Electrocatalytic reduction of CO_(2) into fuels and commodity chemicals has emerged as a potential way to balance the carbon cycle and produce reusable carbon fuels.However,the challenges of the competing reaction of ...Electrocatalytic reduction of CO_(2) into fuels and commodity chemicals has emerged as a potential way to balance the carbon cycle and produce reusable carbon fuels.However,the challenges of the competing reaction of hydrogen evolution reaction,low CO_(2) concentration on the catalyst surface and the diversity of products significantly limit the catalytic activity and selectivity.Hereby,metal nanomaterials,protected by surface sta-bilizing ligands,have been widely studied in the field of CO_(2) reduction due to their structural diversity and outstanding physical and chemical properties.Nevertheless,the surface organic ligands may lower the activity of electrocatalysts,while ligand detachment would cause original structure collapse and selectivity reduction.Therefore,the implementation of strategies based on designing nano-metal catalysts to promote CO_(2) reduction from the perspective of metals and ligands has attracted increasing attention.Herein,we highlight the recent studies on the regulation of surface ligands of metal clusters and metal nanoparticles to promote CO_(2) electro-reduction.Meanwhile,we further summarize the relationship between the surface structure of metal nano-catalysts and the catalytic performance for CO_(2) reduction reaction(CO_(2) RR).This mini review offers an inspiration in remaining challenges and future directions on nano-metal catalysts for electrocatalytic CO_(2) RR.展开更多
With the rapid development of economy,the increasing energy crisis and environmental pollution urge us to develop sustainable and clean novel energy systems.Among them,the electrochemical energy conversion technology ...With the rapid development of economy,the increasing energy crisis and environmental pollution urge us to develop sustainable and clean novel energy systems.Among them,the electrochemical energy conversion technology is considered as one of the ideal potential alternative energy systems,and the electrocatalysts play critical roles but are still challenging.Metal-organic frameworks(MOFs),thanks to their regular channels,atomically dispersed active centers,adjustable chemical and pore environments,have severed as promising electrocatalysts for electrochemical energy conversion.However,the relatively low conductivities and instabilities of MOFs limit their wide application in this field.In this case,fabricating hybrids of MOFs and carbon-based materials is an effective way to overcome above deficiencies.In addition,the synergistic effects between MOFs and carbons could optimize the electronic structures of active sites and promote the active surface areas,and thus improve the electrocatalytic performances of the composites.Herein,we outline the current development of MOF/carbon composites,including the fabrication methods of MOFs hybridized with various dimensions of carbon-based materials and the electrocatalysis utilization for water splitting,including the hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and the oxygen reduction reaction(ORR).Finally,the advantages and challenges of such catalysts are highlighted and future endeavors on the development of MOF/carbon composites for the HER,OER and ORR are discussed.展开更多
To design efficient and low-cost core-shell electrocatalysts with an ultrathin platinum shell, the balance between platinum dosage and durability in acid solution is of great importance. In the present work, trimetall...To design efficient and low-cost core-shell electrocatalysts with an ultrathin platinum shell, the balance between platinum dosage and durability in acid solution is of great importance. In the present work, trimetallic Au@PdPt core-shell nanoparticles(NPs)with Pd/Pt molar ratios ranging from 0.31:1 to 4.20:1 were synthesized based on the Au catalytic reduction strategy and the subsequent metallic replacement reaction. When the Pd/Pt molar ratio is 1.19:1(designated as Au@Pd_(1.19) Pt_1 NPs), the superior electrochemical activity and stability were achieved for oxygen reduction reaction(ORR) in acid solution. Especially, the specific and mass activities of Au@Pd_(1.19) Pt_1 NPs are 1.31 and 6.09 times higher than those of commercial Pt/C catalyst. In addition, the Au@Pd_(1.19) Pt_1 NPs presented a good durability in acid solution. After 3000 potential cycles between 0.1 and 0.7 V(vs. Ag/AgCl), the oxygen reduction activity is almost unchanged. This study provides a simple strategy to synthesize highperformance trimetallic ORR electrocatalyst for fuel cells.展开更多
基金supported by the Natural Science Foundation of Guangxi Province(2019GXNSFGA245003,2021GXNSFBA220058)Na-tional Natural Science Foundation of China(Nos.22002026,22272036)and Guangxi Normal University Research Grant(2022TD).
