Synergetic Effect of Ultrasmall Metal Clusters and Zeolites Promoting Hydrogen Generation

Sun, Qiming; Wang, Ning; Bai, Risheng; Hui, Yu; Zhang, Tianjun; Do, David A.; Zhang, Peng; Song, Lijuan; Miao, Shu; Yu, Jihong

doi:10.1002/advs.201802350

Synergetic Effect of Ultrasmall Metal Clusters and Zeolites Promoting Hydrogen Generation

Journal Article · Mon Mar 25 00:00:00 EDT 2019 · Advanced Science

DOI:https://doi.org/10.1002/advs.201802350· OSTI ID:1513308

Sun, Qiming ^[1]; Wang, Ning ^[1]; Bai, Risheng ^[1]; Hui, Yu ^[2]; Zhang, Tianjun ^[1]; Do, David A. ^[3]; Zhang, Peng ^[3]; Song, Lijuan ^[2]; Miao, Shu ^[4]; ^[5]

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University 2699 Qianjin Street Changchun 130012 P. R. China
Key Laboratory of Petrochemical Catalytic Science and Technology Liaoning Province Liaoning Shihua University Fushun 113001 China
Department of Chemistry Dalhousie University Halifax Nova Scotia B3H 4R2 Canada
Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University 2699 Qianjin Street Changchun 130012 P. R. China, International Center of Future Science Jilin University 2699 Qianjin Street Changchun 130012 P. R. China

Abstract

Taking advantage of the synergetic effect of confined ultrasmall metal clusters and zeolite frameworks is an efficient strategy for improving the catalytic performance of metal nanocatalysts. Herein, it is demonstrated that the synergetic effect of ultrasmall ruthenium (Ru) clusters and intrinsic Brønsted acidity of zeolite frameworks can significantly promote the hydrogen generation of ammonia borane (AB) hydrolysis. Ultrasmall Ru clusters are embedded onto the silicoaluminophosphate SAPO‐34 ( CHA ) and various aluminosilicate zeolites ( MFI, * BEA , and FAU ) with tunable acidities by a facile incipient wetness impregnation method. Evidenced by high‐resolution scanning transmission electron microscopy, the sub‐nanometric Ru clusters are uniformly distributed throughout the zeolite crystals. The X‐ray absorption spectroscopy measurements reveal the existence of Ru‐H species between Ru clusters and adjacent Brønsted acid sites of zeolites, which could synergistically activate AB and water molecules, significantly enhancing the hydrogen evolution rate of AB hydrolysis. Notably, the Ru/SAPO‐34‐0.8Si (Si/Al = 0.8) and Ru/FAU (Si/Al = 30) catalysts with strong acidities afford high turnover frequency values up to 490 and 627 min ⁻¹ , respectively. These values are more than a 13‐fold enhancement than that of the commercial Ru/C catalyst, and among the top level over other heterogeneous catalysts tested under similar conditions.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)

Sponsoring Organization:: National Key Research and Development Program of China; National Natural Science Foundation of China; USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1513308

Alternate ID(s):: OSTI ID: 1503365
OSTI ID: 1531019

Journal Information:: Advanced Science, Journal Name: Advanced Science Journal Issue: 10 Vol. 6; ISSN 2198-3844

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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