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Electroreductive Defluorination Enables 1,1-Deuterocarboxylation of Difluoro-and Trifluoromethylarenes 认领 引用
1
作者 Cheng Zhong Peng Li +4 位作者 Jianye Zhang Mingming Yu Yuan Zhou Aiwen Lei Zhaoliang Yang 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2026年第12期1949-1955,共7页
The defluorination-enabled functionalization not only provides an effective strategy to mitigate fluoride pollution,but also opens new avenues for constructing molecular diversity.Although numerous methods for C-F bon... The defluorination-enabled functionalization not only provides an effective strategy to mitigate fluoride pollution,but also opens new avenues for constructing molecular diversity.Although numerous methods for C-F bond activation have been developed,their applications are typically confined to single defluorination-monofunctionalization processes.Traditional approaches to achieve 1,1-dual modification rely on multistep reaction sequences or precious-metal catalytic systems,which suffer from inefficiency,high cost,and significant environmental burden.In this study,we report the first electroreductive strategy for one-pot 1,1-deuterocarboxylation of C(sp3)-F bonds using cost-effective deuterium oxide(D2O)as the deuterium source and carbon dioxide(CO2)as a sustainable C1 feedstock.This method demonstrates broad substrate compatibility with difluoro-rifluoroalkylarenes and enables late-stage drug functionalization without pre-activation.Mechanistic studies confirmed that the reaction proceeds via a sequential pathway:the substrate undergoes initial reduction at the cathode,reacts with CO2,and then undergoes reduction by deuterium protonation in the presence of D2O,ultimately leading to the formation of the final product. 展开更多
关键词 Electroreductive Defluorination 1,1-Deuterocarboxylation Carboarylation Deuteration Tifluoromethylarenes CO2 D2O
Dynamic evolution of copper-based catalysts during CO2 electroreduction 认领 引用 被引量：3
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作者 Zhizheng Wu Pengpeng Yang Minrui Gao 《Nano Materials Science》 EI CAS CSCD 2026年第3期687-702,共16页
The CO2 electroreduction reaction(CO2RR)is a promising approach of using renewable electricity to synthesize fuels and value-added chemicals.At present,Cu is generally considered to be the major monometallic cat... The CO2 electroreduction reaction(CO2RR)is a promising approach of using renewable electricity to synthesize fuels and value-added chemicals.At present,Cu is generally considered to be the major monometallic catalyst capable of producing multicarbon products(C2+)with high current densities from the CO2RR,but it still suffers from the low activity and high overpotential.The challenge of sluggish CO2RR kinetics can be overcome by developing efficient Cu-based catalysts,which undergo the dynamic evolution during the reaction process.The dynamic evolution of the Cu-based catalysts taking place under working conditions makes it difficult to study the structure-activity correlation and reaction mechanism present during CO2RR.Recently,a number of important works have observed and revealed the dynamic evolution process of Cu-based catalysts by operando characterization techniques.This aspect,however,remains less summarized and prospected in the CO2RR literature.In this Review,we summarize the dynamic evolution of Cu-based catalysts during the CO2RR from aspects of structure,composition and oxidation state.We highlight the correlations between evolution behaviors and catalytic properties.Then,we discuss the dynamic deactivation process of Cu-based catalysts during CO2RR,including metal impurities contamination and carbon accumulation.In particular,we introduce recent advancements in in situ characterization techniques those are employed to probe the dynamic evolution under operating conditions.We end the Review by outlining the challenges and offering personal perspectives on the future development opportunities in this field. 展开更多
关键词 Copper-based catalysts CO2electroreduction reaction Dynamic evolution
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Regulating the proton supply effect on chlorine-doped bismuth for enhanced electroreduction CO2 to formate 认领 引用 被引量：1
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作者 Xiao Li Chaoqiong Fang +1 位作者 Riming Hu Jiayuan Yu 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第1期611-615,共5页
