It is generally considered that the hydrogenation of CO₂ is the critical bottleneck of the CO₂ electroreduction. In this work, with the aid of density functional theory (DFT) calculations, the catalytic hydrogenation of CO₂ molecules over Indium-doped SnP₃ catalyst were systematically studied. Through doping with indium (In) atom, the energy barrier of CO₂ protonation is reduced and OCHO* species could easily be generated. This is mainly due to the p orbital of In exhibits strong hybridization with the p orbital of O, indicating that there is a strong interaction between OCHO* and In-doped SnP₃ catalyst. As a result, In-doped SnP₃ possesses high-efficiency and high-selectivity for converting CO₂ into HCOOH with a low limiting potential of −0.17 V. Our findings will offer theoretical guidance to CO₂ electroreduction.

通常认为，CO ₂的氢化是CO ₂电还原的关键瓶颈。在这项工作中，借助密度泛函理论（DFT）的计算，系统地研究了铟掺杂SnP ₃催化剂上CO ₂分子的催化加氢。通过掺杂铟（In）原子，可以减少CO ₂质子化的能垒，并且可以轻松生成OCHO *物种。这主要是由于这样的p轨道在表现出与强杂交的p轨道的O，指示存在OCHO之间*和In掺杂SNP存在强烈的相互作用₃催化剂。结果，掺In SnP₃具有在-0.17 V的低极限电势下将CO ₂转化为HCOOH的高效和高选择性。我们的发现将为CO ₂电还原提供理论指导。