As an alternative to conventional energy conversion and storage reactions,gas-involved electrochemical reactions,including the carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and hydrogen e...As an alternative to conventional energy conversion and storage reactions,gas-involved electrochemical reactions,including the carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and hydrogen evolution reaction(HER),have become an emerging research direction and have gained increasing attention due to their advantages of environmental friendliness and sustainability.Various studies have been designed to accelerate sluggish kinetics but with limited results.Most of them promote the reaction by modulating the intrinsic properties of the catalyst,ignoring the synergistic effect of the reaction as a whole.Due to the introduction of gas,traditional liquid-solid two-phase reactions are no longer applicable to future research.Since gas-involved electrochemical reactions mostly occur at the junctions of gaseous reactants,liquid electrolytes and solid catalysts,the focus of future research on reaction kinetics should gradually shift to three-phase reaction interfaces.In this review,we briefly introduce the formation and constraints of the three-phase interface and propose three criteria to judge its merit,namely,the active site,mass diffusion and electron mass transfer.Subsequently,a series of modulation methods and relevant works are discussed in detail from the three improvement directions of‘exposing more active sites,promoting mass diffusion and accelerating electron transfer’.Definitively,we provide farsighted insights into the understanding and research of three-phase interfaces in the future and point out the possible development direction of future regulatory methods,hoping that this review can broaden the future applications of the three-phase interface,including but not limited to gas-involved electrochemical reactions.展开更多
Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with pro...Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with production performance co-benefits. This study presents three PM reduction methods based on controlling operating parameters, i.e., lowering electrolyte temperature, H2SO4 concentration, and current density of the cathode. The optimized conditions were also investigated using the response surface methodology to balance the PM reduction effect and Zn production. The results showed that lowering electrolyte temperature is the most efficient, with an 89.0% reduction in the PM generation flux (GFPM). Reducing H2SO4 concentration led to the minimum side effects on the current efficiency of Zn deposition (CEZn) or power consumption (PC). With the premise of non-deteriorating CEZn and PC, GFPM can be reduced by 86.3% at the optimal condition (electrolyte temperature = 295 K, H2SO4 = 110 g/L, current density = 373 A/m^(2)). In addition, the reduction mechanism was elucidated by comprehensively analyzing bubble characteristics, electrochemical reactions, and surface tension. Results showed that lower electrolyte temperature inhibited the oxygen evolution reaction (OER) and compressed gas volume. Lower H2SO4 concentration inhibited the hydrogen evolution reaction (HER) and reduced electrolyte surface tension. Lower current density inhibited both OER and HER by decreasing the reaction current. The inhibited gas evolutions reduced the microbubbles’ number and size, thereby reducing GFPM. These results may provide energy-efficient PM reduction methods and theoretical hints of exploring cleaner PM reduction approaches for industrial electrolysis.展开更多
Mass transfer can tune the surface concentration of reactants and products and subsequently infl uence the catalytic perfor-mance.The morphology of nanomaterials plays an important role in the mass transfer of reactio...Mass transfer can tune the surface concentration of reactants and products and subsequently infl uence the catalytic perfor-mance.The morphology of nanomaterials plays an important role in the mass transfer of reaction microdomains,but related studies are lacking.Herein,a facile electrospinning technique utilizing cellulose was employed to fabricate a series of carbon nanofi bers with diff erent diameters,which exhibited excellent electrochemical nitrate reduction reaction and oxygen evolu-tion reaction activities.Furthermore,the microstructure of electrocatalysts could infl uence the gas-liquid-solid interfacial mass transfer,resulting in diff erent electrochemical performances.展开更多
Heterogeneous nanostructures that are defined as a hybrid structure consisting of two or more nanoscale domains with distinct chemical compositions or physical characteristics have attracted intense efforts in recent ...Heterogeneous nanostructures that are defined as a hybrid structure consisting of two or more nanoscale domains with distinct chemical compositions or physical characteristics have attracted intense efforts in recent years.In this review,we focus on the introduction of a number of heterogeneous nanostructures derived using core-shell Ag-Pt nanoparticles as starting materials,including hollow,dimeric and composite structures and also highlight their application in catalyzing electrochemical reactions,e.g.,methanol oxidation reaction and oxygen reduction reaction.This review not only shows the capability of core-shell Ag-Pt nanoparticles in producing various heterogeneous nanostructures as starting templates,but also highlights the structural design or electronic interaction that endows the heterogeneous nanostructures with enhanced catalytic properties either in methanol oxidation or in oxygen reduction.Further,we also make some perspectives for more heterogeneous nanostructures that may be prepared by using core-shell Ag-Pt particles or their derivatives so as to offer the readers the opportunities and challenges in this field.展开更多
Zn_(2)Ti_(3)O_(8),as a new type of anode material for lithium-ion batteries,is attracting enormous attention because of its low cost and excellent safety.Though decent capacities have been reported,the electrochemical...Zn_(2)Ti_(3)O_(8),as a new type of anode material for lithium-ion batteries,is attracting enormous attention because of its low cost and excellent safety.Though decent capacities have been reported,the electrochemical reaction mechanism of Zn_(2)Ti_(3)O_(8)has rarely been studied.In this work,a porous Zn_(2)Ti_(3)O_(8)anode with considerably high capacity(421 mAh/g at 100 mA/g and 209 mAh/g at 5000 mA/g after 1500 cycles)was reported,which is even higher than ever reported titanium-based anodes materials including Li_(4)Ti_(5)O_(12),TiO_(2)and Li_(2)ZnTi_(3)O_(8).Here,for the first time,the accurate theoretical capacity of Zn_(2)Ti_(3)O_(8)was confirmed to be 266.4 mAh/g.It was also found that both intercalation reaction and pseudocapacitance contribute to the actual capacity of Zn_(2)Ti_(3)O_(8),making it possibly higher than the theoretical value.Most importantly,the porous structure of Zn_(2)Ti_(3)O_(8)not only promotes the intercalation reaction,but also induces high pseudocapacitance capacity(225.4 mAh/g),which boosts the reversible capacity.Therefore,it is the outstanding pseudocapacitance capacity of porous Zn_(2)Ti_(3)O_(8)that accounts for high actual capacity exceeding the theoretical one.This work elucidates the superiorities of porous structure and provides an example in designing high-performance electrodes for lithium-ion batteries.展开更多
