Photoelectrochemical splitting of water with nanocrystalline Zn 1-xMnxO thin films: First-principle DFT computations supporting the systematic experimental endeavor

Vidhika Sharma; Mudit Dixit; Vibha R. Satsangi; Sahab Dass; Sourav Pal; Rohit Shrivastav

doi:10.1016/j.ijhydene.2013.12.150

Photoelectrochemical splitting of water with nanocrystalline Zn _1-xMn_xO thin films: First-principle DFT computations supporting the systematic experimental endeavor

Vidhika Sharma, Mudit Dixit, Vibha R. Satsangi, Sahab Dass, Sourav Pal, Rohit Shrivastav

Research output: Contribution to journal › Article › peer-review

20 Scopus citations

Abstract

Photoelectrochemical splitting of water with nanocrystalline Zn _1-xMn_xO thin films was investigated. ZnO thin films with 1, 3, 5 and 7% at. Mn incorporation were synthesized by sol-gel method and characterized by X-Ray Diffraction (XRD) analysis, Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), X-ray Photoelectron spectroscopy (XPS), High Resolution Transmission Electron Microscopy (HR-TEM) and UV-Vis spectroscopy. Mn incorporation coupled with variation in sintering temperature led to significant microstructural changes, which tentatively influenced the magnitude of optical absorption and charge carrier mobility, thereby impacting the performance of such systems towards photoelectrochemical splitting of water. Electronic structure computations based on first principle density functional theory (DFT) revealed electronic states of Mn being responsible for the marginally recorded red shift in bandgap energy. Photoelectrochemical measurements using thin films of 1% at. Mn:ZnO sintered at 600 C yielded 3 times enhanced photocurrent at zero bias due to improved optical absorption. Plausible explanations for the effect have also been offered.

Original language	English
Pages (from-to)	3637-3648
Number of pages	12
Journal	International Journal of Hydrogen Energy
Volume	39
Issue number	8
DOIs	https://doi.org/10.1016/j.ijhydene.2013.12.150
State	Published - 6 Mar 2014
Externally published	Yes

Bibliographical note

Funding Information:
Financial assistance from DAE-BRNS, Govt. of India is gratefully acknowledged. VS thanks HRDG-CSIR, Govt. of India, for providing Nehru post-doctoral fellowship. Authors thank Dr. Shyam Prasad, NIO, Goa, India for SEM; and Prof. Sheryl H Ehrman, Chia-Ying Chiang and Dr. Karen Gaskell, University of Maryland, USA, for TEM and XPS analysis. Financial support from DST-NSF under Material World Network Program (Project No. DST/INT/NSF-MWN/Proj-03/07) is also acknowledged.

Funding

Financial assistance from DAE-BRNS, Govt. of India is gratefully acknowledged. VS thanks HRDG-CSIR, Govt. of India, for providing Nehru post-doctoral fellowship. Authors thank Dr. Shyam Prasad, NIO, Goa, India for SEM; and Prof. Sheryl H Ehrman, Chia-Ying Chiang and Dr. Karen Gaskell, University of Maryland, USA, for TEM and XPS analysis. Financial support from DST-NSF under Material World Network Program (Project No. DST/INT/NSF-MWN/Proj-03/07) is also acknowledged.

Funders	Funder number
DST-NSF	DST/INT/NSF-MWN/Proj-03/07

Keywords

Density functional theory
Hydrogen energy
Mn doped ZnO
Optical properties
Photoelectrochemical water splitting

UN SDGs

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

Access to Document

10.1016/j.ijhydene.2013.12.150

Cite this

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title = "Photoelectrochemical splitting of water with nanocrystalline Zn 1-xMnxO thin films: First-principle DFT computations supporting the systematic experimental endeavor",

abstract = "Photoelectrochemical splitting of water with nanocrystalline Zn 1-xMnxO thin films was investigated. ZnO thin films with 1, 3, 5 and 7% at. Mn incorporation were synthesized by sol-gel method and characterized by X-Ray Diffraction (XRD) analysis, Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), X-ray Photoelectron spectroscopy (XPS), High Resolution Transmission Electron Microscopy (HR-TEM) and UV-Vis spectroscopy. Mn incorporation coupled with variation in sintering temperature led to significant microstructural changes, which tentatively influenced the magnitude of optical absorption and charge carrier mobility, thereby impacting the performance of such systems towards photoelectrochemical splitting of water. Electronic structure computations based on first principle density functional theory (DFT) revealed electronic states of Mn being responsible for the marginally recorded red shift in bandgap energy. Photoelectrochemical measurements using thin films of 1% at. Mn:ZnO sintered at 600 C yielded 3 times enhanced photocurrent at zero bias due to improved optical absorption. Plausible explanations for the effect have also been offered.",

