Composite solid-state electrolytes represent a critical pathway that balances the interface compatibility and lithium-ion conductivity in all-solid-state batteries.The quest for stable and highly ion-conductive combin...Composite solid-state electrolytes represent a critical pathway that balances the interface compatibility and lithium-ion conductivity in all-solid-state batteries.The quest for stable and highly ion-conductive combinations between polymers and fillers is vital,but blind attempts are often made due to a lack of understanding of the mechanisms involved in the interaction between polymers and fillers.Herein,we employ in-situ polymerization to prepare a polymer based on an ether-nitrile copolymer with high cathode stability as the foundation and discuss the performance enhancement mechanisms of argyrodite and nano-alumina.With 1%content of sulfide interacting with the polymer at the two-phase interface,the local enhancement of lithium-ion migration capability can be achieved,avoiding the reduction in capacity due to the low ion conductivity of the passivation layer during cycling.The capacity retention after 50cycles at 0.5 C increases from 83.5%to 94.4%.Nano-alumina,through anchoring the anions and interface inhibition functions,eventually poses an initial discharge capacity of 136.8 m A h g^(-1)at 0.5 C and extends the cycling time to 1000 h without short-circuiting in lithium metal batteries.Through the combined action of dual fillers on the composite solid-state electrolyte,promising insights are provided for future material design.展开更多
While TiFe alloy has recently attracted attention as the efficient catalyst to enhance de/hydrogenation rates of Mg/MgH_(2),the difficulty of its activation characteristics has hindered further improvement of reaction...While TiFe alloy has recently attracted attention as the efficient catalyst to enhance de/hydrogenation rates of Mg/MgH_(2),the difficulty of its activation characteristics has hindered further improvement of reaction kinetics.Herein,we report that the TiFe_(0.92)Mn_(0.04)Co_(0.04) catalyst can overcome the abovementioned challenges.The synthesized MgH_(2)-30 wt% TiFe_(0.92)Mn_(0.04)Co_(0.04) can release 4.5 wt%of hydrogen in 16 min at 250℃,three times as fast as MgH_(2).The activation energy of dehydrogenation was as low as 84.6 kJ mol^(-1),which is 46.8%reduced from pure MgH_(2).No clear degradation of reaction rates and hydrogen storage capacity was observed for at least 30 cycles.Structural studies reveal that TiFe_(0.92)Mn_(0.04)Co_(0.04) partially decomposes to in-situ generatedα-Fe particles dispersed on TiFe_(0.92)Mn_(0.04)Co_(0.04).The presence ofα-Fe reduces the formation of an oxide layer on TiFe_(0.92)Mn_(0.04)Co_(0.04),enabling the activation processes.At the same time,the hydrogen incorporation capabilities of TiFe_(0.92)Mn_(0.04)Co_(0.04) can provide more hydrogen diffusion paths,which promote hydrogen dissociation and diffusion.These discoveries demonstrate the advanced nature and importance of combining the in-situ generatedα-Fe with TiFe_(0.92)Mn_(0.04)Co_(0.04).It provides a new strategy for designing highly efficient and stable catalysts for Mg-based hydrogen storage materials.展开更多
The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-...The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-TiO_(2) modified by sulfate radicals,was selected as the catalyst support,which showed superior potassium resistance.The physicochemical properties and K-poisoning resistance of the V_(2)O_(5)-WO_(3)/SO_(4)^(2-)-TiO_(2)(VWSTi) catalyst were carried out by XRD,BET,H2-TPR,NH3-TPD,XPS,in situ DRIFTS and TG.The results pointed out that the introduction of SO_(4)^(2-)significantly increased the NH3-SCR catalytic activity at high temperatures,with an exceptionally high NO_(x) conversion over 90% between 275℃ and 500℃.When 0.5%(mass) K_(2)O was doped on the catalysts,the catalytic performance of the traditional V_(2)O_(5)-WO_(3)/TiO_(2)(VWTi) catalyst decreased significantly,while the VWSTi catalyst could still maintain a NOxconversion over 90%in the range of 300–500℃.The characterizations suggested that the support of SO_(4)^(2-)-TiO_(2) greatly increased the number of acidic sites,thereby enhancing the adsorption capacity of the reactant NH_(3).The results above demonstrated a potential approach to achieve superior potassium resistance for NH3-SCR catalysts using solid superacid.展开更多
Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable development.The typical SLIBs recycling concentrated on separating valuable comp...Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable development.The typical SLIBs recycling concentrated on separating valuable components had limitations,including high energy consumption and complicated separation processes.This work suggests a safe hydrometallurgical process to recover usable metallic cobalt from depleted LiCoO_(2)batteries by utilizing citric acid as leachant and hydrogen peroxide as an oxidizing agent,with ethanol as a selective precipitating agent.The anode graphite was also recovered and converted to graphene oxide(GO).The above components were directly resynthesized to cobaltintegrated nitrogen-doped graphene(Co@NG).The Co@NG showed a decent activity towards oxygen reduction reaction(ORR)with a half-wave potential of 0.880 V vs.RHE,almost similar to Pt/C(0.888 V vs.RHE)and with an onset potential of 0.92 V vs.RHE.The metal-nitrogen-carbon(Co-N-C)having the highest nitrogen content has decreased the barrier for ORR since the reaction was enhanced for Co@NG-800,as confirmed by density functional theory(DFT)simulations.The Co@NG cathode catalyst coupled with commercial Pt-Ru/C as anode catalyst exhibits excellent performance for direct methanol fuel cell(DMFC)with a peak power density of 34.7 mW cm^(-2)at a discharge current density of120 m A cm^(-2)and decent stability,indicating the promising utilization of spent battery materials in DMFC applications.Besides,lithium was recovered from supernatant as lithium carbonate by coprecipitation process.This work avoids sophisticated elemental separation by utilizing SLIBs for other renewable energy applications,lowering the environmental concerns associated with recycling.展开更多
A lead-shielded HPGe detector and offlineγ-ray spectra of the residual product were used to measure the cross section(CS)and ratios of isomeric CS(σm/σg)in^(134)Xe(n,2n)^(133m),gXe reactions at different energies(1...A lead-shielded HPGe detector and offlineγ-ray spectra of the residual product were used to measure the cross section(CS)and ratios of isomeric CS(σm/σg)in^(134)Xe(n,2n)^(133m),gXe reactions at different energies(13.5 MeV,13.8 MeV,14.1 MeV,14.4 MeV,14.8 MeV)relative to the^(93)Nb(n,2n)^(92)mNb reaction CS.The target was high-purity natural Xe gas under high pressure.The T(d,n)4He reaction produces neutrons.TALYS code(version 1.95)for nuclear reactions was used for calculations,with default parameters and nuclear level density models.The uncertainties in the measured CS data were thoroughly analyzed using the covariance analysis method.The results were compared with theoretical values,evaluation data,and previous experimental findings.CS data of the 134Xe(n,2n)133mXe and 134Xe(n,2n)133gXe reactions and the corresponding isomeric CS ratios at 13.5 MeV,13.8 MeV,and 14.1 MeV neutron energies are reported for the first time.This research advances our knowledge of pre-equilibrium emission in the(n,2n)reaction channel by resolving inconsistencies in the Xe data.展开更多
Magnesium-based energy materials, which combine promising energy-related functional properties with low cost, environmental compatibility and high availability, have been regarded as fascinating candidates for sustain...Magnesium-based energy materials, which combine promising energy-related functional properties with low cost, environmental compatibility and high availability, have been regarded as fascinating candidates for sustainable energy conversion and storage. In this review,we provide a timely summary on the recent progress in three types of important Mg-based energy materials, based on the fundamental strategies of composition and structure engineering. With regard to Mg-based materials for batteries, we systematically review and analyze different material systems, structure regulation strategies as well as the relevant performance in Mg-ion batteries(MIBs) and Mg-air batteries(MABs), covering cathodes, electrolytes, anodes for MIBs, and anodes for MABs;as to Mg-based hydrogen storage materials, we discuss how catalyst adding, composite, alloying and nanostructuring improve the kinetic and thermodynamic properties of de/hydrogenation reactions, and in particular, the impacts of composition and structure modification on hydrogen absorption/dissociation processes and free energy modification mechanism are focused;regarding Mg-based thermoelectric materials, the relations between composition/structure and electrical/thermal transport properties of Mg_(3)X_(2)(X = Sb, Bi), Mg_(2)X(X = Si, Ge, Sn) and Mg Ag Sb-based materials, together with the representative research progress of each material system, are summarized and discussed. Finally, by pointing out remaining challenges and providing possible solutions, this review aims to shed light on the directions and perspectives for practical applications of magnesium-based energy materials in the future.展开更多
Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution ...Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution reactions(OER).Herein,we fabricate a range of bifunctional M-N-C(metal-nitrogen-carbon)catalysts containing M-Nx coordination sites and M/MxC nanoparticles(M=Co,Fe,and Cu)using a new class ofγ-cyclodextrin(CD)based metal-organic framework as the precursor.With the two types of active sites interacting with each other in the catalysts,the obtained Fe@C-FeNC and Co@C-CoNC display superior alkaline ORR activity in terms of low half-wave(E1/2)potential(~0.917 and 0.906 V,respectively),which are higher than Cu@C-CuNC(~0.829 V)and the commercial Pt/C(~0.861 V).As a bifunctional electrocatalyst,the Co@C-CoNC exhibits the best performance,showing a bifunctional ORR/OER overpotential(ΔE)of~0.732 V,which is much lower than that of Fe@C-FeNC(~0.831 V)and Cu@C-CuNC(~1.411 V),as well as most of the robust bifunctional electrocatalysts reported to date.Synchrotron X-ray absorption spectroscopy and density functional theory simulations reveal that the strong electronic correlation between metallic Co nanoparticles and the atomic Co-N4 sites in the Co@C-CoNC catalyst can increase the d-electron density near the Fermi level and thus effectively optimize the adsorption/desorption of intermediates in ORR/OER,resulting in an enhanced bifunctional electrocatalytic performance.The Co@C-CoNC-based rechargeable ZAB exhibited a maximum power density of 162.80 mW cm^(−2) at 270.30 mA cm^(−2),higher than the combination of commercial Pt/C+RuO2(~158.90 mW cm^(−2) at 265.80 mA cm^(−2))catalysts.During the galvanostatic discharge at 10 mA cm^(−2),the ZAB delivered an almost stable discharge voltage of 1.2 V for~140 h,signifying the virtue of excellent bifunctional ORR/OER electrocatalytic activity.展开更多
Silver nanoclusters(AgNCs)are a new type of nanomaterials with similar properties to molecules and unique applications.The applications of AgNCs can be significantly expanded by combining them with different matrix ma...Silver nanoclusters(AgNCs)are a new type of nanomaterials with similar properties to molecules and unique applications.The applications of AgNCs can be significantly expanded by combining them with different matrix materials to obtain AgNC composites.Using irradiation techniques,we developed a simple two-step method for preparing silver nanocluster composites.First,polyacrylic acid(PAA)chains were grafted onto the surface of a PE film as templates(PE-g-PAA).Subsequently,silver ions were reduced in situ on the surface of the template material to obtain the AgNC composites(AgNCs@PE-g-PAA).The degree of AgNC loading on the composite film was easily controlled by adjusting the reaction conditions.The loaded AgNCs were anchored to the carboxyl groups of the PAA and wrapped in the graft chain.The particle size of the AgNCs was only 4.38±0.85 nm,with a very uniform particle size distribution.The AgNCs@PE-g-PAA exhibited fluorescence characteristics derived from the AgNCs.The fluorescence of the AgNCs@PE-g-PAA was easily quenched by Cr^(3+)ions.The composite can be used as a fluorescence test paper to realize visual detection of Cr^(3+).展开更多
High voltage fracturing technology was widely used in the field of reservoir reconstruction due to its advantages of being clean, pollution-free, and high-efficiency. However, high-frequency circuit oscillation occurs...High voltage fracturing technology was widely used in the field of reservoir reconstruction due to its advantages of being clean, pollution-free, and high-efficiency. However, high-frequency circuit oscillation occurs during the underwater high voltage pulse discharge process, which brings security risks to the stability of the pulse fracturing system. In order to solve this problem, an underwater pulse power discharge system was established, the circuit oscillation generation conditions were analyzed and the circuit oscillation suppression method was proposed. Firstly, the system structure was introduced and the charging model of the energy storage capacitor was established by the state space average method. Next, the electrode high-voltage breakdown model was established through COMSOL software, the electrode breakdown process was analyzed according to the electron density distribution image, and the plasma channel impedance was estimated based on the conductivity simulation results. Then the underwater pulse power discharge process and the circuit oscillation generation condition were analyzed, and the circuit oscillation suppression strategy of using the thyristor to replace the gas spark switch was proposed. Finally, laboratory experiments were carried out to verify the precision of the theoretical model and the suppression effect of circuit oscillation. The experimental results show that the voltage variation of the energy storage capacitor, the impedance change of the pulse power discharge process, and the equivalent circuit in each discharge stage were consistent with the theoretical model. The proposed oscillation suppression strategy cannot only prevent the damage caused by circuit oscillation but also reduce the damping oscillation time by77.1%, which can greatly improve the stability of the system. This research has potential application value in the field of underwater pulse power discharge for reservoir reconstruction.展开更多
Rotating packed bed(RPB) is one of the most effective gas–liquid mass transfer enhancement reactors, its effective specific mass transfer area(ae) is critical to understand the mass transfer process. By using the NaO...Rotating packed bed(RPB) is one of the most effective gas–liquid mass transfer enhancement reactors, its effective specific mass transfer area(ae) is critical to understand the mass transfer process. By using the NaOH–CO_(2) chemical absorption method, the aevalues of three RPB reactors with different rotor sizes were measured under different operation conditions. The results showed that the high gravity factor and liquid flow rate were major affecting factors, while the gas flow rate exhibited minor influence.The radius of packing is the dominant equipment factor to affect aevalue. The results indicated that the contact area depends on the dispersion of the liquid phase, thus the centrifugal force of rotating packed bed greatly influenced the aevalue. Moreover, the measured ae/ap(effective specific mass transfer area/specific surface area of packing) values were fitted with dimensionless correlation formulas. The unified correlation formula with dimensionless bed size parameter can well predict the experimental data and the prediction errors were within 15%.展开更多
With the growing threat of airborne epidemics,there has been an increasing emphasis on personal protection.Masks serve as our primary external defense against bacteria and viruses that might enter the respiratory trac...With the growing threat of airborne epidemics,there has been an increasing emphasis on personal protection.Masks serve as our primary external defense against bacteria and viruses that might enter the respiratory tract.Hence,it’s crucial to develop a polypropylene(PP)nonwoven fabric with quick antibacterial capabilities as a key component for masks.This study introduces silver nanoclusters(AgNCs)into non-woven PP using radiation technology to infuse antibacterial properties.Initially,a solid ligand(PP-g-PAA)was procured via radiation grafting of the ligand polyacrylic acid(PAA),which was incorporated into the nonwoven PP with the aid of a crosslinking agent at a lower absorbed dosage.Subsequently,AgNCs were synthesized in situ on PP-g-PAA via an interaction between PAA and AgNCs,leading directly to the formation of AgNCs@PP-g-PAA composites.Owing to the hydrophilicity of PAA,AgNCs@PP-g-PAA maintains good moisture permeability even when the voids are heavily saturated with PAA gel,preventing droplet aggregation by diffusing droplets on the surface of the material.This feature enhances the comfort of the masks.Most importantly,due to the incorporation of AgNCs,AgNCs@PP-g-PAA demonstrates outstanding antibacterial effects against Escherichia coli and Staphylococcus aureus,nearly achieving an instant“touch and kill”outcome.In conclusion,we synthesized a modified nonwoven fabric with significant antibacterial activity using a simple synthetic route,offering a promising material that provides improved personal protection.展开更多