Electrochemical CO2 reduction reaction(CO2RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demons... Electrochemical CO2 reduction reaction(CO2RR) into valuable formate provides a strategy for carbon neutrality.Bismuth(Bi) catalysts,attributed to their appropriate energy barrier of OCHO*intermediate,have demonstrated substantial potential for the advancement of electrocatalytic CO2 reduction to formate.However,due to the weak bonding of protons(H*) of Bi,the available protonate of CO2 on Bi is insufficient,which limits the formation of OCHO*.Prediction by theoretical calculation,chlorine doping can effectively promote the dissociation of H2O and thus achieve effective proton supply.We prepare chlorine-doped Bi(Cl-Bi) via an electrochemical conversion strategy for electroreduction of CO2 .An obvious improvement of faradaic efficiency(FE) of formate(96.7% at-0.95 V vs.RHE) can be achieved on Cl-Bi,higher than that of Bi(89.4%).Meanwhile,Cl-Bi has the highest formate production rate of 275 μmol h-1cm-2at-0.95 V vs.RHE,which is 1.2 times higher than that of Bi(224 μmol h-1cm-2).In situ characterizations and kinetic analysis reveal that chlorine doping promotes the activation of H2O and supply sufficient protons to promote the protonation of CO2 to OCHO*,which is consistent with theoretical calculation.The study presents an effective strategy for rational design of highly efficient electrocatalysts to promote green chemical production. 展开更多
关键词 CO2electroreduction Heteroatom doping Proton supply effect Reaction kinetics Bismuth-based catalysts
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Unraveling in-situ electrochemical reconstruction of indium oxide catalysts with oxygen vacancy for enhanced electrocatalytic CO2-to-formate conversion 认领 引用 被引量：1
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作者 Biao Hong Wei Xiao 《International Journal of Minerals,Metallurgy and Materials》 SCIE EI CAS CSCD 2026年第5期1652-1661,I0174-I0197,共10页
Indium-based materials have emerged as promising alternative catalysts for the selective electroreduction of CO2to formate,yet the optimal catalytic configuration remains elusive.Herein,theoretical calculation reve... Indium-based materials have emerged as promising alternative catalysts for the selective electroreduction of CO2to formate,yet the optimal catalytic configuration remains elusive.Herein,theoretical calculation reveals that metallic indium over oxygen vacancycontaining In2O3support(In/In2O3-VO)possesses the lowest energy barriers(0.99 eV)for CO2reduction to formate.A rational air-annealing strategy applied to In3+-adsorbed resin is developed to synthesize indium oxide catalysts containing oxygen vacancy(R-In2O3).In-situ spectroscopy techniques confirm in-situ electrochemical reconstruction of the In/In2O3configuration and the effective stabilization of the key reaction intermediate(HCOO*).Consequently,the catalyst delivers excellent CO2-to-formate conversion performance,maintaining a current efficiency above 92% over 56 h of galvanostatic electrolysis at-250 mA·cm-2.These insights provide an effective strategy for the rational design of high-performance and durable indium-based electrocatalysts for sustainable formate production. 展开更多
关键词 carbon dioxide electroreduction indium oxide formate active sites energy conversion
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Room-Temperature Electroreductiveα-Alkylation of N-Heteroarenes with Styrenes 认领 引用 被引量：1
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作者 Maorui Wang Chengqian Zhang +3 位作者 He Zhao Huanfeng Jiang Pierre HDixneuf Min Zhang 《CCS Chemistry》 CSCD 2024年第2期342-352,共11页
Despite their interesting applications,direct and diverse syntheses of aryl-fused 2-alkyl cyclic amines still remain challenging.Here,the concept of incorporating a C–C coupling process into the N-heteroaryl reductio... Despite their interesting applications,direct and diverse syntheses of aryl-fused 2-alkyl cyclic amines still remain challenging.Here,the concept of incorporating a C–C coupling process into the N-heteroaryl reduction was successfully applied to fulfill such a synthetic purpose.Due to our use of controllable electroreduction coupled with proton abstraction,we can report a room-temperature reductiveα-alkylation of the inert N-heteroarenes with abundantly available styrenes in an undivided Zn(+)/C(−)cell.This proceeds with good substrate compatibility and operational simplicity,utilizes cost-effective sacrificial Zn-anode,exhibits high selectivity,and does not need pressurized H2 gas and transition-metal catalysts.This current work offers a useful platform for direct construction of valuable aryl-fused 2-alkyl cyclic amines that are difficult to access with conventional methods. 展开更多
关键词 electroreductive C-C cross-coupling N-heteroarenes styrenes 2-alkyl cyclic amines alkylation
Sulfur-engineered Ni single-atom catalysts for sustainable tandem CO2-to-chemicals conversion across pH-universal windows 认领 引用
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作者 Jun-Kang Li Pei-Yao Wang +3 位作者 Jia-Lin Zhang Shu-Na Zhao Bo Li Shuang-Quan Zang 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第7期732-738,共7页
