期刊
CHEMICAL SCIENCE
卷 10, 期 22, 页码 5712-5718出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c9sc01539f
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资金
- Japan Society for the Promotion of Science (JSPS) [17H06153]
- JSPS [18J00745]
- Ministry of Science and Technology of the People's Republic of China (MOST) [2018YFA0208603, 2016YFA0200602]
- National Natural Science Foundation of China (NSFC) [21573204]
- Anhui Initiative in Quantum Information Technologies [AHY090400]
- Fundamental Research Funds for the Central Universities
- National Program for Support of Top-Notch Young Professional
- External Cooperation Program of BIC CAS [211134KYSB20130017]
- Grants-in-Aid for Scientific Research [18J00745] Funding Source: KAKEN
Ruthenium (Ru) loaded catalysts are of significant interest for ammonia synthesis under mild reaction conditions. The B-5 sites have been reported as the active sites for ammonia formation, i.e., Ru with other coordinations were inactive, which has limited the utilization efficiency of Ru metal. The implantation of Ru into intermetallic compounds is considered to be a promising approach to tune the catalytic activity and utilization efficiency of Ru. Here we report an acid-durable electride, LnRuSi (Ln = La, Ce, Pr and Nd), as a B-5-site-free Ru catalyst. The active Ru plane with a negative charge is selectively exposed by chemical etching using disodium dihydrogen ethylenediaminetetraacetate (EDTA-2Na) acid, which leads to 2-4-fold enhancement in the ammonia formation rate compared with that of the original catalyst. The turnover frequency (TOF) of LnRuSi is estimated to be approximately 0.06 s(-1), which is 600 times higher than that of pure Ru powder. Density functional theory (DFT) calculations revealed that the dissociation of N-2 occurs easily on the exposed Ru plane of LaRuSi. This systematic study provides firm evidence that layered Ru with a negative charge in LnRuSi is a new type of active site that differs significantly from B-5 sites.
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