Doping heteroatoms into carbon matrix was an efficient strategy to achieve a high-performance non-precious metal oxygen reduction electrocatalyst. Herein, an in situ templated synthesis strategy has been demonstrated ...Doping heteroatoms into carbon matrix was an efficient strategy to achieve a high-performance non-precious metal oxygen reduction electrocatalyst. Herein, an in situ templated synthesis strategy has been demonstrated to fabricate nitrogen, sulfur and iron-tridoped mesoporous carbon nanosheets（NSFC） with FeCl3 as the two-dimensional template. And a protic salt was used as the carbon, nitrogen and sulfur source, which realized one-step preparation of catalyst materials and the co-doping of various heteroatoms simultaneously. As a result, the optimized NSFC catalyst possessed comparable catalytic activity and selectivity, while superior durability and methanol permeability resistance to commercial 30 wt% Pt/C catalyst in alkaline media. Such excellent performance should be ascribed to the efficient multiple-element doping into the large-specific-surface-area and highly stable carbon nanosheets realized by the in situ synthesis route with a novel FeCl3 template.展开更多
The oxygen reduction reaction(ORR)is a cornerstone inelectrochemical energy conversion and chemical synthesis,with its four-electron and two-electron transfer pathwaysserving distinct purposes:efficient fuel cell oper...The oxygen reduction reaction(ORR)is a cornerstone inelectrochemical energy conversion and chemical synthesis,with its four-electron and two-electron transfer pathwaysserving distinct purposes:efficient fuel cell operation andsustainable hydrogen peroxide production,respectively.Akey challenge in ORR is the development of low-cost andefficient electrocatalysts that can achieve selective controlover either the two-electron or four-electron pathway.Car-bonaceous materials have emerged as promising candidatesfor addressing this challenge due to their abundance,highefficiency,and versatile structural tunability.By manipulat-ing the type of heteroatoms or the configuration of defectsin the carbon materials,it is possible to effectively regulateselectivity toward distinct pathways.This review provides anoverview of recent advancements in the design and engi-neering of carbonaceous materials to regulate ORR selectivi-ty,focusing on the three strate gies of heteroatom doping,defect engineering,and their synergistic integration.In theend,we discuss the current challenges and future perspec-tives on advancing the rational design of carbonaceouscatalysts with tailored selectivity for different ORR path-ways.These insights will aid in the development of sustain-able and highly selective electrocatalysts for clean energytechnologies and other industrial applications.展开更多
Controlling the surface structure and composi- tion at the atomic level is an effective way to tune the cat- alytic properties of bimetallic catalysts. Herein, we demon- strate a generalized strategy to synthesize hig...Controlling the surface structure and composi- tion at the atomic level is an effective way to tune the cat- alytic properties of bimetallic catalysts. Herein, we demon- strate a generalized strategy to synthesize highly monodis- perse, surfactant-free octahedral PtxNi1-x nanoparticles with tunable surface structure and composition. With increasing the Ni content in the bulk composition, the degree of concave- ness of the octahedral PtxNi1-x nanoparticles increases. We systematically studied the correlation between their surface structure/composition and their observed oxygen reduction activity. Electrochemical studies have shown that all the octa- hedral PtxNi1-x nanoparticles exhibit enhanced oxygen reduc- tion activity relative to the state-of-the-art commercial Pt/C catalyst. More importantly, we find that the surface struc- ture and composition of the octahedral PtxNi1-x nanoparti- cles have significant effect on their oxygen reduction activ- ity. Among the studied PtxNi1-x nanoparticles, the octahedral PtlNi1 nauoparticles with slight concaveness in its （111） facet show the highest activity. At 0.90 V vs. RHE, the Pt mass and specific activity of the octahedral PhNil nanoparticles are 7.0 and 7.5-fold higher than that of commercial Pt/C catalyst, re- spectively. The present work not only provides a generalized strategy to synthesize highly monodisperse, surfactant-free octahedral PtxNi1-x nanoparticles with tunable surface struc- ture and composition, but also provides insights to the struc- ture-activity correlation.展开更多
基金supported by the National Natural Science Foundation of China(21273114,21771107)Natural Science Foundation of Jiangsu Province(BK20161484)+3 种基金the Fundamental Research Funds for the Central Universities(NE2015003)the "Six Talent Peaks Program" of Jiangsu Province(2013-XNY-010)Project Funded by the Priority Academic Program Development of Jiangsu Higher Education Institutionthe Foundation of Graduate Innovation Center in NUAA(kfjj20160613)~~
文摘Doping heteroatoms into carbon matrix was an efficient strategy to achieve a high-performance non-precious metal oxygen reduction electrocatalyst. Herein, an in situ templated synthesis strategy has been demonstrated to fabricate nitrogen, sulfur and iron-tridoped mesoporous carbon nanosheets（NSFC） with FeCl3 as the two-dimensional template. And a protic salt was used as the carbon, nitrogen and sulfur source, which realized one-step preparation of catalyst materials and the co-doping of various heteroatoms simultaneously. As a result, the optimized NSFC catalyst possessed comparable catalytic activity and selectivity, while superior durability and methanol permeability resistance to commercial 30 wt% Pt/C catalyst in alkaline media. Such excellent performance should be ascribed to the efficient multiple-element doping into the large-specific-surface-area and highly stable carbon nanosheets realized by the in situ synthesis route with a novel FeCl3 template.