Tandem CO2 electroreduction integrated with carbonylation reactions offers a promising pathway for transforming greenhouse gases into valuable chemical products.The development of efficient CO2-to-CO electrocata... Tandem CO2 electroreduction integrated with carbonylation reactions offers a promising pathway for transforming greenhouse gases into valuable chemical products.The development of efficient CO2-to-CO electrocatalysts operational across wide potential ranges is crucial to address renewable energy fluctuations and facilitate integrated cascade systems.Herein,a Ni single-atom catalyst(SAC)with sulfur doping in the second shell of Ni-N4 is reported.In situ measurements and theoretical calculations demonstrate that the incorporation S atoms not only modulates the electronic configuration of Ni active sites but also enhances H2O adsorption,enabling rapid CO2 hydrogenation into *COOH intermediates even at high potentials.Consequently,the Ni-N-S/CNS catalyst achieves a Faradaic efficiency for CO2-to-CO(FeCO)of 99.3% at-0.7 VRHE and maintains over 90%across pH-universal conditions with ultrawide potential windows:1400 mV(from-0.3 VRHE to-1.7 VRHE)in alkaline media,1200 mV(from-0.7 VRHE to-1.9VRHE)in neutral conditions,and 1000 mV(from-1.3 VRHE to-2.3 VRHE)in acidic environments.Remarkably,this catalyst enables the tandem CO2RR and N-alkylaniline carbonylation process for synthesizing o-aminobenzoates and isatoic anhydrides with high yield.Our findings demonstrate an electrothermocatalytic tandem strategy for cost-effective CO2 conversion and synthesis of high valuable fine chemicals,thereby broadening the scope of its utilization. 展开更多
关键词 Tandem system CO2electroreduction Carbonylation reaction Single atom catalyst Ultrawide potential window
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Catalysts and modification strategies for CO2 capture and in-situ electroreduction 认领 引用
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作者 Qingman Niu Mingzhu Yue +5 位作者 Bingkun Li Lu Liu Wenfu Xie Min Li Tianyu Zhang Qiang Wang 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第3期287-318,共32页
As atmospheric CO2 concentration continues to rise,carbon capture and utilization(CCU)technology has emerged as a critical strategy toward achieving carbon neutrality.CCU offers a dual advantage of mitigating CO_(2... As atmospheric CO2 concentration continues to rise,carbon capture and utilization(CCU)technology has emerged as a critical strategy toward achieving carbon neutrality.CCU offers a dual advantage of mitigating CO2 emissions while producing value-added chemicals and fuels.However,conventional CCU strategies typically decouple the CO2 capture and electrochemical conversion processes,resulting in increased system complexity,higher energy demands,and limited economic viability.Building an integrated system of CO2 capture and in-situ electroreduction can bridge the technological gap,reduce costs,and ultimately enhance carbon cycle efficiency.In this review,we highlight recent advances in CO2 capture and in-situ electroreduction technologies.We first evaluate the strengths and limitations of conventional CCU technologies and the emerging CO2 capture and direct utilization technologies.Subsequently,we summarize the breakthroughs in multifunctional catalyst systems and key catalyst optimization strategies,and analyze the mechanisms behind the performance improvement.Meanwhile,we also discuss the application progress of in-situ techniques and theoretical calculations in CO2 capture and in-situ electroreduction.Finally,we outline the unresolved scientific and engineering challenges and propose future research directions to accelerate the development of CO2 capture and in-situ electroreduction. 展开更多
关键词 CO2capture In-situ electroreduction Carbon capture and utilization Electrocatalysts Optimization strategies Catalytic mechanism
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Rare earth single atom supported on C2N catalysts for electrochemical CO2reduction:A DFT study 认领 引用
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作者 Yu Ren Qiannan Zhou +4 位作者 Xiaofei Song Yangyang Song Zean Xie Xuehua Yu Zhen Zhao 《Journal of Rare Earths》 SCIE EI CAS CSCD 2026年第4期1085-1090,I0004,共6页
The electrochemical CO2reduction reaction(CO2RR)can convert CO2into high value-added chemicals,which is conducive to improving climate change and energy crisis.Rare earth single-atom catalysts(SACs)have recen... The electrochemical CO2reduction reaction(CO2RR)can convert CO2into high value-added chemicals,which is conducive to improving climate change and energy crisis.Rare earth single-atom catalysts(SACs)have recently been widely studied in the field of CO2reduction due to their unique properties.Herein,a series of rare earth single-atom metals(abbreviated as RM,which are Sc,Y,La,Ce,Pr,Nd,Sm,Eu,Gd,Tb,Dy,Ho,Er,Tm,Yb,Lu)supported on C2N were designed and systematically studied for their CO2RR performance.Results show that CH4is the main product on RM@C2N and the limiting potentials are in range of-0.46 to-0.61 V except for Eu@C2N and Yb@C2N.Among them,Tb@C2N,Sm@C2N,and Gd@C2N show high activity and selectivity with limiting potentials of-0.46,-0.47,and-0.48 V.The binding energy of adsorbed oxygen atoms on rare earth SACs can be used as a good descriptor of activity from volcano plot.These results provide insights into the design of rare earth catalysts for CO2RR and valuable guidance for screening single-atom catalysts in theory. 展开更多
关键词 CO2electroreduction Single-atom catalysts Rare earths Density functional theory C2N
