用于水氧化的 Co 和 S 原子对掺杂 Fe3O4 的动态稳定电子调节和电化学重构,Small

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用于水氧化的 Co 和 S 原子对掺杂 Fe3O4 的动态稳定电子调节和电化学重构
Small ( IF 13.0 ) Pub Date : 2023-04-22 , DOI: 10.1002/smll.202301255
Hai-Jun Liu ₁ , Shuo Zhang ₁ , Ya-Nan Zhou ₁ , Wen-Li Yu ₁ , Yu Ma ₁ , Shu-Tao Wang ₁ , Yong-Ming Chai ₁ , Bin Dong ₁

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地球上丰富的电催化剂的电子调节和表面重建对于高效的析氧反应（OER）至关重要。在这里，在泡沫铁（Co,S-Fe 3 O 4 /IF）上生长的_反尖晶石_Co , S原子对共掺杂Fe ₃ O _{4被制造为一种经济有效的OER电催化剂。}这种 Co 和 S 原子对定向共掺杂特征的策略加速了表面重建并动态稳定了电子调节。_{Fe 3} O ₄晶体中掺杂的Co - S原子对有利于通过硫浸出进行可控表面重构，在重构的FeOOH（Co-FeOOH-O _v /IF）表面形成氧空位和Co掺杂。在通过原位电化学过程进行表面重构之前和之后，具有八面体场的Fe位点动态地保持OER中间体适当的电子结构，从而表现出始终如一的优异的OER性能。^{电化学调谐的铁基电极在1000 mA cm -2}的电流密度下表现出349 mV的低过电势、 43.3 mV dec ^-1的轻微塔菲尔斜率以及在碱性介质中200小时的优异长期电解稳定性。密度泛函理论计算说明了 Fe 位点的电子调节、吉布斯自由能的变化以及 OER 中间体之间限制性标度关系的打破。这项工作为开发大规模水分解系统的预催化剂提供了一种有前景的定向共掺杂策略。

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Dynamically Stabilized Electronic Regulation and Electrochemical Reconstruction in Co and S Atomic Pair Doped Fe3O4 for Water Oxidation

The electronic regulation and surface reconstruction of earth-abundant electrocatalysts are essential to efficient oxygen evolution reaction (OER). Here, an inverse-spinel Co,S atomic pair codoped Fe₃O₄ grown on iron foam (Co,S-Fe₃O₄/IF) is fabricated as a cost-effective electrocatalyst for OER. This strategy of Co and S atomic pair directional codoping features accelerates surface reconstruction and dynamically stabilizes electronic regulation. CoS atomic pairs doped in the Fe₃O₄ crystal favor controllable surface reconstruction via sulfur leaching, forming oxygen vacancies and Co doping on the surface of reconstructed FeOOH (Co-FeOOH-O_v/IF). Before and after surface reconstruction via in situ electrochemical process, the Fe sites with octahedral field dynamically maintains an appropriate electronic structure for OER intermediates, thus exhibiting consistently excellent OER performance. The electrochemically tuned Fe-based electrodes exhibit a low overpotential of 349 mV at a current density of 1000 mA cm⁻², a slight Tafel slope of 43.3 mV dec⁻¹, and exceptional long-term electrolysis stability of 200 h in an alkaline medium. Density functional theory calculations illustrate the electronic regulation of Fe sites, changes in Gibbs free energies, and the breaking of the restrictive scaling relation between OER intermediates. This work provides a promising directional codoping strategy for developing precatalysts for large-scale water-splitting systems.

更新日期：2023-04-22

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