Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silic...Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.展开更多
As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates hav...As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.展开更多
By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variationa...By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variational Zn-salen ligands RZn and NADH(reduced nicotinamide adenine dinucleotide)mimic modified tridentate ligands with square-planar Pd ions.UV-Vis and luminescence spectra experiments reveal that different anions could selec-tively interact with different sites of Zn-salen modified metal-organic cages to achieve the structural regulation of cage compound,by using the differentiated host-guest electrostatic interactions of counter ions with metal-organic hosts.Compared to other anions,the presence of chloride ions caused the most significant fluorescence emission enhancement of Pd‑R(Zn),meanwhile,the UV-Vis absorption band attributed to the salen aromatic backbone showed an absorption decrease,and the metal-to-ligand induced peak displayed a blue shift effect.Circular dichro-ism and ^(1)H NMR spectra further demonstrate that the introduction of chloride anions is beneficial to keeping a more rigid scaffold.展开更多
Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction int...Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the catalyst.Here,a family of n%-Co_(3)O_(4)/SiC(n=5,8,12,20)catalysts with a delicate percentage of Co^(2+)and Co^(3+)were prepared for NO_(3)RR.We found that Co^(3+)primarily acts as the active site for NO_(3)^(−)reduction to NO_(2)^(−),while Co^(2+)is responsible for the conversion of NO_(2)^(−)to NH_(3).Moreover,the conversion of these intermediates over the active sites is autonomous and separately controllable.Both processes synergistically accomplish the reduction of nitrate ions to synthesize ammonia.Combining the experimental studies and density functional theory(DFT)calculations,it is discovered the pathway(^(*)NHO→^(*)NHOH→^(*)NH_(2)OH→^(*)NH_(2)→^(*)NH_(3))is more favorable due to the lowerΔG value(0.25 eV)for the rate-limiting step(^(*)NO→^(*)NHO).The NH_(3)yield rate of 8%-Co_(3)O_(4)/SiC reached 1.08 mmol/(cm^(2)h)with a Faradaic efficiency of 96.4%at−0.89 V versus the reversible hydrogen electrode(RHE),surpassing those of most reported non-noble NO_(3)RR catalysts.This strategy not only provides an efficient catalyst for NO_(3)RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites,thereby presenting a new approach to enhance the efficiency of intricate reactions.展开更多
Lithium-sulfur batteries(LSBs)are widely regarded as promising next-generation batteries due to their high theoretical specific capacity and low material cost.However,the practical applications of LSBs are limited by ...Lithium-sulfur batteries(LSBs)are widely regarded as promising next-generation batteries due to their high theoretical specific capacity and low material cost.However,the practical applications of LSBs are limited by the shuttle effect of lithium polysulfides(LiPSs),electronic insulation of charge and discharge products,and slow LiPSs conversion reaction kinetics.Accordingly,the introduction of catalysts into LSBs is one of the effective strategy to solve the issues of the sluggished LiPS conversion.Because of their nearly 100%atom utilization and high electrocatalytic activity,single-atom catalysts(SACs)have been widely used as reaction mediators for LSBs’reactions.Excitingly,the SACs with asymmetric coordination structures have exhibited intriguing electronic structures and superior catalytic activities when compared to the traditional M-N_(4)active sites.In this review,we systematically describe the recent advancements in the installation of asymmetrically coordinated single-atom structure as reactions catalysts in LSBs,including asymmetrically nitrogen coordinated SACs,heteroatom coordinated SACs,support effective asymmetrically coordinated SACs,and bimetallic coordinated SACs.Particularly noteworthy is the discussion of the catalytic conversion mechanism of LiPSs spanning asymmetrically coordinated SACs.Finally,a perspective on the future developments of asymmetrically coordinated SACs in LSB applications is provided.展开更多
Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipat...Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts(bda=2,2'-bipyrdine-6,6'-dicarbonoxyl acid)and aliphatic chain decorated electrode surfaces,forming lipid bilayer membrane(LBM)-like structures.The Ru(bda)catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms.However,compared to the slow charge transfer process,the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes,and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs.Instead,charge transfer plays a decisive role in the PEC water oxidation rate.When an indolo[3,2-b]carbazole derivative was introduced between the Ru(bda)catalysts and aliphatic chain-modified photosensitizer in LBM films,serving as a charge transfer mediator for the tyrosine-histidine pair in PSⅡ,the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.展开更多
Pesticide adjuvants,as crop protection products,have been widely used to reduce drift loss and improve utilization efficiency by regulating droplet spectrum.However,the coordinated regulation mechanisms of adjuvants a...Pesticide adjuvants,as crop protection products,have been widely used to reduce drift loss and improve utilization efficiency by regulating droplet spectrum.However,the coordinated regulation mechanisms of adjuvants and nozzles on droplet spectrum remain unclear.Here,we established the relationship between droplet spectrum evolution and liquid atomization by investigating the typical characteristics of droplet diameter distribution near the nozzle.Based on this,the regulation mechanisms of distinctive pesticide adjuvants on droplet spectrum were clarified,and the corresponding drift reduction performances were quantitively evaluated by wind tunnel experiments.It shows that the droplet diameter firstly shifts to the smaller due to the liquid sheet breakup and then prefers to increase caused by droplet interactions.Reducing the surface tension of sprayed liquid facilitates the uniform liquid breakup and increasing the viscosity inhibits the liquid deformation,which prolong the atomization process and effectively improve the droplet spectrum.As a result,the drift losses of flat-fan and hollow cone nozzles are reduced by about 50%after adding organosilicon and vegetable oil adjuvants.By contrast,the air induction nozzle shows a superior anti-drift ability,regardless of distinctive adjuvants.Our findings provide insights into rational adjuvant design and nozzle selection in the field application.展开更多
