The electrocatalytic reduction of carbon dioxide(CO_(2))to multi-carbon(C_(2+))products represents a promising route for sustainable chemical synthesis and carbon neutrality.However,the efficiency and selectivity of C...The electrocatalytic reduction of carbon dioxide(CO_(2))to multi-carbon(C_(2+))products represents a promising route for sustainable chemical synthesis and carbon neutrality.However,the efficiency and selectivity of C-C coupling remain major challenges.This review provides a comprehensive and multidimensional overview of recent advances in enhancing C_(2+)yield through rational catalyst design,reaction environment modulation,and reaction pathway engineering,with a particular emphasis on sustainable strategies.We highlight that atomic-level active site engineering,nanostructure control,support interactions,and heteroatom doping can optimize intermediate adsorption and facilitate C-C coupling.Beyond catalysts,we discuss sustainable reaction systems,including electrolyte optimization,advanced reactor design,and external field assistance that synergistically improve selectivity and energy efficiency.The integration of theoretical simulations and operando characterization offers deep mechanistic insights into dynamic catalyst behavior under working conditions.We further outline future directions for achieving industrially viable and sustainable CO_(2) electroreduction,underscoring the role of interdisciplinary approaches in advancing carbon-neutral technologies.展开更多
Seawater electrolysis for green hydrogen production is a promising approach toward achieving carbon neutrality.However,the abundance of Cl^(−)in seawater can severely corrode catalytic sites,significantly reducing the...Seawater electrolysis for green hydrogen production is a promising approach toward achieving carbon neutrality.However,the abundance of Cl^(−)in seawater can severely corrode catalytic sites,significantly reducing the lifespan of seawater electrolysis systems.Herein,we present metal ion-chelated tannic acid nanoparticles anchored on the CoFe layered double hydroxide nanosheet array on nickel foam(CoFe LDH@CoFe-TA/NF),synthesized via an interfacial coordination assembly method,serving as an efficient and stable electrocatalyst for alkaline seawater oxidation(ASO).The formed CoFe-TA nanoparticles promote the transformation of Co^(3+)into the more robust acid Co^(4+),thereby favoring the adsorption of the hard base OH^(−)rather than the soft base Cl^(−).In addition,the CoFe-TA ligand network effectively inhibits metal ion leaching and stabilizes active sites.As a result,the CoFe LDH@CoFe-TA/NF electrode requires a low overpotential of only 379 mV to obtain a current density of 1000 mA cm^(−2)in 1 M KOH+seawater.Furthermore,the electrode also shows a stable operation for 450 h at an industrial-level current density,underscoring its potential for sustainable energy applications.展开更多
基金supported by the National Natural Science Foundation of China(52272222)Taishan Scholar Young Talent Program(tsqn201909114,tsqn201909123)University Youth Innovation Team of Shandong Province(202201010318).
文摘The electrocatalytic reduction of carbon dioxide(CO_(2))to multi-carbon(C_(2+))products represents a promising route for sustainable chemical synthesis and carbon neutrality.However,the efficiency and selectivity of C-C coupling remain major challenges.This review provides a comprehensive and multidimensional overview of recent advances in enhancing C_(2+)yield through rational catalyst design,reaction environment modulation,and reaction pathway engineering,with a particular emphasis on sustainable strategies.We highlight that atomic-level active site engineering,nanostructure control,support interactions,and heteroatom doping can optimize intermediate adsorption and facilitate C-C coupling.Beyond catalysts,we discuss sustainable reaction systems,including electrolyte optimization,advanced reactor design,and external field assistance that synergistically improve selectivity and energy efficiency.The integration of theoretical simulations and operando characterization offers deep mechanistic insights into dynamic catalyst behavior under working conditions.We further outline future directions for achieving industrially viable and sustainable CO_(2) electroreduction,underscoring the role of interdisciplinary approaches in advancing carbon-neutral technologies.
基金the Deanship of Scientific Research at King Khalid University for funding support through a large group research project under Grant No.RGP2/119/45.
文摘Seawater electrolysis for green hydrogen production is a promising approach toward achieving carbon neutrality.However,the abundance of Cl^(−)in seawater can severely corrode catalytic sites,significantly reducing the lifespan of seawater electrolysis systems.Herein,we present metal ion-chelated tannic acid nanoparticles anchored on the CoFe layered double hydroxide nanosheet array on nickel foam(CoFe LDH@CoFe-TA/NF),synthesized via an interfacial coordination assembly method,serving as an efficient and stable electrocatalyst for alkaline seawater oxidation(ASO).The formed CoFe-TA nanoparticles promote the transformation of Co^(3+)into the more robust acid Co^(4+),thereby favoring the adsorption of the hard base OH^(−)rather than the soft base Cl^(−).In addition,the CoFe-TA ligand network effectively inhibits metal ion leaching and stabilizes active sites.As a result,the CoFe LDH@CoFe-TA/NF electrode requires a low overpotential of only 379 mV to obtain a current density of 1000 mA cm^(−2)in 1 M KOH+seawater.Furthermore,the electrode also shows a stable operation for 450 h at an industrial-level current density,underscoring its potential for sustainable energy applications.