IN the study of antigen and antibody reaction with ellipsometric spectroscopy, most researchers calculated the thickness of antibody film, absorbance and film constant by mathematic models.But by using simple mathemat...IN the study of antigen and antibody reaction with ellipsometric spectroscopy, most researchers calculated the thickness of antibody film, absorbance and film constant by mathematic models.But by using simple mathematic models, it is very hard to describe accurately the real state of the system. Huang and Ord proposed a new physical measurement (optical tracking rate,V<sub>op</sub>), indicating the total change of △, Ψ in study of oxidation and reduction reaction of the iron electrode in alkaline solution. Many experimental results showed that the spectral peaks in V<sub>op</sub>～t figure correspond to the turning points on the polarization curve. This work展开更多
The electrochemical nitrogen reduction reaction(NRR)to directly produce NH3 from N_(2) and H_(2)O under ambient conditions has attracted significant attention due to its ecofriendliness.Nevertheless,the electrochemica...The electrochemical nitrogen reduction reaction(NRR)to directly produce NH3 from N_(2) and H_(2)O under ambient conditions has attracted significant attention due to its ecofriendliness.Nevertheless,the electrochemical NRR presents several practical challenges,including sluggish reaction and low selectivity.Here,bi-atom catalysts have been proposed to achieve excellent activity and high selectivity toward the electrochemical NRR by Ma and his co-workers.It could accelerate the kinetics of N_(2)-to-NH_(3) electrochemical conversion and possess better electrochemical NRR selectivity.This work sheds light on the introduction of bi-atom catalysts to enhance the performance of the electrochemical NRR.展开更多
The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are u...The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.展开更多
A single-sweep oscillopolarographic procedure is descrital which allows detethenahon of rateconstants for reachons of oH. For a wide range of compounds, the results fit well with rate constantspreviously obtained with...A single-sweep oscillopolarographic procedure is descrital which allows detethenahon of rateconstants for reachons of oH. For a wide range of compounds, the results fit well with rate constantspreviously obtained with other methods. Rate constants for reactions of six kinds of active compoundscontalned in rheum, a tradihonal Chinese herb, have been deteboned by this method. Rcationmechanism ha5 also been discussed.展开更多
The electrocatalytic conversion of reactive nitrogen species to ammonia is a promising strategy for efficient NH_(3) synthesis.In this study,we reveal that the hybrid Cu^(+)/Cu~0 interface is catalytically active for ...The electrocatalytic conversion of reactive nitrogen species to ammonia is a promising strategy for efficient NH_(3) synthesis.In this study,we reveal that the hybrid Cu^(+)/Cu~0 interface is catalytically active for electrochemical ammonia synthesis from nitrate reduction.To maintain the hybrid Cu^(+)/Cu~0 state at negative reaction potentials,hydrophilic zeolite is used to modify Cu/Cu_(2)O electrocatalyst,which demonstrates an impressive NH_(3) production rate of 41.65 mg h^(-1) cm^(-2)with ~100% Faradaic efficiency of ammonia synthesis at-0.6 V vs.RHE.In-situ Raman spectroscopy unveil the high activity originates from the zeolite reconstruction at the electrode–electrolyte interface,which protects the valence state of Cu~0/Cu^(+) site under negative potential and promotes electrochemical activity towards NH_(3) synthesis.展开更多
Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to i...Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.展开更多
Owing to the rapidly increasing consumption of fossil fuels,finding clean and reliable new energy sources is of the utmost importance.Thus,developing highly efficient and low-cost catalysts for electrochemical reactio...Owing to the rapidly increasing consumption of fossil fuels,finding clean and reliable new energy sources is of the utmost importance.Thus,developing highly efficient and low-cost catalysts for electrochemical reactions in energy conversion devices is crucial.Single-atom catalysts(SACs)with maximum metal atom utilization efficiency and superior catalytic performance have attracted significant attention,especially for electrochemical reactions.However,because of the highly unsaturated coordination environment,the stability of SACs can be a challenge for practical applications.In this review,we will summarize the strategies to increase the stability of SACs and synthesizing stable SACs,as well as the application of SACs in electrochemical reactions.Finally,we offer a perspective on the development of advanced SACs through rational design and a deeper understanding of SACs with the help of in situ or operando techniques in electrochemical reactions.展开更多
Non-noble metal electrocatalysis has witnessed rapid and profound performance improvements owing to the emergence of advanced nanosynthetic techniques.Integration of these nanotechniques can lead to synergistic perfor...Non-noble metal electrocatalysis has witnessed rapid and profound performance improvements owing to the emergence of advanced nanosynthetic techniques.Integration of these nanotechniques can lead to synergistic performance enhancement,but such system-engineering strategies are difficult to achieve because of the lack of effective synthesis method.We hereby demonstrate an integrated approach that combines most of the existing nanotechniques in a facile one-pot synthesis.Material characterization reveals that the product shows key features intended by techniques including morphological,structural,doping,heterointerface,and surface wetting engineering.The as-obtained nitrogen-doped hierarchical heterostructured MoS_(x)/Ni_(3)S_(2)nanowires show an overpotential that is only50 mV higher than commercial Pt/C for hydrogen evolution reaction over current densities from 10 to 150 mA cm^(-2).Correlations between the adopted nanotechniques and the electrochemical reaction rates are established by evaluating the impacts of individual techniques on the activation energy,pre-exponential factor,and transfer coefficient.This indepth analysis provides a full account of the synergistic effects and the overall improvement in electrocatalytic performance of hydrogen evolution reaction.This work manifests a generic strategy for multipurpose material design in non-noble metal electrocatalysis.展开更多
The interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes is a serious problem,leading to poor electrochemical properties of all-solid-state lithium batteries(ASSLB).The chemical/elec...The interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes is a serious problem,leading to poor electrochemical properties of all-solid-state lithium batteries(ASSLB).The chemical/electrochemical side reactions are considered to be the origin of the interfacial deterioration.However,the influence of chemical and electrochemical side reactions on the interfacial deterioration is rarely studied specifically.In this work,the deterioration mechanism of the interface between LiNi0.85-xCo0.15AlxO2 and Li10GeP2S12 is investigated in detail by combining in/ex-situ Raman spectra and Electrochemical Impedance Spectroscopy(EIS).It can be determined that chemical side reaction between LiNi0.8Co0.15Al0.05O2 and Li10GeP2S12 will occur immediately once contacted,and the interfacial deterioration becomes more serious after charge-discharge process under the dual effects of chemical and electrochemical side reactions.Moreover,our research reveals that the interfacial stability and the cycle performance of ASSLB can be greatly enhanced by increasing Al-substitution for Ni in LiNi0.85-xCo0.15AlxO2.In particular,the capacity retention of LiNi0.6Co0.15Al0.25O2 cathode after 200 cycles can reach 81.9%,much higher than that of LiNi0.8Co0.15Al0.05O2 cathode(12.5%@200 cycles).This work gives an insight to study the interfacial issues between Ni-rich layered oxide cathode and sulfide electrolyte for ASSLBs.展开更多
Developing efficient and low-cost electrocatalysts is essential for the electroreduction of N_(2) to NH_(3).Here,highly monodispersed MoO_(3) clusters loaded on a coral-like CeO_(x)compound with abundant oxygen vacanc...Developing efficient and low-cost electrocatalysts is essential for the electroreduction of N_(2) to NH_(3).Here,highly monodispersed MoO_(3) clusters loaded on a coral-like CeO_(x)compound with abundant oxygen vacancies are successfully prepared by an impregnation-reduction method.The MoO_(3) clusters with small sizes of 2.6±0.5 nm are induced and anchored by the oxygen vacancies of CeO_(x),resulting in excellent nitrogen reduction reaction(NRR)performance.Additionally,the synergistic effects between MoO_(3) and CeO_(x)lead to a further improvement of the electrochemical performance.The as-prepared MoO_(3)-CeO_(x)catalyst shows an NH_(3) yield rate of 32.2 μg h^(-1) mg^(-1) cat and a faradaic efficiency of 7.04%at-0.75 V(vs.reversible hydrogen electrode)in 0.01 M Dulbecco’s Phosphate Buffered Saline.Moreover,it displays decent electrochemical stability over 30,000 s.Besides,the electrochemical NRR mechanism for MoO_(3)-CeO_(x)is investigated by in-situ Fourier transform infrared spectroscopy.N-H stretching,H-N-H bending,and N-N stretching are detected during the reaction,suggesting that an associative pathway is followed.This work provides an approach to designing and synthesizing potential electrocatalysts for NRR.展开更多
Electrochemical CO_(2) reduction(eCO_(2)RR) is an emerging strategy to address the global carbon balance issues and fulfill the carbon-neutral goal through converting CO_(2) to value-added chemicals/fuels driven by re...Electrochemical CO_(2) reduction(eCO_(2)RR) is an emerging strategy to address the global carbon balance issues and fulfill the carbon-neutral goal through converting CO_(2) to value-added chemicals/fuels driven by renewable energy sources. The production of highly reduced carbon compounds beyond CO and formate, especially oxygenate alcohol products with high energy densities and large global market capacities, is particularly desirable for practical applications. However, the building of alcohol-selective e CO_(2)RR electrocatalysis systems to overcome the high overpotential and poor durability remains a big challenge.Recently, diverse strategies have been developed for rational catalyst design towards alcohol productions from e CO_(2)RR on the basis of the corresponding reaction mechanisms. In this review article, we firstly highlight recent advances in fundamental understanding of mechanisms in three electrochemical CO_(2)-alcohol reaction pathways. Then, the design strategies focused on catalyst and interface design are summarized for building alcohol-selective e CO_(2)RR electrocatalysis systems. The advanced characterization techniques are also discussed to provide more insights into e CO_(2) RR-to-alcohols processes. Finally, the remaining challenges and perspectives for promoting e CO_(2)RR to alcohols are proposed.展开更多
The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high c...The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.展开更多
Electrocatalytic CO_(2)reduction reaction(CO_(2)RR),driven by clean electric energy such as solar and wind,can not only alleviate environmental greenhouse effect stemming from excessive CO_(2)emissions,but also realiz...Electrocatalytic CO_(2)reduction reaction(CO_(2)RR),driven by clean electric energy such as solar and wind,can not only alleviate environmental greenhouse effect stemming from excessive CO_(2)emissions,but also realize the storage of renewable energy,for it guarantees the production of value-added chemicals and fuels.Among CO_(2)RR products,formic acid shows great advantages in low energy consumption and high added-value,and thus producing formic acid is generally considered as a profitable line for CO_(2)RR.Bismuth-based electrocatalysts exhibit high formic acid selectivity in CO_(2)RR.Herein,we review the recent progress in bismuth-based electrocatalysts for CO_(2)RR,including material synthesis,performance optimization/validation,and electrolyzers.The effects of morphologies,structure,and composition of bismuth-based electrocatalysts on CO_(2)RR performance are highlighted.Simultaneously,in situ spectroscopic characterization and DFT calculations for reaction mechanism of CO_(2)RR on Bi-based catalysts are emphasized.The applications and optimization of electrolyzers with high current density for CO_(2)RR are summarized.Finally,conclusions and future directions in this field are prospected.展开更多
