The DOI matches its Crossref record; 1 of the 1 references it cites were found in a registry or an index.
Efficient Subnanometric Gold-Catalyzed Hydrogen Generation via Formic Acid Decomposition under Ambient Conditions
Abstract
Formic acid (FA) has tremendous potential as a safe and convenient source of hydrogen for sustainable chemical synthesis and renewable energy storage, but controlled and efficient dehydrogenation of FA by a robust solid catalyst under ambient conditions constitutes a major challenge. Here, we report that a previously unappreciated combination of subnanometric gold and an acid-tolerant oxide support facilitates the liberation of CO-free H(2) from FA. Applying an ultradispersed gold catalyst comprising TEM-invisible gold subnanoclusters deposited on zirconia to a FA-amine mixture affords turnover frequencies (TOFs) up to 1590 per hour and a turnover number of more than 118,400 at 50 °C. The reaction was accelerated at higher temperatures, but even at room temperature, a significant H(2) evolution (TOFs up to 252 h(-1) after 20 min) can still be obtained. Preliminary mechanistic studies suggest that the reaction is unimolecular in nature and proceeds via a unique amine-assisted formate decomposition mechanism on Au-ZrO(2) interface.
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Citations
Cites
Efficient Dehydrogenation of Formic Acid Using an Iron Catalyst
Boddien, A., Mellmann, D., Gärtner, F., Jackstell, R., Junge, H., Dyson, P. J., Laurenczy, G., Ludwig, R., & Beller, M. (2011) · Science · doi:10.1126/science.1206613 · Cited by 832
Cited by
Jiang, K., Xu, K., Zou, S., & Cai, W.-B. (2014) · Journal of the American Chemical Society · doi:10.1021/ja5008917 · Cited by 434
Yoo, J. S., Christensen, R., Vegge, T., Nørskov, J. K., & Studt, F. (2016) · ChemSusChem · doi:10.1002/cssc.201501197 · Cited by 429
Zhang, S., Metin, Ö., Su, D., & Sun, S. (2013) · Angewandte Chemie International Edition · doi:10.1002/anie.201300276 · Cited by 384
Sun, Q., Wang, N., Bing, Q., Si, R., Liu, J., Bai, R., Zhang, P., Jia, M., & Yu, J. (2017) · Chem · doi:10.1016/j.chempr.2017.07.001 · Cited by 303
Li, Z., Yang, X., Tsumori, N., Liu, Z., Himeda, Y., Autrey, T., & Xu, Q. (2017) · ACS Catalysis · doi:10.1021/acscatal.7b00053 · Cited by 216
Metadata
- Authors
- Bi, Q.-Y., Du, X.-L., Liu, Y.-M., Cao, Y., He, H.-Y., & Fan, K.-N.
- Venue
- Journal of the American Chemical Society
- Publisher
- American Chemical Society (ACS)
- Published
- 2012-05-15
- Volume
- 134
- Issue
- 21
- Pages
- 8926-8933
- ISSN
- 0002-7863 (ISSN-L)
- 1520-5126
- OpenAlex
- W2319191734
- Cited by
- 439
- References
- 1
- FWCI
- 17.41
- Type
- journal article
- Language
- en
- Open access
- closed
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