The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actu...The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actual,oil-contaminated seawater remains a critical challenge,because the transport channels and evaporation interfaces of the current solar evaporators are easily blocked by the oil slicks,resulting in undermined evaporation rate and conversion efficiency.Herein,we propose a facile strategy for fabricating a modularized solar evaporator based on flexible MXene aerogels with arbitrarily tunable,highly ordered cellular/lamellar pore structures for high-efficiency oil interception and desalination.The core design is the creation of 1D fibrous MXenes with sufficiently large aspect ratios,whose superior flexibility and plentiful link forms lay the basis for controllable 3D assembly into more complicated pore structures.The cellular pore structure is responsible for effective contaminants rejection due to the multi-sieving effect achieved by the omnipresent,isotropic wall apertures together with underwater superhydrophobicity,while the lamellar pore structure is favorable for rapid evaporation due to the presence of continuous,large-area evaporation channels.The modularized solar evaporator delivers the best evaporation rate(1.48 kg m-2h-1)and conversion efficiency(92.08%)among all MXene-based desalination materials on oil-contaminated seawater.展开更多
The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy density.However,the poor redox kinetics and the"shuttle effect"of polysulfide...The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy density.However,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of Li-S batteries in practical applications.Herein,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling stopper.The three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination temperature.In conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance Li-S batteries.Particularly,the Li-S cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 C.Even with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 cycles.This work paves a new avenue for the rational design of materials for separator modification in high-performance Li-S batteries.展开更多
Ambient electrocatalytic nitrogen fixation is an emerging technology for green ammonia synthesis,but the absence of optimized,stable and performant catalysts can render its practical application challenging.Herein,bim...Ambient electrocatalytic nitrogen fixation is an emerging technology for green ammonia synthesis,but the absence of optimized,stable and performant catalysts can render its practical application challenging.Herein,bimetallic NiCo boride nanoparticles confined in MXene are shown to accomplish highperformance nitrogen reduction electrolysis.Ta king advantage of the synergistic effect in specific compositions with unique electronic d and p orbits and typical architecture of rich nanosized particles embedded in the interconnected conductive network,the synthesized MXene@NiCoB composite demonstrates extensive improvements in nitrogen molecule chemisorption,active area exposure and charge transport.As a result,optimal NH3 yield rate of 38.7μg h^(-1) mgcat^(-1).and Faradaic efficiency of 6.92%are acquired in0.1 M Na_(2)SO_(4) electrolyte.Moreover,the great catalytic performance can be almost entirely maintained in the cases of repeatedly-cycled and long-term electrolysis.Theoretical investigations reveal that the nitrogen reduction reaction on MXene@NiCoB catalyst proceeds according to the distal pathway,with a distinctly-reduced energy barrier relative to the Co2B counterpart.This work may inspire a new route towards the rational catalyst design for the nitrogen reduction reaction.展开更多
BiOBr/ZnO composite photocatalysts were prepared by a simple hydrothermal method. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microsco...BiOBr/ZnO composite photocatalysts were prepared by a simple hydrothermal method. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), high-resolution transmission electron microscopy(HRTEM), UV–Vis diffusion reflectance spectroscopy(DRS) and photoluminescence(PL) spectroscopy, respectively. The photocatalytic activities were evaluated by the degradation of methyl blue(MB) under the simulated sunlight irradiation. Among all the samples, the BiOBr/ZnO composite with a mole ratio of 3:1(Bi:Zn) exhibited the best photocatalytic activity. The improvement of photocatalytic activity was mainly attributed to the low recombination ratio of photo-induced electron-hole pairs. The possible photocatalytic mechanism was discussed on the basis of the band structures of BiOBr and ZnO.展开更多
Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via el...Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via electrocatalytic water splitting.The hydrogen evolution reaction(HER,a half-reaction of water splitting)plays a pivotal role in decreasing the price and increasing the catalytic efficiency of hydrogen production and is efficiently promoted by metal phosphides in different electrolytes.Herein,we summarize the recent advances in the development of metal phosphides as HER electrocatalysts,focus on their synthesis(post-treatment,in situ generation,and electrodeposition methods)and the enhancement of their electrocatalytic activity(via elemental doping,interface and vacancy engineering,construction of specific supports and nanostructures,and the design of bior polymetallic phosphides),and highlight the crucial issues and challenges of future development.展开更多