The development of inexpensive metal-nitrogen-carbon(M-N-C)catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR)on an industrial scale has come to a standstill.Although the number of related studies and rev...The development of inexpensive metal-nitrogen-carbon(M-N-C)catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR)on an industrial scale has come to a standstill.Although the number of related studies and reviews has grown fast,the complexity of the M-N-C composite has limited researchers to focus on only a few variables and carry out sluggish trial-and-error optimizations in their studies.As a result,the conclusions are drawn only by artificial analysis based on a few orthogonal experimental results.To obtain more general design strategies,we have innovatively introduced machine learning(ML)into this field to address this bottleneck.A standard workflow that comprehensively utilizes different ML algorithms and black-box interpretation methods is proposed for this purpose.Besides predicting CO_(2)RR performance metrics for M-N-C catalysts,such as maximum faradaic efficiency with great accuracy,the ML models have also indicated simple and clear design strategies that would guide future exploration from a data science perspective.Besides,we have also demonstrated the potential of the models in guiding the development of new material systems.We thereby believe that the new research paradigm proposed may accelerate the development of this field soon.展开更多
Electrochemical C–N coupling has generated intense research interest as a promising approach to reduce carbon and nitrogen emissions and store excess renewable electricity in valuable chemicals(e.g.,urea,amides,and a...Electrochemical C–N coupling has generated intense research interest as a promising approach to reduce carbon and nitrogen emissions and store excess renewable electricity in valuable chemicals(e.g.,urea,amides,and amines).In this review,we discuss the emerging trends in electrocatalytic C–N coupling reactions using CO_(2) and inorganic nitrogenous species(i.e.,dinitrogen(N_(2))),nitrate(NO_(2)^(-)),nitrite(NO_(3)^(-)),and ammonia(NH_(3))as raw materials.The related reaction mechanisms and potential design principles for advanced electrocatalysts are outlined.In addition,the effects of different reactors,including H-cells,membrane-based flow reactors,and membrane electrode assembly electrolyzers,on the coupling reactions are emphasized.Finally,the current challenges and future opportunities in this field are described.We aim to provide an up-to-date overview of the electrochemical C–N coupling system to advance progress toward its practical application.展开更多
基金supported by the National Natural Science Foundation of China(U21A20332,52103226,52202275,52203314,and 12204253)the Distinguished Young Scholars Fund of Jiangsu Province(BK20220061)the Fellowship of China Postdoctoral Science Foundation(2021 M702382)。
文摘As an alternative to conventional energy conversion and storage reactions,gas-involved electrochemical reactions,including the carbon dioxide reduction reaction(CO_(2)RR),nitrogen reduction reaction(NRR)and hydrogen evolution reaction(HER),have become an emerging research direction and have gained increasing attention due to their advantages of environmental friendliness and sustainability.Various studies have been designed to accelerate sluggish kinetics but with limited results.Most of them promote the reaction by modulating the intrinsic properties of the catalyst,ignoring the synergistic effect of the reaction as a whole.Due to the introduction of gas,traditional liquid-solid two-phase reactions are no longer applicable to future research.Since gas-involved electrochemical reactions mostly occur at the junctions of gaseous reactants,liquid electrolytes and solid catalysts,the focus of future research on reaction kinetics should gradually shift to three-phase reaction interfaces.In this review,we briefly introduce the formation and constraints of the three-phase interface and propose three criteria to judge its merit,namely,the active site,mass diffusion and electron mass transfer.Subsequently,a series of modulation methods and relevant works are discussed in detail from the three improvement directions of‘exposing more active sites,promoting mass diffusion and accelerating electron transfer’.Definitively,we provide farsighted insights into the understanding and research of three-phase interfaces in the future and point out the possible development direction of future regulatory methods,hoping that this review can broaden the future applications of the three-phase interface,including but not limited to gas-involved electrochemical reactions.
基金supported by the National Natural Science Foundation of China(No.22106081)the Natural Science of Foundation of Shandong Province,China(No.ZR202103040646)+2 种基金the special fund of State Key Joint Laboratory of Environment Simulation and Pollution Control(China)(No.20K09ESPCT)the Major Basic Research Projects of Natural Science Foundation of Shandong Province(China)(No.ZR2020KE025)the Fundamental Research Funds for the Central Universities(China)(No.22120220166).
文摘Heavy particulate matter (PM) pollution and high energy consumption are the bottlenecks of hydrometallurgy, especially in the electrolysis process. Therefore, an urgent need is to explore PM reduction methods with production performance co-benefits. This study presents three PM reduction methods based on controlling operating parameters, i.e., lowering electrolyte temperature, H2SO4 concentration, and current density of the cathode. The optimized conditions were also investigated using the response surface methodology to balance the PM reduction effect and Zn production. The results showed that lowering electrolyte temperature is the most efficient, with an 89.0% reduction in the PM generation flux (GFPM). Reducing H2SO4 concentration led to the minimum side effects on the current efficiency of Zn deposition (CEZn) or power consumption (PC). With the premise of non-deteriorating CEZn and PC, GFPM can be reduced by 86.3% at the optimal condition (electrolyte temperature = 295 K, H2SO4 = 110 g/L, current density = 373 A/m^(2)). In addition, the reduction mechanism was elucidated by comprehensively analyzing bubble characteristics, electrochemical reactions, and surface tension. Results showed that lower electrolyte temperature inhibited the oxygen evolution reaction (OER) and compressed gas volume. Lower H2SO4 concentration inhibited the hydrogen evolution reaction (HER) and reduced electrolyte surface tension. Lower current density inhibited both OER and HER by decreasing the reaction current. The inhibited gas evolutions reduced the microbubbles’ number and size, thereby reducing GFPM. These results may provide energy-efficient PM reduction methods and theoretical hints of exploring cleaner PM reduction approaches for industrial electrolysis.
