Journal
ACS CATALYSIS
Volume 11, Issue 18, Pages 11696-11705Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.1c01939
Keywords
metal-organic framework; CO2 reduction; ethylene production; supported copper catalyst
Categories
Funding
- Ministry of Science and Technology of China [2016YFA0200702]
- National Natural Science Foundation of China [22071207, 21721001]
- NFFTBS [J1310024]
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A new tandem route for the conversion of CO2 to C2H4 via CO2 hydrogenation to ethanol followed by ethanol dehydration is presented in this study. Multiple Cu(I) centers loaded onto a Ti-based metal-organic framework catalyzed the conversion, achieving high CO2-to-C2H4 generation rates. This work opens up another path for selectively producing C2H4 through the hydrogenation of CO2.
Hydrogenation of carbon dioxide (CO2) to ethylene (C2H4) can be achieved in two routes via tandem reactions: (1) CO2 hydrogenation to methanol (CH3OH) followed by methanol-to-olefin conversion and (2) reverse water-gas shift reaction followed by Fischer-Tropsch synthesis. Here we present another tandem route for CO2-to-C2H4 conversion via (3) CO2 hydrogenation to ethanol (C2H5OH) followed by C2H5OH dehydration. Multiple cuprous (Cu-I) centers were loaded onto the Ti-8(mu(2)-O)(8)(mu(2)-OH)(4) secondary building units of a Ti-based metal-organic framework (MOF), MIL-125-NH2, via deprotonation and ion exchange of the mu(2)-OH groups. These multiple Cu-I centers catalyzed CO2 hydrogenation to C2H5OH, while the Ti-2-mu(2)-O-M+ (M+ = H+, Li+) sites converted C2H5OH to C2H4. The MOF achieved CO2-to-C2H4 generation rates of up to 2598 mu mol g(Cat)(-1) h(-1) in supercritical CO2 (CO2 30 MPa, H-2 5 MPa) at 85 degrees C and 514 mu mol g(Cat)(-1) h(-1) in the gas phase at 5 MPa (H-2:CO2 = 3) and 100 degrees C, respectively. This work opens another path to selectively producing C2H4 via the hydrogenation of CO2.
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