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Molecular proton-reservoir interfaces directing CO2electroreduction toward methane 认领 引用
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作者 Jing Zhang Lin Yang +7 位作者 Zi-Yuan Dong Hai-wen Chen Jin-Yu Ye Jun Chen Peng-Xiang Lin Jun-Tao Li Zhao-Yu Jin Yao Zhou 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第7期892-903,I0021,共12页
Precise control over the reaction pathway of the electrochemical CO2reduction reaction(eCO2RR)remains challenging,particularly under alkaline conditions where interfacial proton activity is intrinsically low.Her... Precise control over the reaction pathway of the electrochemical CO2reduction reaction(eCO2RR)remains challenging,particularly under alkaline conditions where interfacial proton activity is intrinsically low.Here,we demonstrate that Cu-based coordination polymers bearing polar functional groups function as molecular proton-reservoir interfaces that deterministically steer Cu2O toward methane production.In situ interfacial pH measurements and spectroscopic analyses show that these functional groups undergo a reversible protonation-deprotonation cycle:they can accumulate protons prior to electrolysis and subsequently release them during rapid proton depletion induced by eCO2RR and competing hydrogen evolution reaction(HER).Their conjugate-base forms further extract protons from the electrical double layer,leading to sustained proton enrichment on the Cu2O surface.Concurrently,their strong polarity reorganizes the interfacial hydrogen-bonding network,enhancing proton transport kinetics.This combined molecular-level proton buffering and hydrogen-bond network reinforcement significantly increase the local proton chemical potential,enabling deep hydrogenation of*CO and suppressing C-C coupling.Consequently,Cu2O-polymer interfaces achieve high CH4 selectivity at industrial current densities(Cu2O@CuTAB exhibits a methane Faradaic efficiency of 61%at-400 mA/cm2with a CH4/C2H4 ratio of 6.4),whereas bare Cu2O predominantly yields C2H4.These results establish molecular proton-reservoir interfaces as an effective means to modulate interfacial reaction environments and provide a mechanistic foundation for directing alkaline eCO2RR toward methane. 展开更多
关键词 CO2electroreduction Proton reservoir Interfacial pH CO2to methane conversion
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Synergistic confinement and alloying effects in Pd-based catalysts for efficient and stable CO2reduction 认领 引用
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作者 Yujun Cheng Xi Li +6 位作者 Ziyi Gao Yao Yao Chuan Long Jiasi Zuo Haikun Xu Qi Liu Xiaoqing Chen 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第7期1-11,I0002,共11页
Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limi... Palladium(Pd)has long been constrained as a potential catalyst for CO2reduction reactions(CO2RR)due to significant deactivation caused by strongly adsorbed carbonaceous intermediates on its surface,severely limiting its catalytic activity and stability.To address this critical bottleneck,this study proposes and implements a synergistic regulation strategy combining alloying and spatial confinement effects.This approach designs a composite catalyst by encapsulating boron-silver co-doped palladium alloy nanoparticles(B-Ag4Pd6)within hollow porous resin carbon spheres(HPRCS).In an H-cell,this catalyst achieved a CO Faradaic efficiency of 96.19%at jCO=24.8 mA/cm2 and maintained stable performance for 80 h.Even under flow cell conditions,it sustained 91.23%CO selectivity at jCO=157.86 mA/cm2 over 60 h.Experimental comparisons confirmed the significant promoting effect of spatial confinement on CO2RR.Furthermore,in situ ATR-FTIR spectroscopy and density functional theory(DFT)calculations reveal that B/Ag alloying downshifts the Pd d-band center,optimizes(*)^COOH and(*)^CO adsorption,and the confined Hmicroenvironment accelerates CO formation while suppressing hydrogen evolution.This study not only successfully addressed the issue of carbon intermediate poisoning on Pd surfaces through alloying and microenvironmental regulation,but also provides novel insights and approaches for designing high-performance CO2RR catalysts that integrate electronic structure control with microenvironmental engineering. 展开更多
关键词 CO2electroreduction Pd‑based alloy catalysts Confinement effect Interfacial microenvironment engineering
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Carboxylated Carbon Nanotube-Supported Copper-Indium Bimetallic Catalysts for Electroreduction of CO2 to Dimethyl Carbonate via Membrane-Free Cascade Electrosynthesis 认领 引用
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作者 Youjia Wang Xin Ma +4 位作者 Yuxin Tian Wenchao Wang Bochen Tian Yansheng Liu Junwei Hou 《Carbon and Hydrogen》 SCIE CAS CSCD 2026年第2期226-243,共18页
