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Solar-Driven CO2 Conversion via Optimized Photothermal Catalysis in a Lotus Pod Structure
Authors:Hongmin Wang  Shuting Fu  Bo Shang  Sungho Jeon  Yiren Zhong  Nia J. Harmon  Chungseok Choi  Eric A. Stach  Hailiang Wang
Affiliation:1. Department of Chemistry, Yale University, CT 06520 New Haven, USA;2. Department of Chemistry, Yale University, CT 06520 New Haven, USA

Energy Sciences Institute, Yale University, CT 06516 West Haven, USA;3. Department of Materials Science and Engineering, University of Pennsylvania, PA 19104 Philadelphia, USA

Abstract:Photothermal CO2 reduction is one of the most promising routes to efficiently utilize solar energy for fuel production at high rates. However, this reaction is currently limited by underdeveloped catalysts with low photothermal conversion efficiency, insufficient exposure of active sites, low active material loading, and high material cost. Herein, we report a potassium-modified carbon-supported cobalt (K+−Co−C) catalyst mimicking the structure of a lotus pod that addresses these challenges. As a result of the designed lotus-pod structure which features an efficient photothermal C substrate with hierarchical pores, an intimate Co/C interface with covalent bonding, and exposed Co catalytic sites with optimized CO binding strength, the K+−Co−C catalyst shows a record-high photothermal CO2 hydrogenation rate of 758 mmol gcat−1 h−1 (2871 mmol gCo−1 h−1) with a 99.8 % selectivity for CO, three orders of magnitude higher than typical photochemical CO2 reduction reactions. We further demonstrate with this catalyst effective CO2 conversion under natural sunlight one hour before sunset during the winter season, putting forward an important step towards practical solar fuel production.
Keywords:CO2 Hydrogenation  Hybrid Material  Photothermal Catalysis  Reverse Water-Gas Shift  Solar Fuel
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