Fluoride ferrous(FeF_(2))is viewed as a promising conversion cathode material for next-generation lithiumion batteries(LIBs)due to its high theoretical specific capacity and low cost.Unfortunately,issues such as poor ...Fluoride ferrous(FeF_(2))is viewed as a promising conversion cathode material for next-generation lithiumion batteries(LIBs)due to its high theoretical specific capacity and low cost.Unfortunately,issues such as poor intrinsic conductivity,iron dissolution,and phase separation hinder the application of FeF_(2)in highenergy cathodes.Here,a pressure-induced morphology control method is designed to prepare coralloidlike FeF_(2)nanocrystals with nitrogen-rich carbon coating(c-FeF_(2)@NC).The coralloid-like interconnected crystal structure of c-FeF_(2)@NC contributes to reducing interfacial resistance and enhancing the topotactic transformation during the conversion reaction,and the nitrogen-rich carbon(NC)coating can enhance interfacial stability and kinetic performance.When used as a conversion cathode for LIBs,c-FeF_(2)@NC exhibits a high initial reversible capacity of 503.57 mA h g^(-1)and excellent cycling stability of497.61 m A h g^(-1)with a low capacity decay of 1.19%over 50 cycles at 0.1 A/g.Even at 1 A/g,a stable capacity of 263.78 mA h g^(-1)can still be retained after 200 cycles.The capability of c-FeF_(2)@NC as a conversion cathode for sodium-ion batteries(SIBs)was also evaluated to expand its field of application.Furthermore,two kinds of full batteries have been assembled by employing c-FeF_(2)@NC as cathodes and quantitative limited-Li(LLi)and pre-lithiated reduced graphene oxide(PGO)as anodes,respectively,to envisage the feasibility of practical applications of conversion materials.展开更多
Lithium(Li)metal electrodes show significantly different reversibility in the electrolytes with different salts.However,the understanding on how the salts impact on the Li loss remains unclear.Herein,using the electro...Lithium(Li)metal electrodes show significantly different reversibility in the electrolytes with different salts.However,the understanding on how the salts impact on the Li loss remains unclear.Herein,using the electrolytes with different salts(e.g.,lithium hexafluorophosphate(LiPF_(6)),lithium difluoro(oxalato)borate(LiDFOB),and lithium bis(fluorosulfonyl)amide(LiFSI))as examples,we decouple the irreversible Li loss(SEI Li^(+)and“dead”Li)during cycling.It is found that the accumulation of both SEI Li^(+)and“dead”Li may be responsible to the irreversible Li loss for the Li metal in the electrolyte with LiPF_(6)salt.While for the electrolytes with LiDFOB and LiFSI salts,the accumulation of“dead”Li predominates the Li loss.We also demonstrate that lithium nitrate and fluoroethylene carbonate additives could,respectively,function as the“dead”Li and SEI Li^(+)inhibitors.Inspired by the above understandings,we propose a universal procedure for the electrolyte design of Li metal batteries(LMBs):(i)decouple and find the main reason for the irreversible Li loss;(ii)add the corresponding electrolyte additive.With such a Li-loss-targeted strategy,the Li reversibility was significantly enhanced in the electrolytes with 1,2-dimethoxyethane,triethyl phosphate,and tetrahydrofuran solvents.Our strategy may broaden the scope of electrolyte design toward practical LMBs.展开更多
With the depletion of shallow resources,the exploration of deep earth resources has become a global strategy.The study of the different patterns in the physical mechanical properties of rocks at different occurrence d...With the depletion of shallow resources,the exploration of deep earth resources has become a global strategy.The study of the different patterns in the physical mechanical properties of rocks at different occurrence depths is the basis for exploring deep into the earth,with the core and premise being the acquisition and testing of deep in-situ core specimens.Based on the original idea of deep in-situ condition preserved coring(ICP-Coring)and testing,combined with theoretical modeling,numerical analysis,test platform development,indoor testing and engineering application,the principles and technologies of deep ICP-Coring are developed.This principle and technology consists of five parts:in-situ pressurepreserved coring(IPP-Coring),in-situ substance-preserved coring(ISP-Coring),in-situ temperaturepreserved coring(ITP-Coring),in-situ light-preserved coring(ILP-Coring),and in-situ moisturepreserved coring(IMP-Coring).The theory and technology of temperature and pressure reconstruction at different occurrence depths and in different environments are proposed,and prototype trial production was completed by following the principle of displacement and tests based on the in-situ reconstructed environment.The notable advances are as follows:(1)Deep in-situ coring system:A pressure-preserved controller with an ultimate bearing capacity greater than 140 MPa,highperformance(temperature-resistant,pressure-resistant,and low thermally conductive)temperaturepreserved materials,an active temperature control system,and high-barrier quality-preserved membrane materials were developed;a deep ICP-Coring capacity calibration platform was independently developed,a deep in-situ coring technology system was developed,and the acquisition of deep in-situ cores was realized.(2)In-situ storage displacement system:Following the dual-circuit hydraulic design idea,a single-drive source push-pull composite grabbing mechanism was designed;the design of the overall structure for the deep in-situ displacement storage system and ultrahigh pressure cabin structure was completed,which could realize docking the coring device and core displacement in the in-situ reconstructed environment.(3)Test analysis system:A noncontact acoustic-electric-magnetic test system was developed under the in-situ reconstructed environment,and the errors between the test results and traditional contact test results were mostly less than 10%;a detachable deep in-situ core true triaxial test system was developed,which could perform loading tests for deep in-situ cores.The relevant technological achievements were successfully applied to the exploration and development of deep resources,such as deep mines,deep-sea natural gas hydrates,and deep oil and gas.The research results provide technical and equipment support for the construction of a theoretical system for deep in-situ rock mechanics,the development of deep earth resources and energy,and the scientific exploration of different layers and occurrence depths(deep and ultradeep)of the Earth.展开更多
Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a ...Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a 2D/2D carbon nitride VDW heterojunction in carbon nitride(g-C_(3)N_(4))with carbon-rich carbon nitride.The created 2D semiconducting channel in the VDW structure exhibits enhanced electric field exposure and radiation absorption,which facilitates the separation of the charge carriers and their mobility.Consequently,compared with bulk g-C_(3)N_(4)and its nanosheets,the photocatalytic performance of the fabricated carbon nitride VDW heterojunction in the water splitting reaction to hydrogen is improved by 8.6 and 3.3 times,respectively,while maintaining satisfactory photo-stability.Mechanistically,the finite element method(FEM)was employed to evaluate and clarify the contributions of the formation of VDW heterojunction to enhanced photocatalysis,in agreement quantitatively with experimental ones.This study provides a new and effective strategy for the modification and more insights to performance improvement on polymeric semiconductors in photocatalysis and energy conversion.展开更多
Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance...Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).展开更多
