Precisely regulating the electronic structures of metal active species deposited on carbon support is highly desirable for electrocatalysis.

Date:2021-05-10

Recently, a research team led by Prof. Liu Jian from the Dalian Institute of Chemical Physics (DICP) of the Chinese Academy of Sciences (CAS), and Prof. Zhou Si from Dalian University of Technology, in collaboration with Prof. Liang Ji from Tianjin University, used single atoms to modify the carbon substrate to enhance the interaction between substrate and supported metal nanoparticles, and precisely tailored the electronic structures of metal nanoparticles.

 

 

This work was published in Angew. Chem. Int. Ed., 2021, 60, 16044 and is supported by the NSFC,

Dalian National Laboratory for Clean Energy (DNL) Cooperation Fund, Chinese Academy of Sciences

 

 

Carbon-based substrates usually with inert surface provide weak interaction with the supported metal active species and thus are unable to modulate their electronic structures effectively.In this study, single Co atoms were dispersed on carbon substrate to enhance the interaction between substrate and the ruthenium (Ru) nanoreactor, which enables remote regulation of the electronic states of Ru nanoparticles, and thereby tuning their electrocatalytic activity. Taking hydrogen evolution reaction (HER) as a model reaction, the cobalt single-atom doped carbon-supported Ru nanoreactor shows ultrahigh catalytic activity and stability, which is one of the highest activities reported in the literature.Theoretical calculations show that decoration of oxygen-containing graphene by single metal atoms induce electron redistribution on the carbon surface, such that the carbon atoms surrounding the single atoms are electron deficient, which significantly enhances the electron transfer from Ru nanoparticles to the carbon substrate, and thereby optimizes the binding capability of Ru nanoreactor and its HER performance.



http://www.dicp.cas.cn/xwdt/ttxw/202105/t20210510_6011493.html