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Biomolecule-inspired synthesis of framework zinc in MFI zeolite for propane dehydrogenation
Microporous and Mesoporous Materials ( IF 4.8 ) Pub Date : 2022-11-24 , DOI: 10.1016/j.micromeso.2022.112371
Xunming Su , Zhong-Pan Hu , Jingfeng Han , Yuhong Jia , Shutao Xu , Jin Zhang , Dong Fan , Yingxu Wei , Zhongmin Liu

The development of environment-friendly, stable, and efficient catalysts to substitute Pt and Cr-based catalysts for propane dehydrogenation (PDH) is of great importance but challenging to make. Herein, we use zinc gluconate (Zn(C6H12O7)2), an organometallic biomolecule, to embed Zn atoms into pure silica MFI zeolite framework (Zn-MFI) for PDH reaction. Due to the protection by the glucosyl groups in Zn(C6H12O7)2, Zn atoms can be well embedded into the MFI zeolite framework. Multi-scale characterizations (e.g., Cs-corrected HAADF-STEM, FTIR, UV–vis, and NMR spectroscopy) and DFT calculations demonstrate the formation of uniform tetrahedrally coordinated Zn sites in the MFI zeolite framework with two Zn–O–Si and two Zn⋯OH–Si linkages ({(≡SiO)2Zn(HO–Si≡)2}). The Zn-MFI zeolites are used for PDH, exhibiting excellent catalytic performance. Pyridine-FTIR, C3H6-FTIR, C3H6-TPD/MS, and contrast experiments reveal the unique Zn active sites in Zn-MFI zeolites can promote the C–H bond cleavage and weaken the propylene adsorption, thus guaranteeing high activity and selectivity for PDH. The excellent catalytic performance of Zn-MFI zeolites indicates their promising utilization in industry.



中文翻译:

生物分子启发合成 MFI 沸石骨架锌用于丙烷脱氢

开发环境友好、稳定、高效的催化剂来替代 Pt 和 Cr 基丙烷脱氢 (PDH) 催化剂具有重要意义,但制造难度很大。在此,我们使用葡萄糖酸锌 (Zn(C 6 H 12 O 7 ) 2 ),一种有机金属生物分子,将 Zn 原子嵌入纯二氧化硅 MFI 沸石骨架 (Zn-MFI) 中进行 PDH 反应。由于Zn(C 6 H 12 O 7 ) 2中的糖基保护,Zn原子可以很好地嵌入到MFI沸石骨架中。多尺度表征(例如,C s-校正的 HAADF-STEM、FTIR、UV-vis 和 NMR 光谱)和 DFT 计算表明在具有两个 Zn-O-Si 和两个 Zn⋯OH-Si 键的 MFI 沸石骨架中形成了均匀的四面体配位 Zn 位点({ (≡SiO) 2 Zn(HO–Si≡) 2 })。Zn-MFI沸石用于PDH,表现出优异的催化性能。吡啶-FTIR、C 3 H 6 -FTIR、C 3 H 6 -TPD/MS和对比实验表明,Zn-MFI沸石中独特的Zn活性位点可以促进C-H键断裂,削弱丙烯吸附,从而保证对 PDH 具有高活性和选择性。Zn-MFI 沸石优异的催化性能表明其在工业上的应用前景广阔。

更新日期:2022-11-28
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