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Photoelectrochemical CO reduction (COR) is an appealing solution for converting carbon dioxide into higher-value products. However, COR in aqueous electrolytes suffers from poor selectivity due to the competitive hydrogen evolution reaction that is dominant on semiconductor surfaces in aqueous electrolytes. We demonstrate that functionalizing gold/p-type gallium nitride devices with a film derived from diphenyliodonium triflate suppresses hydrogen generation from 90% to 18%. As a result, we observe increases in the Faradaic efficiency and partial current density for carbon monoxide of 50% and 3-fold, respectively. Furthermore, we demonstrate through optical absorption measurements that the molecular film employed herein, regardless of thickness, does not affect the photocathode's light absorption. Altogether, this study provides a rigorous platform for elucidating the catalytic structure-property relationships to enable engineering of active, stable, and selective materials for photoelectrochemical COR.
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http://dx.doi.org/10.1021/acs.nanolett.3c03590 | DOI Listing |
J Mater Chem A Mater
December 2024
Department of Materials Engineering, Ben-Gurion University of the Negev Beer Sheva 8410500 Israel
Zinc ferrite (ZnFeO, ZFO) has gained attention as a candidate material for photoelectrochemical water oxidation. However, champion devices have achieved photocurrents far below that predicted by its bandgap energy. Herein, strong optical interference is employed in compact ultrathin film (8-14 nm) Ti-doped ZFO films deposited on specular back reflectors to boost photoanode performance through enhanced light trapping, resulting in a roughly fourfold improvement in absorption as compared to films deposited on transparent substrates.
View Article and Find Full Text PDFAdv Sci (Weinh)
December 2024
Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology (KAIST), 291 Daehak-ro, Yuseong-gu, Daejeon, 34141, South Korea.
Photoelectrochemical (PEC) CO reduction using a photocathode is an attractive method for making valuable chemical products due to its simplicity and lower overpotential requirements. However, previous PEC processes have often been diffusion-limited leading to low production rates of the CO reduction reaction, due to inefficient gas diffusion through the liquid electrolyte to the catalyst surface, particularly at high current densities. In this study, a gas-permeable photocathode in a continuous flow PEC reactor is incorporated, which facilitates the direct supply of CO gas to the photocathode-electrolyte interface, unlike dark reaction-based flow reactors.
View Article and Find Full Text PDFBiosens Bioelectron
December 2024
National Engineering Research Center for Carbohydrate Synthesis, Key Lab of Fluorine and Silicon for Energy Materials and Chemistry of Ministry of Education, Key Laboratory for Green Chemistry of Jiangxi Province, College of Chemistry and Materials, Jiangxi Normal University, Nanchang, 330022, People's Republic of China. Electronic address:
Traditional p-type CuO (pCuO), valued for its tunable band gap and p-type conductivity, has been widely used in photoelectrochemical biosensors. However, its weak conductivity leads to unsatisfied photoelectrochemical signals and limits its use in in situ vulcanization reactions. We synthesized n-type CuO (nCuO) with abundant oxygen vacancies through a simple chemical reduction for the first time, which was applied as efficient photoactive material.
View Article and Find Full Text PDFJ Phys Chem C Nanomater Interfaces
December 2024
Department of Physics, Technical University of Denmark, Fysikvej 307, 2800 Kongens Lyngby, Denmark.
Adv Sci (Weinh)
December 2024
Institute of Materials Research and Engineering (IMRE), Agency for Science, Technology and Research (A*STAR), 2 Fusionopolis Way, Singapore, 138634, Singapore.
Solar hydrogen peroxide (HO) production has garnered increased research interest owing to its safety, cost-effectiveness, environmental friendliness, and sustainability. The synthesis of HO relies mainly on renewable resources such as water, oxygen, and solar energy, resulting in minimal waste. Bismuth vanadate (BiVO) stands out among various oxide semiconductors for selective HO production under visible light via direct two-electron oxygen reduction reaction (ORR) and two-electron water oxidation reaction (WOR) pathways.
View Article and Find Full Text PDFEnter search terms and have AI summaries delivered each week - change queries or unsubscribe any time!