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Molecular Additives Improve the Selectivity of CO 2 Photoelectrochemical Reduction over Gold Nanoparticles on Gallium Nitride
Journal article   Peer reviewed

Molecular Additives Improve the Selectivity of CO 2 Photoelectrochemical Reduction over Gold Nanoparticles on Gallium Nitride

Aisulu Aitbekova, Nicholas Watkins, Matthias H Richter, Phillip Jahelka, Jonas C Peters, Theodor Agapie, Harry A Atwater and California Institute of Technology (CalTech), Pasadena, CA (United States)
Nano letters, v 24(4), pp 1090-1095
17 Jan 2024
PMID: 38230969

Abstract

catalyst microenvironment photoelectrochemistry solar fuels semiconductor
Photoelectrochemical CO reduction (CO R) is an appealing solution for converting carbon dioxide into higher-value products. However, CO R 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 CO R.

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UN Sustainable Development Goals (SDGs)

This publication has contributed to the advancement of the following goals:

#7 Affordable and Clean Energy
#13 Climate Action

Source: SDGs in the Output

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Web of Science research areas
Chemistry, Multidisciplinary
Chemistry, Physical
Materials Science, Multidisciplinary
Nanoscience & Nanotechnology
Physics, Applied
Physics, Condensed Matter
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