Direct Microenvironment Modulation of CO2 Electroreduction: Negatively Charged Ag Sites Going beyond Catalytic Surface Reactions.

ABSTRACT

Electrochemical reduction of CO2 is an important way to achieve carbon neutrality, and much effort has been devoted to the design of active sites. Apart from elevating intrinsic activity, expanding the functionality of active site may also boost catalytic performance. Here we have designed "negatively charged Ag (nc-Ag)" active sites featuring both the intrinsic activity and the capability of regulating microenvironment, through modifying Ag nanoparticles with atomically dispersed Sn species. Different from conventional active sites (which only govern surface process by bonding with the intermediates), the nc-Ag sites could manipulate environmental species. Therefore, the sites could not only activate CO2, but also regulate interfacial H2O and CO2, as confirmed by operando spectroscopies. The catalyst delivers a high current density with CO faradaic efficiency of 97%. Our work here opens up new opportunities for the design of multifunctional electrocatalytic active sites.