Journal
ACS CATALYSIS
Volume 9, Issue 12, Pages 11335-11340Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b04187
Keywords
CO2 hydrogenation; cobalt catalyst; nickel; ethanol; reaction intermediate; C-C coupling
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Funding
- National Key Research and Development Program of China [2018YFB0604801]
- National Natural Science Foundation of China [21822203, 91645105, 91634201]
- Natural Science Foundation of Zhejiang Province [LR18B030002]
- Fundamental Research Funds for the Central Universities
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Selective hydrogenation of CO2 into valuable ethanol proceeds by the coupling of appropriate C-1 intermediates to form C-2-oxygenates. Matching the different C-1 intermediates is crucial for this process but is difficult to control. We found that incorporation of nickel species into the cobalt catalyst could boost the formation of relatively stable *CHx intermediate from CO2 hydrogenation, which significantly avoids an occurrence of methanation. The *CHx species subsequently insert into the *HCOO, another intermediate that is easily formed, to produce C-2-oxygenates. Following this pathway, the optimized catalyst, Co0.52Ni0.48AlOx, gives the ethanol yield at 15.8 mmol g(cat)(-1) with selectivity at 85.7% in the CO2 hydrogenation at 200 degrees C for 12 h, which even outperforms those of noble metal catalysts.
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