Rechargeable batteries and supercapacitors are widely investigated as the most important electrochemical energy storage devices nowadays due to the booming energy demand for electric vehicles and hand-held electronics...Rechargeable batteries and supercapacitors are widely investigated as the most important electrochemical energy storage devices nowadays due to the booming energy demand for electric vehicles and hand-held electronics. The large surface-area-to-volume ratio and internal surface areas endow two-dimensional(2D) materials with high mobility and high energy density; therefore, 2D materials are very promising candidates for Li ion batteries and supercapacitors with comprehensive investigations. In 2011, a new kind of 2D transition metal carbides, nitrides and carbonitrides, MXene, were successfully obtained from MAX phases. Since then about 20 different kinds of MXene have been prepared. Other precursors besides MAX phases and even other methods such as chemical vapor deposition(CVD) were also applied to prepare MXene, opening new doors for the preparation of new MXene. Their 2D nature and good electronic properties ensure the inherent advantages as electrode materials for electrochemical energy storage. In this review, we summarize the recent progress in the development of MXene with emphasis on the applications to electrochemical energy storage. Also, future perspective and challenges of MXene-based materials are briefly discussed regrading electrochemical energy storage.展开更多
Taking wall-flow diesel particulate filter(DPF) as the research objective and separately assuming its filtering wall to be composed of numerous spherical or cylindrical elements, two different mathematical models of s...Taking wall-flow diesel particulate filter(DPF) as the research objective and separately assuming its filtering wall to be composed of numerous spherical or cylindrical elements, two different mathematical models of steady filtration for wall-flow diesel particulate filter were developed and verified by experiments as well as numerically solved. Furthermore, the effects of the macroand micro-structural parameters of filtering wall and exhaust-flow characteristic parameters on trapping efficiency were also analyzed and researched. The results show that: 1) The two developed mathematical models are consistent with the prediction of variation of particulate size; the influence of various factors on the steady trapping efficiency is exactly the same. Compared to model 2, model 1 is more suitable for describing the steady filtration process of wall-flow diesel particulate filter; 2)The major influencing factors on steady trapping efficiency of wall-flow diesel particulate filter are the macro-and micro-structural parameters of filtering wall; and the secondary influencing factors are the exhaust-flow characteristic parameters and macro-structural parameters of filter; 3)The steady trapping efficiency will be improved by increasing filter body volume, pore density as well as wall thickness and by decreasing exhaust-flow, but effects will be weakened when particulate size exceeds a certain critical value; 4) The steady trapping efficiency will be significantly improved by increasing exhaust-flow temperature and filtering wall thickness, but effects will be also weakened when particulate size exceeds a certain critical value; 5) The steady trapping efficiency will approximately linearly increase with reducing porosity, micropore aperture and pore width.展开更多
Post-combustion CO_2 capture(PCC) process faces significant challenge of high regeneration energy consumption.Biphasic absorbent is a promising alternative candidate which could significantly reduce the regeneration e...Post-combustion CO_2 capture(PCC) process faces significant challenge of high regeneration energy consumption.Biphasic absorbent is a promising alternative candidate which could significantly reduce the regeneration energy consumption because only the CO_2-concentrated phase should be regenerated. In this work, aqueous solutions of triethylenetetramine(TETA) and N,N-diethylethanolamine(DEEA) are found to be efficient biphasic absorbents of CO_2. The effects of the solvent composition, total amine concentration, and temperature on the absorption behavior, as well as the effect of temperature on the desorption behavior of TETA–DEEA–H2 O system were investigated. An aqueous solution of 1 mol·L-1 TETA and 4 mol·L-1 DEEA spontaneously separates into two liquid phases after a certain amount of CO_2 is absorbed and it shows high CO_2 absorption/desorption performance.About 99.4% of the absorbed CO_2 is found in the lower phase, which corresponds to a CO_2 absorption capacity of 3.44 mol·kg-1. The appropriate absorption and desorption temperatures are found to be 30 °C and 90 °C,respectively. The thermal analysis indicates that the heat of absorption of the 1 mol·L-1 TETA and 4 mol·L-1 DEEA solution is-84.38 kJ·(mol CO_2)-1 which is 6.92 kJ·(mol CO_2)-1 less than that of aqueous MEA. The reaction heat, sensible heat, and the vaporization heat of the TETA–DEEA–H2 O system are lower than that of the aqueous MEA, while its CO_2 capacity is higher. Thus the TETA–DEEA–H2 O system is potentially a better absorbent for the post-combustion CO_2 capture process.展开更多
Aiming at obtaining an accurate porosity of gas shale,various approaches are attempted.Therein,nuclear magnetic resonance(NMR),being treated as a kind of new-developed technique,possesses the representative significan...Aiming at obtaining an accurate porosity of gas shale,various approaches are attempted.Therein,nuclear magnetic resonance(NMR),being treated as a kind of new-developed technique,possesses the representative significance.However,as a booming technique,the reliability of NMR-based porosity of shale is not exactly defined.Depending on NMR device,this work measured the porosity of shale experiencing different water soaking time,accordingly,judging the reliability of NMR-based porosity.Results indicate the NMR outcomes vary with the water soaking time,making a doubt about the objectivity of NMRbased porosity in reflecting the real shale porosity.Furthermore,some supplementary means were adopted to verify the water soaking-induced variation in the pore system of shale sample,which intensities the suspicion if the NMR-based porosity is reliable or not.To sum up,this work considers that the NMR-based porosity of shale is not reliable enough when water is used as the probe.Besides,this work also offers some suggestions on how to enhance the reliability of NMR-based porosity of shale sample.Basically,this work selects a fresh perspective to analyze the NMR approach in determining shale porosity,which is hopefully helpful in promoting the development of NMR technique in the shale-related field.展开更多
基金supported by the Science and Technology Commission of Shanghai Municipality(No.19DZ2270100),China。
文摘Composite solid-state electrolytes represent a critical pathway that balances the interface compatibility and lithium-ion conductivity in all-solid-state batteries.The quest for stable and highly ion-conductive combinations between polymers and fillers is vital,but blind attempts are often made due to a lack of understanding of the mechanisms involved in the interaction between polymers and fillers.Herein,we employ in-situ polymerization to prepare a polymer based on an ether-nitrile copolymer with high cathode stability as the foundation and discuss the performance enhancement mechanisms of argyrodite and nano-alumina.With 1%content of sulfide interacting with the polymer at the two-phase interface,the local enhancement of lithium-ion migration capability can be achieved,avoiding the reduction in capacity due to the low ion conductivity of the passivation layer during cycling.The capacity retention after 50cycles at 0.5 C increases from 83.5%to 94.4%.Nano-alumina,through anchoring the anions and interface inhibition functions,eventually poses an initial discharge capacity of 136.8 m A h g^(-1)at 0.5 C and extends the cycling time to 1000 h without short-circuiting in lithium metal batteries.Through the combined action of dual fillers on the composite solid-state electrolyte,promising insights are provided for future material design.
基金supported by The National Key Research and Development Program of China(2023YFB3809100)the National Natural Science Foundation of China(U23A200722)the Fundamental Research Funds for the Central Universities(2023CDJXY-016).