基金financially supported by the National Nature Science Foundation of China (Nos. 62001097, 22208048)the Provincial Natural Science Foundation Joint Guidance Project (No. LH2020F001)+2 种基金the Young Elite Scientists Sponsorship Program by CAST (No. YESS20210262)the China Postdoctoral Science Foundation-Funded Project (No. 2021M690571)the Heilongjiang Postdoctoral Fund (No. LBH-Z21096)
文摘Mass transfer can tune the surface concentration of reactants and products and subsequently infl uence the catalytic perfor-mance.The morphology of nanomaterials plays an important role in the mass transfer of reaction microdomains,but related studies are lacking.Herein,a facile electrospinning technique utilizing cellulose was employed to fabricate a series of carbon nanofi bers with diff erent diameters,which exhibited excellent electrochemical nitrate reduction reaction and oxygen evolu-tion reaction activities.Furthermore,the microstructure of electrocatalysts could infl uence the gas-liquid-solid interfacial mass transfer,resulting in diff erent electrochemical performances.
基金Financial supports from the Beijing Natural Science Foundation(No.Z200012)National Natural Science Foundation of China(Nos.22075290,21972068,21776292 and 21706265)State Key Laboratory of Multiphase Complex Systems,Institute of Process Engineering,Chinese Academy of Sciences(No.MPCS-2019-A-09)。
文摘Heterogeneous nanostructures that are defined as a hybrid structure consisting of two or more nanoscale domains with distinct chemical compositions or physical characteristics have attracted intense efforts in recent years.In this review,we focus on the introduction of a number of heterogeneous nanostructures derived using core-shell Ag-Pt nanoparticles as starting materials,including hollow,dimeric and composite structures and also highlight their application in catalyzing electrochemical reactions,e.g.,methanol oxidation reaction and oxygen reduction reaction.This review not only shows the capability of core-shell Ag-Pt nanoparticles in producing various heterogeneous nanostructures as starting templates,but also highlights the structural design or electronic interaction that endows the heterogeneous nanostructures with enhanced catalytic properties either in methanol oxidation or in oxygen reduction.Further,we also make some perspectives for more heterogeneous nanostructures that may be prepared by using core-shell Ag-Pt particles or their derivatives so as to offer the readers the opportunities and challenges in this field.
基金the support of Project Supported by Keypoint Research and Invention in Shaanxi Province of China(No.2020GY-270)Service local special plan project of Education Department of Shaanxi Province(No.19JC009)。
文摘Zn_(2)Ti_(3)O_(8),as a new type of anode material for lithium-ion batteries,is attracting enormous attention because of its low cost and excellent safety.Though decent capacities have been reported,the electrochemical reaction mechanism of Zn_(2)Ti_(3)O_(8)has rarely been studied.In this work,a porous Zn_(2)Ti_(3)O_(8)anode with considerably high capacity(421 mAh/g at 100 mA/g and 209 mAh/g at 5000 mA/g after 1500 cycles)was reported,which is even higher than ever reported titanium-based anodes materials including Li_(4)Ti_(5)O_(12),TiO_(2)and Li_(2)ZnTi_(3)O_(8).Here,for the first time,the accurate theoretical capacity of Zn_(2)Ti_(3)O_(8)was confirmed to be 266.4 mAh/g.It was also found that both intercalation reaction and pseudocapacitance contribute to the actual capacity of Zn_(2)Ti_(3)O_(8),making it possibly higher than the theoretical value.Most importantly,the porous structure of Zn_(2)Ti_(3)O_(8)not only promotes the intercalation reaction,but also induces high pseudocapacitance capacity(225.4 mAh/g),which boosts the reversible capacity.Therefore,it is the outstanding pseudocapacitance capacity of porous Zn_(2)Ti_(3)O_(8)that accounts for high actual capacity exceeding the theoretical one.This work elucidates the superiorities of porous structure and provides an example in designing high-performance electrodes for lithium-ion batteries.
文摘IN the study of antigen and antibody reaction with ellipsometric spectroscopy, most researchers calculated the thickness of antibody film, absorbance and film constant by mathematic models.But by using simple mathematic models, it is very hard to describe accurately the real state of the system. Huang and Ord proposed a new physical measurement (optical tracking rate,V<sub>op</sub>), indicating the total change of △, Ψ in study of oxidation and reduction reaction of the iron electrode in alkaline solution. Many experimental results showed that the spectral peaks in V<sub>op</sub>～t figure correspond to the turning points on the polarization curve. This work
文摘The electrochemical nitrogen reduction reaction(NRR)to directly produce NH3 from N_(2) and H_(2)O under ambient conditions has attracted significant attention due to its ecofriendliness.Nevertheless,the electrochemical NRR presents several practical challenges,including sluggish reaction and low selectivity.Here,bi-atom catalysts have been proposed to achieve excellent activity and high selectivity toward the electrochemical NRR by Ma and his co-workers.It could accelerate the kinetics of N_(2)-to-NH_(3) electrochemical conversion and possess better electrochemical NRR selectivity.This work sheds light on the introduction of bi-atom catalysts to enhance the performance of the electrochemical NRR.
