题目：高压二氧化碳电化学还原

时间：2023年12月22日 15:00-16:30

地点：机械与动力工程学院 F310会议室

邀请人：周宝文 副教授（新能源动力研究所）

报告人简介

卢旭博士，2017至2020年于美国耶鲁大学化学系进行博士后研究，2021年3月于沙特阿卜杜拉国王科技大学（KAUST）独立建组，专注高压二氧化碳电还原。团队成立迄今，原创科研成果已发表在Nature Communications（3篇）、Journal of the American Chemical Society、Angewandte Chemie、Chemical Engineering Journal、Journal of the Energy Chemistry等国际顶级期刊，与美国西北大学、多伦多大学、巴黎大学、伦敦大学学院、清华大学、宾夕法尼亚大学、新加坡国立大学等高校保持紧密科研合作，并由沙特阿美、ACWA Power等公司资助进行千瓦级直接太阳能驱动质子交换膜/离子交换膜电解槽研发。

报告摘要

Electrochemical reduction of CO₂ (CO₂R) is a strategy aimed at completing the carbon cycle for chemical production. Until now, this field has primarily concentrated on performing electrolysis on CO₂ at atmospheric pressure. Nevertheless, in industrial settings, CO₂ is typically pressurized during its capture, transportation, and storage, often existing in dissolved state or gas phase. We discovered that subjecting CO₂ to a pressure of 50 bar shifts the CO₂R pathways towards formate, a phenomenon consistently observed across commonly used metal catalysts such as Cu, Ag, Au and Sn. By creating operando techniques that can operate effectively under high pressures, including a quantitative operando Raman spectroscopy, we have established a connection between the heightened preference for formate and the increased coverage of CO₂ on the cathode surface. The interplay of theoretical models and experimental data supports this mechanism and guides us to enhance the cathode surface of a copper electrode with a layer that resists protons, thereby amplifying the formate-selective impact caused by pressure. Besides C1 products, we have uncovered the potential to electrochemically convert high-pressure gas-phase CO₂ into C2 products, especially ethylene (C₂H₄). Our approach involved conducting density functional theory calculations to pinpoint a selection of copper alloys that facilitate the crucial C-C dimerization step under high pressure.