文摘While TiFe alloy has recently attracted attention as the efficient catalyst to enhance de/hydrogenation rates of Mg/MgH_(2),the difficulty of its activation characteristics has hindered further improvement of reaction kinetics.Herein,we report that the TiFe_(0.92)Mn_(0.04)Co_(0.04) catalyst can overcome the abovementioned challenges.The synthesized MgH_(2)-30 wt% TiFe_(0.92)Mn_(0.04)Co_(0.04) can release 4.5 wt%of hydrogen in 16 min at 250℃,three times as fast as MgH_(2).The activation energy of dehydrogenation was as low as 84.6 kJ mol^(-1),which is 46.8%reduced from pure MgH_(2).No clear degradation of reaction rates and hydrogen storage capacity was observed for at least 30 cycles.Structural studies reveal that TiFe_(0.92)Mn_(0.04)Co_(0.04) partially decomposes to in-situ generatedα-Fe particles dispersed on TiFe_(0.92)Mn_(0.04)Co_(0.04).The presence ofα-Fe reduces the formation of an oxide layer on TiFe_(0.92)Mn_(0.04)Co_(0.04),enabling the activation processes.At the same time,the hydrogen incorporation capabilities of TiFe_(0.92)Mn_(0.04)Co_(0.04) can provide more hydrogen diffusion paths,which promote hydrogen dissociation and diffusion.These discoveries demonstrate the advanced nature and importance of combining the in-situ generatedα-Fe with TiFe_(0.92)Mn_(0.04)Co_(0.04).It provides a new strategy for designing highly efficient and stable catalysts for Mg-based hydrogen storage materials.
基金supported by the National Natural Science Foundation of China (22108184)China Postdoctoral Science Foundation (2021TQ0221)+1 种基金the Sichuan Science and Technology Program (2021JDRC0117)Chengdu Science and Technology Program (2021-YF05-00378-SN)。
文摘The significant decrease of acid sites caused by alkali metal poisoning is the major factor in the deactivation of commercial V_(2)O_(5)-WO_(3)/TiO_(2)NH_(3)-SCR catalysts.In this work,the solid superacid SO_(4)^(2-)-TiO_(2) modified by sulfate radicals,was selected as the catalyst support,which showed superior potassium resistance.The physicochemical properties and K-poisoning resistance of the V_(2)O_(5)-WO_(3)/SO_(4)^(2-)-TiO_(2)(VWSTi) catalyst were carried out by XRD,BET,H2-TPR,NH3-TPD,XPS,in situ DRIFTS and TG.The results pointed out that the introduction of SO_(4)^(2-)significantly increased the NH3-SCR catalytic activity at high temperatures,with an exceptionally high NO_(x) conversion over 90% between 275℃ and 500℃.When 0.5%(mass) K_(2)O was doped on the catalysts,the catalytic performance of the traditional V_(2)O_(5)-WO_(3)/TiO_(2)(VWTi) catalyst decreased significantly,while the VWSTi catalyst could still maintain a NOxconversion over 90%in the range of 300–500℃.The characterizations suggested that the support of SO_(4)^(2-)-TiO_(2) greatly increased the number of acidic sites,thereby enhancing the adsorption capacity of the reactant NH_(3).The results above demonstrated a potential approach to achieve superior potassium resistance for NH3-SCR catalysts using solid superacid.
基金supported by the Basic Science Research Program through the National Research Foundation of Korea(NRF)the South Korea grant funded by the Korean government(MSIT)(2021R1A4A2000934,2023R1A2C3004336)+1 种基金The computational part of the work was supported by Department of Chemical and Biomolecular Engineering,Institute of Emergent Materials,Sogang University,via NRF Korea grant 2015M3D3A1A01064929a generous supercomputing time from KISTI。
文摘Recycling spent lithium-ion batteries(SLIBs)has become essential to preserve the environment and reclaim vital resources for sustainable development.The typical SLIBs recycling concentrated on separating valuable components had limitations,including high energy consumption and complicated separation processes.This work suggests a safe hydrometallurgical process to recover usable metallic cobalt from depleted LiCoO_(2)batteries by utilizing citric acid as leachant and hydrogen peroxide as an oxidizing agent,with ethanol as a selective precipitating agent.The anode graphite was also recovered and converted to graphene oxide(GO).The above components were directly resynthesized to cobaltintegrated nitrogen-doped graphene(Co@NG).The Co@NG showed a decent activity towards oxygen reduction reaction(ORR)with a half-wave potential of 0.880 V vs.RHE,almost similar to Pt/C(0.888 V vs.RHE)and with an onset potential of 0.92 V vs.RHE.The metal-nitrogen-carbon(Co-N-C)having the highest nitrogen content has decreased the barrier for ORR since the reaction was enhanced for Co@NG-800,as confirmed by density functional theory(DFT)simulations.The Co@NG cathode catalyst coupled with commercial Pt-Ru/C as anode catalyst exhibits excellent performance for direct methanol fuel cell(DMFC)with a peak power density of 34.7 mW cm^(-2)at a discharge current density of120 m A cm^(-2)and decent stability,indicating the promising utilization of spent battery materials in DMFC applications.Besides,lithium was recovered from supernatant as lithium carbonate by coprecipitation process.This work avoids sophisticated elemental separation by utilizing SLIBs for other renewable energy applications,lowering the environmental concerns associated with recycling.
基金supported by the National Natural science Foundation of China(Nos.11875016,12165006).
文摘A lead-shielded HPGe detector and offlineγ-ray spectra of the residual product were used to measure the cross section(CS)and ratios of isomeric CS(σm/σg)in^(134)Xe(n,2n)^(133m),gXe reactions at different energies(13.5 MeV,13.8 MeV,14.1 MeV,14.4 MeV,14.8 MeV)relative to the^(93)Nb(n,2n)^(92)mNb reaction CS.The target was high-purity natural Xe gas under high pressure.The T(d,n)4He reaction produces neutrons.TALYS code(version 1.95)for nuclear reactions was used for calculations,with default parameters and nuclear level density models.The uncertainties in the measured CS data were thoroughly analyzed using the covariance analysis method.The results were compared with theoretical values,evaluation data,and previous experimental findings.CS data of the 134Xe(n,2n)133mXe and 134Xe(n,2n)133gXe reactions and the corresponding isomeric CS ratios at 13.5 MeV,13.8 MeV,and 14.1 MeV neutron energies are reported for the first time.This research advances our knowledge of pre-equilibrium emission in the(n,2n)reaction channel by resolving inconsistencies in the Xe data.
基金financial support from the National Key Research and Development Program of China (No.2021YFB3502200)the National Natural Science Foundation of China (Grants Nos.52271202,51971040,52171101)+2 种基金the Shanghai Rising-Star Program (No.21QA1403200)supported by a start-up fund from Chongqing University (02110011044171)Liuchuang Program of Chongqing Municipality (cx2022038)。
文摘Magnesium-based energy materials, which combine promising energy-related functional properties with low cost, environmental compatibility and high availability, have been regarded as fascinating candidates for sustainable energy conversion and storage. In this review,we provide a timely summary on the recent progress in three types of important Mg-based energy materials, based on the fundamental strategies of composition and structure engineering. With regard to Mg-based materials for batteries, we systematically review and analyze different material systems, structure regulation strategies as well as the relevant performance in Mg-ion batteries(MIBs) and Mg-air batteries(MABs), covering cathodes, electrolytes, anodes for MIBs, and anodes for MABs;as to Mg-based hydrogen storage materials, we discuss how catalyst adding, composite, alloying and nanostructuring improve the kinetic and thermodynamic properties of de/hydrogenation reactions, and in particular, the impacts of composition and structure modification on hydrogen absorption/dissociation processes and free energy modification mechanism are focused;regarding Mg-based thermoelectric materials, the relations between composition/structure and electrical/thermal transport properties of Mg_(3)X_(2)(X = Sb, Bi), Mg_(2)X(X = Si, Ge, Sn) and Mg Ag Sb-based materials, together with the representative research progress of each material system, are summarized and discussed. Finally, by pointing out remaining challenges and providing possible solutions, this review aims to shed light on the directions and perspectives for practical applications of magnesium-based energy materials in the future.
