纤维状中孔硅胶KCC-1负载的钯纳米颗粒上甲酸催化脱氢反应

doi:10.1016/S1872-2067(19)63303-6

催化学报 ›› 2019, Vol. 40 ›› Issue (11): 1704-1712.DOI: 10.1016/S1872-2067(19)63303-6

纤维状中孔硅胶KCC-1负载的钯纳米颗粒上甲酸催化脱氢反应

Siqian Zhan, Yingjie Qia, Wha-Seung Ahn

仁荷大学化学与化学工程系, 仁川 402-751, 韩国

收稿日期:2018-12-09 修回日期:2019-01-14 出版日期:2019-11-18 发布日期:2019-09-06
通讯作者: Wha-Seung Ahn
基金资助:
This work was supported by C1 Gas Refinery Program (2015M3D3A1A01064899) by the Ministry of Science, ICT & Future Planning, and also by Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (Grant No.:NRF-2015R1A4A1042434).

Catalytic dehydrogenation of formic acid over palladium nanoparticles immobilized on fibrous mesoporous silica KCC-1

Siqian Zhang, Yingjie Qian, Wha-Seung Ahn

Department of Chemistry and Chemical Engineering, Inha University, Incheon 402-751, Republic of Korea

Received:2018-12-09 Revised:2019-01-14 Online:2019-11-18 Published:2019-09-06
Contact: Wha-Seung Ahn
Supported by:
This work was supported by C1 Gas Refinery Program (2015M3D3A1A01064899) by the Ministry of Science, ICT & Future Planning, and also by Basic Science Research Program through the National Research Foundation of Korea funded by the Ministry of Education (Grant No.:NRF-2015R1A4A1042434).

摘要/Abstract

摘要： 在N-（3-三甲氧基硅丙基）二乙烯三胺（PDETA）功能化的纤维状硅胶KCC-1上负载了均一的、平均粒径为2.8 nm的Pd纳米粒子（Pd/KCC-1-PDETA），采用粉末X射线衍射、X射线光电子能谱和N₂吸附-脱附等温线对其进行了表征，并将其作为催化剂用于无添加剂的甲酸脱氢制H₂的反应中.同时还制备了另外两个中孔硅胶材料（MSF和KIT-6）负载的Pd纳米粒子，以考察反应中催化剂的载体效应.结果表明，Pd/KCC-1-PDETA催化剂表现出很高的催化性能（323 K时TOF值为332 h^-1，氢气选择性100%）.这归结为KCC-1独特的纤维状形貌和胺基基团的存在，从而降低了Pd颗粒尺寸，促进了反应物与催化活性位Pd的接触.还考察了Pd负载量（2-10 wt%）、反应温度和反应时间对脱氢反应性能的影响.反应结束后，Pd/KCC-1-PDETA催化剂容易回收，可重复使用5次而催化性能未见明显下降，表现出较好的重复使用性能.

关键词: 纤维状纳米硅胶, KCC-1, 钯纳米颗粒, 储氢, 甲酸脱氢

Abstract: Uniform Pd nanoparticles immobilized on N-(3-trimethoxysilylpropyl)diethylenetriamine (PDETA)-functionalized fibrous silica KCC-1 (Pd/KCC-1-PDETA) were prepared with a mean Pd particle size of 2.8 nm. After characterization using powder X-ray diffraction, X-ray photoelectron spectroscopy, and N₂ adsorption-desorption isotherms, Pd/KCC-1-PDETA was used as catalyst for additive-free dehydrogenation of formic acid to produce H₂. Pd nanoparticle catalysts supported on two other mesoporous silica materials (MSF and KIT-6) were also synthesized to examine how the support affects the reaction. Among the three catalysts, Pd/KCC-1-PDETA exhibited significant catalytic activity (a turnover frequency of 332 h^-1 at 323 K and 100% selectivity towards hydrogen), owing to the unique fibrous morphology of KCC-1 and the presence of amine groups that reduced the Pd particle size and improved the access of reactant to the catalytically active Pd sites. The influence of Pd loading (2-10 wt.%), reaction temperature, and reaction time was also examined for the dehydrogenation reaction. Pd/KCC-1-PDETA was recovered easily after the reaction and showed good reusability up to five times without any significant loss in catalytic performance.

Key words: Fibrous nanosilica, KCC-1, Palladium nanoparticles, Hydrogen storage, Formic acid dehydrogenation

Siqian Zhan, Yingjie Qia, Wha-Seung Ahn. 纤维状中孔硅胶KCC-1负载的钯纳米颗粒上甲酸催化脱氢反应[J]. 催化学报, 2019, 40(11): 1704-1712.

Siqian Zhang, Yingjie Qian, Wha-Seung Ahn. Catalytic dehydrogenation of formic acid over palladium nanoparticles immobilized on fibrous mesoporous silica KCC-1[J]. Chinese Journal of Catalysis, 2019, 40(11): 1704-1712.

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纤维状中孔硅胶KCC-1负载的钯纳米颗粒上甲酸催化脱氢反应

Catalytic dehydrogenation of formic acid over palladium nanoparticles immobilized on fibrous mesoporous silica KCC-1

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