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Photoelectrocatalytic reduction of CO2 to formate using immobilized molecular manganese catalysts on oxidized porous silicon

Journal Article · · Chem
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  1. Yale University, New Haven, CT (United States); Sogang University, Seoul (Korea, Republic of)
  2. Yale University, New Haven, CT (United States)
  3. University of North Carolina at Chapel Hill, NC (United States)
  4. University of Pennsylvania, Philadelphia, PA (United States)
+ Show Author Affiliations
The reduction of carbon dioxide (CO2) to formate using molecular catalysts immobilized on high surface area porous silicon is described. Manganese complexes of the type (Rbpy)Mn(CO)3Br (bpy = 2,2′-bipyridine) were prepared with silatrane groups on the bpy ligand for attachment to oxide-coated porous silicon (SiOx-porSi). SiOx-porSi wafers were formed by heating hydrogen-terminated p-type porous silicon wafers under air, and the manganese complexes were immobilized on SiOx-porSi by heating at 80°C. The resulting hybrid photoelectrodes are photoelectrocatalysts for CO2 reduction in acetonitrile containing 2.0 M triethylamine and 2.0 M isopropanol, yielding formate with high selectivity (>96%) and current density (∼0.6 mA/cm2), excellent reproducibility, and a photovoltage of 280 mV at −1.75 V (versus ferrocenium/ferrocene) under 1 sun illumination. Here, the applied potential is close to the equilibrium potential for CO2 reduction to formate. This work presents rare examples of immobilized molecular catalysts for CO2 reduction to formate and the first on semiconducting silicon.
Research Organization:
Sogang University, Seoul (Korea, Republic of); University of North Carolina at Chapel Hill, NC (United States); University of Pennsylvania, Philadelphia, PA (United States); Yale University, New Haven, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0021173
OSTI ID:
2575196
Journal Information:
Chem, Journal Name: Chem Journal Issue: 7 Vol. 11; ISSN 2451-9294; ISSN CHEMVE
Publisher:
Cell PressCopyright Statement
Country of Publication:
United States
Language:
English

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Photoelectrochemical CO2 Reduction to CO Enabled by a Molecular Catalyst Attached to High-Surface-Area Porous Silicon
Journal Article · Thu Mar 14 20:00:00 EDT 2024 · Journal of the American Chemical Society · OSTI ID:2377746

Related Subjects

13 HYDRO ENERGY
14 SOLAR ENERGY
17 WIND ENERGY
29 ENERGY PLANNING, POLICY, AND ECONOMY
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATION
CO2 reduction
base-metal catalysis
formate production
immobilized catalysts
photoelectrocatalysis
porous silicon