دورية أكاديمية

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

التفاصيل البيبلوغرافية
العنوان: Tailoring atomic chemistry to refine reaction pathway for the most enhancement by magnetization in water oxidation.
المؤلفون: Tianze Wu, Jingjie Ge, Qian Wu, Xiao Ren, Fanxu Meng, Jiarui Wang, Shibo Xi, Xin Wang, Elouarzaki, Kamal, Fisher, Adrian, Zhichuan J. Xu
المصدر: Proceedings of the National Academy of Sciences of the United States of America; 5/7/2024, Vol. 121 Issue 19, p1-9, 23p
مصطلحات موضوعية: CHEMICAL reactions, OXIDATION of water, MAGNETIC domain walls, OXYGEN evolution reactions, MAGNETIZATION
مستخلص: 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. [ABSTRACT FROM AUTHOR]
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قاعدة البيانات: Complementary Index
الوصف
تدمد:00278424
DOI:10.1073/pnas.2318652121