To accelerate the kinetics of the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells,ultrafine Pt nanoparticles modified with trace amounts of cobalt were fabricated and decorated on carbon black thr...To accelerate the kinetics of the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells,ultrafine Pt nanoparticles modified with trace amounts of cobalt were fabricated and decorated on carbon black through a strategy involving modified glycol reduction and chemical etching.The obtained Pt36Co/C catalyst exhibits a much larger electrochemical surface area(ECSA)and an improved ORR electrocatalytic activity compared to commercial Pt/C.Moreover,an electrode prepared with Pt36Co/C was further evaluated under H2-air single cell test conditions,and exhibited a maximum specific power density of 10.27 W mgPt^-1,which is 1.61 times higher than that of a conventional Pt/C electrode and also competitive with most state-of-the-art Pt-based architectures.In addition,the changes in ECSA,power density,and reacting resistance during the accelerated degradation process further demonstrate the enhanced durability of the Pt36Co/C electrode.The superior performance observed in this work can be attributed to the synergy between the ultrasmall size and homogeneous distribution of catalyst nanoparticles,bimetallic ligand and electronic effects,and the dissolution of unstable Co with the rearrangement of surface structure brought about by acid etching.Furthermore,the accessible raw materials and simplified operating procedures involved in the fabrication process would result in great cost-effectiveness for practical applications of PEMFCs.展开更多
Three-dimensional(3D)ordered porous carbon is generally believed to be a promising electromagnetic wave(EMW)absorbing material.However,most research works targeted performance improvement of 3D ordered porous carbon,a...Three-dimensional(3D)ordered porous carbon is generally believed to be a promising electromagnetic wave(EMW)absorbing material.However,most research works targeted performance improvement of 3D ordered porous carbon,and the specific attenuation mechanism is still ambiguous.Therefore,in this work,a novel ultra-light egg-derived porous carbon foam(EDCF)structure has been successfully constructed by a simple carbonization combined with the silica microsphere template-etching process.Based on an equivalent substitute strategy,the influence of pore volume and specific surface area on the electromagnetic parameters and EMW absorption properties of the EDCF products was confirmed respectively by adjusting the addition content and diameter of silica microspheres.As a primary attenuation mode,the dielectric loss originates from the comprehensive effect of conduction loss and polarization loss in S-band and C band,and the value is dominated by polarization loss in X band and Ku band,which is obviously greater than that of conduction loss.Furthermore,in all samples,the largest effective absorption bandwidth of EDCF-3 is 7.12 GHz under the thickness of 2.13 mm with the filling content of approximately 5 wt%,covering the whole Ku band.Meanwhile,the EDCF-7 sample with optimized pore volume and specific surface area achieves minimum reflection loss(RL_(min))of−58.08 dB at 16.86 GHz while the thickness is 1.27 mm.The outstanding research results not only provide a novel insight into enhancement of EMW absorption properties but also clarify the dominant dissipation mechanism for the porous carbon-based absorber from the perspective of objective experiments.展开更多
In this study,Ni_(2)P-Cd_(0.9)Zn_(0.1)S(NPCZS)composites were synthesized by coupling tetrapod bundle Cd_(0.9)Zn_(0.1)S(CZS)and coralline-like Ni_(2)P(NP)via a simple calcination method.CZS shows outstanding activity ...In this study,Ni_(2)P-Cd_(0.9)Zn_(0.1)S(NPCZS)composites were synthesized by coupling tetrapod bundle Cd_(0.9)Zn_(0.1)S(CZS)and coralline-like Ni_(2)P(NP)via a simple calcination method.CZS shows outstanding activity in photocatalytic hydrogen evolution(1.31 mmol h^(‒1)),owing to its unique morphology and heterophase homojunctions(ZB/WZ),which accelerate the separation and transfer of photogenerated charges.After coupling with NP,the photoactivity of NPCZS was enhanced,and the maximum hydrogen evolution rate of 1.88 mmol h^(‒1)was reached at a NP content of 12 wt%,which was 1.43 times higher than that of pure CZS.The experimental results of the photocatalytic activity,viz.photoluminescence spectra,surface photovoltage spectra,and electrochemical test showed that the enhanced photoactivity of NPCZS should be attributed to the synergistic effects of the novel tetrapod-bundle morphology,heterophase homojunctions,and decoration of the NP co-catalyst.Moreover,the as-prepared NPCZS composites exhibited excellent photostability and recyclability.Herein,we propose a possible mechanism for the enhanced photocatalytic activity.展开更多
The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane s...The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane sultone and trifluoromethanesulfonic acid(TfOH).The prepared ILs were characterized by infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy,and their thermal stability was determined by thermal gravimetry.The synthesized polyether ILs coupled with TfOH were used to catalyze the alkylation reaction of isobutane and isobutene for the preparation of alkylate gasoline.The polyether ILs could improve the substrate dissolution and promote the separation of the catalyst from the products.The ideal IL(n=94)was determined.The optimized alkylation reaction conditions covered:a VTfOH/VIL ratio of 0.35,a reaction temperature of 40℃,a reaction time of 50 min,and a stirring speed of 800 r/min.The conversion of isobutene was 92.4%and the selectivity for the C8-product was 81.6%.Under optimal conditions,the catalyst life was determined and TfOH showed improved cyclic performance in the polyether ILs.After 8 operating cycles,the catalytic activity of the catalyst showed negligible decline.展开更多
Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air ...Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.展开更多
Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication ...Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.展开更多
A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was furt...A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.展开更多
Ternary TiO2/WO3/graphene （TWG） nanocomposites were prepared by a facile salt-ultrasonic assisted hydrothermal method. The products were characterized by X-ray diffraction, scanning electron microscopy, transmission...Ternary TiO2/WO3/graphene （TWG） nanocomposites were prepared by a facile salt-ultrasonic assisted hydrothermal method. The products were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption--desorption. Both anatase TiO2 and orthorhombic WO3 formed in the nanocomposites, along with a highly disordered overlay of individual graphene nanosheets. Polyhedral and spherical TiO/and WO3 nanoparticles of uniform size 10-30 nm were densely anchored to the graphene sheets. The maximum specific surface area of the products was 144.59 m2·g^-1. The products showed clear abilities for the removal of Rhodamine B in the absence of illumination. Furthermore, the adsorption activity of the products exhibited only a slight decrease after three successive cycles. The results demonstrate that the ternary nanocomposites could be used as a high-efficiency adsorbent for the removal of environmental contaminants.展开更多
Trace zeolitic imidazolate framework-8(ZIF-8)-decorated activated carbon(AC)pellets were synthesized by a facile wet impregnation technique.After pyrolysis of the above composite material,the obtained carbon had a lar...Trace zeolitic imidazolate framework-8(ZIF-8)-decorated activated carbon(AC)pellets were synthesized by a facile wet impregnation technique.After pyrolysis of the above composite material,the obtained carbon had a large surface area and pore volume,with traces of Zn on its surface.Subsequently,the capacity of the ZIF8/AC samples to adsorb and remove phenol from aqueous media was evaluated in both batch and column experimental setups.The equilibrium adsorption capacity reached 155.24 mg·g^(-1),which was 2.3 times greater than that of the pure AC(46.24 mg·g^(-1)).In addition,adsorption kinetics were examined by pseudofirst and pseudosecond order models,and adsorption isotherms were fitted into Langmuir and Freundlich equations.The adsorbent could be easily filtered from the solution and washed with methanol and water,while maintaining an efficiency N90% after 4 cycles.The above results make it a potentially reusable candidate for water purification.展开更多
Nanocrystalline cellulose(NCC)/poly(lactic acid)(PLLA) composite membranes were prepared by the solution casting method.Physical and chemical modifications were performed to improve the compatibility of NCC and PLLA.T...Nanocrystalline cellulose(NCC)/poly(lactic acid)(PLLA) composite membranes were prepared by the solution casting method.Physical and chemical modifications were performed to improve the compatibility of NCC and PLLA.The results indicated that the NCC dispersibility of the composite membranes with chemical modification were superior to that of the composite membranes with physical modification.Moreover,the chemical modification NCC not only had a large effect on the nucleation and growth of the crystals,but also affected the crystal forms of PLLA.This was because chemical reactions took place between the silicone of silane coupling agent(KH-570) and the hydroxyl groups of NCC during blending.The chemical modification NCC could be dispersed stably in the PLLA matrix,and it played the role of a nucleating agent.展开更多
A polyetheramine(PEA)-based Br?nsted-acidic ionic liquid(IL)was firstly prepared and used to promote the alkylation of isobutane with isobutene catalyzed by trifluoromethanesulfonic acid(TfOH).PEA-IL not only can reso...A polyetheramine(PEA)-based Br?nsted-acidic ionic liquid(IL)was firstly prepared and used to promote the alkylation of isobutane with isobutene catalyzed by trifluoromethanesulfonic acid(TfOH).PEA-IL not only can resolve the persistent problem of poor solubility of the volatile and refractory reactants,but also can satisfactorily exhibit the separation of the catalyst from product oil for reuse.The PEA-IL/TfOH catalytic system with an adjustable acidity ensures a high alkylate selectivity.Under the conditions covering a VIL/VTfOH ratio of 10:3,a temperature of 25°C,and a reaction time of 25 min,the C8-product selectivity reaches 86.63%.The PEA-IL/TfOH catalyst can be reused 13 times without a decrease in the catalytic performance.After many operating cycles,the hydrophobic PEA-IL can be easily regenerated by simply adding water.This study provides a green,economic,and highly efficient method for producing high-octane alkylate gasoline.展开更多
For high-efficiency NH_(3)synthesis via ambient-condition electrohydrogenation of inert N_(2),it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency,good ...For high-efficiency NH_(3)synthesis via ambient-condition electrohydrogenation of inert N_(2),it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency,good conductivity and large surface area.Here,oxygen-deficient SnO_(2)nanoparticles encapsulated by ultrathin carbon layer(d-SnO_(2)@C)are developed by hydrothermal deposition coupled with annealing process,as promising catalysts for ambient electrocatalytic N_(2)reduction.d-SnO_(2)@C exhibits high activity and excellent selectivity for electrocatalytic conversion of N_(2)to NH_(3)in acidic electrolytes,with Faradic efficiency as high as 12.7%at-0.15 V versus the reversible hydrogen electrode(RHE)and large NH_(3)yield rate of 16.68μg h^(-1)mgcat^(-1)at-0.25 V vs.RHE in 0.1 mol L^(-1)HCl.Benefiting from the structural superiority of enhanced charge transfer efficiency and optimized surface states,d-SnO_(2)@C also achieves excellent long-term stability.展开更多
