高选择性铜基电催化材料在二氧化碳还原反应中的应用研究

Research News

Intermediates Adsorption Engineering of CO2 Electroreduction Reaction in Highly Selective Heterostructure Cu‐Based Electrocatalysts for CO Production

Hao Yang, Yu-wen Hu, Jun-jie Chen, M.-Sadeeq (Jie Tang) Balogun, Ping-ping Fang Shanqing Zhang,* Jian Chen,* Yexiang Tong*

DOI: 10.1002/aenm.201901396

The challenge in the artificial CO2 reduction to fuel is achieving high selective electrocatalysts. In this research news article, a highly selective Cu2O/CuO heterostructure electrocatalyst is developed for CO2 electroreduction. The Cu2O/CuO nanowires modified by Ni nanoparticles exhibit superior catalytic performance with high faradic efficiency (95% for CO). Theoretical and experimental analyses show that the hybridization of Cu2O/CuO nanowires and Ni nanoparticles can not only adjust the d‐band center of electrocatalysts to enhance the intrinsic catalytic activity but also improve the adsorption of COOH* intermediates and suppress the hydrogen evolution reaction to promote the CO conversion efficiency during CO2 reduction reaction. In situ Raman spectroscopic study further confirms the existence of COOH* species and the engineering intermediates adsorption.

社会能源消费在未来很长一段时间内还将强烈依赖于石油、煤和天然气等化石燃料,可以预期所排放出来大量 CO2 将继续加剧日趋严重的温室效应和海洋酸化等全球性环境问题。要解决这一问题,除了减少 CO2 的排放,发展 CO2 的捕获和固定工作技术外,更具可持续性发展的思路是发展 CO2 转化技术。CO2 电催化还原不仅条件温和,而且能将太阳能、风能等产生的间歇性电能,转化为可储存运输的燃料和高值化学品,已成为一条非常具有发展潜力的 CO2 转化技术。

近日,中山大学童叶翔课题组,陈建课题组与澳大利亚格里菲斯大学张山青课题组合作,提出了一种金属纳米粒子修饰的Cu2O/CuO纳米线材料应用于CO2 电催化还原反应。金属镍修饰的Cu2O/CuO纳米线表现出优异的催化性能和高法拉第效率。理论计算和实验分析表明,金属镍与Cu2O/CuO纳米线复合不仅可以提高材料本身的催化活性,还可以抑制水溶液体系中析氢反应的进行,提高CO转化效率。原位拉曼光谱研究进一步发现金属镍的修饰和科研调控电极对CO2 电催化还原反应中间体COOH*的吸附,达到提高反应选择性的目的。这项工作为非贵金属过渡金属化合物催化材料的设计及从从分子水平阐明理解CO2电催化还原反应提供了新的方向。相关论文以题为“Intermediates Adsorption Engineering of CO2 Electroreduction Reaction in Highly Selective Heterostructure Cu‐Based Electrocatalysts for CO Production”发表在Advanced Energy Materials (DOI: 10.1002/aenm.201901396)上。