能源催化中单原子催化剂的可控非对称配位研究进展  

Progress in controllable asymmetric coordination studies of single-atom catalysts in energy catalysis

作　　者：程颖 张呈旭 李鑫培 胡觉[1,2] CHENG Ying;ZHANG Chengxu;LI Xinpei;HU Jue(Faculty of Metallurgical and Energy Engineering,Kunming University of Science and Technology,Kunming 650093,China;Key Laboratory of Unconventional Metallurgy,Kunming University of Science and Technology,Kunming 650093,China)

机构地区：[1]昆明理工大学冶金与能源工程学院,昆明650093 [2]昆明理工大学非常规冶金重点实验室,昆明650093

出　　处：《工程科学学报》2025年第4期940-957,共18页Chinese Journal of Engineering

基　　金：国家自然科学基金资助项目(52364041);云南省杰出青年基金资助项目(202401AV070011)。

摘　　要：能源已成为人类社会发展的重要基础,在国民经济中占有举足轻重的地位.单原子催化剂(SACs)已成为一种很有前途的材料,并且在化学和能源领域都有广泛的应用.因此,开发具有高活性、高稳定性和低成本的SACs具有重要的实际意义.特别是SACs中的不对称配位结构,在催化性能上超越了传统的M—N_(4)活性位点,引起了人们的迅速关注.在氧还原反应(ORR)这一燃料电池技术的关键步骤中,具有不对称配位结构的SACs通过优化活性位点的电子性质来提高催化效率.这将导致活化能的大幅降低,从而提高电流密度和能量转换效率,从而加速燃料电池的商业化.同样,在CO_(2)还原反应(CO_(2)RR)中,这些催化剂可以精细地调节CO_(2)分子的吸附和活化,促进CO_(2)选择性和有效地转化为有价值的化学物质,如甲醇和一氧化碳.这种能力为碳回收技术提供了巨大的潜力.此外,不对称SACs在解决环境挑战方面显示出显着的希望,特别是在硝酸盐还原反应(NO_(3)RR)中,它们有效地将有害硝酸盐转化为惰性氮,从而有助于环境保护和水质改善.本文总结了几种典型的非对称单原子催化剂结构,即M—N_(4)—Y(Y为轴向杂原子),M—N_(x)—Y(Y为非金属原子),M—N_(x)和M—M结构.系统介绍了这些先进催化剂的可控合成及其在氧还原反应(ORR)、CO_(2)还原反应(CO_(2)RR)和硝酸根还原反应(NO_(3)RR)等电催化反应中的研究进展和应用.最后,对目前SACs的挑战和未来的发展前景进行了展望.Energy is foundational for the advancement of human society,occupying a pivotal role in the national economy.Single-atom catalysts(SACs)are a promising catalyst material in the chemistry and energy fields owing to their high activity,high efficiency,adjustable electronic structure,and low price.Therefore,the development of SACs with high activity,superior stability,and low cost holds significant practical importance.In particular,asymmetric coordination structures in SACs have gained attention over traditional M—N_(4) active sites in terms of catalytic performance.In the context of the oxygen reduction reaction(ORR),a key step in fuel cell technology,SACs with asymmetric coordination structures have demonstrated enhanced catalytic efficiency by optimizing the electronic properties of active sites.This leads to a substantial reduction in activation energy,resulting in improved current densities and energy conversion efficiencies,thus accelerating the commercialization of fuel cells.Similarly,in the CO_(2) reduction reaction(CO_(2)RR),these catalysts can fine-tune the adsorption and activation of CO_(2) molecules,promoting the selective and efficient conversion of CO_(2) into valuable chemicals such as methanol and carbon monoxide.This capability offers significant potential for carbon recycling technologies.Moreover,asymmetric SACs have shown remarkable promise in addressing environmental challenges,particularly in the nitrate reduction reaction(NO_(3)RR)by efficiently converting harmful nitrates into inert nitrogen,which contributes to environmental protection and water quality improvement.In general,axial coordination in electrocatalysts enhances electrocatalytic reactions such as CO_(2)RR and ORR by fine-tuning the electronic structure of metal centers to optimize reaction kinetics and stabilize the catalyst.This coordination facilitates the efficient desorption of catalytic intermediates while mitigating side reactions,leading to improved catalyst durability and enhanced electrochemical stability.This review

关 键 词：单原子 催化剂 非对称配位 电催化 调控策略 

分 类 号：O646[理学—物理化学]