As a critical role in battery systems,polymer binders have been shown to efficiently suppress the lithium polysulfide shuttling and accommodate volume changes in recent years.However,preparation processes and safety,a...As a critical role in battery systems,polymer binders have been shown to efficiently suppress the lithium polysulfide shuttling and accommodate volume changes in recent years.However,preparation processes and safety,as the key criterions for Li-S batteries'practical applications,still attract less attention.Herein,an aqueous multifunction binder(named PEI-TIC)is prepared via an easy and fast epoxy-amine ring-opening reaction(10 min),which can not only give the sulfur cathode a stable mechanical property,a strong chemical adsorption and catalytic conversion ability,but also a fire safety improvement.The Li-S batteries based on the PEI-TIC binder display a high discharge capacity(1297.8 mAh g^(-1)),superior rate performance(823.0 mAh g^(-1)at 2 C),and an ultralow capacity decay rate of 0.035%over more than 800 cycles.Even under 7.1 mg cm^(-2)S-loaded,the PEI-TIC electrode can also achieve a high areal capacity of 7.2 mA h g^(-1)and excellent cycling stability,confirming its application potential.Moreover,it is also noted that TG-FTIR test is performed for the first time to explore the flame-retardant mechanism of polymer binders.This work provides an economically and environmentally friendly binder for the practical application and inspires the exploration of the flame-retardant mechanism of all electrode components.展开更多
Preferential orientation control of metal—organic framework(MOF)films is advantageous for maximizing pore uniformity and minimizing grain-boundary defects.Nonetheless,the preparation of MOF films with both in-plane a...Preferential orientation control of metal—organic framework(MOF)films is advantageous for maximizing pore uniformity and minimizing grain-boundary defects.Nonetheless,the preparation of MOF films with both in-plane and out-of-plane orientations remains a grand challenge.In this study,we reported the preparation of three-dimensionally oriented MIL-96 layers through combining morphology control of MIL-96 seeds with addition of polyvinylpyrrolidone surfactants and arachidonic acids.The three-dimensionally oriented MIL-96 film was readily obtained through in-plane epitaxial growth.It is anticipated that the aforementioned protocol can be effective for obtaining diverse MOF films with a three-dimensionally oriented organization.展开更多
Artificial skin involves multidisciplinary efforts,including materials science,biology,medicine,and tissue engineering.Recent studies have aimed at creating skins that are multifunctional,intelligent,and capable of re...Artificial skin involves multidisciplinary efforts,including materials science,biology,medicine,and tissue engineering.Recent studies have aimed at creating skins that are multifunctional,intelligent,and capable of regenerating tissue.In this work,we present a specialized 3D printing ink composed of polyurethane and bioactive glass(PU-BG)and prepare dual-function skin patch by microfluidic-regulated 3D bioprinting(MRBP)technique.The MRBP endows the skin patch with a highly controlled microstructure and superior strength.Besides,an asymmetric tri-layer is further constructed,which promotes cell attachment and growth through a dual transport mechanism based on hydrogen bonds and gradient structure from hydrophilic to superhydrophilic.More importantly,by combining the features of biomedical skin with electronic skin(e-skin),we achieved a biomedical and electronic dual-function skin patch.In vivo experiments have shown that this skin patch can enhance hemostasis,resist bacterial growth,stimulate the regeneration of blood vessels,and accelerate the healing process.Meanwhile,it also mimics the sensory functions of natural skin to realize signal detection,where the sensitivity reached up to 5.87 kPa1,as well as cyclic stability(over 500 cycles),a wide detection range of 0–150 kPa,high pressure resolution of 0.1%under the pressure of 100 kPa.This work offers a versatile and effective method for creating dual-function skin patches and provide new insights into wound healing and tissue repair,which have significant implications for clinical applications.展开更多
This study presents the synthesis of three dinuclear cobalt complexes based on three imine derivatives:bis-[4-(2-pyridylmethyleneamino)-phenyl]thioether(L1),bis-[4-(2-pyridylmethyleneamino)-phenyl]ether(L2),and bis-[4...This study presents the synthesis of three dinuclear cobalt complexes based on three imine derivatives:bis-[4-(2-pyridylmethyleneamino)-phenyl]thioether(L1),bis-[4-(2-pyridylmethyleneamino)-phenyl]ether(L2),and bis-[4-(2-pyridylmethyleneamino)-phenyl]methane(L3).Single-crystal X-ray diffraction analysis reveals that the complexes[Co_(2)(L1)3](ClO_(4))4·2CH_(3)CN(1),[Co_(2)(L2)3](ClO_(4))4·2CH_(3)OH(2),and[Co_(2)(L3)3](ClO_(4))4·2CH_(3)OH(3)all exhibit a dinuclear structure.Magnetic test results show that complex 3 exhibited irreversible SCO behavior induced by loss of solvent at 300 K,with the average Co-N bond length increasing from 0.2139(3)to 0.2153(3)nm.Meanwhile,the desolvated complex 3 exhibited paramagnetic behavior similar to that of complexes 1 and 2.Variable-temperature UV-Vis spectroscopic studies also indicate that complex 3 undergoes a solvent-loss-induced spin-state transition.CCDC:2347354,1(120 K);2347355,2(120 K);2347356,3(120 K);2347357,3(400 K).展开更多
Acetic acid and furfural are known as prevalent inhibitors deriving from pretreatment during lignocellulosic ethanol production.They negatively impact cell growth,glucose uptake and ethanol biosynthesis of Saccharomyc...Acetic acid and furfural are known as prevalent inhibitors deriving from pretreatment during lignocellulosic ethanol production.They negatively impact cell growth,glucose uptake and ethanol biosynthesis of Saccharomyces cerevisiae strains.Development of industrial S.cerevisiae strains with high tolerance towards these inhibitors is thus critical for efficient lignocellulosic ethanol production.In this study,the acetic acid or furfural tolerance of different S.cerevisiae strains could be significantly enhanced after adaptive evolution via serial cultivation for 40 generations under stress conditions.The acetic acid-based adaptive strain SPSC01-TA9 produced 30.5 g·L^(-1)ethanol with a yield of 0.46 g·g^(-1)in the presence of 9 g·L^(-1)acetic acid,while the acetic acid/furfural-based adaptive strain SPSC01-TAF94 produced more ethanol of 36.2 g·L^(-1)with increased yield up to 0.49 g·g^(-1)in the presence of both 9 g·L^(-1)acetic acid and 4 g·L^(-1)furfural.Significant improvements were also observed during non-detoxified corn stover hydrolysate culture by SPSC01-TAF94,which achieved ethanol production and yield of 29.1 g·L^(-1)and 0.49 g·g^(-1),respectively,the growth and fermentation efficiency of acetic acid/furfural-based adaptive strain in hydrolysate was 95%higher than those of wildtype strains,indicating the acetic acid-and furfural-based adaptive evolution strategy could be an effective approach for improving lignocellulosic ethanol production.The adapted strains developed in this study with enhanced tolerance against acetic acid and furfural could be potentially contribute to economically feasible and sustainable lignocellulosic biorefinery.展开更多
