Journal
ACS CATALYSIS
Volume 11, Issue 11, Pages 6398-6405Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c01386
Keywords
transfer hydrogenation; reduction of aldehydes; single site catalysts; hydrogen donor; 5-hydroxymethylfurfural
Categories
Funding
- National Key Research and Development Program of China [2019YFB1503903]
- National Natural Science Foundation of China [21978248]
- Natural Science Foundation of Fujian Province of China [2019 J06005]
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The usage of ethanol as a hydrogen source for the transfer hydrogenation of aldehydes/ketones shows high activity and selectivity with single-atom Ni-N-4 site catalysts. The presence of single-atom Ni at the pyridinic N active center reduces electron density and achieves high catalytic activity, demonstrating the possibility of catalytic reactions over metal-free sites.
Transfer hydrogenation (TH) of aldehydes/ketones with renewable and nontoxic ethanol is an attractive solution to produce alcohols. Here, we found that single-atom Ni-N-4 site catalysts bring high activity and selectivity for the reduction of hydroxymethyl-functionalized aldehydes/ketones using renewable and nontoxic ethanol as the hydrogen source. When biomass-derived 5-hydroxymethylfurfural was used as the substrate, a turnover frequency (TOF) value of 22 h(-1) for the as-prepared catalyst was achieved. Experiments and simulating computation revealed that pyridinic N of the Ni-N-4 site is the active center and the presence of single-atom Ni reduces the electron density of its coordinated pyridinic N and thus achieves the high catalytic activity, demonstrating the possibility of catalytic TH reactions over metal-free sites.
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