A Ru(II)-catalyzed ortho allylation reaction of N-aryl-7-azaindole with readily available 2-methylidene cyclic carbonate has been developed.This reaction is an effective pathway for synthesizing 7-azaindole derivative...A Ru(II)-catalyzed ortho allylation reaction of N-aryl-7-azaindole with readily available 2-methylidene cyclic carbonate has been developed.This reaction is an effective pathway for synthesizing 7-azaindole derivatives with a wide scope of substrates and high yields.In addition,the method can be extended to the allylation of other heterocyclic compounds and several cyclic carbonates,highlighting the practicality of this strategy for synthesis.展开更多
A straightforward electrochemical reduction of benzo[b]thiophene 1,1-dioxides with HFIP as the hydrogen donor has been reported in an undivided cell under metal-free conditions.Moreover,the tolerance of various functi...A straightforward electrochemical reduction of benzo[b]thiophene 1,1-dioxides with HFIP as the hydrogen donor has been reported in an undivided cell under metal-free conditions.Moreover,the tolerance of various functional groups and scaled-up experiments showed the practicability and potential applications of this methodology.展开更多
An efficient electrochemical approach has been developed for the construction of 3-sulfanylquinoline derivatives by treating phenylethynylbenzoxazinanones with disulfides in an undivided cell.The protocol provided a c...An efficient electrochemical approach has been developed for the construction of 3-sulfanylquinoline derivatives by treating phenylethynylbenzoxazinanones with disulfides in an undivided cell.The protocol provided a convenient route to functionalized quinolines with good functional group tolerance.Moreover,it does not require any metal catalysts or additives,furnishing a series of biologicalquinolines inmoderatetogoodyields.展开更多
基金support from the National Natural Science Foundation of China(G.Nos.52173055,21961132024,and 51925302)the Ministry of Science and Technology of China(G.No.2021YFE0105100)+3 种基金the Textile Vision Basic Research Program(No.J202201)the International Cooperation Fund of Science and Technology Commission of Shanghai Municipality(G.No.21130750100)the Fundamental Research Funds for the Central Universitiesthe DHU Distinguished Young Professor Program(G.No.LZA2020001)。
文摘The seawater desalination based on solardriven interfacial evaporation has emerged as a promising technique to alleviate the global crisis on freshwater shortage.However,achieving high desalination performance on actual,oil-contaminated seawater remains a critical challenge,because the transport channels and evaporation interfaces of the current solar evaporators are easily blocked by the oil slicks,resulting in undermined evaporation rate and conversion efficiency.Herein,we propose a facile strategy for fabricating a modularized solar evaporator based on flexible MXene aerogels with arbitrarily tunable,highly ordered cellular/lamellar pore structures for high-efficiency oil interception and desalination.The core design is the creation of 1D fibrous MXenes with sufficiently large aspect ratios,whose superior flexibility and plentiful link forms lay the basis for controllable 3D assembly into more complicated pore structures.The cellular pore structure is responsible for effective contaminants rejection due to the multi-sieving effect achieved by the omnipresent,isotropic wall apertures together with underwater superhydrophobicity,while the lamellar pore structure is favorable for rapid evaporation due to the presence of continuous,large-area evaporation channels.The modularized solar evaporator delivers the best evaporation rate(1.48 kg m-2h-1)and conversion efficiency(92.08%)among all MXene-based desalination materials on oil-contaminated seawater.
基金supported by the National Natural Science Foundation of China(51972184,22005169)the Key Basic Research Project of Shandong Province(ZR2019ZD49)+2 种基金the Natural Science Foundation of Shandong Province(ZR2020QB121)the Taishan Scholars Project of Shandong Provincethe Taishan Scholar Young Talent Program(tsqn201909114)。
文摘The lithium-sulfur(Li-S)battery,as one of the energy storage devices,has been in the limelight due to its high theoretical energy density.However,the poor redox kinetics and the"shuttle effect"of polysulfides severely restrict the use of Li-S batteries in practical applications.Herein,a novel bimetallic LaNiO_(3) functional material with high electrical conductivity and catalytic property is prepared to act as a high-efficiency polysulfide shuttling stopper.The three LaNiO_(3) samples with different physical/chemical characteristics are obtained by controlling the calcination temperature.In conjunction with the high electrical conductivity and excellent catalytic properties of the as-prepared materials,the appropriate chemisorption toward polysulfides offers great potential to enhance electrochemical stability for highperformance Li-S batteries.Particularly,the Li-S cell with the separator modified by such functional material gives a specific capacity of 658 mA h g^(-1) after 500 cycles at a high current density of 2 C.Even with high sulfur loading of 6.05 mg cm^(-2),the Li-S battery still exhibits an areal specific capacity of 2.81 m A h cm^(-2)after 150 cycles.This work paves a new avenue for the rational design of materials for separator modification in high-performance Li-S batteries.