K4Ce2Nb10O30 ultrafine powders were prepared by stearic acid method (SAM). The obtained products were analyzed by X-ray diffraction, transmission electron microscopy, energy dispersive X-ray spectrometry, scanning ele...K4Ce2Nb10O30 ultrafine powders were prepared by stearic acid method (SAM). The obtained products were analyzed by X-ray diffraction, transmission electron microscopy, energy dispersive X-ray spectrometry, scanning electron microscopy and UV-visible absorption spectra. XRD patterns revealed that K4Ce2Nb10O30 powders treated at 900 oC for 2 h presented tetragonal structure without the presence of deleterious phases. Furthermore, the K4Ce2Nb10O30 prepared by SAM had considerable activity under visible light irradiation.展开更多
Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a...Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a set of characterizations,and its catalytic activity was investigated for hydrodesulfurization(HDS)of 4,6-dimethyldibenzothiophene.It has confirmed that the incorporation of La profoundly facilitate the generation of“Type II”NiMoS phase by weakening the interaction of Mo–O–Al leakage and promoting the sulfidation of both Ni and Mo oxides as well as changing the morphology of Ni promoted MoS2 slabs,thereafter boosting the HDS performance substantially.The finding here may contribute to the fundamental understanding of structure-activity in ultra-deep desulfurization and inspire the advancement of highly-efficient HDS catalyst in future.展开更多
Measuring the dust explosion characteristics of aluminum-based activated fuels was a prerequisite for developing effective prevention and control measures.In this paper,ignition sensitivity,flame propagation behaviors...Measuring the dust explosion characteristics of aluminum-based activated fuels was a prerequisite for developing effective prevention and control measures.In this paper,ignition sensitivity,flame propagation behaviors and explosion severity of aluminum/polytetrafluoroethylene(Al/PTFE)compositions including 2 PT(2.80 wt.%F),4 PT(7.18 wt.%F)and 8 PT(11.90 wt.%F)were studied.When the content of F increased from 2.80 wt.%to 11.90 wt.%,the minimum explosive concentration MEC decreased from380 g/m^(3)to 140 g/m^(3),due to the dual effects of increased internal active aluminum and enhanced reactivity.The average flame propagation velocities increased as the percentage of F increased.The maximum explosion pressure Pmof 500 g/m3aluminum-based activated fuels increased from 247 k Pa to299 kPa.Scanning electron microscopy demonstrated that with the increase of PTFE content,the reaction was more complete.On this basis,the explosion mechanism of aluminum-based activated fuels was revealed.展开更多
Development and utilization of hydrogen energy is an effective way to achieve carbon neutrality,only hydrogen production through electrolytic water splitting meets the goal of zero carbon emission.To facilitate the la...Development and utilization of hydrogen energy is an effective way to achieve carbon neutrality,only hydrogen production through electrolytic water splitting meets the goal of zero carbon emission.To facilitate the large-scale commercialization of water splitting devices,the development of highly efficient and low-cost catalysts to reduce the energy consumption is essential.MoS_(2)has been regarded as a promising electrocatalyst to replace platinum in hydrogen evolution reaction due to its low price and unique 2D layered structure.However,the poor conductivity and inert basal planes of MoS_(2)limited its wide-spread application.Recently,researches have demonstrated that the conductivity and active sites of MoS_(2)can be improved by heteroatoms doping or constructing of heterogeneous structures.In this review,the recent progress of Mo-based catalysts are summarized centered on MoS_(2)based on interface engineering and anion engineering,including MoS_(2)–MoO_(2),MoS_(2)–Mo_(2)C,MoS_(2)–MoN_(x),MoS_(2)–MoP,and MoS_(2)–MoSe_(2).The preparation method,structure,and performance of the catalysts are introduced and the possible mechanism behind the improved catalytic activity are revealed to give readers an overall comprehension on the progress of the Mo-based electrocatalysts for hydrogen evolution reaction.In addition,an outlook on future opportunities and development directions of Mo-based catalysts are proposed to facilitate the development of Mo-based catalysts for hydrogen production.展开更多
Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of ...Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of gravity.W-MEL membranes were grown on stainless steel (SS) meshes through in-situ hydrothermal growth method facilitated with (3-aminopropyl)triethoxysilane (APTES) modification of stainless steel meshes,which promote the heterogeneous nucleation and crystal growth of W-MEL zeolites onto the mesh surface.W-MEL membranes were grown on different mesh size supports to investigate the effect of mesh size on the separation performance of the membrane.The assynthesized W-MEL membrane supported on 500 mesh (25μm)(W-MEL-500) exhibit the hydrophilic nature with a water contact angle of 11.8°and delivers the best hexane/water mixture separation with a water flux and separation efficiency of 46247 L·m^(-2)·h^(-1)and 99.5%,respectively.The wettability of W-MEL membranes was manipulated from hydrophilic to hydrophobic nature by chemically modifying with the fluorine-free compounds (hexadecyltrimethoxysilane (HDTMS) and dodecyltrimethoxysilane(DDTMS)) to achieve efficient oil-permselective separation of heavy oils from water.Among the hydrophobically modified W-MEL membranes,W-MEL-500-HDTMS having a water contact angle of146.4°delivers the best separation performance for dichloromethane/water mixtures with a constant oil flux and separation efficiency of 61490 L·m^(-2)·h^(-1)and 99.2%,respectively along with the stability tested up to 20 cycles.Both W-MEL-500-HDTMS and W-MEL-500-DDTMS membranes also exhibit similar separation performances for the separation of heavy oil from sea water along with a 20-fold lower corrosion rate in comparison with the bare stainless-steel mesh,indicating their excellent stability in seawater.Compared to the reported zeolite membranes for oil/water separation,the as-synthesized and hydrophobically modified W-MEL membranes shows competitive separation performances in terms of flux and separation efficiency,demonstrating the good potentiality for oil/water separation.展开更多
NH_(3) selective catalytic reduction(SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperat...NH_(3) selective catalytic reduction(SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperatures are essential to denitration. In this work, a series of bimetallic CeCu-SAPO-34 molecular sieves were synthesized by one-step hydrothermal method. The Ce Cu-SAPO-34 maintained good crystallinity and a regular hexahedron appearance of Cu-SAPO-34 after introducing Ce species, while exhibiting a higher specific surface area and pore volume. The as-prepared CeCu-SAPO-34 with 0.02%(mass) Ce constituent exhibited the best catalytic activity below 300℃ and a maximum NO_(x) conversion of 99% was attained;the NO_(x) removal rates of more than 68% and 94% were achieved at 150℃ and 200℃, respectively. And the introduction of cerium species in Cu-SAPO-34 improves the low-temperature hydrothermal stability of the catalyst towards NH_(3)-SCR reaction. Additionally, the introduced Ce species could enhance the formation of abundant weak Br?nsted acid centers and promote the synergistic effect between CuO grains and isolated Cu^(2+) to enhance the redox cycle, which benefit the NH_(3)-SCR reaction.This work provides a facile synthesis method of high-efficiency SCR denitration catalysts towards diesel vehicles exhaust treatment under low temperature.展开更多
