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Boosting oxygen evolution kinetics via sulfur/phosphorus dynamic migration induced surface enrichment in an anion-regulated iron selenide
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-09-02 , DOI: 10.1039/d4ta01867b Bezawit Z. Desalegan , Reibelle Q. Raguindin , Gaojun Jiang , Hyung-Ho Park , Jeong Gil Seo
Journal of Materials Chemistry A ( IF 10.7 ) Pub Date : 2024-09-02 , DOI: 10.1039/d4ta01867b Bezawit Z. Desalegan , Reibelle Q. Raguindin , Gaojun Jiang , Hyung-Ho Park , Jeong Gil Seo
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Optimizing the energetics of the elementary steps of Oxygen Evolution Reaction (OER) by tuning the electrode-intermediate/product interaction through d-band center energy tailoring is an essential yet under-explored concept in oxygen electrocatalysis. Herein, the interplay between sulfur/phosphorus and selenium toward improved OER kinetics is investigated and the synergistic interaction between these task-specific anions along with additional metal–anion interaction provides suitable tailoring of the d-band center for facilitating efficient electrocatalysis. S/P regulation of FeSe2 resulted in a transition from high-spin Fe2+/3+ to intermediate-spin Fe2+/3+ affording simultaneous adsorption/desorption optimization leading to ultralow overpotentials of <300 mV at a current density of 600 mA cm−2 [376 A g−1] with highly stable performance for 50 h. These improvements stem from the strong electronic modulation arising from anion regulation-induced electron transfer and anion vacancies due to the dynamic migration of P/S to the outermost electrode surface during OER. This dynamic migration brings forth surface enrichment of S/P anions, endowing a hydrophilic surface for accelerating OH− adsorption while the Se-rich core facilitates the desorption of oxygen via reinforced electron repulsion between metal/Se d-band and oxygen p-band electrons. This work paves the way for optimizing oxygen electrocatalysis through descriptor-guided tuning from an experimental standpoint by introducing functional task-specific elements.
中文翻译:
通过硫/磷动态迁移诱导阴离子调节硒化铁表面富集来促进析氧动力学
通过 d 带中心能量调整来调整电极-中间体/产物相互作用来优化析氧反应 (OER) 基本步骤的能量学是氧电催化中一个重要但尚未充分探索的概念。在此,研究了硫/磷和硒之间的相互作用以改善 OER 动力学,并且这些特定任务阴离子之间的协同相互作用以及额外的金属-阴离子相互作用为 d 带中心提供了适当的定制,以促进有效的电催化。 FeSe 2的 S/P 调节导致从高自旋 Fe 2+/3+到中自旋 Fe 2+/3+的转变,提供同时吸附/解吸优化,导致在电流密度为 <300 mV 的超低过电势600 mA cm -2 [376 A g -1 ],50 小时内性能高度稳定。这些改进源于阴离子调节引起的电子转移和阴离子空位(由于 OER 过程中 P/S 动态迁移到最外层电极表面而产生的阴离子空位)所产生的强电子调制。这种动态迁移带来了 S/P 阴离子的表面富集,赋予亲水性表面以加速OH-吸附,而富 Se 核心则通过增强金属/Se d 带和氧 p 带电子之间的电子排斥促进氧的解吸。这项工作通过引入功能性任务特定元素,从实验的角度通过描述符引导的调整,为优化氧电催化铺平了道路。
更新日期:2024-09-05
中文翻译:
![](https://scdn.x-mol.com/jcss/images/paperTranslation.png)
通过硫/磷动态迁移诱导阴离子调节硒化铁表面富集来促进析氧动力学
通过 d 带中心能量调整来调整电极-中间体/产物相互作用来优化析氧反应 (OER) 基本步骤的能量学是氧电催化中一个重要但尚未充分探索的概念。在此,研究了硫/磷和硒之间的相互作用以改善 OER 动力学,并且这些特定任务阴离子之间的协同相互作用以及额外的金属-阴离子相互作用为 d 带中心提供了适当的定制,以促进有效的电催化。 FeSe 2的 S/P 调节导致从高自旋 Fe 2+/3+到中自旋 Fe 2+/3+的转变,提供同时吸附/解吸优化,导致在电流密度为 <300 mV 的超低过电势600 mA cm -2 [376 A g -1 ],50 小时内性能高度稳定。这些改进源于阴离子调节引起的电子转移和阴离子空位(由于 OER 过程中 P/S 动态迁移到最外层电极表面而产生的阴离子空位)所产生的强电子调制。这种动态迁移带来了 S/P 阴离子的表面富集,赋予亲水性表面以加速OH-吸附,而富 Se 核心则通过增强金属/Se d 带和氧 p 带电子之间的电子排斥促进氧的解吸。这项工作通过引入功能性任务特定元素,从实验的角度通过描述符引导的调整,为优化氧电催化铺平了道路。