基金supported by the National Natural ScienceFoundation of china(grant nos.22405066,22375o67,21925104,922612o4,and 224310o5)the National Key Researchand Development Program of China(grant nos.2022YFA1504703and 2o22YFB4002204)+3 种基金Hubei Provincial Science and TechnologyInnovation Team Project(2o22)the Innovational Fund for Sci-entific and Technological Personnel of Hainan Province(grant no.KJRC2o23C1o)the Princess Nourah bint Abdulrahman Uni-versity Researchers Supporting Project number(grant no.PNURSP2025R398)Princess Nourah bint Abdulrahman Univer-sity,Riyadh,Saudi Arabia.
文摘The oxygen reduction reaction(ORR)is a cornerstone inelectrochemical energy conversion and chemical synthesis,with its four-electron and two-electron transfer pathwaysserving distinct purposes:efficient fuel cell operation andsustainable hydrogen peroxide production,respectively.Akey challenge in ORR is the development of low-cost andefficient electrocatalysts that can achieve selective controlover either the two-electron or four-electron pathway.Car-bonaceous materials have emerged as promising candidatesfor addressing this challenge due to their abundance,highefficiency,and versatile structural tunability.By manipulat-ing the type of heteroatoms or the configuration of defectsin the carbon materials,it is possible to effectively regulateselectivity toward distinct pathways.This review provides anoverview of recent advancements in the design and engi-neering of carbonaceous materials to regulate ORR selectivi-ty,focusing on the three strate gies of heteroatom doping,defect engineering,and their synergistic integration.In theend,we discuss the current challenges and future perspec-tives on advancing the rational design of carbonaceouscatalysts with tailored selectivity for different ORR path-ways.These insights will aid in the development of sustain-able and highly selective electrocatalysts for clean energytechnologies and other industrial applications.
基金supported by the National Research Foundation,Prime Minister’s Office,Singapore under its CREATE Programmefinancial support by the Defence Acquisition Program Administration and Agency for Defence Development(UD120080GD),Republic of Korea
文摘Controlling the surface structure and composi- tion at the atomic level is an effective way to tune the cat- alytic properties of bimetallic catalysts. Herein, we demon- strate a generalized strategy to synthesize highly monodis- perse, surfactant-free octahedral PtxNi1-x nanoparticles with tunable surface structure and composition. With increasing the Ni content in the bulk composition, the degree of concave- ness of the octahedral PtxNi1-x nanoparticles increases. We systematically studied the correlation between their surface structure/composition and their observed oxygen reduction activity. Electrochemical studies have shown that all the octa- hedral PtxNi1-x nanoparticles exhibit enhanced oxygen reduc- tion activity relative to the state-of-the-art commercial Pt/C catalyst. More importantly, we find that the surface struc- ture and composition of the octahedral PtxNi1-x nanoparti- cles have significant effect on their oxygen reduction activ- ity. Among the studied PtxNi1-x nanoparticles, the octahedral PtlNi1 nauoparticles with slight concaveness in its （111） facet show the highest activity. At 0.90 V vs. RHE, the Pt mass and specific activity of the octahedral PhNil nanoparticles are 7.0 and 7.5-fold higher than that of commercial Pt/C catalyst, re- spectively. The present work not only provides a generalized strategy to synthesize highly monodisperse, surfactant-free octahedral PtxNi1-x nanoparticles with tunable surface struc- ture and composition, but also provides insights to the struc- ture-activity correlation.
