Modulating Electronic Structure to Improve the Solar to Hydrogen Efficiency of Cobalt Nitride with Lattice Doping

Siqi Liu; Weiliang Qi; Jue Liu; Xiangjian Meng; Samira Adimi; J. Paul Attfield; Minghui Yang

doi:10.1021/acscatal.2c05075

Modulating Electronic Structure to Improve the Solar to Hydrogen Efficiency of Cobalt Nitride with Lattice Doping

Siqi Liu, Weiliang Qi, Jue Liu, Xiangjian Meng, Samira Adimi, J. Paul Attfield, Minghui Yang

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Abstract

Development of state-of-the-art catalytic systems for highly efficient solar to hydrogen energy conversion is desirable but remains a challenge. In this work, transition metal (M = V, Mo, and W) doped cobalt nitride has been synthesized for solar to hydrogen energy conversion. Neutron diffraction results suggest that the composition of our as-prepared cobalt nitride is Co_3.75N_0.14, which contains many lattice defects. Neutron pair distribution function (PDF) analysis confirms the structural defects and lattice distortion in M-Co_3.75N_0.14. The M-doping is demonstrated to tune the electronic structure and properties of Co_3.75N_0.14 due to the formation of M-N bonds, which significantly improves charge carrier separation efficiency and the reaction kinetics. Density functional theory (DFT) calculations suggest that the d-band center of the doped cobalt nitrides exhibit downshifts compared to pure cobalt nitride. This is beneficial for the desorption of hydrogen atoms, promoting hydrogen evolution activity. The hydrogen evolution rate of the optimal V-Co_3.75N_0.14-Eosin-Y system reaches 21.21 μmol·mg^-1·h^-1, with quantum efficiency around 38% at 405 nm excitation wavelength. This remarkable value surpasses those reported for other hybrid photocatalysts.

Original language	English
Pages (from-to)	2214-2222
Number of pages	9
Journal	ACS Catalysis
Volume	13
Issue number	4
DOIs	https://doi.org/10.1021/acscatal.2c05075
State	Published - Feb 17 2023

Funding

This work is supported by National Natural Science Foundation of China (Grant No. 61971405), National Key Research and Development Plan (Grant No. 2016YFB0101205), Zhejiang Provincial Science Foundation for Distinguished Young Scholars of China (Grant No. R20B010002), M. Yang would like to thank for the National “Thousand Youth Talents” Program of China. S. Liu thanks the support from the Fundamental Research Funds for the Central Universities (Grant No. DUT21RC(3)114).

Funders	Funder number
National “Thousand Youth Talents” Program of China
National Natural Science Foundation of China	61971405
National Key Research and Development Program of China	2016YFB0101205
Fundamental Research Funds for the Central Universities	DUT21RC(3)114
Science Fund for Distinguished Young Scholars of Zhejiang Province	R20B010002

Keywords

electronic structure regulation
photocatalysis
solar energy conversion
transition metal doping
transition metal nitrides

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1021/acscatal.2c05075

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title = "Modulating Electronic Structure to Improve the Solar to Hydrogen Efficiency of Cobalt Nitride with Lattice Doping",

abstract = "Development of state-of-the-art catalytic systems for highly efficient solar to hydrogen energy conversion is desirable but remains a challenge. In this work, transition metal (M = V, Mo, and W) doped cobalt nitride has been synthesized for solar to hydrogen energy conversion. Neutron diffraction results suggest that the composition of our as-prepared cobalt nitride is Co3.75N0.14, which contains many lattice defects. Neutron pair distribution function (PDF) analysis confirms the structural defects and lattice distortion in M-Co3.75N0.14. The M-doping is demonstrated to tune the electronic structure and properties of Co3.75N0.14 due to the formation of M-N bonds, which significantly improves charge carrier separation efficiency and the reaction kinetics. Density functional theory (DFT) calculations suggest that the d-band center of the doped cobalt nitrides exhibit downshifts compared to pure cobalt nitride. This is beneficial for the desorption of hydrogen atoms, promoting hydrogen evolution activity. The hydrogen evolution rate of the optimal V-Co3.75N0.14-Eosin-Y system reaches 21.21 μmol·mg-1·h-1, with quantum efficiency around 38% at 405 nm excitation wavelength. This remarkable value surpasses those reported for other hybrid photocatalysts.",

keywords = "electronic structure regulation, photocatalysis, solar energy conversion, transition metal doping, transition metal nitrides",

author = "Siqi Liu and Weiliang Qi and Jue Liu and Xiangjian Meng and Samira Adimi and Attfield, {J. Paul} and Minghui Yang",

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AU - Attfield, J. Paul

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N2 - Development of state-of-the-art catalytic systems for highly efficient solar to hydrogen energy conversion is desirable but remains a challenge. In this work, transition metal (M = V, Mo, and W) doped cobalt nitride has been synthesized for solar to hydrogen energy conversion. Neutron diffraction results suggest that the composition of our as-prepared cobalt nitride is Co3.75N0.14, which contains many lattice defects. Neutron pair distribution function (PDF) analysis confirms the structural defects and lattice distortion in M-Co3.75N0.14. The M-doping is demonstrated to tune the electronic structure and properties of Co3.75N0.14 due to the formation of M-N bonds, which significantly improves charge carrier separation efficiency and the reaction kinetics. Density functional theory (DFT) calculations suggest that the d-band center of the doped cobalt nitrides exhibit downshifts compared to pure cobalt nitride. This is beneficial for the desorption of hydrogen atoms, promoting hydrogen evolution activity. The hydrogen evolution rate of the optimal V-Co3.75N0.14-Eosin-Y system reaches 21.21 μmol·mg-1·h-1, with quantum efficiency around 38% at 405 nm excitation wavelength. This remarkable value surpasses those reported for other hybrid photocatalysts.

AB - Development of state-of-the-art catalytic systems for highly efficient solar to hydrogen energy conversion is desirable but remains a challenge. In this work, transition metal (M = V, Mo, and W) doped cobalt nitride has been synthesized for solar to hydrogen energy conversion. Neutron diffraction results suggest that the composition of our as-prepared cobalt nitride is Co3.75N0.14, which contains many lattice defects. Neutron pair distribution function (PDF) analysis confirms the structural defects and lattice distortion in M-Co3.75N0.14. The M-doping is demonstrated to tune the electronic structure and properties of Co3.75N0.14 due to the formation of M-N bonds, which significantly improves charge carrier separation efficiency and the reaction kinetics. Density functional theory (DFT) calculations suggest that the d-band center of the doped cobalt nitrides exhibit downshifts compared to pure cobalt nitride. This is beneficial for the desorption of hydrogen atoms, promoting hydrogen evolution activity. The hydrogen evolution rate of the optimal V-Co3.75N0.14-Eosin-Y system reaches 21.21 μmol·mg-1·h-1, with quantum efficiency around 38% at 405 nm excitation wavelength. This remarkable value surpasses those reported for other hybrid photocatalysts.

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Modulating Electronic Structure to Improve the Solar to Hydrogen Efficiency of Cobalt Nitride with Lattice Doping

Abstract

Funding

Keywords

UN SDGs

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