Pei Zhihao, Lu Xue Feng, Zhang Huabin, Li Yunxiang, Luan Deyan, Lou Xiong Wen David
School of Chemical and Biomedical Engineering, Nanyang Technological University, 62 Nanyang Drive, Singapore, 637459, Singapore.
KAUST Catalysis Center (KCC), King Abdullah University of Science and Technology (KAUST), Thuwal, 23955-6900, Saudi Arabia.
Angew Chem Int Ed Engl. 2022 Oct 4;61(40):e202207537. doi: 10.1002/anie.202207537. Epub 2022 Aug 22.
Single-atom catalysts (SACs) are being pursued as economical electrocatalysts. However, their low active-site loading, poor interactions, and unclear catalytic mechanism call for significant advances. Herein, atomically dispersed Ni/Co dual sites anchored on nitrogen-doped carbon (a-NiCo/NC) hollow prisms are rationally designed and synthesized. Benefiting from the atomically dispersed dual-metal sites and their synergistic interactions, the obtained a-NiCo/NC sample exhibits superior electrocatalytic activity and kinetics towards the oxygen evolution reaction. Moreover, density functional theory calculations indicate that the strong synergistic interactions from heteronuclear paired Ni/Co dual sites lead to the optimization of the electronic structure and the reduced reaction energy barrier. This work provides a promising strategy for the synthesis of high-efficiency atomically dispersed dual-site SACs in the field of electrochemical energy storage and conversion.
单原子催化剂(SACs)正被视作经济高效的电催化剂。然而,其活性位点负载量低、相互作用差以及催化机理不明等问题亟待重大突破。在此,我们合理设计并合成了锚定在氮掺杂碳(a-NiCo/NC)空心棱柱上的原子分散的镍/钴双位点。得益于原子分散的双金属位点及其协同相互作用,所制备的a-NiCo/NC样品在析氧反应中展现出优异的电催化活性和动力学性能。此外,密度泛函理论计算表明,异核配对的镍/钴双位点之间的强协同相互作用导致了电子结构的优化和反应能垒的降低。这项工作为在电化学储能和转换领域合成高效的原子分散双位点SACs提供了一种有前景的策略。