Transformation of lignin to valuable chemicals via sustainable pathways is recognized as one of the most efficient ways to explore its value and replace the nonrenewable petroleum resource. In this work, an environmen...Transformation of lignin to valuable chemicals via sustainable pathways is recognized as one of the most efficient ways to explore its value and replace the nonrenewable petroleum resource. In this work, an environmental-friendly transfer hydrogenation process has been developed to convert lignin derived2,6-dimethoxybenzoquinone to 1,4-cyclohexanediol. Compared with previous work under hydrogen pressure(30 bar), this process uses isopropanol as both solvent and hydrogen donor, which significantly simply the operation process. The core of this study is the design and preparation of Mn modified Raney Ni catalysts by ball milling process. A series of Raney Ni Mn catalysts with different ball milling time and Mn content were prepared and investigated. Characterizations by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), scanning electron microscope(SEM) and transmission electron microscope(TEM) etc. showed that Ni Mn Al alloy was formed during the ball milling process and then transformed to Ni Mn alloy after treatment by aqueous Na OH. After optimization, a yield as high as 86.1% could be achieved for 1,4-cyclohexanediol at 200℃ in only 1 h.展开更多
With the rapid development of flexible and portable microelectronics,the extreme demand for miniaturized,mechanically flexible,and integrated microsystems are strongly stimulated.Here,biomass-derived carbons(BDCs)are ...With the rapid development of flexible and portable microelectronics,the extreme demand for miniaturized,mechanically flexible,and integrated microsystems are strongly stimulated.Here,biomass-derived carbons(BDCs)are prepared by KOH activation using Qamgur precursor,exhibiting three-dimensional(3D)hierarchical porous structure.Benefiting from unobstructed 3D hierarchical porous structure,BDCs provide an excellent specific capacitance of 433 F g^(-1)and prominent cyclability without capacitance degradation after 50000 cycles at 50 A g^(-1).Furthermore,BDC-based planar micro-supercapacitors(MSCs)without metal collector,prepared by mask-assisted coating,exhibit outstanding areal-specific capacitance of 84 mF cm^(-2)and areal energy density of 10.6μWh cm^(-2),exceeding most of the previous carbon-based MSCs.Impressively,the MSCs disclose extraordinary flexibility with capacitance retention of almost 100%under extreme bending state.More importantly,a flexible planar integrated system composed of the MSC and temperature sensor is assembled to efficiently monitor the temperature variation,providing a feasible route for flexible MSC-based functional micro-devices.展开更多
基金supported by the Fundamental Research Funds for the Central Universities(DUT21LK34)Natural Science Foundation of Liaoning Province(2020-MS-113).
文摘Rational design of oxygen evolution reaction(OER)catalysts at low cost would greatly benefit the economy.Taking advantage of earth-abundant elements Si,Co and Ni,we produce a unique-structure where cobalt-nickel silicate hydroxide[Co_(2.5)Ni_(0.5)Si_(2)O_(5)(OH)_(4)]is vertically grown on a reduced graphene oxide(rGO)support(CNS@rGO).This is developed as a low-cost and prospective OER catalyst.Compared to cobalt or nickel silicate hydroxide@rGO(CS@rGO and NS@rGO,respectively)nanoarrays,the bimetal CNS@rGO nanoarray exhibits impressive OER performance with an overpotential of 307 mV@10 mA cm^(-2).This value is higher than that of CS@rGO and NS@rGO.The CNS@rGO nanoarray has an overpotential of 446 mV@100 mA cm^(-2),about 1.4 times that of the commercial RuO_(2)electrocatalyst.The achieved OER activity is superior to the state-of-the-art metal oxides/hydroxides and their derivatives.The vertically grown nanostructure and optimized metal-support electronic interactions play an indispensable role for OER performance improvement,including a fast electron transfer pathway,short proton/electron diffusion distance,more active metal centers,as well as optimized dualatomic electron density.Taking advantage of interlay chemical regulation and the in-situ growth method,the advanced-structural CNS@rGO nanoarrays provide a new horizon to the rational and flexible design of efficient and promising OER electrocatalysts.
基金financial support from the National Key Research and Development Program of China(2020YFA0710202)the National Natural Science Foundation of China(21978043,U1662130)+1 种基金Inner Mongolia University of Technology Scientific Research Initial Funding(DC2300001240)Talent Introduction Support Project of Inner Mongolia(DC2300001426).
文摘As a common precursor for supercritical CO_(2)(scCO_(2))deposition techniques,solubility data of organometallic complexes in scCO_(2)is crucial for the preparation of nanocomposites.Recently,metal acetylacetonates have shown great potential for the preparation of single-atom catalytic materials.In this study,the solubilities of iron(Ⅲ)acetylacetonate(Fe(acac)3)and nickel(Ⅱ)acetylacetonate(Ni(acac)2)were measured at the temperature from 313.15 to 333.15 K and in the pressure range of 9.5–25.2 MPa to accumulate new solubility data.Solubility was measured using a static weight loss method.The semi-empirical models proposed by Chrastil and Sung et al.were used to correlate the solubility data of Fe(acac)3 and Ni(acac)2.The equations obtained can be used to predict the solubility of the same system in the experimental range.
文摘By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variational Zn-salen ligands RZn and NADH(reduced nicotinamide adenine dinucleotide)mimic modified tridentate ligands with square-planar Pd ions.UV-Vis and luminescence spectra experiments reveal that different anions could selec-tively interact with different sites of Zn-salen modified metal-organic cages to achieve the structural regulation of cage compound,by using the differentiated host-guest electrostatic interactions of counter ions with metal-organic hosts.Compared to other anions,the presence of chloride ions caused the most significant fluorescence emission enhancement of Pd‑R(Zn),meanwhile,the UV-Vis absorption band attributed to the salen aromatic backbone showed an absorption decrease,and the metal-to-ligand induced peak displayed a blue shift effect.Circular dichro-ism and ^(1)H NMR spectra further demonstrate that the introduction of chloride anions is beneficial to keeping a more rigid scaffold.
