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Title: Synergetic Effect of Ultrasmall Metal Clusters and Zeolites Promoting Hydrogen Generation

Journal Article · · Advanced Science
 [1];  [1];  [1];  [2];  [1];  [3];  [3];  [2];  [4]; ORCiD logo [5]
  1. State Key Laboratory of Inorganic Synthesis and Preparative Chemistry College of Chemistry Jilin University 2699 Qianjin Street Changchun 130012 P. R. China
  2. Key Laboratory of Petrochemical Catalytic Science and Technology Liaoning Province Liaoning Shihua University Fushun 113001 China
  3. Department of Chemistry Dalhousie University Halifax Nova Scotia B3H 4R2 Canada
  4. Dalian Institute of Chemical Physics Chinese Academy of Sciences Dalian 116023 P. R. China
  5. 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
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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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE Office of Science (SC); National Key Research and Development Program of China; National Natural Science Foundation of China (NSFC)
Grant/Contract Number:
DE‐AC02‐06CH11357; AC02-06CH11357; 2016YFB0701100; 21835002; 21621001
OSTI ID:
1513308
Alternate ID(s):
OSTI ID: 1503365; OSTI ID: 1531019
Journal Information:
Advanced Science, Journal Name: Advanced Science Vol. 6 Journal Issue: 10; ISSN 2198-3844
Publisher:
Wiley Blackwell (John Wiley & Sons)Copyright Statement
Country of Publication:
Germany
Language:
English
Citation Metrics:
Cited by: 58 works
Citation information provided by
Web of Science

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