Cargando…
Photoelectrochemical CO(2) Reduction at a Direct CuInGaS(2)/Electrolyte Junction
[Image: see text] Photoelectrochemical (PEC) CO(2) reduction has received considerable attention given the inherent sustainability and simplicity of directly converting solar energy into carbon-based chemical fuels. However, complex photocathode architectures with protecting layers and cocatalysts a...
Autores principales: | , , , , , , , |
---|---|
Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2023
|
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10111408/ https://www.ncbi.nlm.nih.gov/pubmed/37090168 http://dx.doi.org/10.1021/acsenergylett.3c00022 |
_version_ | 1785027445278113792 |
---|---|
author | Liu, Yongpeng Xia, Meng Ren, Dan Nussbaum, Simon Yum, Jun-Ho Grätzel, Michael Guijarro, Néstor Sivula, Kevin |
author_facet | Liu, Yongpeng Xia, Meng Ren, Dan Nussbaum, Simon Yum, Jun-Ho Grätzel, Michael Guijarro, Néstor Sivula, Kevin |
author_sort | Liu, Yongpeng |
collection | PubMed |
description | [Image: see text] Photoelectrochemical (PEC) CO(2) reduction has received considerable attention given the inherent sustainability and simplicity of directly converting solar energy into carbon-based chemical fuels. However, complex photocathode architectures with protecting layers and cocatalysts are typically needed for selective and stable operation. We report herein that bare CuIn(0.3)Ga(0.7)S(2) photocathodes can drive the PEC CO(2) reduction with a benchmarking 1 Sun photocurrent density of over 2 mA/cm(2) (at −2 V vs Fc(+)/Fc) and a product selectivity of up to 87% for CO (CO/all products) production while also displaying long-term stability for syngas production (over 44 h). Importantly, spectroelectrochemical analysis using PEC impedance spectroscopy (PEIS) and intensity-modulated photocurrent spectroscopy (IMPS) complements PEC data to reveal that tailoring the proton donor ability of the electrolyte is crucial for enhancing the performance, selectivity, and durability of the photocathode. When a moderate amount of protons is present, the density of photogenerated charges accumulated at the interface drops significantly, suggesting a faster charge transfer process. However, with a high concentration of proton donors, the H(2) evolution reaction is preferred. |
format | Online Article Text |
id | pubmed-10111408 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2023 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-101114082023-04-19 Photoelectrochemical CO(2) Reduction at a Direct CuInGaS(2)/Electrolyte Junction Liu, Yongpeng Xia, Meng Ren, Dan Nussbaum, Simon Yum, Jun-Ho Grätzel, Michael Guijarro, Néstor Sivula, Kevin ACS Energy Lett [Image: see text] Photoelectrochemical (PEC) CO(2) reduction has received considerable attention given the inherent sustainability and simplicity of directly converting solar energy into carbon-based chemical fuels. However, complex photocathode architectures with protecting layers and cocatalysts are typically needed for selective and stable operation. We report herein that bare CuIn(0.3)Ga(0.7)S(2) photocathodes can drive the PEC CO(2) reduction with a benchmarking 1 Sun photocurrent density of over 2 mA/cm(2) (at −2 V vs Fc(+)/Fc) and a product selectivity of up to 87% for CO (CO/all products) production while also displaying long-term stability for syngas production (over 44 h). Importantly, spectroelectrochemical analysis using PEC impedance spectroscopy (PEIS) and intensity-modulated photocurrent spectroscopy (IMPS) complements PEC data to reveal that tailoring the proton donor ability of the electrolyte is crucial for enhancing the performance, selectivity, and durability of the photocathode. When a moderate amount of protons is present, the density of photogenerated charges accumulated at the interface drops significantly, suggesting a faster charge transfer process. However, with a high concentration of proton donors, the H(2) evolution reaction is preferred. American Chemical Society 2023-03-02 /pmc/articles/PMC10111408/ /pubmed/37090168 http://dx.doi.org/10.1021/acsenergylett.3c00022 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by/4.0/Permits the broadest form of re-use including for commercial purposes, provided that author attribution and integrity are maintained (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Liu, Yongpeng Xia, Meng Ren, Dan Nussbaum, Simon Yum, Jun-Ho Grätzel, Michael Guijarro, Néstor Sivula, Kevin Photoelectrochemical CO(2) Reduction at a Direct CuInGaS(2)/Electrolyte Junction |
title | Photoelectrochemical
CO(2) Reduction at a
Direct CuInGaS(2)/Electrolyte Junction |
title_full | Photoelectrochemical
CO(2) Reduction at a
Direct CuInGaS(2)/Electrolyte Junction |
title_fullStr | Photoelectrochemical
CO(2) Reduction at a
Direct CuInGaS(2)/Electrolyte Junction |
title_full_unstemmed | Photoelectrochemical
CO(2) Reduction at a
Direct CuInGaS(2)/Electrolyte Junction |
title_short | Photoelectrochemical
CO(2) Reduction at a
Direct CuInGaS(2)/Electrolyte Junction |
title_sort | photoelectrochemical
co(2) reduction at a
direct cuingas(2)/electrolyte junction |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10111408/ https://www.ncbi.nlm.nih.gov/pubmed/37090168 http://dx.doi.org/10.1021/acsenergylett.3c00022 |
work_keys_str_mv | AT liuyongpeng photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT xiameng photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT rendan photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT nussbaumsimon photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT yumjunho photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT gratzelmichael photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT guijarronestor photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction AT sivulakevin photoelectrochemicalco2reductionatadirectcuingas2electrolytejunction |