基金Y.C.and J.C.are contributed equally to the paper.Project supported by the National Natural Science Foundation of China (U19A2017)the Fundamental Research Funds for the Central South University and the Australian Research Council (DP180100731 and DP180100568)。
文摘The electrochemical carbon dioxide reduction reaction(CO_(2)RR),which can produce value-added chemical feedstocks,is a proton-coupled-electron process with sluggish kinetics.Thus,highly efficient,cheap catalysts are urgently required.Transition metal oxides such as CoO_(x),FeO_(x),and NiO_(x)are low-cost,low toxicity,and abundant materials for a wide range of electrochemical reactions,but are almost inert for CO_(2)RR.Here,we report for the first time that nitrogen doped carbon nanotubes(N-CNT)have a surprising activation effect on the activity and selectivity of transition metal-oxide(MO_(x)where M=Fe,Ni,and Co)nanoclusters for CO_(2)RR.MO_(x)supported on N-CNT,MO_(x)/N-CNT,achieves a CO yield of 2.6–2.8 mmol cm−2 min−1 at an overpotential of−0.55 V,which is two orders of magnitude higher than MO_(x)supported on acid treated CNTs(MO_(x)/O-CNT)and four times higher than pristine N-CNT.The faraday efficiency for electrochemical CO_(2)-to-CO conversion is as high as 90.3%at overpotential of 0.44 V.Both in-situ XAS measurements and DFT calculations disclose that MO_(x)nanoclusters can be hydrated in CO_(2)saturated KHCO_(3),and the N defects of N-CNT effectively stabilize these metal hydroxyl species under carbon dioxide reduction reaction conditions,which can split the water molecules and provide local protons to inhibit the poisoning of active sites under carbon dioxide reduction reaction conditions.
文摘A single-sweep oscillopolarographic procedure is descrital which allows detethenahon of rateconstants for reachons of oH. For a wide range of compounds, the results fit well with rate constantspreviously obtained with other methods. Rate constants for reactions of six kinds of active compoundscontalned in rheum, a tradihonal Chinese herb, have been deteboned by this method. Rcationmechanism ha5 also been discussed.
基金the support from the Fundamental Research Funds for the Central Universities (2022LHJH01-03, 2022ZFJH04, 2022QZJH14)Pioneer R&D Program of Zhejiang Province (2022C03040)+1 种基金the Ecological civilization project, Zhejiang Universitythe support from A Project Supported by Scientific Research Fund of Zhejiang University (XY2022013)。
文摘The electrocatalytic conversion of reactive nitrogen species to ammonia is a promising strategy for efficient NH_(3) synthesis.In this study,we reveal that the hybrid Cu^(+)/Cu~0 interface is catalytically active for electrochemical ammonia synthesis from nitrate reduction.To maintain the hybrid Cu^(+)/Cu~0 state at negative reaction potentials,hydrophilic zeolite is used to modify Cu/Cu_(2)O electrocatalyst,which demonstrates an impressive NH_(3) production rate of 41.65 mg h^(-1) cm^(-2)with ~100% Faradaic efficiency of ammonia synthesis at-0.6 V vs.RHE.In-situ Raman spectroscopy unveil the high activity originates from the zeolite reconstruction at the electrode–electrolyte interface,which protects the valence state of Cu~0/Cu^(+) site under negative potential and promotes electrochemical activity towards NH_(3) synthesis.
基金supported by the Climate Change Response Project (NRF-2019M1A2A2065612)the Brainlink Project (NRF2022H1D3A3A01081140)+3 种基金the NRF-2021R1A4A3027878 and the No. RS-2023-00212273 funded by the Ministry of Science and ICT of Korea via National Research Foundationresearch funds from Hanhwa Solutions Chemicals (1.220029.01)UNIST (1.190013.01)supported by the Institute for Basic Science (IBS-R019-D1)。
文摘Electrochemical N_(2) reduction reaction(eNRR) over Cu-based catalysts suffers from an intrinsically low activity of Cu for activation of stable N_(2) molecules and the limited supply of N_(2) to the catalyst due to its low solubility in aqueous electrolytes.Herein,we propose phosphorus-activated Cu electrocatalysts to generate electron-deficient Cu sites on the catalyst surface to promote the adsorption of N_(2) molecules.The eNRR system is further modified using a gas diffusion electrode(GDE) coated with polytetrafluoroethylene(PTFE) to form an effective three-phase boundary of liquid water-gas N_(2)-solid catalyst to facilitate easy access of N_(2) to the catalytic sites.As a result,the new catalyst in the flow-type cell records a Faradaic efficiency of 13.15% and an NH_(3) production rate of 7.69 μg h^(-1) cm^(-2) at-0.2 V_(RHE),which represent 3.56 and 59.2 times increases from those obtained with a pristine Cu electrode in a typical electrolytic cell.This work represents a successful demonstration of dual modification strategies;catalyst modification and N_(2) supplying system engineering,and the results would provide a useful platform for further developments of electrocatalysts and reaction systems.
基金This study was supported by National Sciences and Engineering Research Council of Canada(NSERC)Canada Research Chair Program(CRC)+2 种基金Canada Foundation for Innovation(CFI)the University of Western OntarioJL was supported by the Chinese Scholarship Council.
文摘Owing to the rapidly increasing consumption of fossil fuels,finding clean and reliable new energy sources is of the utmost importance.Thus,developing highly efficient and low-cost catalysts for electrochemical reactions in energy conversion devices is crucial.Single-atom catalysts(SACs)with maximum metal atom utilization efficiency and superior catalytic performance have attracted significant attention,especially for electrochemical reactions.However,because of the highly unsaturated coordination environment,the stability of SACs can be a challenge for practical applications.In this review,we will summarize the strategies to increase the stability of SACs and synthesizing stable SACs,as well as the application of SACs in electrochemical reactions.Finally,we offer a perspective on the development of advanced SACs through rational design and a deeper understanding of SACs with the help of in situ or operando techniques in electrochemical reactions.
