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在Ga₂O₃表面通过固态NMR光谱直接检测反应性化物种

Hongyu Chen^1,2, Pan Gao¹, Zhengmao Liu^1,2

¹State Key Laboratory of Catalysis, Dalian National Laboratory for Clean Energy, 2011-Collaborative Innovation Center of Chemistry for Energy Materials, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, 457 Zhongshan Road, Dalian 116023, China.

Journal of the American Chemical Society

|September 14, 2022

概括

研究人员使用先进的NMR在氧化 (Ga2O3) 催化剂上直接检测出高度反应的表面化物 (Ga-H). 这一突破揭示了Ga-H中间体在关键催化反应中的关键作用.

科学领域:

不同质的催化
表面化学
固态核磁共振光谱

背景情况:

表面金属化物 (M-H) 在催化中至关重要,但由于高反应性和复杂的催化剂表面,难以表征.
在实际的催化剂上直接检测像化 (Ga-H) 这样的反应性表面物种仍然是一个重大挑战.

研究的目的:

提供第一个在H2激活过程中对Ga2O3催化剂高度反应的表面化物 (Ga-H) 的直接和明确的NMR证据.
阐明Ga-H物种的形成机制,地点规格和结构配置以及H2解离机制.
证明表面Ga-H作为催化反应中无处不在的中间体的关键作用.

主要方法:

与先进的固态NMR光谱相结合即时火捕获.
在1H NMR信号上区分69Ga和71Ga的同位素效应,以清晰识别Ga-H.
量化和二维核磁共振技术,以及密度函数理论 (DFT) 的计算.

主要成果:

在Ga2O3催化剂上直接和明确地检测表面Ga-H.
使用同位素效应清晰区分Ga-H信号与基.
阐明Ga-H形成机制,H2解离途径和特定地点的信息.
确认表面Ga-H中间体在脱和二氧化碳化中的重要作用.

结论:

这项研究提出了一种新的分析方法,用于表层反应性金属化物.
表面的Ga-H物种在重要的催化过程中扮演着关键的,以前未经证实的中间体角色.
这些发现为设计更高效的基催化剂提供了宝贵的见解,并可扩展到其他M-H分析.

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