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Propane Dehydrogenation Catalyzed by Isolated Pt Atoms in ≡SiOZn–OH Nests in Dealuminated Zeolite Beta
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-12-09 , DOI: 10.1021/jacs.1c10261 Liang Qi 1, 2 , Melike Babucci 3 , Yanfei Zhang 1, 2 , Alicia Lund 4 , Lingmei Liu 5, 6 , Jingwei Li 6 , Yizhen Chen 3 , Adam S Hoffman 7 , Simon R Bare 7 , Yu Han 5, 8 , Bruce C Gates 3 , Alexis T Bell 1, 2
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2021-12-09 , DOI: 10.1021/jacs.1c10261 Liang Qi 1, 2 , Melike Babucci 3 , Yanfei Zhang 1, 2 , Alicia Lund 4 , Lingmei Liu 5, 6 , Jingwei Li 6 , Yizhen Chen 3 , Adam S Hoffman 7 , Simon R Bare 7 , Yu Han 5, 8 , Bruce C Gates 3 , Alexis T Bell 1, 2
Affiliation
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.
中文翻译:
脱铝β沸石中≡SiOZn-OH巢中分离的Pt原子催化丙烷脱氢
原子分散的贵金属催化剂作为替代负载金属簇和金属纳米粒子的候选物引起了广泛关注。原子分散可以提供独特的化学性质以及最大限度地利用昂贵的金属。已发现添加第二种金属有助于减小双金属簇中 Pt 系综的尺寸;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。我们现在报告了一种用于设计、合成和表征沸石支撑的丙烷脱氢催化剂的新策略,该催化剂主要包含稳定结合在脱铝沸石 Beta 纳米级孔内的锌原子巢内的孤立 Pt 原子。该催化剂长期运行稳定,表现出高活性和高丙烯选择性。在 X 射线吸收光谱的支持下,原子分辨率图像证明了 Pt 在巢中的主要原子分散,并且利用互补的红外和核磁共振光谱,确定了嵌套 Pt 的结构模型。
更新日期:2021-12-22
中文翻译:
脱铝β沸石中≡SiOZn-OH巢中分离的Pt原子催化丙烷脱氢
原子分散的贵金属催化剂作为替代负载金属簇和金属纳米粒子的候选物引起了广泛关注。原子分散可以提供独特的化学性质以及最大限度地利用昂贵的金属。已发现添加第二种金属有助于减小双金属簇中 Pt 系综的尺寸;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。我们现在报告了一种用于设计、合成和表征沸石支撑的丙烷脱氢催化剂的新策略,该催化剂主要包含稳定结合在脱铝沸石 Beta 纳米级孔内的锌原子巢内的孤立 Pt 原子。该催化剂长期运行稳定,表现出高活性和高丙烯选择性。在 X 射线吸收光谱的支持下,原子分辨率图像证明了 Pt 在巢中的主要原子分散,并且利用互补的红外和核磁共振光谱,确定了嵌套 Pt 的结构模型。