Affiliation:
1. Key Laboratory of Fine Chemicals Frontier Science Center for Smart Materials Liaoning Key Lab for Energy Materials and Chemical Engineering School of Chemical Engineering Dalian University of Technology Dalian 116024 China
2. State Key Laboratory of Chemical Resource Engineering College of Chemical Engineering Beijing University of Chemical Technology Beijing 100029 China
Abstract
AbstractDeveloping metal‐free carbon catalysts with designable high nitrogen (N) content yet well‐organized N distribution within carbon at nanoscale is still one of the paramount challenges for electrochemical CO2 conversion. Herein, a gradient N doping enabled by the energetic microwave irradiation is realized along the radial direction of carbon nanotubes (CNTs), with an ultrahigh surface N content of 30.5 at%, beyond the upper limit of the tradition pyrolysis method. The unique time‐domain features of microwave heating presented as the sub‐minute residence time for precursors and relatively mild surface temperature on CNTs, contributing to the maximum reservation of the surface N species. The catalyst exhibits a prominent performance with great activity and selectivity for electrochemical CO2‐to‐CO conversion. Theoretical calculation confirmed the catalyst with high N‐doping level can promote the adsorption of CO2 molecule, with a low adsorption energy of −3.35 eV. This work provides a novel prototype to construct the distribution‐controlled and space‐intensive active sites over functional gradient metal‐free carbon materials.
Funder
National Natural Science Foundation of China
Fundamental Research Funds for the Central Universities
National Key Research and Development Program of China
Liaoning Revitalization Talents Program