基金supported by the Shenzhen Government’s Plan of Science and Technology(JCYJ20190808121407676 and 20200813142301001)National Natural Science Foundation of China(22178223 and 22262010)+1 种基金Guangxi Science and Technology Fund for Distinguished High-Talent Introduction Program(No.RZ2200002233AC22035091).
文摘Rechargeable zinc-air batteries(ZABs)are a promising energy conversion device,which rely critically on electrocatalysts to accelerate their rate-determining reactions such as oxygen reduction(ORR)and oxygen evolution reactions(OER).Herein,we fabricate a range of bifunctional M-N-C(metal-nitrogen-carbon)catalysts containing M-Nx coordination sites and M/MxC nanoparticles(M=Co,Fe,and Cu)using a new class ofγ-cyclodextrin(CD)based metal-organic framework as the precursor.With the two types of active sites interacting with each other in the catalysts,the obtained Fe@C-FeNC and Co@C-CoNC display superior alkaline ORR activity in terms of low half-wave(E1/2)potential(~0.917 and 0.906 V,respectively),which are higher than Cu@C-CuNC(~0.829 V)and the commercial Pt/C(~0.861 V).As a bifunctional electrocatalyst,the Co@C-CoNC exhibits the best performance,showing a bifunctional ORR/OER overpotential(ΔE)of~0.732 V,which is much lower than that of Fe@C-FeNC(~0.831 V)and Cu@C-CuNC(~1.411 V),as well as most of the robust bifunctional electrocatalysts reported to date.Synchrotron X-ray absorption spectroscopy and density functional theory simulations reveal that the strong electronic correlation between metallic Co nanoparticles and the atomic Co-N4 sites in the Co@C-CoNC catalyst can increase the d-electron density near the Fermi level and thus effectively optimize the adsorption/desorption of intermediates in ORR/OER,resulting in an enhanced bifunctional electrocatalytic performance.The Co@C-CoNC-based rechargeable ZAB exhibited a maximum power density of 162.80 mW cm^(−2) at 270.30 mA cm^(−2),higher than the combination of commercial Pt/C+RuO2(~158.90 mW cm^(−2) at 265.80 mA cm^(−2))catalysts.During the galvanostatic discharge at 10 mA cm^(−2),the ZAB delivered an almost stable discharge voltage of 1.2 V for~140 h,signifying the virtue of excellent bifunctional ORR/OER electrocatalytic activity.
基金supported by the Gansu Natural Science Foundation (Nos.20JR10RA778 and 20JR10RA777)。
文摘Silver nanoclusters(AgNCs)are a new type of nanomaterials with similar properties to molecules and unique applications.The applications of AgNCs can be significantly expanded by combining them with different matrix materials to obtain AgNC composites.Using irradiation techniques,we developed a simple two-step method for preparing silver nanocluster composites.First,polyacrylic acid(PAA)chains were grafted onto the surface of a PE film as templates(PE-g-PAA).Subsequently,silver ions were reduced in situ on the surface of the template material to obtain the AgNC composites(AgNCs@PE-g-PAA).The degree of AgNC loading on the composite film was easily controlled by adjusting the reaction conditions.The loaded AgNCs were anchored to the carboxyl groups of the PAA and wrapped in the graft chain.The particle size of the AgNCs was only 4.38±0.85 nm,with a very uniform particle size distribution.The AgNCs@PE-g-PAA exhibited fluorescence characteristics derived from the AgNCs.The fluorescence of the AgNCs@PE-g-PAA was easily quenched by Cr^(3+)ions.The composite can be used as a fluorescence test paper to realize visual detection of Cr^(3+).
基金financially supported by the National Science and Technology Major Project(No.2016ZX05034004)。
文摘High voltage fracturing technology was widely used in the field of reservoir reconstruction due to its advantages of being clean, pollution-free, and high-efficiency. However, high-frequency circuit oscillation occurs during the underwater high voltage pulse discharge process, which brings security risks to the stability of the pulse fracturing system. In order to solve this problem, an underwater pulse power discharge system was established, the circuit oscillation generation conditions were analyzed and the circuit oscillation suppression method was proposed. Firstly, the system structure was introduced and the charging model of the energy storage capacitor was established by the state space average method. Next, the electrode high-voltage breakdown model was established through COMSOL software, the electrode breakdown process was analyzed according to the electron density distribution image, and the plasma channel impedance was estimated based on the conductivity simulation results. Then the underwater pulse power discharge process and the circuit oscillation generation condition were analyzed, and the circuit oscillation suppression strategy of using the thyristor to replace the gas spark switch was proposed. Finally, laboratory experiments were carried out to verify the precision of the theoretical model and the suppression effect of circuit oscillation. The experimental results show that the voltage variation of the energy storage capacitor, the impedance change of the pulse power discharge process, and the equivalent circuit in each discharge stage were consistent with the theoretical model. The proposed oscillation suppression strategy cannot only prevent the damage caused by circuit oscillation but also reduce the damping oscillation time by77.1%, which can greatly improve the stability of the system. This research has potential application value in the field of underwater pulse power discharge for reservoir reconstruction.
基金the support from the National Natural Science Foundation of China (22008157,21978178)。
文摘Rotating packed bed(RPB) is one of the most effective gas–liquid mass transfer enhancement reactors, its effective specific mass transfer area(ae) is critical to understand the mass transfer process. By using the NaOH–CO_(2) chemical absorption method, the aevalues of three RPB reactors with different rotor sizes were measured under different operation conditions. The results showed that the high gravity factor and liquid flow rate were major affecting factors, while the gas flow rate exhibited minor influence.The radius of packing is the dominant equipment factor to affect aevalue. The results indicated that the contact area depends on the dispersion of the liquid phase, thus the centrifugal force of rotating packed bed greatly influenced the aevalue. Moreover, the measured ae/ap(effective specific mass transfer area/specific surface area of packing) values were fitted with dimensionless correlation formulas. The unified correlation formula with dimensionless bed size parameter can well predict the experimental data and the prediction errors were within 15%.
文摘With the growing threat of airborne epidemics,there has been an increasing emphasis on personal protection.Masks serve as our primary external defense against bacteria and viruses that might enter the respiratory tract.Hence,it’s crucial to develop a polypropylene(PP)nonwoven fabric with quick antibacterial capabilities as a key component for masks.This study introduces silver nanoclusters(AgNCs)into non-woven PP using radiation technology to infuse antibacterial properties.Initially,a solid ligand(PP-g-PAA)was procured via radiation grafting of the ligand polyacrylic acid(PAA),which was incorporated into the nonwoven PP with the aid of a crosslinking agent at a lower absorbed dosage.Subsequently,AgNCs were synthesized in situ on PP-g-PAA via an interaction between PAA and AgNCs,leading directly to the formation of AgNCs@PP-g-PAA composites.Owing to the hydrophilicity of PAA,AgNCs@PP-g-PAA maintains good moisture permeability even when the voids are heavily saturated with PAA gel,preventing droplet aggregation by diffusing droplets on the surface of the material.This feature enhances the comfort of the masks.Most importantly,due to the incorporation of AgNCs,AgNCs@PP-g-PAA demonstrates outstanding antibacterial effects against Escherichia coli and Staphylococcus aureus,nearly achieving an instant“touch and kill”outcome.In conclusion,we synthesized a modified nonwoven fabric with significant antibacterial activity using a simple synthetic route,offering a promising material that provides improved personal protection.
