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脱铝β沸石中≡SiOZn-OH巢状结构中孤立铂原子催化的丙烷脱氢反应

Propane Dehydrogenation Catalyzed by Isolated Pt Atoms in ≡SiOZn-OH Nests in Dealuminated Zeolite Beta.

作者信息

Qi Liang, Babucci Melike, Zhang Yanfei, Lund Alicia, Liu Lingmei, Li Jingwei, Chen Yizhen, Hoffman Adam S, Bare Simon R, Han Yu, Gates Bruce C, Bell Alexis T

机构信息

Lawrence Berkeley National Laboratory, Berkeley, California 94720, United States.

Department of Chemical and Biomolecular Engineering, University of California, Berkeley, California 94720, United States.

出版信息

J Am Chem Soc. 2021 Dec 22;143(50):21364-21378. doi: 10.1021/jacs.1c10261. Epub 2021 Dec 9.

Abstract

Atomically dispersed noble metal catalysts have drawn wide attention as candidates to replace supported metal clusters and metal nanoparticles. Atomic dispersion can offer unique chemical properties as well as maximum utilization of the expensive metals. Addition of a second metal has been found to help reduce the size of Pt ensembles in bimetallic clusters; however, the stabilization of isolated Pt atoms in small nests of nonprecious metal atoms remains challenging. We now report a novel strategy for the design, synthesis, and characterization of a zeolite-supported propane dehydrogenation catalyst that incorporates predominantly isolated Pt atoms stably bonded within nests of Zn atoms located within the nanoscale pores of dealuminated zeolite Beta. The catalyst is stable in long-term operation and exhibits high activity and high selectivity to propene. Atomic resolution images, bolstered by X-ray absorption spectra, demonstrate predominantly atomic dispersion of the Pt in the nests and, with complementary infrared and nuclear magnetic resonance spectra, determine a structural model of the nested Pt.

摘要

原子分散的贵金属催化剂作为替代负载型金属簇和金属纳米颗粒的候选物已引起广泛关注。原子分散可以提供独特的化学性质以及对昂贵金属的最大利用率。已发现添加第二种金属有助于减小双金属簇中Pt团簇的尺寸;然而,在非贵金属原子的小巢中稳定孤立的Pt原子仍然具有挑战性。我们现在报告一种新颖的策略,用于设计、合成和表征一种沸石负载的丙烷脱氢催化剂,该催化剂主要包含稳定键合在脱铝β沸石纳米级孔内的Zn原子巢中的孤立Pt原子。该催化剂在长期运行中稳定,并表现出对丙烯的高活性和高选择性。由X射线吸收光谱支持的原子分辨率图像表明Pt在巢中主要呈原子分散状态,并且通过互补的红外光谱和核磁共振光谱确定了嵌套Pt的结构模型。

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