Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers

doi:10.1016/j.cjche.2020.05.013

中国化学工程学报 ›› 2020, Vol. 28 ›› Issue (10): 2577-2586.DOI: 10.1016/j.cjche.2020.05.013

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers

Guozhu Liu¹, Hairui Liang¹, Yajie Tian², Bofeng Zhang¹, Li Wang¹

1 Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2 College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475001, China

收稿日期:2020-01-23 修回日期:2020-05-07 出版日期:2020-10-28 发布日期:2020-12-03
通讯作者: Guozhu Liu, Hairui Liang, Yajie Tian, Bofeng Zhang, Li Wang
基金资助:
Financial supports by the National Natural Science Foundation of China (21776210) Science and Technology Research Project of Henan Province (No. 202102210048) are gratefully acknowledged.

Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers

Guozhu Liu¹, Hairui Liang¹, Yajie Tian², Bofeng Zhang¹, Li Wang¹

1 Key Laboratory for Green Chemical Technology of Ministry of Education, School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China;
2 College of Chemistry and Chemical Engineering, Henan University, Kaifeng 475001, China

Received:2020-01-23 Revised:2020-05-07 Online:2020-10-28 Published:2020-12-03
Contact: Guozhu Liu, Hairui Liang, Yajie Tian, Bofeng Zhang, Li Wang
Supported by:
Financial supports by the National Natural Science Foundation of China (21776210) Science and Technology Research Project of Henan Province (No. 202102210048) are gratefully acknowledged.

摘要/Abstract

摘要： Direct synthesis of hydrogen peroxide (DSHP) was studied over Pd loaded on HZSM-5 nanosheets (Pd/ZN). Pd nanoparticles with average size of ca. 4.3 nm were introduced into the adjacent nanosheet layers (thickness of ca. 2.9 nm) by impregnation method. Pd/ZN with theoretical Si/Al molar ratio of 25 showed the highest selectivity for H₂O₂ among the prepared catalysts, together with highest formation rate of H₂O₂ (38.0 mmol·(g cat)^-1·h^-1), 1.9 times than that of Pd supported on conventional HZSM-5 zeolite (Pd/CZ-50). Better catalytic performance of nanosheet catalysts was attributed to the promoted Pd dispersion which promoted H₂ dissociation, more Brønsted acid sites and stronger metal-support interaction which inhibited the dissociation of O-O bond in H₂O₂. The embedded structure sufficiently protected the Pd nanoparticles by space confinement which restrained the Pd leaching, leading to a better catalytic stability with 90% activity retained after 3 cycles, which was almost 3 times than that of Pd/CZ-50 (30.4% activity retained).

关键词: HZSM-5 nanosheets, Palladium catalyst, Silica/alumina molar ratio, Metal-support interaction, Direct synthesis of hydrogen peroxide

Abstract: Direct synthesis of hydrogen peroxide (DSHP) was studied over Pd loaded on HZSM-5 nanosheets (Pd/ZN). Pd nanoparticles with average size of ca. 4.3 nm were introduced into the adjacent nanosheet layers (thickness of ca. 2.9 nm) by impregnation method. Pd/ZN with theoretical Si/Al molar ratio of 25 showed the highest selectivity for H₂O₂ among the prepared catalysts, together with highest formation rate of H₂O₂ (38.0 mmol·(g cat)^-1·h^-1), 1.9 times than that of Pd supported on conventional HZSM-5 zeolite (Pd/CZ-50). Better catalytic performance of nanosheet catalysts was attributed to the promoted Pd dispersion which promoted H₂ dissociation, more Brønsted acid sites and stronger metal-support interaction which inhibited the dissociation of O-O bond in H₂O₂. The embedded structure sufficiently protected the Pd nanoparticles by space confinement which restrained the Pd leaching, leading to a better catalytic stability with 90% activity retained after 3 cycles, which was almost 3 times than that of Pd/CZ-50 (30.4% activity retained).

Key words: HZSM-5 nanosheets, Palladium catalyst, Silica/alumina molar ratio, Metal-support interaction, Direct synthesis of hydrogen peroxide

Guozhu Liu, Hairui Liang, Yajie Tian, Bofeng Zhang, Li Wang. Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers[J]. 中国化学工程学报, 2020, 28(10): 2577-2586.

Guozhu Liu, Hairui Liang, Yajie Tian, Bofeng Zhang, Li Wang. Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers[J]. Chinese Journal of Chemical Engineering, 2020, 28(10): 2577-2586.

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Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers

Direct synthesis of hydrogen peroxide over Pd nanoparticles embedded between HZSM-5 nanosheets layers

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