基金financially supported by the National Key Research and Development Program of China (2018YFA0209404)the Fundamental Research Funds for the Central Universities (DUT22LAB601)
文摘Regulating the intermediates involved in the electrocatalytic nitrate reduction reaction(NO_(3)RR)is crucial for the enhancement of reaction efficiency.However,it remains a great challenge to regulate the reaction intermediates through active site manipulation on the surface of the catalyst.Here,a family of n%-Co_(3)O_(4)/SiC(n=5,8,12,20)catalysts with a delicate percentage of Co^(2+)and Co^(3+)were prepared for NO_(3)RR.We found that Co^(3+)primarily acts as the active site for NO_(3)^(−)reduction to NO_(2)^(−),while Co^(2+)is responsible for the conversion of NO_(2)^(−)to NH_(3).Moreover,the conversion of these intermediates over the active sites is autonomous and separately controllable.Both processes synergistically accomplish the reduction of nitrate ions to synthesize ammonia.Combining the experimental studies and density functional theory(DFT)calculations,it is discovered the pathway(^(*)NHO→^(*)NHOH→^(*)NH_(2)OH→^(*)NH_(2)→^(*)NH_(3))is more favorable due to the lowerΔG value(0.25 eV)for the rate-limiting step(^(*)NO→^(*)NHO).The NH_(3)yield rate of 8%-Co_(3)O_(4)/SiC reached 1.08 mmol/(cm^(2)h)with a Faradaic efficiency of 96.4%at−0.89 V versus the reversible hydrogen electrode(RHE),surpassing those of most reported non-noble NO_(3)RR catalysts.This strategy not only provides an efficient catalyst for NO_(3)RR but also serves as an illustrative model for the regulation of multi-step reaction intermediates through the design of distinct active sites,thereby presenting a new approach to enhance the efficiency of intricate reactions.
基金supported by the National Natural Science Foundation of China(Grant Nos.22108133,51972180)Science,Education and Industry Integration of Basic Research Projects of Qilu University of Technology(Grant No.2022PY062,2023PY034,2023PY022)
文摘Lithium-sulfur batteries(LSBs)are widely regarded as promising next-generation batteries due to their high theoretical specific capacity and low material cost.However,the practical applications of LSBs are limited by the shuttle effect of lithium polysulfides(LiPSs),electronic insulation of charge and discharge products,and slow LiPSs conversion reaction kinetics.Accordingly,the introduction of catalysts into LSBs is one of the effective strategy to solve the issues of the sluggished LiPS conversion.Because of their nearly 100%atom utilization and high electrocatalytic activity,single-atom catalysts(SACs)have been widely used as reaction mediators for LSBs’reactions.Excitingly,the SACs with asymmetric coordination structures have exhibited intriguing electronic structures and superior catalytic activities when compared to the traditional M-N_(4)active sites.In this review,we systematically describe the recent advancements in the installation of asymmetrically coordinated single-atom structure as reactions catalysts in LSBs,including asymmetrically nitrogen coordinated SACs,heteroatom coordinated SACs,support effective asymmetrically coordinated SACs,and bimetallic coordinated SACs.Particularly noteworthy is the discussion of the catalytic conversion mechanism of LiPSs spanning asymmetrically coordinated SACs.Finally,a perspective on the future developments of asymmetrically coordinated SACs in LSB applications is provided.
基金conducted by the Fundamental Research Center of Artificial Photosynthesis(FReCAP)financially supported by the National Natural Science Foundation of China(22172011 and 22088102)+1 种基金the National Key R&D Program of China(2022YFA0911904)the Fundamental Research Funds for the Central Universities(DUT22LK06,DUT22QN213 and DUT23LAB611)。
文摘Inspired by the function of crucial components in photosystemⅡ(PSⅡ),electrochemical and dyesensitized photoelectrochemical(DSPEC)water oxidation devices were constructed by the selfassembly of well-designed amphipathic Ru(bda)-based catalysts(bda=2,2'-bipyrdine-6,6'-dicarbonoxyl acid)and aliphatic chain decorated electrode surfaces,forming lipid bilayer membrane(LBM)-like structures.The Ru(bda)catalysts on electrode-supported LBM films demonstrated remarkable water oxidation performance with different O-O formation mechanisms.However,compared to the slow charge transfer process,the O-O formation pathways did not determine the PEC water oxidation efficiency of the dyesensitized photoanodes,and the different reaction rates for similar catalysts with different catalytic paths did not determine the PEC performance of the DSPECs.Instead,charge transfer plays a decisive role in the PEC water oxidation rate.When an indolo[3,2-b]carbazole derivative was introduced between the Ru(bda)catalysts and aliphatic chain-modified photosensitizer in LBM films,serving as a charge transfer mediator for the tyrosine-histidine pair in PSⅡ,the PEC water oxidation performance of the corresponding photoanodes was dramatically enhanced.
基金financially supported by the National Key Research and Development Program of China(2017YFD0200304)。
文摘Pesticide adjuvants,as crop protection products,have been widely used to reduce drift loss and improve utilization efficiency by regulating droplet spectrum.However,the coordinated regulation mechanisms of adjuvants and nozzles on droplet spectrum remain unclear.Here,we established the relationship between droplet spectrum evolution and liquid atomization by investigating the typical characteristics of droplet diameter distribution near the nozzle.Based on this,the regulation mechanisms of distinctive pesticide adjuvants on droplet spectrum were clarified,and the corresponding drift reduction performances were quantitively evaluated by wind tunnel experiments.It shows that the droplet diameter firstly shifts to the smaller due to the liquid sheet breakup and then prefers to increase caused by droplet interactions.Reducing the surface tension of sprayed liquid facilitates the uniform liquid breakup and increasing the viscosity inhibits the liquid deformation,which prolong the atomization process and effectively improve the droplet spectrum.As a result,the drift losses of flat-fan and hollow cone nozzles are reduced by about 50%after adding organosilicon and vegetable oil adjuvants.By contrast,the air induction nozzle shows a superior anti-drift ability,regardless of distinctive adjuvants.Our findings provide insights into rational adjuvant design and nozzle selection in the field application.
