Insights into the Use of Te–O Pairs as Active Centers of Carbon Nanosheets for Efficient Electrochemical Oxygen Reduction
Zeming Wang, Gao Li, Weidong Hou, Huazhang Guo, Liang Wang, Minghong Wu
Abstract
Previous theoretical calculations have predicted that the incorporation of tellurium (Te) into carbon materials can significantly enhance their catalytic activity. Nevertheless, the experimental realization of efficient Te-doped carbon materials remains challenging. Here, we employed theoretical calculations to deduce the possible structure of Te-doped carbon materials. Our findings unveil that the formation of Te-O pairs in carbon materials with a relatively low oxygen coordination microenvironment can impart strong electron-donating capabilities, thereby boosting the electrocatalytic activity of oxygen reduction reaction (ORR). To verify our theoretical predictions, we synthesized Te-O pair-doped carbon materials using a tandem hydrothermal dehydration-pyrolysis strategy. This approach enabled efficient infiltration of Te into carbon materials. Our unconventional Te-O pair-doped carbon materials exhibit expanded interlayer distances and graphene-like nanosheet architectures, which provide enlarged active areas. These structural features contribute to the enhanced ORR catalytic performance of the as-prepared carbon catalyst. Our findings provide molecular-level insights into the design of various carbon-based electrocatalysts with binary-heteroatom-doped active sites.