Under the background of the dual carbon strategy,upgrading CO2 electroreduction from C1 products to high-value C3 esters is an important direction for realizing its resource utilization and valorization.In this wor... Under the background of the dual carbon strategy,upgrading CO2 electroreduction from C1 products to high-value C3 esters is an important direction for realizing its resource utilization and valorization.In this work,Cu100In50 bimetallic catalysts supported on carboxylated carbon nanotubes were prepared,and a membrane-free paired electrolytic cell cascade system was constructed to achieve the directional conversion of CO2→CO→dimethyl carbonate(DMC).The catalyst exhibits enhanced CO supply and interfacial mass transfer capability,with the number of CO adsorption sites increased by 1.8 times and the methanol contact angle reduced from 22°to 8°.Electrochemical measurements show that the catalyst achieves a CO Faraday efficiency(FECO)of 60.9%at−1.8 V versus Ag/AgCl,whereas the FEH2 remains as low as 2.1%.In the cascade reaction,the FEDMC reaches 52.3%at−2.2 V and remains at 49.6%after 5 cycles.The system can also be extended to the electrosynthesis of diethyl carbonate(DEC),giving a FEDEC of 27.8%.In situ Raman spectroscopy combined with DFT calculations reveals that In doping shifts the d-band center of Cu by 0.38 eV,regulates the adsorption behavior of key intermediates,and suppresses HER,whereas carboxyl groups optimize the interfacial electronic structure and mass transfer behavior.This work provides an efficient catalytic strategy and mechanistic insight for the cascade valorization of CO2 into high-value carbonates. 展开更多
关键词 carboxylated carbon nanotubes cascade reaction CO2electroreduction copper-indium bimetallic catalyst DFT dimethyl carbonate insitu Raman spectroscopy
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Optimizing CO production in electrocatalytic CO2 reduction via electron accumulation at Ni sites in Ni3ZnC0.7/Ni on N-doped carbon nanofibers 认领 引用
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作者 Min Wang Ge Bai +6 位作者 Luwei Peng Lulu Li Yadan Yu Wenyi Li Nianjun Yang Daniil I.Kolokolove Jinli Qiao 《Green Energy & Environment》 SCIE EI CAS CSCD 2026年第1期258-268,共11页
The electrocatalytic reduction of carbon dioxide(CO2RR)to valuable products presents a promising solution for addressing global warming and enhancing renewable energy storage.Herein,we construct a novel Ni3ZnC_(... The electrocatalytic reduction of carbon dioxide(CO2RR)to valuable products presents a promising solution for addressing global warming and enhancing renewable energy storage.Herein,we construct a novel Ni3ZnC0.7/Ni heterostructure electrocatalyst,using an electrospinning strategy to prepare metal particles uniformly loaded on nitrogen-doped carbon nanofibers(CNFs).The incorporation of zinc(Zn)into nickel(Ni)catalysts optimizes the adsorption of CO2intermediates,balancing the strong binding affinity of Ni with the comparatively weaker affinity of Zn,which mitigates over-activation.The electron transfer within the Ni3ZnC0.7/Ni@CNFs system facilitates rapid electron transfer to CO2,resulting in great performance with a faradaic efficiency for CO(FECO)of nearly 90%at−0.86 V versus the reversible hydrogen electrode(RHE)and a current density of 17.51 mA cm−2at−1.16 V versus RHE in an H-cell.Furthermore,the catalyst exhibits remarkable stability,maintaining its crystal structure and morphology after 50 h of electrolysis.Moreover,the Ni3ZnC0.7/Ni@CNFs is used in the membrane electrode assembly reactor(MEA),which can achieve a FECO of 91.7%at a cell voltage of−3 V and a current density of 200 mA cm−2 at−3.9 V,demonstrating its potential for practical applications in CO2reduction. 展开更多
关键词 CO2electroreduction CO production Ni3ZnC0.7/Ni Heterostructure Membrane electrode assembly
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Neighboring Ni-Cu dual single-atom sites regulate the local environment of interfacial water for promoting CO2 electroreduction kinetics in CO2-to-CO conversion 认领 引用
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作者 Qi Hao Qi Tang +3 位作者 Junxiu Wu Kai Liu Jun Lu Tianpin Wu 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第8期47-58,共12页
We develop a Ni-Cu dual single-atom catalyst(DSAC)as a model catalyst to investigate the neighboring synergy in dual single-atom sites for promoting the electrocatalytic carbon dioxide reduction reaction(ECO2RR)kin... We develop a Ni-Cu dual single-atom catalyst(DSAC)as a model catalyst to investigate the neighboring synergy in dual single-atom sites for promoting the electrocatalytic carbon dioxide reduction reaction(ECO2RR)kinetics.Through detailed electrochemical tests,in situ spectroscopic observations and theoretical calculations,we found that during ECO2RR,the neighboring Ni-Cu dual single-atom sites synergistically weaken the rigidity of the hydrogen-bond networks of interfacial water and optimize the spatial configuration of water molecules surrounding the Ni-Cu dual single-atom sites,which increases the proportion of easily dissociated water species in the interfacial water,thus accelerating the CO2 protonation kinetics during the conversion of CO2 to CO.As a result,Ni-Cu