基金the support from National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(52222314)CNPC Innovation Fund(2021DQ02-1001)+2 种基金Liao Ning Revitalization Talents Program(XLYC1907144)Xinghai Talent Cultivation Plan(X20200303)Fundamental Research Funds for the Central Universities(DUT22JC02,DUT22LAB605)
文摘As a critical role in battery systems,polymer binders have been shown to efficiently suppress the lithium polysulfide shuttling and accommodate volume changes in recent years.However,preparation processes and safety,as the key criterions for Li-S batteries'practical applications,still attract less attention.Herein,an aqueous multifunction binder(named PEI-TIC)is prepared via an easy and fast epoxy-amine ring-opening reaction(10 min),which can not only give the sulfur cathode a stable mechanical property,a strong chemical adsorption and catalytic conversion ability,but also a fire safety improvement.The Li-S batteries based on the PEI-TIC binder display a high discharge capacity(1297.8 mAh g^(-1)),superior rate performance(823.0 mAh g^(-1)at 2 C),and an ultralow capacity decay rate of 0.035%over more than 800 cycles.Even under 7.1 mg cm^(-2)S-loaded,the PEI-TIC electrode can also achieve a high areal capacity of 7.2 mA h g^(-1)and excellent cycling stability,confirming its application potential.Moreover,it is also noted that TG-FTIR test is performed for the first time to explore the flame-retardant mechanism of polymer binders.This work provides an economically and environmentally friendly binder for the practical application and inspires the exploration of the flame-retardant mechanism of all electrode components.
基金National Natural Science Foundation of China(22078039)Science Fund for Creative Research Groups of the National Natural Science Foundation of China(22021005)+1 种基金National Key Research and Development Program of China(2023YFB3810700)the Fundamental Research Funds for the Central Universities(DUT22LAB602)。
文摘Preferential orientation control of metal—organic framework(MOF)films is advantageous for maximizing pore uniformity and minimizing grain-boundary defects.Nonetheless,the preparation of MOF films with both in-plane and out-of-plane orientations remains a grand challenge.In this study,we reported the preparation of three-dimensionally oriented MIL-96 layers through combining morphology control of MIL-96 seeds with addition of polyvinylpyrrolidone surfactants and arachidonic acids.The three-dimensionally oriented MIL-96 film was readily obtained through in-plane epitaxial growth.It is anticipated that the aforementioned protocol can be effective for obtaining diverse MOF films with a three-dimensionally oriented organization.
基金supported by National Natural Science Foundation of China(22278225,82170581,22308160)Natural Science Foundation of Jiangsu Province(BK20211133,BK20230327)+1 种基金the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_1471)Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD).
文摘Artificial skin involves multidisciplinary efforts,including materials science,biology,medicine,and tissue engineering.Recent studies have aimed at creating skins that are multifunctional,intelligent,and capable of regenerating tissue.In this work,we present a specialized 3D printing ink composed of polyurethane and bioactive glass(PU-BG)and prepare dual-function skin patch by microfluidic-regulated 3D bioprinting(MRBP)technique.The MRBP endows the skin patch with a highly controlled microstructure and superior strength.Besides,an asymmetric tri-layer is further constructed,which promotes cell attachment and growth through a dual transport mechanism based on hydrogen bonds and gradient structure from hydrophilic to superhydrophilic.More importantly,by combining the features of biomedical skin with electronic skin(e-skin),we achieved a biomedical and electronic dual-function skin patch.In vivo experiments have shown that this skin patch can enhance hemostasis,resist bacterial growth,stimulate the regeneration of blood vessels,and accelerate the healing process.Meanwhile,it also mimics the sensory functions of natural skin to realize signal detection,where the sensitivity reached up to 5.87 kPa1,as well as cyclic stability(over 500 cycles),a wide detection range of 0–150 kPa,high pressure resolution of 0.1%under the pressure of 100 kPa.This work offers a versatile and effective method for creating dual-function skin patches and provide new insights into wound healing and tissue repair,which have significant implications for clinical applications.
文摘This study presents the synthesis of three dinuclear cobalt complexes based on three imine derivatives:bis-[4-(2-pyridylmethyleneamino)-phenyl]thioether(L1),bis-[4-(2-pyridylmethyleneamino)-phenyl]ether(L2),and bis-[4-(2-pyridylmethyleneamino)-phenyl]methane(L3).Single-crystal X-ray diffraction analysis reveals that the complexes[Co_(2)(L1)3](ClO_(4))4·2CH_(3)CN(1),[Co_(2)(L2)3](ClO_(4))4·2CH_(3)OH(2),and[Co_(2)(L3)3](ClO_(4))4·2CH_(3)OH(3)all exhibit a dinuclear structure.Magnetic test results show that complex 3 exhibited irreversible SCO behavior induced by loss of solvent at 300 K,with the average Co-N bond length increasing from 0.2139(3)to 0.2153(3)nm.Meanwhile,the desolvated complex 3 exhibited paramagnetic behavior similar to that of complexes 1 and 2.Variable-temperature UV-Vis spectroscopic studies also indicate that complex 3 undergoes a solvent-loss-induced spin-state transition.CCDC:2347354,1(120 K);2347355,2(120 K);2347356,3(120 K);2347357,3(400 K).
