Insights into the Use of Te-O Pairs as Active Centers of Carbon Nanosheets for Efficient Electrochemical Oxygen Reduction.
Zeming WangGao LiWeidong HouHuazhang GuoLiang WangMinghong WuPublished in: ACS nano (2023)
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.