DSAC exhibits a 1.5-fold increase and a 15-fold increase in ECO2RR activity compared to Ni SAC and Cu SAC,respectively.In flow cell electrolyzer,Ni-Cu DSAC achieves almost 100%Faradaic efficiency for CO production(FECO)from applied current density of 50 to 400 mA cm-2,with the optimal full-cell energy efficiency of 61.1%for CO production,reflecting the excellent catalytic performance of neighboring Ni-Cu dual single-atom sites for selective conversion of CO2 to CO.Benefiting from the efficient suppression of carbonates formation in acidic media,Ni-Cu DSAC achieves an outstanding single-pass carbon efficiency of 67.3%for CO2-to-CO conversion at 200 mA cm-2.Additionally,Ni-Cu DSAC also exhibits excellent long-term stability,with less than 10%decay of FECO throughout a 170-h continuous electrolysis in strong acid(pH=1,j=200 mA cm-2). 展开更多
关键词 CO2electroreduction Neighboring synergistic effect Microenvironment regulation Optimized CO2protonation kinetics Industrial-level current densities
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From fundamental flaw to manageable parameter:Engineering salt precipitation out of acidic CO2RR for industrial viability Author links open overlay panel 认领 引用
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作者 Genxiang Wang Zhiwen Lu Zhenhai Wen 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 2026年第2期5-8,共4页
Salt precipitation remains a persistent barrier to industrial CO2 electrolysis.This Perspective analyzes transformative breakthroughs in acidic systems,elegantly connecting Sargent’s cation-focused interface engin... Salt precipitation remains a persistent barrier to industrial CO2 electrolysis.This Perspective analyzes transformative breakthroughs in acidic systems,elegantly connecting Sargent’s cation-focused interface engineering,Xia’s robust catalysteactor design,and Wang’s revolutionary acid humidification strategy into a cohesive industrial pathway.Based on this,we propose that integrating these approaches,combining acid-humidified feeds with durable catalysts and reactor designs,could establish a scalable route to industrial CO2 electrolysis deployment powered by renewable electricity. 展开更多
关键词 CO2electroreduction Salt deposition Acidic electrolysis Volatile acid humidification Industrial feasibility
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Cl-adsorbed Cu(111)/H2O interface selectively realizes electrochemical CO2reduction towards C2H4 product:Mechanistic understanding 认领 引用
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作者 Lihui Ou Zhancheng Liu +1 位作者 Dai-Huo Liu Zhi Zhang 《Chinese Chemical Letters》 SCIE CAS CSCD 2026年第2期523-528,共6页
Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2to various high value-added C2 products like ethylene and alcohols.However,realizing high selectivity of C2 products are still a ... Cu electrocatalysts have been demonstrated to have unique ability to reduce CO2to various high value-added C2 products like ethylene and alcohols.However,realizing high selectivity of C2 products are still a main challenge due to complex CO2electroreduction pathways and small opportunity of C-C coupling reactions.Here,we found the origin of enhanced CO2electroreduction reaction activity and product selectivity towards C2 products and C-C coupling mechanism at halogen atoms-adsorbed Cu/H2O interfaces,the corresponding CO2electroreduction evolution mechanisms at the halogen atoms-modified Cu/H2O interfaces are systematically studied via theoretical modeling and calculations.The calculated results indicate that halide anions modifications are beneficial to CO dimerization into OCCO dimer,especially Cl--adsorbed Cu(111)/H2O interface has the optimum activity and selectivity towards OCCO dimer,subsequent Cl-adsorbed Cu(111)/H2O interface can selectively reduce CO2into C2H4 product.The function relationship between adsorption free energy of Cl atom and electrode potential explain why the adsorption of Cl-can enhance selectivity of C2H4 product.The determinations of onset potentials indicate that electroreduction pathways of CO2towards C2H4 product are facile to take place and further explain the origin of the significantly enhanced CO production activity and C2H4 product selectivity.This work on selective realization of CO2electroreduction towards C2H4 product via Cl--modified Cu(111)/H2O interface provide a theoretical guideline for how to selectively realize other high value-added C2 products. 展开更多
关键词 CO2 Cl-adsorbed Cu(111)surface C2H4product C-C coupling Selective electroreduction
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Recent progress in bismuth-based materials for electrochemical CO2reduction to formate/formic acid 认领 引用 被引量：3
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作者 Xinrui Linghu Jun Chen +1 位作者 Liangliang Jiang Tianshuai Wang 《Nano Materials Science》 EI CAS CSCD 2026年第4期761-778,共18页
