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用于氨选择性催化氧化的ZSM-5上热稳定的高负载单铜位点

Thermally stable high-loading single Cu sites on ZSM-5 for selective catalytic oxidation of NH.

作者信息

Chen Lu, Guan Xuze, Wu Xinbang, Asakura Hiroyuki, Hopkinson David G, Allen Christopher, Callison June, Dyson Paul J, Wang Feng Ryan

机构信息

Department of Chemical Engineering, University College London, London WC1E 7JE, United Kingdom.

Institute of Chemical Sciences and Engineering, École Polytechnique Fedérale de Lausanne (EPFL), Lausanne CH-1015, Switzerland.

出版信息

Proc Natl Acad Sci U S A. 2024 Jul 30;121(31):e2404830121. doi: 10.1073/pnas.2404830121. Epub 2024 Jul 23.

DOI:10.1073/pnas.2404830121
PMID:39042689
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11295017/
Abstract

Rigorous comparisons between single site- and nanoparticle (NP)-dispersed catalysts featuring the same composition, in terms of activity, selectivity, and reaction mechanism, are limited. This limitation is partly due to the tendency of single metal atoms to sinter into aggregated NPs at high loadings and elevated temperatures, driven by a decrease in metal surface free energy. Here, we have developed a unique two-step method for the synthesis of single Cu sites on ZSM-5 (termed Cu/ZSM-5) with high thermal stability. The atomic-level dispersion of single Cu sites was confirmed through scanning transmission electron microscopy, X-ray absorption fine structure (XAFS), and electron paramagnetic resonance spectroscopy. The Cu/ZSM-5 catalyst was compared to a CuO NP-based catalyst (termed Cu/ZSM-5) in the oxidation of NH to N, with the former exhibiting superior activity and selectivity. Furthermore, operando XAFS and diffuse reflectance infrared Fourier transform spectroscopy studies were conducted to simultaneously assess the fate of the Cu and the surface adsorbates, providing a comprehensive understanding of the mechanism of the two catalysts. The study shows that the facile redox behavior exhibited by single Cu sites correlates with the enhanced activity observed for the Cu/ZSM-5 catalyst.

摘要

在活性、选择性和反应机理方面，对具有相同组成的单位点催化剂和纳米颗粒（NP）分散催化剂进行严格比较的研究有限。这种限制部分是由于在高负载和高温下，单金属原子倾向于烧结成聚集的NP，这是由金属表面自由能的降低所驱动的。在此，我们开发了一种独特的两步法，用于在ZSM-5上合成具有高热稳定性的单铜位点（称为Cu/ZSM-5）。通过扫描透射电子显微镜、X射线吸收精细结构（XAFS）和电子顺磁共振光谱证实了单铜位点的原子级分散。在NH氧化为N的反应中，将Cu/ZSM-5催化剂与基于CuO NP的催化剂（称为Cu/ZSM-5）进行了比较，前者表现出优异的活性和选择性。此外，进行了原位XAFS和漫反射红外傅里叶变换光谱研究，以同时评估Cu和表面吸附物的状态，从而全面了解两种催化剂的机理。研究表明，单铜位点表现出的 facile 氧化还原行为与Cu/ZSM-5催化剂观察到的增强活性相关。 （注：“facile”此处可能有误，结合语境推测可能是“易变的、灵活的”等意思，但需确认原文准确表述）

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/1a1aded1b433/pnas.2404830121fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/0403afb3f18b/pnas.2404830121fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/7bd4c25cf4b9/pnas.2404830121fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/7498dc599017/pnas.2404830121fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/4c094b760d62/pnas.2404830121fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/1a1aded1b433/pnas.2404830121fig05.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/0403afb3f18b/pnas.2404830121fig01.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/7bd4c25cf4b9/pnas.2404830121fig02.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/7498dc599017/pnas.2404830121fig03.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/4c094b760d62/pnas.2404830121fig04.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/e0f3/11295017/1a1aded1b433/pnas.2404830121fig05.jpg

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2
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ACS Catal. 2022 Dec 16;12(24):15207-15217. doi: 10.1021/acscatal.2c04863. Epub 2022 Nov 29.
3
Strikingly distinctive NH-SCR behavior over Cu-SSZ-13 in the presence of NO.
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Nat Commun. 2022 Aug 8;13(1):4606. doi: 10.1038/s41467-022-32136-z.
4
Assessing the Influence of Zeolite Composition on Oxygen-Bridged Diamino Dicopper(II) Complexes in Cu-CHA DeNO Catalysts by Machine Learning-Assisted X-ray Absorption Spectroscopy.通过机器学习辅助的X射线吸收光谱法评估沸石组成对Cu-CHA脱硝催化剂中氧桥连二氨基二铜（II）配合物的影响。
J Phys Chem Lett. 2022 Jul 7;13(26):6164-6170. doi: 10.1021/acs.jpclett.2c01107. Epub 2022 Jun 28.
5
A minireview on the synthesis of single atom catalysts.关于单原子催化剂合成的一篇综述短文。
RSC Adv. 2022 Mar 24;12(15):9373-9394. doi: 10.1039/d2ra00657j. eCollection 2022 Mar 21.
6
Single-Site vs. Cluster Catalysis in High Temperature Oxidations.高温氧化中的单中心催化与簇催化
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7
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