keywords = "Density functional theory, Hydrogen energy, Mn doped ZnO, Optical properties, Photoelectrochemical water splitting",

author = "Vidhika Sharma and Mudit Dixit and Satsangi, {Vibha R.} and Sahab Dass and Sourav Pal and Rohit Shrivastav",

note = "Funding Information: Financial assistance from DAE-BRNS, Govt. of India is gratefully acknowledged. VS thanks HRDG-CSIR, Govt. of India, for providing Nehru post-doctoral fellowship. Authors thank Dr. Shyam Prasad, NIO, Goa, India for SEM; and Prof. Sheryl H Ehrman, Chia-Ying Chiang and Dr. Karen Gaskell, University of Maryland, USA, for TEM and XPS analysis. Financial support from DST-NSF under Material World Network Program (Project No. DST/INT/NSF-MWN/Proj-03/07) is also acknowledged.",

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doi = "10.1016/j.ijhydene.2013.12.150",

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volume = "39",

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Photoelectrochemical splitting of water with nanocrystalline Zn _1-xMn_xO thin films: First-principle DFT computations supporting the systematic experimental endeavor. / Sharma, Vidhika; Dixit, Mudit; Satsangi, Vibha R. et al.
In: International Journal of Hydrogen Energy, Vol. 39, No. 8, 06.03.2014, p. 3637-3648.

Research output: Contribution to journal › Article › peer-review

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AU - Dixit, Mudit

AU - Satsangi, Vibha R.

AU - Dass, Sahab

AU - Pal, Sourav

AU - Shrivastav, Rohit

N1 - Funding Information: Financial assistance from DAE-BRNS, Govt. of India is gratefully acknowledged. VS thanks HRDG-CSIR, Govt. of India, for providing Nehru post-doctoral fellowship. Authors thank Dr. Shyam Prasad, NIO, Goa, India for SEM; and Prof. Sheryl H Ehrman, Chia-Ying Chiang and Dr. Karen Gaskell, University of Maryland, USA, for TEM and XPS analysis. Financial support from DST-NSF under Material World Network Program (Project No. DST/INT/NSF-MWN/Proj-03/07) is also acknowledged.

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N2 - Photoelectrochemical splitting of water with nanocrystalline Zn 1-xMnxO thin films was investigated. ZnO thin films with 1, 3, 5 and 7% at. Mn incorporation were synthesized by sol-gel method and characterized by X-Ray Diffraction (XRD) analysis, Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), X-ray Photoelectron spectroscopy (XPS), High Resolution Transmission Electron Microscopy (HR-TEM) and UV-Vis spectroscopy. Mn incorporation coupled with variation in sintering temperature led to significant microstructural changes, which tentatively influenced the magnitude of optical absorption and charge carrier mobility, thereby impacting the performance of such systems towards photoelectrochemical splitting of water. Electronic structure computations based on first principle density functional theory (DFT) revealed electronic states of Mn being responsible for the marginally recorded red shift in bandgap energy. Photoelectrochemical measurements using thin films of 1% at. Mn:ZnO sintered at 600 C yielded 3 times enhanced photocurrent at zero bias due to improved optical absorption. Plausible explanations for the effect have also been offered.

AB - Photoelectrochemical splitting of water with nanocrystalline Zn 1-xMnxO thin films was investigated. ZnO thin films with 1, 3, 5 and 7% at. Mn incorporation were synthesized by sol-gel method and characterized by X-Ray Diffraction (XRD) analysis, Scanning Electron Microscopy (SEM), Atomic Force Microscopy (AFM), X-ray Photoelectron spectroscopy (XPS), High Resolution Transmission Electron Microscopy (HR-TEM) and UV-Vis spectroscopy. Mn incorporation coupled with variation in sintering temperature led to significant microstructural changes, which tentatively influenced the magnitude of optical absorption and charge carrier mobility, thereby impacting the performance of such systems towards photoelectrochemical splitting of water. Electronic structure computations based on first principle density functional theory (DFT) revealed electronic states of Mn being responsible for the marginally recorded red shift in bandgap energy. Photoelectrochemical measurements using thin films of 1% at. Mn:ZnO sintered at 600 C yielded 3 times enhanced photocurrent at zero bias due to improved optical absorption. Plausible explanations for the effect have also been offered.

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