Performance assessment of photoelectrochemical CO₂ reduction photocathodes with patterned electrocatalysts: a multi-physical model-based approach

Chen, Yuzhu1,2; Xiang, Chengxiang3; Lin, Meng1,2

2024-03-01

10.1039/d4ee00575a

ENERGY & ENVIRONMENTAL SCIENCE   影响因子和分区

1754-5692

1754-5706

Photoelectrochemical (PEC) carbon dioxide reduction (CO2R) devices stand as a promising route for converting intermittent solar energy into storable fuels. The performance of the PEC CO2R device requires simultaneous minimization of optical obstruction by the catalyst and maximization of the junction barrier height to facilitate charge separation. A photocathode coated with patterned electrocatalysts is a promising solution due to its flexibility in tuning optics and interfacial charge separation by size and coverage. This study reports typical p-Si photocathodes coated with patterned Ag electrocatalysts for efficient CO2R under various catalyst sizes and coverage designs. Notably, we investigated the effects of patterned electrocatalysts on optical absorption due to obstruction and interfacial barrier height rectification due to the pinch-off effect. A coupled multi-physical model-based framework was developed to quantitatively analyze the trade-offs among optical propagation, charge transport, mass transfer, and electrochemical reactions in a PEC CO2R photocathode. We found that an optimal catalyst coverage of 0.4 can reconcile the interplay between optical reduction and the catalyst's available surface area, leading to an achievable solar-to-carbon monoxide conversion efficiency (eta(CO)) of up to 9.6%, and decreasing the boundary layer thickness of the electrolyte to 25 mu m can achieve a eta(CO) of 11.2%. This modeling framework offers valuable insights into the intricate interplay between optics, charge transport, and electrochemical behavior and provides a potent tool for guiding the engineering of high-performance CO2R photocathodes featuring patterned electrocatalysts.

SCI

英语

第一 ; 通讯

National Natural Science Foundation of China[52376191] ; National Natural Science Foundation of China["GJHZ20210705141808026","20231120185819001","KCXST20221021111207017"] ; Shenzhen Science and Technology Innovation Commission[ZDSYS20220527171403009] ; Shenzhen Key Laboratory of Intelligent Robotics and Flexible Manufacturing Systems[2023A1515011595] ; Guangdong Basic and Applied Basic Research Foundation[2021QN02L562]

Chemistry ; Energy & Fuels ; Engineering ; Environmental Sciences & Ecology

Chemistry, Multidisciplinary ; Energy & Fuels ; Engineering, Chemical ; Environmental Sciences

WOS:001186475300001

ROYAL SOC CHEMISTRY

Web of Science

1.Southern Univ Sci & Technol, Dept Mech & Energy Engn, Shenzhen Key Lab Biomimet Robot & Intelligent Syst, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, SUSTech Energy Inst Carbon Neutral, Shenzhen 518055, Peoples R China
3.CALTECH, Dept Appl Phys & Mat Sci, Liquid Sunlight Alliance, Pasadena, CA 91125 USA

Chen, Yuzhu,Xiang, Chengxiang,Lin, Meng. Performance assessment of photoelectrochemical CO₂ reduction photocathodes with patterned electrocatalysts: a multi-physical model-based approach[J]. ENERGY & ENVIRONMENTAL SCIENCE,2024.

Chen, Yuzhu,Xiang, Chengxiang,&Lin, Meng.(2024).Performance assessment of photoelectrochemical CO₂ reduction photocathodes with patterned electrocatalysts: a multi-physical model-based approach.ENERGY & ENVIRONMENTAL SCIENCE.

Chen, Yuzhu,et al."Performance assessment of photoelectrochemical CO₂ reduction photocathodes with patterned electrocatalysts: a multi-physical model-based approach".ENERGY & ENVIRONMENTAL SCIENCE (2024).