报告题目：Rational Catalyst Design for CO₂Electrochemical Reduction Reaction

报告时间：2024年5月20号（星期一）15:30

报告地点：知化楼423会议室

主办单位：化学化工与资源利用学院

报 告 人：王子运教授

报告人简介：王子运博士，新西兰奥克兰大学Senior Lecturer。2012年本科毕业于华东理工大学，2015年博士毕业于英国女王大学，师从胡培君教授和ChrisHardacre教授。先后在斯坦福大学（合作导师JensK. Nørskov教授）和多伦多大学（合作导师Edward H. Sargent教授）从事博士后研究，主要研究方向包括二氧化碳电还原的理论计算、人工智能辅助多相催化设计和表面微动力学。以通讯作者或（共同）第一作者发表文章45篇，其中Nature2篇，NatureCatalysis5篇，NatureEnergy2篇，NatureCommunications 4篇，J. Am. Chem. Soc. 7篇，Angew.Chem. 4篇。

报告摘要：Selectivity is very important in electrochemical reduction of CO₂(CO₂RR) both scientifically and industrially. Recently, C₂selectivity has exceeded 80% on Cu-based catalyst using the flow cell, and ethylene and ethanol are the main two products. Understanding the mechanism branching the ethylene and ethanol is the key to achieve high selectivity of CO₂RR.

In this work, we first used density functional theory (DFT) calculations to understand the reaction pathways of CO₂RR to ethylene and ethanol. The reaction barriers and enthalpy changes are calculated for the elementary steps considered in the two pathways on Cu(100). Based on the DFT results, we investigated two factors that could affect the ratio between ethylene and ethanol, namely CO coverage and surface decoration. Using DFT calculation, we found that CO coverage could affect the relative energies of intermediates along ethylene and ethanol pathways, thus favoring one product over the other. With the decrease of CO coverage, the ethylene pathway becomes more favorable. Experiment results suggest the same trend and the highest ethylene selectivity is achieved with low CO partial pressure in CORR experiment. We also investigated the effect of surface decoration and found metal oxide and surface condiment favors ethanol.