基金financially supported by the National Natural Science Foundation of China(No.21878063)Key Program of Shandong Provincial Natural Science Foundation(No.ZR2020KB011)+2 种基金Taishan Scholars Program of Shandong Province(No.tsqn201909119)financial support from the Flemish Government through the Moonshot cSBO project P2C(HBC.2019.0108)through long-term structural funding(Methusalem CASAS2,Meth/15/04)。
文摘Ambient electrocatalytic nitrogen fixation is an emerging technology for green ammonia synthesis,but the absence of optimized,stable and performant catalysts can render its practical application challenging.Herein,bimetallic NiCo boride nanoparticles confined in MXene are shown to accomplish highperformance nitrogen reduction electrolysis.Ta king advantage of the synergistic effect in specific compositions with unique electronic d and p orbits and typical architecture of rich nanosized particles embedded in the interconnected conductive network,the synthesized MXene@NiCoB composite demonstrates extensive improvements in nitrogen molecule chemisorption,active area exposure and charge transport.As a result,optimal NH3 yield rate of 38.7μg h^(-1) mgcat^(-1).and Faradaic efficiency of 6.92%are acquired in0.1 M Na_(2)SO_(4) electrolyte.Moreover,the great catalytic performance can be almost entirely maintained in the cases of repeatedly-cycled and long-term electrolysis.Theoretical investigations reveal that the nitrogen reduction reaction on MXene@NiCoB catalyst proceeds according to the distal pathway,with a distinctly-reduced energy barrier relative to the Co2B counterpart.This work may inspire a new route towards the rational catalyst design for the nitrogen reduction reaction.
文摘BiOBr/ZnO composite photocatalysts were prepared by a simple hydrothermal method. The as-prepared samples were characterized by X-ray diffraction(XRD), scanning electron microscopy(SEM), transmission electron microscopy(TEM), high-resolution transmission electron microscopy(HRTEM), UV–Vis diffusion reflectance spectroscopy(DRS) and photoluminescence(PL) spectroscopy, respectively. The photocatalytic activities were evaluated by the degradation of methyl blue(MB) under the simulated sunlight irradiation. Among all the samples, the BiOBr/ZnO composite with a mole ratio of 3:1(Bi:Zn) exhibited the best photocatalytic activity. The improvement of photocatalytic activity was mainly attributed to the low recombination ratio of photo-induced electron-hole pairs. The possible photocatalytic mechanism was discussed on the basis of the band structures of BiOBr and ZnO.
文摘Among the sustainable energy sources,hydrogen is the one most promising for alleviating the pollution issues related to the usage of conventional fuels,as it can be produced in an efficient and eco-friendly way via electrocatalytic water splitting.The hydrogen evolution reaction(HER,a half-reaction of water splitting)plays a pivotal role in decreasing the price and increasing the catalytic efficiency of hydrogen production and is efficiently promoted by metal phosphides in different electrolytes.Herein,we summarize the recent advances in the development of metal phosphides as HER electrocatalysts,focus on their synthesis(post-treatment,in situ generation,and electrodeposition methods)and the enhancement of their electrocatalytic activity(via elemental doping,interface and vacancy engineering,construction of specific supports and nanostructures,and the design of bior polymetallic phosphides),and highlight the crucial issues and challenges of future development.
基金supported by the National Major Research Project(2016YFB0101208)the National Natural Science Foundation of China(21576257)+1 种基金the Natural Science Foundation-Liaoning United Fund(U1508202)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB06050303)~~
文摘To accelerate the kinetics of the oxygen reduction reaction(ORR)in proton exchange membrane fuel cells,ultrafine Pt nanoparticles modified with trace amounts of cobalt were fabricated and decorated on carbon black through a strategy involving modified glycol reduction and chemical etching.The obtained Pt36Co/C catalyst exhibits a much larger electrochemical surface area(ECSA)and an improved ORR electrocatalytic activity compared to commercial Pt/C.Moreover,an electrode prepared with Pt36Co/C was further evaluated under H2-air single cell test conditions,and exhibited a maximum specific power density of 10.27 W mgPt^-1,which is 1.61 times higher than that of a conventional Pt/C electrode and also competitive with most state-of-the-art Pt-based architectures.In addition,the changes in ECSA,power density,and reacting resistance during the accelerated degradation process further demonstrate the enhanced durability of the Pt36Co/C electrode.The superior performance observed in this work can be attributed to the synergy between the ultrasmall size and homogeneous distribution of catalyst nanoparticles,bimetallic ligand and electronic effects,and the dissolution of unstable Co with the rearrangement of surface structure brought about by acid etching.Furthermore,the accessible raw materials and simplified operating procedures involved in the fabrication process would result in great cost-effectiveness for practical applications of PEMFCs.
基金supported by the National Natural Science Foundation of China under Grant No.52072196,52002199,52002200,52102106Major Basic Research Program of Natural Science Foundation of Shandong Province under Grant No.ZR2020ZD09+2 种基金the Natural Science Foundation of Shandong Province under Grant No.ZR2019BEM042,ZR2020QE063the Innovation and Technology Program of Shandong Province under Grant No.2020KJA004the Taishan Scholars Program of Shandong Province under No.ts201511034
文摘Three-dimensional(3D)ordered porous carbon is generally believed to be a promising electromagnetic wave(EMW)absorbing material.However,most research works targeted performance improvement of 3D ordered porous carbon,and the specific attenuation mechanism is still ambiguous.Therefore,in this work,a novel ultra-light egg-derived porous carbon foam(EDCF)structure has been successfully constructed by a simple carbonization combined with the silica microsphere template-etching process.Based on an equivalent substitute strategy,the influence of pore volume and specific surface area on the electromagnetic parameters and EMW absorption properties of the EDCF products was confirmed respectively by adjusting the addition content and diameter of silica microspheres.As a primary attenuation mode,the dielectric loss originates from the comprehensive effect of conduction loss and polarization loss in S-band and C band,and the value is dominated by polarization loss in X band and Ku band,which is obviously greater than that of conduction loss.Furthermore,in all samples,the largest effective absorption bandwidth of EDCF-3 is 7.12 GHz under the thickness of 2.13 mm with the filling content of approximately 5 wt%,covering the whole Ku band.Meanwhile,the EDCF-7 sample with optimized pore volume and specific surface area achieves minimum reflection loss(RL_(min))of−58.08 dB at 16.86 GHz while the thickness is 1.27 mm.The outstanding research results not only provide a novel insight into enhancement of EMW absorption properties but also clarify the dominant dissipation mechanism for the porous carbon-based absorber from the perspective of objective experiments.