基金supported by the National Key Research and Development Program of China(2021YFC2101303)the National Natural Science Foundation of China(U22A20424 and 22378048)+6 种基金the Major Scientific and Technological Projects of Sinopecthe Dalian Technology Talents Project for Distinguished Young Scholars(2021RJ03)the Yunnan Provincial Rural Energy Engineering Key Laboratory(2022KF003)the National Natural Science Foundation of Liaoning Province(2023-MS-110)the Liaoning Revitalization Talents Program(XLYC2202049)the Fundamental Research Funds for the Central Universities(DUT22LK22)the CAS Key Laboratory of Renewable Energy,Guangzhou Institute of Energy Conversion(E229kf0401)。
文摘Acetic acid and furfural are known as prevalent inhibitors deriving from pretreatment during lignocellulosic ethanol production.They negatively impact cell growth,glucose uptake and ethanol biosynthesis of Saccharomyces cerevisiae strains.Development of industrial S.cerevisiae strains with high tolerance towards these inhibitors is thus critical for efficient lignocellulosic ethanol production.In this study,the acetic acid or furfural tolerance of different S.cerevisiae strains could be significantly enhanced after adaptive evolution via serial cultivation for 40 generations under stress conditions.The acetic acid-based adaptive strain SPSC01-TA9 produced 30.5 g·L^(-1)ethanol with a yield of 0.46 g·g^(-1)in the presence of 9 g·L^(-1)acetic acid,while the acetic acid/furfural-based adaptive strain SPSC01-TAF94 produced more ethanol of 36.2 g·L^(-1)with increased yield up to 0.49 g·g^(-1)in the presence of both 9 g·L^(-1)acetic acid and 4 g·L^(-1)furfural.Significant improvements were also observed during non-detoxified corn stover hydrolysate culture by SPSC01-TAF94,which achieved ethanol production and yield of 29.1 g·L^(-1)and 0.49 g·g^(-1),respectively,the growth and fermentation efficiency of acetic acid/furfural-based adaptive strain in hydrolysate was 95%higher than those of wildtype strains,indicating the acetic acid-and furfural-based adaptive evolution strategy could be an effective approach for improving lignocellulosic ethanol production.The adapted strains developed in this study with enhanced tolerance against acetic acid and furfural could be potentially contribute to economically feasible and sustainable lignocellulosic biorefinery.
基金Project supported by the National Natural Science Foundation of China (20872051) "Zijin Star" of NJUST
文摘K4Ce2Nb10O30 ultrafine powders were prepared by stearic acid method (SAM). The obtained products were analyzed by X-ray diffraction, transmission electron microscopy, energy dispersive X-ray spectrometry, scanning electron microscopy and UV-visible absorption spectra. XRD patterns revealed that K4Ce2Nb10O30 powders treated at 900 oC for 2 h presented tetragonal structure without the presence of deleterious phases. Furthermore, the K4Ce2Nb10O30 prepared by SAM had considerable activity under visible light irradiation.
基金financial support of the National Natural Science Foundation of China(22002050,22178154)the Project of Jiangsu University Senior Talents Foundation(20JDG35)+1 种基金Postdoctoral Science Foundation of China(2022T150765,2020M683154)National Engineering Laboratory for Mobile Source Emission Control Technology(NELMS2020B01).
文摘Herein,we designed and constructed a mesoporous LaAlOx via a solvent evaporation induced self-assembly protocol.The structure and physicochemical property of the corresponding NiMo supported catalyst was analyzed by a set of characterizations,and its catalytic activity was investigated for hydrodesulfurization(HDS)of 4,6-dimethyldibenzothiophene.It has confirmed that the incorporation of La profoundly facilitate the generation of“Type II”NiMoS phase by weakening the interaction of Mo–O–Al leakage and promoting the sulfidation of both Ni and Mo oxides as well as changing the morphology of Ni promoted MoS2 slabs,thereafter boosting the HDS performance substantially.The finding here may contribute to the fundamental understanding of structure-activity in ultra-deep desulfurization and inspire the advancement of highly-efficient HDS catalyst in future.
基金financially supported by National Natural Science Foundation of China(No.51922025 and No.51874066)China Postdoctoral Science Foundation(No.2020M670759)the Fundamental Research Funds for the Central Universities(No.DUT20GJ201)。
文摘Measuring the dust explosion characteristics of aluminum-based activated fuels was a prerequisite for developing effective prevention and control measures.In this paper,ignition sensitivity,flame propagation behaviors and explosion severity of aluminum/polytetrafluoroethylene(Al/PTFE)compositions including 2 PT(2.80 wt.%F),4 PT(7.18 wt.%F)and 8 PT(11.90 wt.%F)were studied.When the content of F increased from 2.80 wt.%to 11.90 wt.%,the minimum explosive concentration MEC decreased from380 g/m^(3)to 140 g/m^(3),due to the dual effects of increased internal active aluminum and enhanced reactivity.The average flame propagation velocities increased as the percentage of F increased.The maximum explosion pressure Pmof 500 g/m3aluminum-based activated fuels increased from 247 k Pa to299 kPa.Scanning electron microscopy demonstrated that with the increase of PTFE content,the reaction was more complete.On this basis,the explosion mechanism of aluminum-based activated fuels was revealed.
基金This work has been financially supported by the National Natural Science Foun-dation of China (No.51972293,51772039,and 21902189)Key Scientific Research Projects of Universities in Henan Province (21A150062)Young Backbone Teacher of Zhongyuan University of Technology.
文摘Development and utilization of hydrogen energy is an effective way to achieve carbon neutrality,only hydrogen production through electrolytic water splitting meets the goal of zero carbon emission.To facilitate the large-scale commercialization of water splitting devices,the development of highly efficient and low-cost catalysts to reduce the energy consumption is essential.MoS_(2)has been regarded as a promising electrocatalyst to replace platinum in hydrogen evolution reaction due to its low price and unique 2D layered structure.However,the poor conductivity and inert basal planes of MoS_(2)limited its wide-spread application.Recently,researches have demonstrated that the conductivity and active sites of MoS_(2)can be improved by heteroatoms doping or constructing of heterogeneous structures.In this review,the recent progress of Mo-based catalysts are summarized centered on MoS_(2)based on interface engineering and anion engineering,including MoS_(2)–MoO_(2),MoS_(2)–Mo_(2)C,MoS_(2)–MoN_(x),MoS_(2)–MoP,and MoS_(2)–MoSe_(2).The preparation method,structure,and performance of the catalysts are introduced and the possible mechanism behind the improved catalytic activity are revealed to give readers an overall comprehension on the progress of the Mo-based electrocatalysts for hydrogen evolution reaction.In addition,an outlook on future opportunities and development directions of Mo-based catalysts are proposed to facilitate the development of Mo-based catalysts for hydrogen production.