The electrochemical reduction of carbon dioxide(CO2)to formate/formic acid represents a significant pathway for sustainable fuel production,addressing both environmental sustainability and the growing demand for re... The electrochemical reduction of carbon dioxide(CO2)to formate/formic acid represents a significant pathway for sustainable fuel production,addressing both environmental sustainability and the growing demand for renewable energy sources.Recently,bismuth-based(Bi-based)catalysts have attracted significant attention for this field due to their high selectivity,cost-effectiveness,and environmental friendliness.However,a critical challenge remains:developing catalysts that can achieve industrial-scale current density,high Faradaic efficiency,and robust stability simultaneously.Various emerging strategies have been explored to overcome this challenge.This review provides a comprehensive overview of recent advancements in this area.We begin with a discussion of the reaction mechanisms an d theoretical optimization techniques for CO2reduction using Bi-based electrocatalysts.We then highlight recent optimization strategies for designing high-performance Bi-based catalysts,including approaches such as morphology con trol,crystal plane effects,doping engineerin g,interface engineering,and single-atom alloy engineering.Finally,we discuss future research directions for designing Bi-based catalysts capable of operating under industrial conditions for the electroreduction of CO2to formate/formic acid. 展开更多
关键词 CO2electroreduction Bismuth Formate Formic acid Modification strategy
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Surface-immobilized cross-linking tetraalkylammonium cations networks mitigate hydrogen evolution for pure acidic CO2reduction in proton-exchange membrane electrolyzers 认领 引用 被引量：1
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作者 Min Zhang Zengyi Tan +3 位作者 Mufan Xing Yang Wang Xun Zhu Qian Fu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2026年第1期90-96,I0004,共7页
The scaling-up of electrochemical CO2reduction requires circumventing the CO2loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative... The scaling-up of electrochemical CO2reduction requires circumventing the CO2loss as carbonates under alkaline conditions.Zero-gap MEA cell configurations with a proton exchange membrane represent an alternative solution in a pure acidic system,but the catalyst layer in direct contact with the hydrated proton environment usually leads to H2evolution dominating.Herein,we show that polydimethyldiallyl-ammonium-chloride-coated Ag(Ag@PDDA)electrode exhibits outstanding performance with a FE of 86%,a single-pass conversion of 72%,and a stability of 28 h for CO production in pure-acid MEA compared with ammonium poly(N-methyl-piperidine-co-pterphenyl)decorated Ag(Ag/QAPPT)and cetyltrimethylammonium bromide decorated Ag(Ag/CTAB).The in situ ATR-SEIRAS reveal that PDDA creates a positive charge-rich protective outer layer and an N-rich hybrid inner layer,which not only suppresses the migration of H+during the electrolysis process and blocks the direct contact between H2O and Ag catalyst,but also promotes the generation from CO2to*COOH in a pure-acid system.This work highlights the importance of polyelectrolyte engineering in regulating the electrocatalytic interface and accelerates the development of proton exchange membrane CO2electrolysis. 展开更多
关键词 Pure acidic CO2electroreduction Mitigate hydrogen evolution Polyelectrolyte cations MEA electrolyzer
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A Review of CO2 Electroreduction to Ethanol:C-C Coupling Mechanistic Insights and Catalyst Design 认领 引用
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作者 Fang Zhao Bo Huang +3 位作者 Yingzheng Zhang Tianxin Wei Jiatao Zhang Di Zhao 《Nano-Micro Letters》 SCIE EI CAS CSCD 2026年第9期449-486,共38页
As a major contributor to climate change,CO2 has imposed severe detrimental effects on global ecosystems.Among various CO2 conversion strategies,the electrocatalytic CO2 reduction reaction(eCO2RR)stands ou... As a major contributor to climate change,CO2 has imposed severe detrimental effects on global ecosystems.Among various CO2 conversion strategies,the electrocatalytic CO2 reduction reaction(eCO2RR)stands out due to its ability to operate under mild conditions using renewable electricity.Compared to gaseous C2 products such as ethylene,ethanol as a liquid fuel demonstrates greater economic potential and broader market prospects.In recent years,copper-based electrocatalysts have emerged as leading materials for the electrochemical conversion of CO2-to-ethanol.Meanwhile,a number of non-copper-based electrocatalysts have also been developed to produce ethanol via C–C coupling pathways distinct from those on Cu-based materials.However,few reviews have systematically addressed the reaction mechanisms and material design principles specific to ethanol production through eCO2RR.In this review,we highlight the most recent advancements in this field of study.We begin by assessing the economic viability of ethanol as a CO2 reduction product.This is followed by a systematic summary of the reaction mechanisms and advanced characterization methods