Tailoring atomic chemistry to refine reaction pathway for the most enhancement by magnetization in water oxidation

• 成果类型: Article
• 署名作者: Wu, Tianze; Ge, Jingjie; Wu, Qian; Ren, Xiao; Meng, Fanxu; Wang, Jiarui; Xi, Shibo; Wang, Xin; Elouarzaki, Kamal; Fisher, Adrian; Xu, Zhichuan J.
• 署名单位: Nanyang Technological University; Hong Kong Polytechnic University; Peking University; Agency for Science Technology & Research (A*STAR); City University of Hong Kong; Nanyang Technological University; University of Cambridge; Nanyang Technological University
• 刊物名称: PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
• ISSN/ISSBN: 0027-13483
• DOI: 10.1073/pnas.2318652121
• 发表日期: 2024-05-07
• 关键词: oxygen; catalysis; oxides; STABILITY

摘要

Water oxidation on magnetic catalysts has generated significant interest due to the spin - polarization effect. Recent studies have revealed that the disappearance of magnetic domain wall upon magnetization is responsible for the observed oxygen evolution reaction (OER) enhancement. However, an atomic picture of the reaction pathway remains unclear, i.e., which reaction pathway benefits most from spin - polarization, the adsorbent evolution mechanism, the intermolecular mechanism (I2M), the lattice oxygen - mediated one, or more? Here, using three model catalysts with distinguished atomic chemistries of active sites, we are able to reveal the atomic - level mechanism. We found that spin - polarized OER mainly occurs at interconnected active sites, which favors direct coupling of neighboring ligand oxygens (I2M). Furthermore, our study reveals the crucial role of lattice oxygen participation in spin - polarized OER, significantly facilitating the coupling kinetics of neighboring oxygen radicals at active sites.