Electrochemical CO<sub>2</sub> Reduction on SnO: Insights into C<sub>1</sub> Product Dynamic Distribution and Reaction Mechanisms
Zhongyuan Guo, Tianyi Wang, Heng Liu, Xue Jia, Di Zhang, Wei Li, Jiang Xu, Hao Li
Abstract
High Resolution Image Download MS PowerPoint Slide The precise synthesis of desirable products from the electrochemical CO 2 reduction reaction (CO 2 RR) remains challenging, primarily due to unclear structure–activity relationships under in situ reaction conditions. Recognized by their cost-effectiveness and nontoxic nature, Sn-based materials are extensively utilized in CO 2 RR to produce valuable chemicals. Notably, our large-scale data mining of the experimental CO 2 RR literature reveals a significant trend: SnO 2 -based electrocatalysts primarily generate HCOOH, while SnO-based counterparts demonstrate the ability to produce both HCOOH and CO in comparable quantities. Furthermore, our findings indicate that SnO remains underexplored in terms of its surface speciation and structure–activity relationships for the CO 2 RR compared to SnO 2 -based materials. Addressing these issues is crucial in the field of electrocatalysis, as understanding them will not only clarify why SnO uniquely influences the distribution of C 1 products but also provide insights into how to precisely control electrocatalytic processes for targeted product synthesis. Herein, we employed a constant-potential method combined with surface coverage and reconstruction analyses to simulate the energetics of CO 2 RR intermediates and to elucidate the dynamic distribution of C 1 products on the in situ resting surface of SnO under typical CO 2 RR conditions. Our analysis of surface coverage and reconstruction effectively identifies the active surface of SnO involved in the CO 2 RR. Furthermore, comparative simulations between pristine and reconstructed SnO surfaces reveal how electrochemistry-induced oxygen vacancies direct C 1 product distribution. By addressing these critical issues, we aim to advance electrocatalysis and contribute to chemical production from CO 2, stimulating future exploration of structure–activity relationships and reaction conditions in other electrocatalytic systems.