Journal
ACS NANO
Volume 14, Issue 2, Pages 2099-2108Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsnano.9b08792
Keywords
CO2 reduction; energy; solar-driven; copper; electrochemistry; in situ Raman; hydrocarbons
Categories
Funding
- Illinois Institute of Technology
- Wanger Institute for Sustainable Energy Research (WISER) [262029 221E 2300]
- Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource seed funding at Northwestern University
- NSF [DMR-1809439]
- MRSEC Materials Preparation and Measurement Laboratory [NSF DMR1420709]
- MRSEC program at the Materials Research Center [NSF DMR-1121262]
- Nanoscale Science and Engineering Center at the International Institute for Nano technology [NSF EEC -0647560]
- State of Illinois, through the International Institute for Nanotechnology
- MRI-R2 grant from the National Science Foundation [DMR-0959470]
- Department of Energy
- DOE Office of Science [DE-AC02-06CH 11357]
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Solar conversion of carbon dioxide (CO2) into hydrocarbon fuels offers a promising approach to fulfill the world's ever-increasing energy demands in a sustainable way. However, a highly active catalyst that can also tune the selectivity toward desired products must be developed for an effective process. Here, we present oxygen functionalized copper (OFn-Cu) nanoparticles as a highly active and methane (CH4) selective catalyst for the electrocatalytic CO2 reduction reaction. Our electrochemical results indicate that OFn-Cu (5nm) nanoparticles with an oxidized layer at the surface reach a maximum CH4 formation current density and turnover frequency of 36.24 mA/cm(2) and of 0.17 s(-1) at the potential of -1.05 V vs RHE, respectively, exceeding the performance of existing Cu and Cu-based catalysts. Characterization results indicate that the surface of the OFn-Cu nanoparticles consists of an oxygen functionalized layer in the form of Cu2+ (CuO) separated from the underneath elemental Cu by a Cu+ (Cu2O) sublayer. Density functional theory calculations also confirm that presence of the 0 site at the CuO (101) surface is the main reason for the enhanced activity and selectivity. Using this catalyst, we have demonstrated a flow cell with an active area of 25 cm 2 that utilizes solar energy to produce 7.24 L of CH4 after 10 h of continuous process at a cell power density of 30 mW/cm(2).
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