文摘In this study,Ni_(2)P-Cd_(0.9)Zn_(0.1)S(NPCZS)composites were synthesized by coupling tetrapod bundle Cd_(0.9)Zn_(0.1)S(CZS)and coralline-like Ni_(2)P(NP)via a simple calcination method.CZS shows outstanding activity in photocatalytic hydrogen evolution(1.31 mmol h^(‒1)),owing to its unique morphology and heterophase homojunctions(ZB/WZ),which accelerate the separation and transfer of photogenerated charges.After coupling with NP,the photoactivity of NPCZS was enhanced,and the maximum hydrogen evolution rate of 1.88 mmol h^(‒1)was reached at a NP content of 12 wt%,which was 1.43 times higher than that of pure CZS.The experimental results of the photocatalytic activity,viz.photoluminescence spectra,surface photovoltage spectra,and electrochemical test showed that the enhanced photoactivity of NPCZS should be attributed to the synergistic effects of the novel tetrapod-bundle morphology,heterophase homojunctions,and decoration of the NP co-catalyst.Moreover,the as-prepared NPCZS composites exhibited excellent photostability and recyclability.Herein,we propose a possible mechanism for the enhanced photocatalytic activity.
基金supported by the National Natural Science Foundation of China (21476120)the Shandong Province Prioritized Development Plan (2017GGX40107)the Taishan Scholar Project of Shandong Province in China (ts201511033)
文摘The Br?nsted-acidic polyether ionic liquids(ILs)with different polymerization degrees(n value)were prepared via the reaction of tetramethylguanidine and epoxy ethane,followed by successive reactions with 1,3-propane sultone and trifluoromethanesulfonic acid(TfOH).The prepared ILs were characterized by infrared spectroscopy and 1H nuclear magnetic resonance spectroscopy,and their thermal stability was determined by thermal gravimetry.The synthesized polyether ILs coupled with TfOH were used to catalyze the alkylation reaction of isobutane and isobutene for the preparation of alkylate gasoline.The polyether ILs could improve the substrate dissolution and promote the separation of the catalyst from the products.The ideal IL(n=94)was determined.The optimized alkylation reaction conditions covered:a VTfOH/VIL ratio of 0.35,a reaction temperature of 40℃,a reaction time of 50 min,and a stirring speed of 800 r/min.The conversion of isobutene was 92.4%and the selectivity for the C8-product was 81.6%.Under optimal conditions,the catalyst life was determined and TfOH showed improved cyclic performance in the polyether ILs.After 8 operating cycles,the catalytic activity of the catalyst showed negligible decline.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51772162)the Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and Technologythe Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)。
文摘Non-noble-metal-based electrocatalysts with superior oxygen reduction reaction(ORR)activity to platinum(Pt)are highly desirable but their fabrications are challenging and thus impeding their applications in metal-air batteries and fuel cells.Here,we report a facile molten salt assisted two-step pyrolysis strategy to construct carbon nanosheets matrix with uniformly dispersed Fe_(3) N/Fe nanoparticles and abundant nitrogen-coordinated Fe single atom moieties(Fe@Fe_(SA)-N-C).Thermal exfoliation and etching effect of molten salt contribute to the formation of carbon nanosheets with high porosity,large surface area and abundant uniformly immobilized active sites.Aberration-corrected high-angle annular dark-field scanning transmission electron microscopy(HAADF-STEM)image,X-ray absorption fine spectroscopy,and X-ray photoelectron spectroscopy indicate the generation of Fe(mainly Fe_(3) N/Fe)and Fe_(SA)-N-C moieties,which account for the catalytic activity for ORR.Further study on modulating the crystal structure and composition of Fe_(3) N/Fe nanoparticles reveals that proper chemical environment of Fe in Fe_(3) N/Fe notably optimizes the ORR activity.Consequently,the presence of abundant Fe_(SA)-N-C moieties,and potential synergies of Fe_(3) N/Fe nanoparticles and carbon shells,markedly promote the reaction kinetics.The as-developed Fe@Fe_(SA)-N-C-900 electrocatalyst displays superior ORR performance with a half-wave potential(E_(1/2))of 0.83 V versus reversible hydrogen electrode(RHE)and a diffusion limited current density of 5.6 mA cm^(-2).In addition,a rechargeable Zn-air battery device assembled by the Fe@Fe_(SA)-N-C-900 possesses remarkably stable performance with a small voltage gap without obvious voltage loss after500 h of operation.The facile synthesis strategy for the high-performance composites represents another viable avenue to stable and low-cost electrocatalysts for ORR catalysis.
