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铁-硫双调制吸附质演化与晶格氧兼容的析氧机制

Fe-S dually modulated adsorbate evolution and lattice oxygen compatible mechanism for water oxidation.

作者信息

Luo Xu, Zhao Hongyu, Tan Xin, Lin Sheng, Yu Kesong, Mu Xueqin, Tao Zhenhua, Ji Pengxia, Mu Shichun

机构信息

State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan, 430070, China.

State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, Wuhan, 430070, China.

出版信息

Nat Commun. 2024 Sep 27;15(1):8293. doi: 10.1038/s41467-024-52682-y.

DOI:10.1038/s41467-024-52682-y
PMID:39333518
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11436974/
Abstract

Simultaneously activating metal and lattice oxygen sites to construct a compatible multi-mechanism catalysis is expected for the oxygen evolution reaction (OER) by providing highly available active sites and mediate catalytic activity/stability, but significant challenges remain. Herein, Fe and S dually modulated NiFe oxyhydroxide (R-NiFeOOH@SO) is conceived by complete reconstruction of NiMoO·xHO@Fe,S during OER, and achieves compatible adsorbate evolution mechanism and lattice oxygen oxidation mechanism with simultaneously optimized metal/oxygen sites, as substantiated by in situ spectroscopy/mass spectrometry and chemical probe. Further theoretical analyses reveal that Fe promotes the OER kinetics under adsorbate evolution mechanism, while S excites the lattice oxygen activity under lattice oxygen oxidation mechanism, featuring upshifted O 2p band centers, enlarged d-d Coulomb interaction, weakened metal-oxygen bond and optimized intermediate adsorption free energy. Benefiting from the compatible multi-mechanism, R-NiFeOOH@SO only requires overpotentials of 251 ± 5/291 ± 1 mV to drive current densities of 100/500 mA cm in alkaline media, with robust stability for over 300 h. This work provides insights in understanding the OER mechanism to better design high-performance OER catalysts.

摘要

通过提供高度可用的活性位点并调节催化活性/稳定性，同时激活金属和晶格氧位点以构建兼容的多机制催化有望用于析氧反应（OER），但仍存在重大挑战。在此，通过在OER过程中对NiMoO·xH₂O@Fe,S进行完全重构，设计出了铁和硫双重调制的氢氧化镍铁（R-NiFeOOH@SO），并实现了兼容的吸附质演化机制和晶格氧氧化机制，同时优化了金属/氧位点，原位光谱/质谱和化学探针证实了这一点。进一步的理论分析表明，铁在吸附质演化机制下促进OER动力学，而硫在晶格氧氧化机制下激发晶格氧活性，其特征为O 2p带中心上移、d-d库仑相互作用增大、金属-氧键减弱以及中间吸附自由能优化。受益于兼容的多机制，R-NiFeOOH@SO在碱性介质中驱动100/500 mA cm⁻²的电流密度仅需251±5/291±1 mV的过电位，具有超过300小时的稳健稳定性。这项工作为理解OER机制以更好地设计高性能OER催化剂提供了见解。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/8c94abf946df/41467_2024_52682_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/031a8e14fe98/41467_2024_52682_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/4dd525fb09ad/41467_2024_52682_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/20afda55d143/41467_2024_52682_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/fa95b1896099/41467_2024_52682_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/8c94abf946df/41467_2024_52682_Fig5_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/031a8e14fe98/41467_2024_52682_Fig1_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/4dd525fb09ad/41467_2024_52682_Fig2_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/20afda55d143/41467_2024_52682_Fig3_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/fa95b1896099/41467_2024_52682_Fig4_HTML.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/234b/11436974/8c94abf946df/41467_2024_52682_Fig5_HTML.jpg

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