Journal
ISCIENCE
Volume 16, Issue -, Pages 390-+Publisher
CELL PRESS
DOI: 10.1016/j.isci.2019.06.005
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Funding
- National Natural Science Foundation of China [51801235, 11875258, 11505187]
- Start-up Funding of Central South University [502045005]
- Fundamental Research Funds for the Central Universities of Central South University [2018zzts402]
- Fundamental Research Funds for the Central Universities [WK2310000066, WK2060190081]
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N-functionalization of amines with CO2 and H-2 is one of the most important processes to make use of CO2. Although noble metal-based catalysts with remarkable performance have been widely used in this process, developing efficient non-noble-metal-based catalysts remains a grand challenge. Herein, we report In2O3 nanocrystals with high density of grain boundaries (HGB-In2O3), which show excellent activity toward methylation of amines. Impressively, HGB-In2O3 achieved the optimal yield of 82.7% for N,N-dimethylaniline with a mass activity of 21.2 mmol.g(-1) h(-1) in methylation of N-methylaniline, comparable to noble-metal-based catalysts. As a bonus, HGB-In2O3 held noticeable stability, remarkable selectivity, and comprehensive applicability. Further mechanistic studies revealed that the presence of high density of grain boundaries not only facilitated the adsorption and activation of CO2 to generate CH3OH as the intermediate but also enhanced the activation of N-H bond in amines, contributing to the attractive activity of HGB-In2O3 toward methylation of amines.
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