Revealing interaction of pyridinic N in N‐doped carbon with Sn sites for improved CO <sub>2</sub> reduction
Huijuan Yang, Xu-Hong Yan, Cheng Yan, Zi-Qin Min, Lei Chai, Chun-Ran Wang, Lina Chen, Wei Xiao, Tao Wang, Chong Xie, Dawei Pang, Xifei Li
Abstract
N‐doped carbon (NC) materials have emerged as attractive supports for metal‐based catalysts, enhancing their catalytic performance through the metal–support interactions. However, gaining fundamental insights into the metal–support interaction between NC support and Sn metal sites for improving the electrocatalytic CO 2 reduction reaction (CO 2 RR) performance remains challenging. Here, we reveal that pyridinic N in NC support indirectly induces the net electron distribution of Sn sites to exhibit optimal adsorption of HCOO* and HCOOH* by combining theoretical simulations and experiments, while pyrrolic N and graphitic N present weaker adsorption of HCOO* and stronger adsorption of HCOOH*, respectively. Consequently, the catalyst comprising NC with abundant pyridinic N loaded SnO 2 quantum dots exhibits excellent CO 2 RR performance, achieving high partial formate activity (over 90 mA. cm −2 in an H‐cell and 200 mA. cm −2 in a flow cell) and impressive Faradaic efficiency for formate (approximately 90%). This work provides valuable insights into intricate metal–support interactions, thereby offering guidance for the future design and development of CO 2 RR electrocatalysts.