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A Theory-Guided X-ray Absorption Spectroscopy Approach for Identifying Active Sites in Atomically Dispersed Transition-Metal Catalysts
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-11-22 , DOI: 10.1021/jacs.1c07116 Yizhen Chen 1 , Rachita Rana 1 , Tyler Sours 1 , Fernando D Vila 2 , Shaohong Cao 3 , Thomas Blum 4 , Jiyun Hong 5 , Adam S Hoffman 5 , Chia-Yu Fang 6 , Zhennan Huang 3 , Chunyan Shang 7 , Chuanhao Wang 7 , Jie Zeng 7 , Miaofang Chi 3 , Coleman X Kronawitter 1 , Simon R Bare 5 , Bruce C Gates 1 , Ambarish R Kulkarni 1
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-11-22 , DOI: 10.1021/jacs.1c07116 Yizhen Chen 1 , Rachita Rana 1 , Tyler Sours 1 , Fernando D Vila 2 , Shaohong Cao 3 , Thomas Blum 4 , Jiyun Hong 5 , Adam S Hoffman 5 , Chia-Yu Fang 6 , Zhennan Huang 3 , Chunyan Shang 7 , Chuanhao Wang 7 , Jie Zeng 7 , Miaofang Chi 3 , Coleman X Kronawitter 1 , Simon R Bare 5 , Bruce C Gates 1 , Ambarish R Kulkarni 1
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Atomically dispersed supported metal catalysts offer new properties and the benefits of maximized metal accessibility and utilization. The characterization of these materials, however, remains challenging. Using atomically dispersed platinum supported on crystalline MgO (chosen for its well-defined bonding sites) as a prototypical example, we demonstrate how systematic density functional theory calculations for assessing all the potentially stable platinum sites, combined with automated analysis of extended X-ray absorption fine structure (EXAFS) spectra, leads to unbiased identification of isolated, surface-enveloped platinum cations as the catalytic species for CO oxidation. The catalyst has been characterized by atomic-resolution imaging and EXAFS and high-energy resolution fluorescence detection X-ray absorption near edge spectroscopy. The proposed platinum sites are in agreement with experiment. This theory-guided workflow leads to rigorously determined structural models and provides a more detailed picture of the structure of the catalytically active site than what is currently possible with conventional EXAFS analyses. As this approach is efficient and agnostic to the metal, support, and catalytic reaction, we posit that it will be of broad interest to the materials characterization and catalysis communities.
中文翻译：
一种用于识别原子分散过渡金属催化剂活性位点的理论引导 X 射线吸收光谱方法
原子分散的负载型金属催化剂提供了新的特性以及最大限度地提高金属可及性和利用率的好处。然而，这些材料的表征仍然具有挑战性。以结晶 MgO 上负载的原子分散铂（因其明确定义的键合位点而选择）作为典型示例，我们展示了系统密度泛函理论计算如何评估所有潜在稳定的铂位点，并结合扩展 X 射线吸收的自动分析精细结构 (EXAFS) 光谱，导致对孤立的、表面包覆的铂阳离子作为 CO 氧化的催化物质的无偏鉴定。该催化剂已通过原子分辨率成像和 EXAFS 以及高能分辨率荧光检测 X 射线吸收近边光谱表征。提议的铂位点与实验一致。这种以理论为指导的工作流程导致了严格确定的结构模型，并提供了比目前传统 EXAFS 分析更详细的催化活性位点结构图。由于这种方法对金属、载体和催化反应有效且不可知，因此我们认为它将对材料表征和催化界产生广泛的兴趣。
更新日期：2021-12-08
中文翻译：
一种用于识别原子分散过渡金属催化剂活性位点的理论引导 X 射线吸收光谱方法
原子分散的负载型金属催化剂提供了新的特性以及最大限度地提高金属可及性和利用率的好处。然而，这些材料的表征仍然具有挑战性。以结晶 MgO 上负载的原子分散铂（因其明确定义的键合位点而选择）作为典型示例，我们展示了系统密度泛函理论计算如何评估所有潜在稳定的铂位点，并结合扩展 X 射线吸收的自动分析精细结构 (EXAFS) 光谱，导致对孤立的、表面包覆的铂阳离子作为 CO 氧化的催化物质的无偏鉴定。该催化剂已通过原子分辨率成像和 EXAFS 以及高能分辨率荧光检测 X 射线吸收近边光谱表征。提议的铂位点与实验一致。这种以理论为指导的工作流程导致了严格确定的结构模型，并提供了比目前传统 EXAFS 分析更详细的催化活性位点结构图。由于这种方法对金属、载体和催化反应有效且不可知，因此我们认为它将对材料表征和催化界产生广泛的兴趣。
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