单原子催化剂具有原子利用率高、活性中心明确、催化中心原子配位数低等优点,有望提高电催化性能.具有相邻杂原子的双原子催化剂(DAC)有望发挥两个原子的协同作用,从而进一步提高活性.在本文中,我们报道了一种PtNi-NC催化剂,该催化剂由...单原子催化剂具有原子利用率高、活性中心明确、催化中心原子配位数低等优点,有望提高电催化性能.具有相邻杂原子的双原子催化剂(DAC)有望发挥两个原子的协同作用,从而进一步提高活性.在本文中,我们报道了一种PtNi-NC催化剂,该催化剂由固定在氮掺杂碳基底上的PtNi双原子构成,该基底采用原子层沉积技术合成.X射线吸收光谱证实了Pt–Ni双原子的存在.所制备的PtNi-NC催化剂具有优异的催化活性,在10 m A cm^(-2)的电流密度下,酸性介质中析氢反应(HER)的过电位为30 m V,与市售20 wt%Pt/C相当.特别值得注意的是,PtNi-NC具有比20 wt%Pt/C更高的质量活性,约为其21倍.密度泛函理论计算表明,Pt–Ni双原子通过调节局部电子结构和优化电荷分布产生协同效应,有助于优化吸附性能和增强电催化性能.这项工作为DAC的制备提供了新途径,揭示了它们在电催化HER等领域的应用潜力.展开更多
The development of cost-effective and highly efficient electrocatalysts to accelerate distinct electrochemical reactions is essential to help the industry to achieve a low-carbon footprint.Single-atom alloys(SAAs)with...The development of cost-effective and highly efficient electrocatalysts to accelerate distinct electrochemical reactions is essential to help the industry to achieve a low-carbon footprint.Single-atom alloys(SAAs)with the characteristics of unique electronic structures,well-defined active sites,and maximum atom utilization demonstrate promising potential to replace traditional noble metal catalysts.SAAs are expected to tailor the adsorption properties of reaction species,thus promoting electrocatalytic behaviors.Herein,representative synthetic strategies including wet chemistry,galvanic replacement,dealloying,and atomic layer deposition are introduced,followed by a summary of applications of SAAs in hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,carbon dioxide reduction reaction,and ethanol electro-oxidation to provide an in-depth understanding of the structure–activity relationship.Moreover,the challenges and perspectives in this emerging field of SAAs are discussed.展开更多
基金supported by the National Natural Science Foundation of China(52122107 and 51972224)the National Research Foundation,SingaporeA*STAR under its LCER FI program Award(U2102d2002)。
文摘单原子催化剂具有原子利用率高、活性中心明确、催化中心原子配位数低等优点,有望提高电催化性能.具有相邻杂原子的双原子催化剂(DAC)有望发挥两个原子的协同作用,从而进一步提高活性.在本文中,我们报道了一种PtNi-NC催化剂,该催化剂由固定在氮掺杂碳基底上的PtNi双原子构成,该基底采用原子层沉积技术合成.X射线吸收光谱证实了Pt–Ni双原子的存在.所制备的PtNi-NC催化剂具有优异的催化活性,在10 m A cm^(-2)的电流密度下,酸性介质中析氢反应(HER)的过电位为30 m V,与市售20 wt%Pt/C相当.特别值得注意的是,PtNi-NC具有比20 wt%Pt/C更高的质量活性,约为其21倍.密度泛函理论计算表明,Pt–Ni双原子通过调节局部电子结构和优化电荷分布产生协同效应,有助于优化吸附性能和增强电催化性能.这项工作为DAC的制备提供了新途径,揭示了它们在电催化HER等领域的应用潜力.
基金National Natural Science Foundation of China,Grant/Award Numbers:51972224,52122107National Research Foundation,Singapore,and A*STAR(Agency for Science,Technology and Research)under its LCER FI program Award,Grant/Award Number:U2102d2002。
文摘The development of cost-effective and highly efficient electrocatalysts to accelerate distinct electrochemical reactions is essential to help the industry to achieve a low-carbon footprint.Single-atom alloys(SAAs)with the characteristics of unique electronic structures,well-defined active sites,and maximum atom utilization demonstrate promising potential to replace traditional noble metal catalysts.SAAs are expected to tailor the adsorption properties of reaction species,thus promoting electrocatalytic behaviors.Herein,representative synthetic strategies including wet chemistry,galvanic replacement,dealloying,and atomic layer deposition are introduced,followed by a summary of applications of SAAs in hydrogen evolution reaction,oxygen evolution reaction,oxygen reduction reaction,carbon dioxide reduction reaction,and ethanol electro-oxidation to provide an in-depth understanding of the structure–activity relationship.Moreover,the challenges and perspectives in this emerging field of SAAs are discussed.