基金financial support from the NSFC(Grant No.21403119)the Science and Technology Bureau of Shenzhen(Grant No.JCYJ20170306171540744)
文摘Non-noble metal electrocatalysis has witnessed rapid and profound performance improvements owing to the emergence of advanced nanosynthetic techniques.Integration of these nanotechniques can lead to synergistic performance enhancement,but such system-engineering strategies are difficult to achieve because of the lack of effective synthesis method.We hereby demonstrate an integrated approach that combines most of the existing nanotechniques in a facile one-pot synthesis.Material characterization reveals that the product shows key features intended by techniques including morphological,structural,doping,heterointerface,and surface wetting engineering.The as-obtained nitrogen-doped hierarchical heterostructured MoS_(x)/Ni_(3)S_(2)nanowires show an overpotential that is only50 mV higher than commercial Pt/C for hydrogen evolution reaction over current densities from 10 to 150 mA cm^(-2).Correlations between the adopted nanotechniques and the electrochemical reaction rates are established by evaluating the impacts of individual techniques on the activation energy,pre-exponential factor,and transfer coefficient.This indepth analysis provides a full account of the synergistic effects and the overall improvement in electrocatalytic performance of hydrogen evolution reaction.This work manifests a generic strategy for multipurpose material design in non-noble metal electrocatalysis.
基金financially supported partly by the National Key Research and Development Program of China(2018YFE0111600)Tianjin Sci.&Tech.Program(17YFZCGX00560,18ZXJMTG00040,19JCZDJC31800)。
文摘The interfacial instability between Ni-rich layered oxide cathodes and sulfide electrolytes is a serious problem,leading to poor electrochemical properties of all-solid-state lithium batteries(ASSLB).The chemical/electrochemical side reactions are considered to be the origin of the interfacial deterioration.However,the influence of chemical and electrochemical side reactions on the interfacial deterioration is rarely studied specifically.In this work,the deterioration mechanism of the interface between LiNi0.85-xCo0.15AlxO2 and Li10GeP2S12 is investigated in detail by combining in/ex-situ Raman spectra and Electrochemical Impedance Spectroscopy(EIS).It can be determined that chemical side reaction between LiNi0.8Co0.15Al0.05O2 and Li10GeP2S12 will occur immediately once contacted,and the interfacial deterioration becomes more serious after charge-discharge process under the dual effects of chemical and electrochemical side reactions.Moreover,our research reveals that the interfacial stability and the cycle performance of ASSLB can be greatly enhanced by increasing Al-substitution for Ni in LiNi0.85-xCo0.15AlxO2.In particular,the capacity retention of LiNi0.6Co0.15Al0.25O2 cathode after 200 cycles can reach 81.9%,much higher than that of LiNi0.8Co0.15Al0.05O2 cathode(12.5%@200 cycles).This work gives an insight to study the interfacial issues between Ni-rich layered oxide cathode and sulfide electrolyte for ASSLBs.
基金financially supported by the National Key Research and Development Program of China(2017YFA0206500)NSFC(Grant Nos.21673198,91934303,21621091)。
文摘Developing efficient and low-cost electrocatalysts is essential for the electroreduction of N_(2) to NH_(3).Here,highly monodispersed MoO_(3) clusters loaded on a coral-like CeO_(x)compound with abundant oxygen vacancies are successfully prepared by an impregnation-reduction method.The MoO_(3) clusters with small sizes of 2.6±0.5 nm are induced and anchored by the oxygen vacancies of CeO_(x),resulting in excellent nitrogen reduction reaction(NRR)performance.Additionally,the synergistic effects between MoO_(3) and CeO_(x)lead to a further improvement of the electrochemical performance.The as-prepared MoO_(3)-CeO_(x)catalyst shows an NH_(3) yield rate of 32.2 μg h^(-1) mg^(-1) cat and a faradaic efficiency of 7.04%at-0.75 V(vs.reversible hydrogen electrode)in 0.01 M Dulbecco’s Phosphate Buffered Saline.Moreover,it displays decent electrochemical stability over 30,000 s.Besides,the electrochemical NRR mechanism for MoO_(3)-CeO_(x)is investigated by in-situ Fourier transform infrared spectroscopy.N-H stretching,H-N-H bending,and N-N stretching are detected during the reaction,suggesting that an associative pathway is followed.This work provides an approach to designing and synthesizing potential electrocatalysts for NRR.
基金supported by the National Natural Science Foundation of China(Grant No.51972191)the National Key Research and Development Program of China(Grant No.2021YFA1200800)。
文摘Electrochemical CO_(2) reduction(eCO_(2)RR) is an emerging strategy to address the global carbon balance issues and fulfill the carbon-neutral goal through converting CO_(2) to value-added chemicals/fuels driven by renewable energy sources. The production of highly reduced carbon compounds beyond CO and formate, especially oxygenate alcohol products with high energy densities and large global market capacities, is particularly desirable for practical applications. However, the building of alcohol-selective e CO_(2)RR electrocatalysis systems to overcome the high overpotential and poor durability remains a big challenge.Recently, diverse strategies have been developed for rational catalyst design towards alcohol productions from e CO_(2)RR on the basis of the corresponding reaction mechanisms. In this review article, we firstly highlight recent advances in fundamental understanding of mechanisms in three electrochemical CO_(2)-alcohol reaction pathways. Then, the design strategies focused on catalyst and interface design are summarized for building alcohol-selective e CO_(2)RR electrocatalysis systems. The advanced characterization techniques are also discussed to provide more insights into e CO_(2) RR-to-alcohols processes. Finally, the remaining challenges and perspectives for promoting e CO_(2)RR to alcohols are proposed.
