Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration

Abstract Solar photoelectrochemical reactions have been considered one of the most promising paths for sustainable energy production. To date, however, there has been no demonstration of semiconductor photoelectrodes with long-term stable operation in a two-electrode configuration, which is required...

Full description

Bibliographic Details
Main Authors: Yixin Xiao, Xianghua Kong, Srinivas Vanka, Wan Jae Dong, Guosong Zeng, Zhengwei Ye, Kai Sun, Ishtiaque Ahmed Navid, Baowen Zhou, Francesca M. Toma, Hong Guo, Zetian Mi
Format: Article
Language:English
Published: Nature Portfolio 2023-04-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-023-37754-9
_version_ 1797845889672282112
author Yixin Xiao
Xianghua Kong
Srinivas Vanka
Wan Jae Dong
Guosong Zeng
Zhengwei Ye
Kai Sun
Ishtiaque Ahmed Navid
Baowen Zhou
Francesca M. Toma
Hong Guo
Zetian Mi
author_facet Yixin Xiao
Xianghua Kong
Srinivas Vanka
Wan Jae Dong
Guosong Zeng
Zhengwei Ye
Kai Sun
Ishtiaque Ahmed Navid
Baowen Zhou
Francesca M. Toma
Hong Guo
Zetian Mi
author_sort Yixin Xiao
collection DOAJ
description Abstract Solar photoelectrochemical reactions have been considered one of the most promising paths for sustainable energy production. To date, however, there has been no demonstration of semiconductor photoelectrodes with long-term stable operation in a two-electrode configuration, which is required for any practical application. Herein, we demonstrate the stable operation of a photocathode comprising Si and GaN, the two most produced semiconductors in the world, for 3,000 hrs without any performance degradation in two-electrode configurations. Measurements in both three- and two-electrode configurations suggest that surfaces of the GaN nanowires on Si photocathode transform in situ into Ga-O-N that drastically enhances hydrogen evolution and remains stable for 3,000 hrs. First principles calculations further revealed that the in-situ Ga-O-N species exhibit atomic-scale surface metallization. This study overcomes the conventional dilemma between efficiency and stability imposed by extrinsic cocatalysts, offering a path for practical application of photoelectrochemical devices and systems for clean energy.
first_indexed 2024-04-09T17:46:16Z
format Article
id doaj.art-96623d46ccbb4d18b923e52e11a5b6b4
institution Directory Open Access Journal
issn 2041-1723
language English
last_indexed 2024-04-09T17:46:16Z
publishDate 2023-04-01
publisher Nature Portfolio
record_format Article
series Nature Communications
spelling doaj.art-96623d46ccbb4d18b923e52e11a5b6b42023-04-16T11:18:04ZengNature PortfolioNature Communications2041-17232023-04-0114111010.1038/s41467-023-37754-9Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configurationYixin Xiao0Xianghua Kong1Srinivas Vanka2Wan Jae Dong3Guosong Zeng4Zhengwei Ye5Kai Sun6Ishtiaque Ahmed Navid7Baowen Zhou8Francesca M. Toma9Hong Guo10Zetian Mi11Department of Electrical Engineering and Computer Science, University of MichiganDepartment of Physics, McGill UniversityDepartment of Electrical Engineering and Computer Science, University of MichiganDepartment of Electrical Engineering and Computer Science, University of MichiganLawrence Berkeley National Laboratory, Chemical Sciences DivisionDepartment of Electrical Engineering and Computer Science, University of MichiganDepartment of Materials Science and Engineering, University of MichiganDepartment of Electrical Engineering and Computer Science, University of MichiganDepartment of Electrical Engineering and Computer Science, University of MichiganLawrence Berkeley National Laboratory, Chemical Sciences DivisionDepartment of Physics, McGill UniversityDepartment of Electrical Engineering and Computer Science, University of MichiganAbstract Solar photoelectrochemical reactions have been considered one of the most promising paths for sustainable energy production. To date, however, there has been no demonstration of semiconductor photoelectrodes with long-term stable operation in a two-electrode configuration, which is required for any practical application. Herein, we demonstrate the stable operation of a photocathode comprising Si and GaN, the two most produced semiconductors in the world, for 3,000 hrs without any performance degradation in two-electrode configurations. Measurements in both three- and two-electrode configurations suggest that surfaces of the GaN nanowires on Si photocathode transform in situ into Ga-O-N that drastically enhances hydrogen evolution and remains stable for 3,000 hrs. First principles calculations further revealed that the in-situ Ga-O-N species exhibit atomic-scale surface metallization. This study overcomes the conventional dilemma between efficiency and stability imposed by extrinsic cocatalysts, offering a path for practical application of photoelectrochemical devices and systems for clean energy.https://doi.org/10.1038/s41467-023-37754-9
spellingShingle Yixin Xiao
Xianghua Kong
Srinivas Vanka
Wan Jae Dong
Guosong Zeng
Zhengwei Ye
Kai Sun
Ishtiaque Ahmed Navid
Baowen Zhou
Francesca M. Toma
Hong Guo
Zetian Mi
Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
Nature Communications
title Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
title_full Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
title_fullStr Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
title_full_unstemmed Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
title_short Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
title_sort oxynitrides enabled photoelectrochemical water splitting with over 3 000 hrs stable operation in practical two electrode configuration
url https://doi.org/10.1038/s41467-023-37754-9
work_keys_str_mv AT yixinxiao oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT xianghuakong oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT srinivasvanka oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT wanjaedong oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT guosongzeng oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT zhengweiye oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT kaisun oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT ishtiaqueahmednavid oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT baowenzhou oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT francescamtoma oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT hongguo oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration
AT zetianmi oxynitridesenabledphotoelectrochemicalwatersplittingwithover3000hrsstableoperationinpracticaltwoelectrodeconfiguration