Zhou Yixiang, Yao Yebo, Zhao Rui, Wang Xiaoxuan, Fu Zhenzhen, Wang Dewei, Wang Huaizhi, Zhao Liang, Ni Wei, Yang Zhiyu, Yan Yi-Ming
State Key Lab of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, Beijing, 100029, P. R. China.
Beijing Aerospace Propulsion Institute, Beijing, 100076, China.
Angew Chem Int Ed Engl. 2022 Aug 1;61(31):e202205832. doi: 10.1002/anie.202205832. Epub 2022 Jun 23.
Copper oxide-based materials effectively electrocatalyze carbon dioxide reduction (CO RR). To comprehend their role and achieve high CO RR activity, Cu in copper oxides must be stabilized. As an electrocatalyst, Cu O nanoparticles were decorated with hexagonal boron nitride (h-BN) nanosheets to stabilize Cu . The C H /CO ratio increased 1.62-fold in the CO RR with Cu O-BN compared to that with Cu O. Experimental and theoretical studies confirmed strong electronic interactions between the two components in Cu O-BN, which strengthens the Cu-O bonds. Electrophilic h-BN receives partial electron density from Cu O, protecting the Cu-O bonds from electron attack during the CO RR and stabilizing the Cu species during long-term electrolysis. The well-retained Cu species enhanced the C product selectivity and improved the stability of Cu O-BN. This work offers new insight into the metal-valence-state-dependent selectivity of catalysts, enabling the design of advanced catalysts.
基于氧化铜的材料能有效电催化二氧化碳还原反应（CO₂RR）。为了理解它们的作用并实现高CO₂RR活性，氧化铜中的铜必须被稳定下来。作为一种电催化剂，用六方氮化硼（h-BN）纳米片修饰CuO纳米颗粒以稳定铜。与CuO相比，在CO₂RR中，CuO-BN的C₂H₄/CO比率提高了1.62倍。实验和理论研究证实了CuO-BN中两种组分之间存在强烈的电子相互作用，这强化了Cu-O键。亲电子的h-BN从CuO接收部分电子密度，在CO₂RR过程中保护Cu-O键免受电子攻击，并在长期电解过程中稳定铜物种。保留良好的铜物种提高了C₂H₄产物的选择性，并改善了CuO-BN的稳定性。这项工作为催化剂的金属价态依赖性选择性提供了新的见解，有助于设计先进的催化剂。