基金supported financially by the National Natural Science Foundation of China,China(Grant No.51702180,51572136,91963113,21703116,51372127,51873096)The Scientific and Technical Development Project of Qingdao,China(Grant No.18-2-2-52-jch)+1 种基金The Taishan Scholar Advantage and Characteristic Discipline Team of Eco Chemical Process and TechnologyThe Natural Science Foundation of Hebei Province(B2019204009)。
文摘Efficient bifunctional oxygen electrocatalysts for ORR and OER are fundamental to the development of high performance metal-air batteries.Herein,a facile cost-efficient two-step pyrolysis strategy for the fabrication of a bifunctional oxygen electrocatalyst has been proposed.The efficient non-preciousmetal-based electrocatalyst,Fe/Fe_(3)C@Fe-N_(x)-C consists of highly curved onion-like carbon shells that encapsulate Fe/Fe_(3)C nanoparticles,distributed on an extensively porous graphitic carbon aerogel.The obtained Fe/Fe_(3)C@Fe-N_(x)-C aerogel exhibited superb electrochemical activity,excellent durability,and high methanol tolerance.The experimental results indicated that the assembly of onion-like carbon shells with encapsulated Fe/Fe_(3)C yielded highly curved carbon surfaces with abundant Fe-Nxactive sites,a porous structure,and enhanced electrocatalytic activity towards ORR and OER,hence displaying promising potential for application as an air cathode in rechargeable Zn-air batteries.The constructed Zn-air battery possessed an exceptional peak power density of~147 mW cm^(-2),outstanding cycling stability(200 cycles,1 h per cycle),and a small voltage gap of 0.87 V.This study offers valuable insights regarding the construction of low-cost and highly active bifunctional oxygen electrocatalysts for efficient air batteries.
基金the financial supports from the Shandong Provincial Natural Science Foundation(Grant No.ZR201910220216)the Key Research and Development Plan of Shandong Province(2019GGX104034)+1 种基金the Foundation of State Key Laboratory of High-efficiency Utilization of Coal,and Green Chemical Engineering(Grant No.2020-KF-18)the Taishan Scholar Program of Shandong Province(No.ts201712045)。
文摘A 2 D-2 D titanium dioxide nanosheet-reduced graphene oxide(TNS-r GO)composite with better electronic conductivity and hydrophilicity was prepared by the hydrothermal method.The as-obtained TNS-r GO composite was further functionalized with 3-aminopropyltriethoxysilane(APTES)to provide a large amount of-NH2 groups on the surface for anchoring ultrafine Pd Ag alloy nanoparticles with an average particle size of 1.69 nm by a facile wet reduction approach.Benefiting from the combined effects of well-dispersed Pd Ag alloy nanoparticles,facilitated electron transfer from TNS-r GO to Pd,and increased electron density of active sites,the Pd8 Ag_(1)/NH_(2)-TNS-r GO catalyst exhibited excellent activity towards dehydrogenation of formic acid without adding any additives at 298 K,corresponding to an initial turn over frequency as high as 1090 h-1,which is much higher than that of most other state-of-theart catalysts.
基金financially supported by the National Natural Science Foundation of China (No. 41340037)the Science Foundation for Youth Scholars of State Oceanic Administration (No. 2012508)+2 种基金the Scientific Research Program of Shandong Province (No. 2013G0021701)the Natural Science Foundation of Shandong Province, China (No. ZR2011BL012 and ZR2012EMM015)the Scientific Research Program of Qingdao (No.11-2-4-3-15-jch)
文摘Ternary TiO2/WO3/graphene （TWG） nanocomposites were prepared by a facile salt-ultrasonic assisted hydrothermal method. The products were characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy, and nitrogen adsorption--desorption. Both anatase TiO2 and orthorhombic WO3 formed in the nanocomposites, along with a highly disordered overlay of individual graphene nanosheets. Polyhedral and spherical TiO/and WO3 nanoparticles of uniform size 10-30 nm were densely anchored to the graphene sheets. The maximum specific surface area of the products was 144.59 m2·g^-1. The products showed clear abilities for the removal of Rhodamine B in the absence of illumination. Furthermore, the adsorption activity of the products exhibited only a slight decrease after three successive cycles. The results demonstrate that the ternary nanocomposites could be used as a high-efficiency adsorbent for the removal of environmental contaminants.
基金This work was supported by National Natural Science Foundation of China (21606252)the Key Research and Development Program of Xuzhou (KC19214)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Trace zeolitic imidazolate framework-8(ZIF-8)-decorated activated carbon(AC)pellets were synthesized by a facile wet impregnation technique.After pyrolysis of the above composite material,the obtained carbon had a large surface area and pore volume,with traces of Zn on its surface.Subsequently,the capacity of the ZIF8/AC samples to adsorb and remove phenol from aqueous media was evaluated in both batch and column experimental setups.The equilibrium adsorption capacity reached 155.24 mg·g^(-1),which was 2.3 times greater than that of the pure AC(46.24 mg·g^(-1)).In addition,adsorption kinetics were examined by pseudofirst and pseudosecond order models,and adsorption isotherms were fitted into Langmuir and Freundlich equations.The adsorbent could be easily filtered from the solution and washed with methanol and water,while maintaining an efficiency N90% after 4 cycles.The above results make it a potentially reusable candidate for water purification.
