Engineering of Ag@Pd/Al2O3 with varied Pd-shell thickness: Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation

doi:10.1016/j.cjche.2023.06.012

中国化学工程学报 ›› 2023, Vol. 64 ›› Issue (12): 139-148.DOI: 10.1016/j.cjche.2023.06.012

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Engineering of Ag@Pd/Al₂O₃ with varied Pd-shell thickness: Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation

Mingbo Yang¹, Tianxing Yang², Rui Ma³, Sha Li³, Yufei He^1,4,5, Dianqing Li^1,4,5

1. State Key Laboratory of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2. Department of Medicine and Chemical Engineering, Lianyungang Technical College, Lianyungang 222006, China;
3. Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515031, China;
4. Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China;
5. Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China

收稿日期:2023-04-03 修回日期:2023-06-10 出版日期:2023-12-28 发布日期:2024-02-05
通讯作者: Rui Ma,E-mail:marui1840@163.com;Sha Li,E-mail:lisha@ccelab.com.cn;Yufei He,E-mail:yfhe@mail.buct.edu.cn
基金资助:
This work was supported by National Key Research & Development Program of China (2022YFA1506200), the National Natural Science Foundations of China (22078007, 21627813, 21706009, 22002085), Guangdong Basic and Applied Basic Research Foundation (2020A1515110832), the Fundamental Research Funds for the Central Universities (buctrc201921, JD2223), Innovative Achievement Commercialization Service-Platform of Industrial Catalysis, MIIT. R.M. would like to thank Chemistry and Chemical Engineering Guangdong Laboratory for a startup funding support (2111001).

Engineering of Ag@Pd/Al₂O₃ with varied Pd-shell thickness: Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation

Mingbo Yang¹, Tianxing Yang², Rui Ma³, Sha Li³, Yufei He^1,4,5, Dianqing Li^1,4,5

1. State Key Laboratory of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China;
2. Department of Medicine and Chemical Engineering, Lianyungang Technical College, Lianyungang 222006, China;
3. Chemistry and Chemical Engineering Guangdong Laboratory, Shantou 515031, China;
4. Quzhou Institute for Innovation in Resource Chemical Engineering, Quzhou 324000, China;
5. Beijing Engineering Center for Hierarchical Catalysts, Beijing University of Chemical Technology, Beijing 100029, China

Received:2023-04-03 Revised:2023-06-10 Online:2023-12-28 Published:2024-02-05
Contact: Rui Ma,E-mail:marui1840@163.com;Sha Li,E-mail:lisha@ccelab.com.cn;Yufei He,E-mail:yfhe@mail.buct.edu.cn
Supported by:
This work was supported by National Key Research & Development Program of China (2022YFA1506200), the National Natural Science Foundations of China (22078007, 21627813, 21706009, 22002085), Guangdong Basic and Applied Basic Research Foundation (2020A1515110832), the Fundamental Research Funds for the Central Universities (buctrc201921, JD2223), Innovative Achievement Commercialization Service-Platform of Industrial Catalysis, MIIT. R.M. would like to thank Chemistry and Chemical Engineering Guangdong Laboratory for a startup funding support (2111001).

摘要/Abstract

摘要： Bimetallic nanoparticles exhibit a synergistic effect that critically depends on their surface composition, but such promotion mechanisms become vague with varying surface compositions. Here, alumina supported Ag@Pd core–shell and PdAg alloy structure with controlled size and surface compositions were prepared to demonstrate synergetic mechanisms, particularly, ligand and strain effects on activity and ethylene selectivity for acetylene hydrogenation. The performance evaluation indicates that Ag@Pd catalysts with well-controlled Pd-shell thickness can effectively lower apparent activation energy and improve ethylene selectivity. Hydrogenation activity increases from 0.019 to 0.062 s^-1 with decreasing Pd-shell thickness under mild conditions, which is 3–6 times higher than their alloyed and monometallic counterparts. Combined characterizations and density functional theory are conducted to reveal such shell-thickness-dependent performance. The ligand effect arising from Ag alloying in the interface of Ag@Pd_2ML observes the strongest binding of acetylene, but it diminished sharply and the strain effect gets more prevailing with increasing shell thickness. The competition of ethylene desorption and deep-hydrogenation were also investigated to understand the selectivity governing factors, and the selectivity descriptor (0.5BE(C₂H₄) – BE(H)) was built to match the contribution of ligand and strain effect on the different surfaces of Pd-Ag bimetallic NPs. The exploration of synergetic mechanisms among bimetallic NPs with varied structure and surface compositions in this work can help us to deepen the understanding catalyst structure–activity relationship and provide a feasible way to optimize the overall catalytic performance.

关键词: Catalyst, Hydrogenation, Nanostructure, Shell-thickness-dependent performance, Ligand and strain effect

Abstract: Bimetallic nanoparticles exhibit a synergistic effect that critically depends on their surface composition, but such promotion mechanisms become vague with varying surface compositions. Here, alumina supported Ag@Pd core–shell and PdAg alloy structure with controlled size and surface compositions were prepared to demonstrate synergetic mechanisms, particularly, ligand and strain effects on activity and ethylene selectivity for acetylene hydrogenation. The performance evaluation indicates that Ag@Pd catalysts with well-controlled Pd-shell thickness can effectively lower apparent activation energy and improve ethylene selectivity. Hydrogenation activity increases from 0.019 to 0.062 s^-1 with decreasing Pd-shell thickness under mild conditions, which is 3–6 times higher than their alloyed and monometallic counterparts. Combined characterizations and density functional theory are conducted to reveal such shell-thickness-dependent performance. The ligand effect arising from Ag alloying in the interface of Ag@Pd_2ML observes the strongest binding of acetylene, but it diminished sharply and the strain effect gets more prevailing with increasing shell thickness. The competition of ethylene desorption and deep-hydrogenation were also investigated to understand the selectivity governing factors, and the selectivity descriptor (0.5BE(C₂H₄) – BE(H)) was built to match the contribution of ligand and strain effect on the different surfaces of Pd-Ag bimetallic NPs. The exploration of synergetic mechanisms among bimetallic NPs with varied structure and surface compositions in this work can help us to deepen the understanding catalyst structure–activity relationship and provide a feasible way to optimize the overall catalytic performance.

Key words: Catalyst, Hydrogenation, Nanostructure, Shell-thickness-dependent performance, Ligand and strain effect

Mingbo Yang, Tianxing Yang, Rui Ma, Sha Li, Yufei He, Dianqing Li. Engineering of Ag@Pd/Al₂O₃ with varied Pd-shell thickness: Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation[J]. 中国化学工程学报, 2023, 64(12): 139-148.

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Engineering of Ag@Pd/Al₂O₃ with varied Pd-shell thickness: Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation

Engineering of Ag@Pd/Al₂O₃ with varied Pd-shell thickness: Dynamic evolution of ligand and strain effects on acetylene selective hydrogenation

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