基金Financial support from the Science Fund for Creative Research Groups of the National Science Foundation of China (22021005)the National Natural Science Foundation of China (21776032)the Innovation Team of Dalian University of Technology (DUT2017TB01)。
文摘Tungsten (W) incorporated mobil-type eleven (MEL) zeolite membrane (referred to as W-MEL membrane) with high separation performance was firstly explored for the separation of oil/water mixtures under the influence of gravity.W-MEL membranes were grown on stainless steel (SS) meshes through in-situ hydrothermal growth method facilitated with (3-aminopropyl)triethoxysilane (APTES) modification of stainless steel meshes,which promote the heterogeneous nucleation and crystal growth of W-MEL zeolites onto the mesh surface.W-MEL membranes were grown on different mesh size supports to investigate the effect of mesh size on the separation performance of the membrane.The assynthesized W-MEL membrane supported on 500 mesh (25μm)(W-MEL-500) exhibit the hydrophilic nature with a water contact angle of 11.8°and delivers the best hexane/water mixture separation with a water flux and separation efficiency of 46247 L·m^(-2)·h^(-1)and 99.5%,respectively.The wettability of W-MEL membranes was manipulated from hydrophilic to hydrophobic nature by chemically modifying with the fluorine-free compounds (hexadecyltrimethoxysilane (HDTMS) and dodecyltrimethoxysilane(DDTMS)) to achieve efficient oil-permselective separation of heavy oils from water.Among the hydrophobically modified W-MEL membranes,W-MEL-500-HDTMS having a water contact angle of146.4°delivers the best separation performance for dichloromethane/water mixtures with a constant oil flux and separation efficiency of 61490 L·m^(-2)·h^(-1)and 99.2%,respectively along with the stability tested up to 20 cycles.Both W-MEL-500-HDTMS and W-MEL-500-DDTMS membranes also exhibit similar separation performances for the separation of heavy oil from sea water along with a 20-fold lower corrosion rate in comparison with the bare stainless-steel mesh,indicating their excellent stability in seawater.Compared to the reported zeolite membranes for oil/water separation,the as-synthesized and hydrophobically modified W-MEL membranes shows competitive separation performances in terms of flux and separation efficiency,demonstrating the good potentiality for oil/water separation.
基金supported by Project of Central Government for Local Science and Technology Development of China (2022JH6/100100050)the National Natural Science Foundation of China (21776028)Liaoning Key Laboratory of Chemical Additive Synthesis and Separation (ZJKF2001)。
文摘NH_(3) selective catalytic reduction(SCR) has been widely recognized as a promising technique for reducing nitrogen oxides from diesel vehicle exhausts. High-efficiency SCR catalysts that could perform at low temperatures are essential to denitration. In this work, a series of bimetallic CeCu-SAPO-34 molecular sieves were synthesized by one-step hydrothermal method. The Ce Cu-SAPO-34 maintained good crystallinity and a regular hexahedron appearance of Cu-SAPO-34 after introducing Ce species, while exhibiting a higher specific surface area and pore volume. The as-prepared CeCu-SAPO-34 with 0.02%(mass) Ce constituent exhibited the best catalytic activity below 300℃ and a maximum NO_(x) conversion of 99% was attained;the NO_(x) removal rates of more than 68% and 94% were achieved at 150℃ and 200℃, respectively. And the introduction of cerium species in Cu-SAPO-34 improves the low-temperature hydrothermal stability of the catalyst towards NH_(3)-SCR reaction. Additionally, the introduced Ce species could enhance the formation of abundant weak Br?nsted acid centers and promote the synergistic effect between CuO grains and isolated Cu^(2+) to enhance the redox cycle, which benefit the NH_(3)-SCR reaction.This work provides a facile synthesis method of high-efficiency SCR denitration catalysts towards diesel vehicles exhaust treatment under low temperature.
基金supported by the Fundamental Research Funds for the Central Universities (BLX202132)the Foreign expert program (G2022109001L)+1 种基金the Beijing Forestry University Outstanding Young Talent Cultivation Project (2019JQ03005)the Young Tip-top Talent Project of Science and Technology Innovation by National Forestry and Grassland Administration of China(2019132609)。
文摘Transformation of lignin to valuable chemicals via sustainable pathways is recognized as one of the most efficient ways to explore its value and replace the nonrenewable petroleum resource. In this work, an environmental-friendly transfer hydrogenation process has been developed to convert lignin derived2,6-dimethoxybenzoquinone to 1,4-cyclohexanediol. Compared with previous work under hydrogen pressure(30 bar), this process uses isopropanol as both solvent and hydrogen donor, which significantly simply the operation process. The core of this study is the design and preparation of Mn modified Raney Ni catalysts by ball milling process. A series of Raney Ni Mn catalysts with different ball milling time and Mn content were prepared and investigated. Characterizations by X-ray diffraction(XRD), X-ray photoelectron spectroscopy(XPS), scanning electron microscope(SEM) and transmission electron microscope(TEM) etc. showed that Ni Mn Al alloy was formed during the ball milling process and then transformed to Ni Mn alloy after treatment by aqueous Na OH. After optimization, a yield as high as 86.1% could be achieved for 1,4-cyclohexanediol at 200℃ in only 1 h.
基金support from Liao Ning Revitalization Talents Program(XLYC1907144)Dalian Youth Science and Technology Star Project Support Program(No.2017RQ104)+6 种基金National Key Research and Development Program of China(No.2020YFB0311600)National Natural Science Foundation of China(Grant Nos.22125903,51872283,22075279)Liaoning BaiQianWan Talents Program(Grant XLYC1807153)Dalian Innovation Support Plan for High Level Talents(2019RT09)Dalian National Laboratory For Clean Energy(DNL),CAS,DNL Cooperation Fund,CAS(DNL201912,DNL201915,DNL202016,DNL202019)DICP(DICP ZZBS201802,DICP I2020032)The Joint Fund of the Yulin University and the Dalian National Laboratory for Clean Energy(YLU-DNL Fund 2021002,2021009).
文摘With the rapid development of flexible and portable microelectronics,the extreme demand for miniaturized,mechanically flexible,and integrated microsystems are strongly stimulated.Here,biomass-derived carbons(BDCs)are prepared by KOH activation using Qamgur precursor,exhibiting three-dimensional(3D)hierarchical porous structure.Benefiting from unobstructed 3D hierarchical porous structure,BDCs provide an excellent specific capacitance of 433 F g^(-1)and prominent cyclability without capacitance degradation after 50000 cycles at 50 A g^(-1).Furthermore,BDC-based planar micro-supercapacitors(MSCs)without metal collector,prepared by mask-assisted coating,exhibit outstanding areal-specific capacitance of 84 mF cm^(-2)and areal energy density of 10.6μWh cm^(-2),exceeding most of the previous carbon-based MSCs.Impressively,the MSCs disclose extraordinary flexibility with capacitance retention of almost 100%under extreme bending state.More importantly,a flexible planar integrated system composed of the MSC and temperature sensor is assembled to efficiently monitor the temperature variation,providing a feasible route for flexible MSC-based functional micro-devices.
