H2 dissociation barrier governed by antibonding-state center in defective graphene-supported Cu19 cluster

IF 1.8 4区化学 Q3 CHEMISTRY, PHYSICAL

Surface Science Pub Date : 2025-06-10 DOI:10.1016/j.susc.2025.122801

Naigui Liu , Delu Gao , Dunyou Wang

引用次数: 0

Abstract

The dissociation of H₂ is crucial for hydrogen storage and industrial hydrogenation processes. This study employs ab initio molecular dynamics calculations to explore the mechanisms of H₂ dissociation on Cu₁₉ clusters and Cu₁₉ clusters supported by defective graphene. The findings indicate that the defective graphene-supported Cu₁₉ cluster exhibits more dissociation processes compared to the standalone Cu₁₉ cluster, with each corresponding process also having a lower energy barrier. Analysis using crystal orbital Hamilton population at the transition states reveals that for both cluster types, a higher center of the H₂ antibonding state correlates with a reduced dissociation barrier. Furthermore, the reduction in the dissociation barrier on the defective graphene-supported Cu₁₉ cluster is linked to an upward shift in the H₂ antibonding-state center relative to that on the Cu₁₉ cluster alone.

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缺陷石墨烯支持的Cu19簇中H2解离势垒由反键态中心控制

氢气的解离是氢储存和工业加氢过程的关键。本研究采用从头算分子动力学方法探讨了H2在Cu19团簇和缺陷石墨烯支持的Cu19团簇上的解离机制。研究结果表明，与独立的Cu19团簇相比，缺陷石墨烯支持的Cu19团簇表现出更多的解离过程，每个相应的解离过程也具有更低的能垒。利用过渡态的晶体轨道Hamilton居群分析表明，对于这两种类型的簇，H2反键态中心越高，解离势垒越低。此外，在有缺陷的石墨烯支持的Cu19簇上，解离势垒的减少与H2反键态中心相对于单独的Cu19簇的向上移动有关。

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.