基金supported by Foundation for the Sichuan University and Zigong City Joint research project(2021CDZG-2)the Foundation for the Sichuan University and Yibin City Strategic Cooperation Project(2020CDYB-32)the Guangxi Key Laboratory of Low Carbon Energy Material(2020GKLLCEM02)。
文摘Fluoride ferrous(FeF_(2))is viewed as a promising conversion cathode material for next-generation lithiumion batteries(LIBs)due to its high theoretical specific capacity and low cost.Unfortunately,issues such as poor intrinsic conductivity,iron dissolution,and phase separation hinder the application of FeF_(2)in highenergy cathodes.Here,a pressure-induced morphology control method is designed to prepare coralloidlike FeF_(2)nanocrystals with nitrogen-rich carbon coating(c-FeF_(2)@NC).The coralloid-like interconnected crystal structure of c-FeF_(2)@NC contributes to reducing interfacial resistance and enhancing the topotactic transformation during the conversion reaction,and the nitrogen-rich carbon(NC)coating can enhance interfacial stability and kinetic performance.When used as a conversion cathode for LIBs,c-FeF_(2)@NC exhibits a high initial reversible capacity of 503.57 mA h g^(-1)and excellent cycling stability of497.61 m A h g^(-1)with a low capacity decay of 1.19%over 50 cycles at 0.1 A/g.Even at 1 A/g,a stable capacity of 263.78 mA h g^(-1)can still be retained after 200 cycles.The capability of c-FeF_(2)@NC as a conversion cathode for sodium-ion batteries(SIBs)was also evaluated to expand its field of application.Furthermore,two kinds of full batteries have been assembled by employing c-FeF_(2)@NC as cathodes and quantitative limited-Li(LLi)and pre-lithiated reduced graphene oxide(PGO)as anodes,respectively,to envisage the feasibility of practical applications of conversion materials.
基金This work was supported by the National Key Research and Development Program(2021YFB2400300)the National Natural Science Foundation of China(52272203)the Fundamental Research Funds for the Central Universities(2021GCRC001).
文摘Lithium(Li)metal electrodes show significantly different reversibility in the electrolytes with different salts.However,the understanding on how the salts impact on the Li loss remains unclear.Herein,using the electrolytes with different salts(e.g.,lithium hexafluorophosphate(LiPF_(6)),lithium difluoro(oxalato)borate(LiDFOB),and lithium bis(fluorosulfonyl)amide(LiFSI))as examples,we decouple the irreversible Li loss(SEI Li^(+)and“dead”Li)during cycling.It is found that the accumulation of both SEI Li^(+)and“dead”Li may be responsible to the irreversible Li loss for the Li metal in the electrolyte with LiPF_(6)salt.While for the electrolytes with LiDFOB and LiFSI salts,the accumulation of“dead”Li predominates the Li loss.We also demonstrate that lithium nitrate and fluoroethylene carbonate additives could,respectively,function as the“dead”Li and SEI Li^(+)inhibitors.Inspired by the above understandings,we propose a universal procedure for the electrolyte design of Li metal batteries(LMBs):(i)decouple and find the main reason for the irreversible Li loss;(ii)add the corresponding electrolyte additive.With such a Li-loss-targeted strategy,the Li reversibility was significantly enhanced in the electrolytes with 1,2-dimethoxyethane,triethyl phosphate,and tetrahydrofuran solvents.Our strategy may broaden the scope of electrolyte design toward practical LMBs.
基金the National Natural Science Foundation of China(No.51827901)the Program for Guangdong Introducing Innovative and Enterpreneurial Teams(No.2019ZT08G315)Shenzhen Key Research Projects(No.JSGG20220831105002005).
文摘With the depletion of shallow resources,the exploration of deep earth resources has become a global strategy.The study of the different patterns in the physical mechanical properties of rocks at different occurrence depths is the basis for exploring deep into the earth,with the core and premise being the acquisition and testing of deep in-situ core specimens.Based on the original idea of deep in-situ condition preserved coring(ICP-Coring)and testing,combined with theoretical modeling,numerical analysis,test platform development,indoor testing and engineering application,the principles and technologies of deep ICP-Coring are developed.This principle and technology consists of five parts:in-situ pressurepreserved coring(IPP-Coring),in-situ substance-preserved coring(ISP-Coring),in-situ temperaturepreserved coring(ITP-Coring),in-situ light-preserved coring(ILP-Coring),and in-situ moisturepreserved coring(IMP-Coring).The theory and technology of temperature and pressure reconstruction at different occurrence depths and in different environments are proposed,and prototype trial production was completed by following the principle of displacement and tests based on the in-situ reconstructed environment.The notable advances are as follows:(1)Deep in-situ coring system:A pressure-preserved controller with an ultimate bearing capacity greater than 140 MPa,highperformance(temperature-resistant,pressure-resistant,and low thermally conductive)temperaturepreserved materials,an active temperature control system,and high-barrier quality-preserved membrane materials were developed;a deep ICP-Coring capacity calibration platform was independently developed,a deep in-situ coring technology system was developed,and the acquisition of deep in-situ cores was realized.(2)In-situ storage displacement system:Following the dual-circuit hydraulic design idea,a single-drive source push-pull composite grabbing mechanism was designed;the design of the overall structure for the deep in-situ displacement storage system and ultrahigh pressure cabin structure was completed,which could realize docking the coring device and core displacement in the in-situ reconstructed environment.(3)Test analysis system:A noncontact acoustic-electric-magnetic test system was developed under the in-situ reconstructed environment,and the errors between the test results and traditional contact test results were mostly less than 10%;a detachable deep in-situ core true triaxial test system was developed,which could perform loading tests for deep in-situ cores.The relevant technological achievements were successfully applied to the exploration and development of deep resources,such as deep mines,deep-sea natural gas hydrates,and deep oil and gas.The research results provide technical and equipment support for the construction of a theoretical system for deep in-situ rock mechanics,the development of deep earth resources and energy,and the scientific exploration of different layers and occurrence depths(deep and ultradeep)of the Earth.
基金the National Natural Science Foundation of China(51676096)supported by the Australian Research Council(DP170104264 and DP190103548).
文摘Van der Waals(VDW)heterojunctions in a 2D/2D contact provide the highest area for the separation and transfer of charge carriers.In this work,a top-down strategy with a gas erosion process was employed to fabricate a 2D/2D carbon nitride VDW heterojunction in carbon nitride(g-C_(3)N_(4))with carbon-rich carbon nitride.The created 2D semiconducting channel in the VDW structure exhibits enhanced electric field exposure and radiation absorption,which facilitates the separation of the charge carriers and their mobility.Consequently,compared with bulk g-C_(3)N_(4)and its nanosheets,the photocatalytic performance of the fabricated carbon nitride VDW heterojunction in the water splitting reaction to hydrogen is improved by 8.6 and 3.3 times,respectively,while maintaining satisfactory photo-stability.Mechanistically,the finite element method(FEM)was employed to evaluate and clarify the contributions of the formation of VDW heterojunction to enhanced photocatalysis,in agreement quantitatively with experimental ones.This study provides a new and effective strategy for the modification and more insights to performance improvement on polymeric semiconductors in photocatalysis and energy conversion.
