Asymmetric distortion of orbital hybridization at halogen-doped IrO2 monolayers for acidic water electrolysis

IF 2.1 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science Pub Date : 2024-06-23 DOI:10.1016/j.susc.2024.122542

Ming Meng , Yiming Liu , Yun Shan , Yi Song , Jian Li , Yang Shao , Lizhe Liu

引用次数: 0

Abstract

The unsatisfactory reactive activity and structural stability in acidic oxygen evolution reaction (OER) have been the main bottleneck in exploiting hydrogen energy from water splitting. Herein, we suggest a halogen (H)-doping strategy in 1T phase iridium dioxide (IrO₂) monolayer to optimize its electronic structure for accelerating the reaction kinetics process, in which the bonding interaction difference between Ir-H and Ir-O bonds causes an electronic reconfiguration through asymmetric orbital hybridization. The doped F elements with a lower valence state make more valence electrons revert to the Ir-5d orbitals to reduce the activation energy, leading to a higher catalytic activity. In addition, a stronger bonding interaction at Ir-F bonds also can lead to a higher structural stability. However, this advantage cannot occur at Cl-doped or Br-doped IrO₂ monolayer. This work provides a new insight into designing new-type catalysts for acidic OER.

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用于酸性水电解的卤素掺杂 IrO2 单层轨道杂化的不对称畸变

酸性氧进化反应（OER）的反应活性和结构稳定性不尽如人意，一直是利用水分裂产生氢能的主要瓶颈。在此，我们提出了一种在 1T 相二氧化铱（IrO2）单层中掺杂卤素（H）的策略，以优化其电子结构，从而加速反应动力学过程，其中 Ir-H 键和 Ir-O 键之间的成键相互作用差异通过不对称轨道杂化引起了电子重构。掺杂的 F 元素具有较低的价态，使更多的价电子回到 Ir-5d 轨道，从而降低了活化能，提高了催化活性。此外，Ir-F 键上更强的成键作用也能带来更高的结构稳定性。然而，这种优势在掺Cl或掺Br的IrO2单层中并不存在。这项研究为设计新型酸性 OER 催化剂提供了新的思路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Surface Science 化学-物理：凝聚态物理

CiteScore

3.30

自引率

5.30%

发文量

137

审稿时长

25 days

期刊介绍： Surface Science is devoted to elucidating the fundamental aspects of chemistry and physics occurring at a wide range of surfaces and interfaces and to disseminating this knowledge fast. The journal welcomes a broad spectrum of topics, including but not limited to: • model systems (e.g. in Ultra High Vacuum) under well-controlled reactive conditions • nanoscale science and engineering, including manipulation of matter at the atomic/molecular scale and assembly phenomena • reactivity of surfaces as related to various applied areas including heterogeneous catalysis, chemistry at electrified interfaces, and semiconductors functionalization • phenomena at interfaces relevant to energy storage and conversion, and fuels production and utilization • surface reactivity for environmental protection and pollution remediation • interactions at surfaces of soft matter, including polymers and biomaterials. Both experimental and theoretical work, including modeling, is within the scope of the journal. Work published in Surface Science reaches a wide readership, from chemistry and physics to biology and materials science and engineering, providing an excellent forum for cross-fertilization of ideas and broad dissemination of scientific discoveries.