文摘Electrocatalytic reduction of CO_(2) into fuels and commodity chemicals has emerged as a potential way to balance the carbon cycle and produce reusable carbon fuels.However,the challenges of the competing reaction of hydrogen evolution reaction,low CO_(2) concentration on the catalyst surface and the diversity of products significantly limit the catalytic activity and selectivity.Hereby,metal nanomaterials,protected by surface sta-bilizing ligands,have been widely studied in the field of CO_(2) reduction due to their structural diversity and outstanding physical and chemical properties.Nevertheless,the surface organic ligands may lower the activity of electrocatalysts,while ligand detachment would cause original structure collapse and selectivity reduction.Therefore,the implementation of strategies based on designing nano-metal catalysts to promote CO_(2) reduction from the perspective of metals and ligands has attracted increasing attention.Herein,we highlight the recent studies on the regulation of surface ligands of metal clusters and metal nanoparticles to promote CO_(2) electro-reduction.Meanwhile,we further summarize the relationship between the surface structure of metal nano-catalysts and the catalytic performance for CO_(2) reduction reaction(CO_(2) RR).This mini review offers an inspiration in remaining challenges and future directions on nano-metal catalysts for electrocatalytic CO_(2) RR.
基金This work was supported by the Natural Science Foundation of Guangxi Province(Nos.2019GXNSFGA245003 and 2021GXNSFBA220058)the National Natural Science Foundation of China(Nos.22002026 and 22272036)the Guangxi Normal University Research Grant(2022TD).
文摘With the rapid development of economy,the increasing energy crisis and environmental pollution urge us to develop sustainable and clean novel energy systems.Among them,the electrochemical energy conversion technology is considered as one of the ideal potential alternative energy systems,and the electrocatalysts play critical roles but are still challenging.Metal-organic frameworks(MOFs),thanks to their regular channels,atomically dispersed active centers,adjustable chemical and pore environments,have severed as promising electrocatalysts for electrochemical energy conversion.However,the relatively low conductivities and instabilities of MOFs limit their wide application in this field.In this case,fabricating hybrids of MOFs and carbon-based materials is an effective way to overcome above deficiencies.In addition,the synergistic effects between MOFs and carbons could optimize the electronic structures of active sites and promote the active surface areas,and thus improve the electrocatalytic performances of the composites.Herein,we outline the current development of MOF/carbon composites,including the fabrication methods of MOFs hybridized with various dimensions of carbon-based materials and the electrocatalysis utilization for water splitting,including the hydrogen evolution reaction(HER),oxygen evolution reaction(OER),and the oxygen reduction reaction(ORR).Finally,the advantages and challenges of such catalysts are highlighted and future endeavors on the development of MOF/carbon composites for the HER,OER and ORR are discussed.
基金supported by the National Natural Science Foundation of China (21773224, 21633008, 21575134, 11374297, 21405149)the National Key Research and Development Plan (2016YFA0203200)K. C. Wong Education Foundation
文摘To design efficient and low-cost core-shell electrocatalysts with an ultrathin platinum shell, the balance between platinum dosage and durability in acid solution is of great importance. In the present work, trimetallic Au@PdPt core-shell nanoparticles(NPs)with Pd/Pt molar ratios ranging from 0.31:1 to 4.20:1 were synthesized based on the Au catalytic reduction strategy and the subsequent metallic replacement reaction. When the Pd/Pt molar ratio is 1.19:1(designated as Au@Pd_(1.19) Pt_1 NPs), the superior electrochemical activity and stability were achieved for oxygen reduction reaction(ORR) in acid solution. Especially, the specific and mass activities of Au@Pd_(1.19) Pt_1 NPs are 1.31 and 6.09 times higher than those of commercial Pt/C catalyst. In addition, the Au@Pd_(1.19) Pt_1 NPs presented a good durability in acid solution. After 3000 potential cycles between 0.1 and 0.7 V(vs. Ag/AgCl), the oxygen reduction activity is almost unchanged. This study provides a simple strategy to synthesize highperformance trimetallic ORR electrocatalyst for fuel cells.