基金the National Science Fund for Distinguished Young Scholars(Grant No.52125103)the National Natural Science Foundation of China(Grant Nos.52301232,52071041,12074048,and 12147102)China Postdoctoral Science Foundation(Grant No.2022M720552).
文摘Electrocatalytic reduction of CO_(2) converts intermittent renewable electricity into value-added liquid products with an enticing prospect,but its practical application is hampered due to the lack of high-performance electrocatalysts.Herein,we elaborately design and develop strongly coupled nanosheets composed of Ag nanoparticles and Sn-SnO_(2) grains,designated as Ag/Sn-SnO_(2) nanosheets(NSs),which possess optimized electronic structure,high electrical conductivity,and more accessible sites.As a result,such a catalyst exhibits unprecedented catalytic performance toward CO_(2)-to-formate conversion with near-unity faradaic efficiency(≥90%),ultrahigh partial current density(2,000 mA cm^(−2)),and superior long-term stability(200 mA cm^(−2),200 h),surpassing the reported catalysts of CO_(2) electroreduction to formate.Additionally,in situ attenuated total reflection-infrared spectra combined with theoretical calculations revealed that electron-enriched Sn sites on Ag/Sn-SnO_(2)NSs not only promote the formation of*OCHO and alleviate the energy barriers of*OCHO to*HCOOH,but also impede the desorption of H*.Notably,the Ag/Sn-SnO_(2)NSs as the cathode in a membrane electrode assembly with porous solid electrolyte layer reactor can continuously produce~0.12 M pure HCOOH solution at 100 mA cm^(−2)over 200 h.This work may inspire further development of advanced electrocatalysts and innovative device systems for promoting practical application of producing liquid fuels from CO_(2).
基金supported by Tianjin Municipal Science and Technology Commission(16PTSYJC00010)in China
文摘Rechargeable batteries and supercapacitors are widely investigated as the most important electrochemical energy storage devices nowadays due to the booming energy demand for electric vehicles and hand-held electronics. The large surface-area-to-volume ratio and internal surface areas endow two-dimensional(2D) materials with high mobility and high energy density; therefore, 2D materials are very promising candidates for Li ion batteries and supercapacitors with comprehensive investigations. In 2011, a new kind of 2D transition metal carbides, nitrides and carbonitrides, MXene, were successfully obtained from MAX phases. Since then about 20 different kinds of MXene have been prepared. Other precursors besides MAX phases and even other methods such as chemical vapor deposition(CVD) were also applied to prepare MXene, opening new doors for the preparation of new MXene. Their 2D nature and good electronic properties ensure the inherent advantages as electrode materials for electrochemical energy storage. In this review, we summarize the recent progress in the development of MXene with emphasis on the applications to electrochemical energy storage. Also, future perspective and challenges of MXene-based materials are briefly discussed regrading electrochemical energy storage.
基金Projects(5117604551276056)supported by the National Natural Science Foundation of China+1 种基金Projects(201208430262201306130031)supported by the National Studying Abroad Foundation of the China Scholarship Council
文摘Taking wall-flow diesel particulate filter(DPF) as the research objective and separately assuming its filtering wall to be composed of numerous spherical or cylindrical elements, two different mathematical models of steady filtration for wall-flow diesel particulate filter were developed and verified by experiments as well as numerically solved. Furthermore, the effects of the macroand micro-structural parameters of filtering wall and exhaust-flow characteristic parameters on trapping efficiency were also analyzed and researched. The results show that: 1) The two developed mathematical models are consistent with the prediction of variation of particulate size; the influence of various factors on the steady trapping efficiency is exactly the same. Compared to model 2, model 1 is more suitable for describing the steady filtration process of wall-flow diesel particulate filter; 2)The major influencing factors on steady trapping efficiency of wall-flow diesel particulate filter are the macro-and micro-structural parameters of filtering wall; and the secondary influencing factors are the exhaust-flow characteristic parameters and macro-structural parameters of filter; 3)The steady trapping efficiency will be improved by increasing filter body volume, pore density as well as wall thickness and by decreasing exhaust-flow, but effects will be weakened when particulate size exceeds a certain critical value; 4) The steady trapping efficiency will be significantly improved by increasing exhaust-flow temperature and filtering wall thickness, but effects will be also weakened when particulate size exceeds a certain critical value; 5) The steady trapping efficiency will approximately linearly increase with reducing porosity, micropore aperture and pore width.
基金Supported by the National Natural Science Foundation of China(21606154)
文摘Post-combustion CO_2 capture(PCC) process faces significant challenge of high regeneration energy consumption.Biphasic absorbent is a promising alternative candidate which could significantly reduce the regeneration energy consumption because only the CO_2-concentrated phase should be regenerated. In this work, aqueous solutions of triethylenetetramine(TETA) and N,N-diethylethanolamine(DEEA) are found to be efficient biphasic absorbents of CO_2. The effects of the solvent composition, total amine concentration, and temperature on the absorption behavior, as well as the effect of temperature on the desorption behavior of TETA–DEEA–H2 O system were investigated. An aqueous solution of 1 mol·L-1 TETA and 4 mol·L-1 DEEA spontaneously separates into two liquid phases after a certain amount of CO_2 is absorbed and it shows high CO_2 absorption/desorption performance.About 99.4% of the absorbed CO_2 is found in the lower phase, which corresponds to a CO_2 absorption capacity of 3.44 mol·kg-1. The appropriate absorption and desorption temperatures are found to be 30 °C and 90 °C,respectively. The thermal analysis indicates that the heat of absorption of the 1 mol·L-1 TETA and 4 mol·L-1 DEEA solution is-84.38 kJ·(mol CO_2)-1 which is 6.92 kJ·(mol CO_2)-1 less than that of aqueous MEA. The reaction heat, sensible heat, and the vaporization heat of the TETA–DEEA–H2 O system are lower than that of the aqueous MEA, while its CO_2 capacity is higher. Thus the TETA–DEEA–H2 O system is potentially a better absorbent for the post-combustion CO_2 capture process.
基金financially supported by the Science and Technology Department of Sichuan Province(Grant Nos.2021YFH0048 and 2021YFH0118)the Project funded by China Postdoctoral Science Foundation(Grant No.2020M683253)
文摘Aiming at obtaining an accurate porosity of gas shale,various approaches are attempted.Therein,nuclear magnetic resonance(NMR),being treated as a kind of new-developed technique,possesses the representative significance.However,as a booming technique,the reliability of NMR-based porosity of shale is not exactly defined.Depending on NMR device,this work measured the porosity of shale experiencing different water soaking time,accordingly,judging the reliability of NMR-based porosity.Results indicate the NMR outcomes vary with the water soaking time,making a doubt about the objectivity of NMRbased porosity in reflecting the real shale porosity.Furthermore,some supplementary means were adopted to verify the water soaking-induced variation in the pore system of shale sample,which intensities the suspicion if the NMR-based porosity is reliable or not.To sum up,this work considers that the NMR-based porosity of shale is not reliable enough when water is used as the probe.Besides,this work also offers some suggestions on how to enhance the reliability of NMR-based porosity of shale sample.Basically,this work selects a fresh perspective to analyze the NMR approach in determining shale porosity,which is hopefully helpful in promoting the development of NMR technique in the shale-related field.