文摘Nanocrystalline cellulose(NCC)/poly(lactic acid)(PLLA) composite membranes were prepared by the solution casting method.Physical and chemical modifications were performed to improve the compatibility of NCC and PLLA.The results indicated that the NCC dispersibility of the composite membranes with chemical modification were superior to that of the composite membranes with physical modification.Moreover,the chemical modification NCC not only had a large effect on the nucleation and growth of the crystals,but also affected the crystal forms of PLLA.This was because chemical reactions took place between the silicone of silane coupling agent(KH-570) and the hydroxyl groups of NCC during blending.The chemical modification NCC could be dispersed stably in the PLLA matrix,and it played the role of a nucleating agent.
基金financially supported by the National Natural Science Foundation of China(Nos.21476120,21805158)the Shandong Province Priority Development Plan of China(Nos.2017GGX40107,2019GGX102021)。
文摘A polyetheramine(PEA)-based Br?nsted-acidic ionic liquid(IL)was firstly prepared and used to promote the alkylation of isobutane with isobutene catalyzed by trifluoromethanesulfonic acid(TfOH).PEA-IL not only can resolve the persistent problem of poor solubility of the volatile and refractory reactants,but also can satisfactorily exhibit the separation of the catalyst from product oil for reuse.The PEA-IL/TfOH catalytic system with an adjustable acidity ensures a high alkylate selectivity.Under the conditions covering a VIL/VTfOH ratio of 10:3,a temperature of 25°C,and a reaction time of 25 min,the C8-product selectivity reaches 86.63%.The PEA-IL/TfOH catalyst can be reused 13 times without a decrease in the catalytic performance.After many operating cycles,the hydrophobic PEA-IL can be easily regenerated by simply adding water.This study provides a green,economic,and highly efficient method for producing high-octane alkylate gasoline.
基金supported by Taishan Scholar Program of Shandong Province,China(ts201712045)the Doctoral Found of QUST(0100229001)2019 Research Funds(1.190002.01)of Ulsan National Institute of Science and Technology(UNIST)。
文摘For high-efficiency NH_(3)synthesis via ambient-condition electrohydrogenation of inert N_(2),it is pivotal to ingeniously design an active electrocatalyst with multiple features of abundant surfacial deficiency,good conductivity and large surface area.Here,oxygen-deficient SnO_(2)nanoparticles encapsulated by ultrathin carbon layer(d-SnO_(2)@C)are developed by hydrothermal deposition coupled with annealing process,as promising catalysts for ambient electrocatalytic N_(2)reduction.d-SnO_(2)@C exhibits high activity and excellent selectivity for electrocatalytic conversion of N_(2)to NH_(3)in acidic electrolytes,with Faradic efficiency as high as 12.7%at-0.15 V versus the reversible hydrogen electrode(RHE)and large NH_(3)yield rate of 16.68μg h^(-1)mgcat^(-1)at-0.25 V vs.RHE in 0.1 mol L^(-1)HCl.Benefiting from the structural superiority of enhanced charge transfer efficiency and optimized surface states,d-SnO_(2)@C also achieves excellent long-term stability.
基金supported by the Natural Science Foundation of Shandong Province(ZR2019BB011)the Scientific Research Foundation of Qingdao University of Science&Technology(010029022).
文摘A Ru(II)-catalyzed ortho allylation reaction of N-aryl-7-azaindole with readily available 2-methylidene cyclic carbonate has been developed.This reaction is an effective pathway for synthesizing 7-azaindole derivatives with a wide scope of substrates and high yields.In addition,the method can be extended to the allylation of other heterocyclic compounds and several cyclic carbonates,highlighting the practicality of this strategy for synthesis.
基金supported by the National Natural Science Foundation of China(21801152 and 21572110)We thank the Youth Innovation Science and Technology Plan of Colleges and Universities in Shandong Province(2021KJ076).
文摘A straightforward electrochemical reduction of benzo[b]thiophene 1,1-dioxides with HFIP as the hydrogen donor has been reported in an undivided cell under metal-free conditions.Moreover,the tolerance of various functional groups and scaled-up experiments showed the practicability and potential applications of this methodology.
基金supported by the National Natural Science Foundation of China(21801152 and 21572110)the Youth Innovation Science and Technology Plan of Colleges and Universities in Shandong Province(2021KJ076).
文摘An efficient electrochemical approach has been developed for the construction of 3-sulfanylquinoline derivatives by treating phenylethynylbenzoxazinanones with disulfides in an undivided cell.The protocol provided a convenient route to functionalized quinolines with good functional group tolerance.Moreover,it does not require any metal catalysts or additives,furnishing a series of biologicalquinolines inmoderatetogoodyields.
