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

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
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引用次数: 0

摘要

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

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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来源期刊
Surface Science
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.
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