involved in ethanol production via eCO2RR across various pathways.Next,we discuss and compare the catalytic active sites and key electrochemical performance metrics for ethanol generation on different types of electrocatalysts.Finally,we propose several promising strategies to guide the rational design and synthesis of next-generation high-performance electrocatalysts for selective ethanol production.This review comprehensively summarizes the latest research progress in the field of ethanol production via eCO2RR from multiple dimensions,including the economic value of ethanol,reaction mechanisms,an introduction to various electrocatalysts and strategies for improving electrocatalysts.It not only promotes in-depth basic research,but also provides theoretical guidance for electrocatalyst design,reaction condition optimization,and industrial applications,making it of great research value and practical significance. 展开更多
关键词 CO2electroreduction Ethanol Dynamic mechanism Electrocatalysts Optimization strategy
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Br-doped CuO promotes water dissociation and enables efficient asymmetric C-C coupling during electrochemical reduction of CO2 to ethylene 认领 引用
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作者 Canyan Yang Wei Liu +6 位作者 Zhao Zuo Jinhua Xiao Huawang Zhao Bihong Lv Zuoming Zhou Xiaomin Wu Guohua Jing 《Journal of Environmental Sciences》 SCIE EI CAS CSCD 2026年第7期261-268,共8页
Carbon-carbon(C-C)coupling,the rate-determining step in electrocatalytic CO2reduction reaction(CO2RR)to C2+ products,has low efficiency and poor stability.It originates from an ineffective water dissociation ... Carbon-carbon(C-C)coupling,the rate-determining step in electrocatalytic CO2reduction reaction(CO2RR)to C2+ products,has low efficiency and poor stability.It originates from an ineffective water dissociation capability and a high energy barrier for the C-C coupling pathway on existing catalysts.Herein,an efficient and facile Br-CuO electrocatalyst was synthesized to promote water dissociation and achieve an impressive Faradic Efficiency(FE)of around 60% C2H4 at a current density of up to-350 mA/cm2 with stability of 16 h.Combinative theoretical and experimental protocols strongly evidence that the architecture of Cu0-Cu+ sites is crucial for the enhancement in CO2 RR activity.Cu0 activates CO2and Cu+ strengthens *CO adsorption to further boost C-C coupling.Furthermore,Br doping can facilitate the dissociation of water to generate *H,which promotes the protonation of *CO to *CHO,thereby enabling the low energy barrier asymmetric *CHO-*CO coupling.The in situ ATR-FTIR and Density functional theory(DFT) was analyzed to explain the reaction mechanism and pathway.This study elucidates the critical function of water dissociation and provides a promising avenue to efficient CO2-to-C2H4 electrocatalysis. 展开更多
关键词 Br-doped CuO catalyst Ethylene selectivity CO2electroreduction Water dissociation
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Recent engineering strategies for enhancing C2+product formation in copper-catalyzed CO2electroreduction 认领 引用
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作者 Muhammad Shakir Hussain Sheraz Ahmed +4 位作者 Muhammad Irshad Syeda Sidra Bibi Muhammad Asif Farooq Sher Muhammad Kashif Khan 《Nano Materials Science》 EI CAS CSCD 2026年第1期207-233,共27页
The conversion of carbon dioxide(CO2)into hydrocarbons through electrochemical CO2reduction reaction(eCO2RR)shows a promising method to reduce CO2levels and decrease reliance on fossil fuels in the years t... The conversion of carbon dioxide(CO2)into hydrocarbons through electrochemical CO2reduction reaction(eCO2RR)shows a promising method to reduce CO2levels and decrease reliance on fossil fuels in the years to come.Copper-based electrocatalysts exhibit a pronounced inclination for C-C coupling,drawing considerable interest as a favored metal catalyst for generating C2+products through CO2RR.However,CO2RR still has some obstacles including product selectivity,higher overpotential,low Faradic efficiency(FE),stability,and current density(CD).Therefore,advancement in this field enables us to comprehend the complex multi-proton electron transfer during C-C coupling and engineering strategies to improve FE and CD.Herein,this review presents some key features of Cu-based catalysts as an electrocatalyst for C2 product formation while addressing the industrial challenges that hinder commercialization of CO2RR.In addition,recent strategies on Cu-based catalysts,synthesis strategies,advanced characterizations,and mechanistic investigations via theoretical simulations have been presented.Furthermore,recent approaches towards the composition,oxidation states,and active facets have been presented.Thus,the most favorable mechanism and possible pathways to synthesize C2+products have been explained using theoretical calculations. 展开更多
关键词 Electroreduction Cu-based catalysts C2products Structural engineering Operando techniques
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