基金supported by the National Natural Science Foundation of China (NSFC)(22075201)the National Key Research and Development Program of China (2022YFB4101800)。
文摘The electrochemical CO_(2)reduction reaction to produce multi-carbon(C_(2+)) hydrocarbons or oxygenate compounds is a promising route to obtain a renewable fuel of high energy density.However,producing C_(2+)at high current densities is still a challenge.Herein,we develop a Cu-Zn alloy/Cu-Zn aluminate oxide composite electrocatalytic system for enhanced conversion of CO_(2)to C_(2+)products.The Cu-Zn-Al-Layered Double Hydroxide(LDH) is used as a precursor to decompose into uniform Cu-Zn oxide/Cu-Zn aluminate pre-catalyst.Under electrochemical reduction,Cu-Zn oxide generates Cu-Zn alloy while Cu-Zn aluminate oxide remains unchanged.The alloy and oxide are closely stacked and arranged alternately,and the aluminate oxide induces the strong electron interaction of Cu,Zn and Al,creating a large number of highly active reaction interfaces composed of 0 to+3 valence metal sites.With the help of the interface effect,the optimized Cu_(9)Zn_(1)/Cu_(0.8)Zn_(0.2)Al_(2)O_(4)catalyst achieves a Faradaic efficiency of 88.5% for C_(2+)products at a current density of 400 mA cm^(-2)at-1.15 V versus reversible hydrogen electrode.The in-situ Raman and attenuate total reflectance-infrared absorption spectroscopy(ATR-IRAS) spectra show that the aluminate oxide at the interface significantly enhances the adsorption and activation of CO_(2)and the dissociation of H2O and strengthens the adsorption of CO intermediates,and the alloy promotes the C-C coupling to produce C_(2+)products.This work provides an efficient strategy to construct highly active reaction interfaces for industrial-scale electrochemical CO_(2)RR.
基金This work was financially supported by grants from the National Key Research and Development Program of China(2021YFA1501504)Natural Science Foundation of China(22172135,22288102,92045302,and 22021001).
文摘Electrocatalytic CO_(2)reduction reaction(CO_(2)RR),driven by clean electric energy such as solar and wind,can not only alleviate environmental greenhouse effect stemming from excessive CO_(2)emissions,but also realize the storage of renewable energy,for it guarantees the production of value-added chemicals and fuels.Among CO_(2)RR products,formic acid shows great advantages in low energy consumption and high added-value,and thus producing formic acid is generally considered as a profitable line for CO_(2)RR.Bismuth-based electrocatalysts exhibit high formic acid selectivity in CO_(2)RR.Herein,we review the recent progress in bismuth-based electrocatalysts for CO_(2)RR,including material synthesis,performance optimization/validation,and electrolyzers.The effects of morphologies,structure,and composition of bismuth-based electrocatalysts on CO_(2)RR performance are highlighted.Simultaneously,in situ spectroscopic characterization and DFT calculations for reaction mechanism of CO_(2)RR on Bi-based catalysts are emphasized.The applications and optimization of electrolyzers with high current density for CO_(2)RR are summarized.Finally,conclusions and future directions in this field are prospected.
基金This work was partially supported by the National Natural Science Foundation of China(Nos.22125205 and 92045302).
文摘The development of inexpensive metal-nitrogen-carbon(M-N-C)catalysts for electrochemical CO_(2)reduction reaction(CO_(2)RR)on an industrial scale has come to a standstill.Although the number of related studies and reviews has grown fast,the complexity of the M-N-C composite has limited researchers to focus on only a few variables and carry out sluggish trial-and-error optimizations in their studies.As a result,the conclusions are drawn only by artificial analysis based on a few orthogonal experimental results.To obtain more general design strategies,we have innovatively introduced machine learning(ML)into this field to address this bottleneck.A standard workflow that comprehensively utilizes different ML algorithms and black-box interpretation methods is proposed for this purpose.Besides predicting CO_(2)RR performance metrics for M-N-C catalysts,such as maximum faradaic efficiency with great accuracy,the ML models have also indicated simple and clear design strategies that would guide future exploration from a data science perspective.Besides,we have also demonstrated the potential of the models in guiding the development of new material systems.We thereby believe that the new research paradigm proposed may accelerate the development of this field soon.
基金This work was financially supported in part by the National Key R&D Program of China(2020YFA0406103)NSFC(21725102,22122506,91961106,U1832156,22105192,22075267)+4 种基金Strategic Priority Research Program of the CAS(XDPB14)the Open Funding Project of National Key Laboratory of Human Factors Engineering(SYFD062010K)Anhui Provincial Natural Science Foundation(2008085J05)Youth Innovation Promotion Association of CAS(2019444)China Post-doctoral Science Foundation(2021M693065,2021TQ0322).
文摘Electrochemical C–N coupling has generated intense research interest as a promising approach to reduce carbon and nitrogen emissions and store excess renewable electricity in valuable chemicals(e.g.,urea,amides,and amines).In this review,we discuss the emerging trends in electrocatalytic C–N coupling reactions using CO_(2) and inorganic nitrogenous species(i.e.,dinitrogen(N_(2))),nitrate(NO_(2)^(-)),nitrite(NO_(3)^(-)),and ammonia(NH_(3))as raw materials.The related reaction mechanisms and potential design principles for advanced electrocatalysts are outlined.In addition,the effects of different reactors,including H-cells,membrane-based flow reactors,and membrane electrode assembly electrolyzers,on the coupling reactions are emphasized.Finally,the current challenges and future opportunities in this field are described.We aim to provide an up-to-date overview of the electrochemical C–N coupling system to advance progress toward its practical application.
