Metal-based electrocatalysts with different sizes(single atoms,nanoclusters,and nanoparticles)show different catalytic behaviors for various electrocatalytic reactions.Regulating the coordination environment of active...Metal-based electrocatalysts with different sizes(single atoms,nanoclusters,and nanoparticles)show different catalytic behaviors for various electrocatalytic reactions.Regulating the coordination environment of active sites with precision to rationally design an efficient electrocatalyst is of great significance for boosting electrocatalytic reactions.This review summarizes the recent process of heterogeneous supported single atoms,nanoclusters,and nanoparticles catalysts in electrocatalytic reactions,respectively,and figures out the construct strategies and design concepts based on their strengths and weaknesses.Specifically,four key factors for enhancing electrocatalytic performance,including electronic structure,coordination environment,support property,and interfacial interactions are proposed to provide an overall comprehension to readers in this field.Finally,some insights into the current challenges and future opportunities of the heterogeneous supported electrocatalysts are provided.展开更多
Metal-based atomically dispersed catalysts have attracted more attention because of their excellent catalytic performance and nearly 100%atom utilization.Therefore,it is very important to comprehensively and systemati...Metal-based atomically dispersed catalysts have attracted more attention because of their excellent catalytic performance and nearly 100%atom utilization.Therefore,it is very important to comprehensively and systematically understand the relationship between catalytic active sites and catalytic performance at atomic scale.Here,we discuss and summarize in detail the key and fundamental factors affecting the active site,and relate them to the catalytic performance.First,we describe the effectiveness of active site design by coordination effects.Then,the role of chemical bonds in the active sites in changing the reaction performance is discussed.In addition,for intermetallic compounds,we explore how the spacing of active atoms affects the catalytic behavior.Moreover,the importance of synergistic effect in catalyst design is further discussed.Finally,the key parameters affecting the catalytic performance at atomic scale are summarized,and the main challenges and development prospects of atomic catalysts in the future are put forward.展开更多
基金the National Key R&D Program of China(No.2018YFA0702003)the National Natural Science Foundation of China(Nos.21890383 and 21871159)+1 种基金the science and Technology Key Project of Guangdong Province of China(No.2020B010188002)the China Postdoctoral Science Foundation(Nos.2021M691757,2021M690086,and 2021TQ0170).
文摘Metal-based electrocatalysts with different sizes(single atoms,nanoclusters,and nanoparticles)show different catalytic behaviors for various electrocatalytic reactions.Regulating the coordination environment of active sites with precision to rationally design an efficient electrocatalyst is of great significance for boosting electrocatalytic reactions.This review summarizes the recent process of heterogeneous supported single atoms,nanoclusters,and nanoparticles catalysts in electrocatalytic reactions,respectively,and figures out the construct strategies and design concepts based on their strengths and weaknesses.Specifically,four key factors for enhancing electrocatalytic performance,including electronic structure,coordination environment,support property,and interfacial interactions are proposed to provide an overall comprehension to readers in this field.Finally,some insights into the current challenges and future opportunities of the heterogeneous supported electrocatalysts are provided.
文摘作为一种稳定性好、抗辐射能力强、原材料丰富的宽禁带半导体, ZnO在光催化的研究领域中成为热点材料,但是其仅能吸收可见光中的紫光,因此如何扩大ZnO对可见光的响应范围是一个值得研究的问题.掺杂改性是解决这个问题的常用方法.基于以上考量,本文应用第一性原理计算方法研究了N与Pr掺杂对ZnO的电子结构和光学性质的影响.研究结果表明:共掺体系比单掺体系更容易形成,且共掺体系的稳定性随Pr浓度的增加先增强后变弱;同一体系的最短Zn—O键与最长Zn—O键的布居数比例随杂质浓度的增大先增大后减小,说明杂质的掺入对体系的晶格畸变有很大的影响,有利于光生空穴-电子对的分离,从而提高材料的光催化活性. N 2p态与Pr 4f态发生杂化对晶体的完整性产生了破坏,在杂质原子周围形成晶场,造成能级劈裂,带隙减小;介电函数虚部的主峰位均向低能区域移动,吸收光谱中各掺杂体系发生红移,各共掺体系随着杂质原子Pr浓度的增加,在可见光区的响应范围依次扩大,吸收能力也依次增加,说明N与Pr的共掺杂对提高ZnO的光催化性是有利的.
基金the National Natural Science Foundation of China(Nos.22171157,21871159,and 21890383)Science and Technology Key Project of Guangdong Province of China(No.2020B010188002)the National Key R&D Program of China(No.2018YFA0702003).
文摘Metal-based atomically dispersed catalysts have attracted more attention because of their excellent catalytic performance and nearly 100%atom utilization.Therefore,it is very important to comprehensively and systematically understand the relationship between catalytic active sites and catalytic performance at atomic scale.Here,we discuss and summarize in detail the key and fundamental factors affecting the active site,and relate them to the catalytic performance.First,we describe the effectiveness of active site design by coordination effects.Then,the role of chemical bonds in the active sites in changing the reaction performance is discussed.In addition,for intermetallic compounds,we explore how the spacing of active atoms affects the catalytic behavior.Moreover,the importance of synergistic effect in catalyst design is further discussed.Finally,the key parameters affecting the catalytic performance at atomic scale are summarized,and the main challenges and development prospects of atomic catalysts in the future are put forward.
