Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting

Unraveling the role of transition-metal doping in affecting the native spinel-structured nanosheets' water splitting remains a grand challenge. In this work, a series of spinel-structured nanosheets wrapped hollow nitrogen-doped carbon polyhedrons were constructed, and doped transition-metal do...

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Main Authors: Lai, Feili, Feng, Jianrui, Ye, Xiaobin, Zong, Wei, He, Guanjie, Miao, Yue-E, Han, Xuemei, Ling, Xing Yi, Parkin, Ivan P., Pan, Bicai, Sun, Yongfu, Liu, Tianxi
Other Authors: School of Physical and Mathematical Sciences
Format: Article
Language:English
Published: 2021
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Online Access:https://hdl.handle.net/10356/151596
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Institution: Nanyang Technological University
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spelling sg-ntu-dr.10356-1515962021-07-23T04:57:33Z Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting Lai, Feili Feng, Jianrui Ye, Xiaobin Zong, Wei He, Guanjie Miao, Yue-E Han, Xuemei Ling, Xing Yi Parkin, Ivan P. Pan, Bicai Sun, Yongfu Liu, Tianxi School of Physical and Mathematical Sciences Science::Chemistry Highly Efficient Oxygen Evolution Unraveling the role of transition-metal doping in affecting the native spinel-structured nanosheets' water splitting remains a grand challenge. In this work, a series of spinel-structured nanosheets wrapped hollow nitrogen-doped carbon polyhedrons were constructed, and doped transition-metal domains were deliberately introduced on the surface. Theoretical investigations show that their energy level can be finely tuned via direct transition-metal doping engineering. As a prototype, an Fe-doped NiCo₂O₄ nanosheets wrapped hollow nitrogen-doped carbon polyhedron (Fe–NiCo₂O₄@HNCP) exhibits outstanding bifunctional electrocatalytic performances with low overpotentials (η = 270 mV for OER, η = 84 mV for HER), low Tafel slopes (b = 42 mV dec⁻¹ for OER, b = 47 mV dec⁻¹ for HER), and high durability. The enhanced performance is attributed to the synergistic effects of energy level matching for electron transfer, and partial charge delocalization-induced rich active sites for reactant adsorption via thermodynamic and kinetic acceleration. This work may open a new pathway to design highly active and stable transition-metal doped electrocatalysts by manipulated energy levels for efficient overall water splitting. We are really grateful for the financial support from the National Natural Science Foundation of China (51433001, 21674019, 21604010), the Science and Technology Commission of Shanghai Municipality (16520722100), the Program of Shanghai Academic Research Leader (17XD1400100), the “Chenguang Program” supported by the Shanghai Education Development Foundation and Shanghai Municipal Education Commission (16CG39) and the Engineering and Physical Sciences Research Council (EPSRC, EP/L015862/1). The computational center of USTC is acknowledged for computational support. 2021-07-23T04:57:33Z 2021-07-23T04:57:33Z 2019 Journal Article Lai, F., Feng, J., Ye, X., Zong, W., He, G., Miao, Y., Han, X., Ling, X. Y., Parkin, I. P., Pan, B., Sun, Y. & Liu, T. (2019). Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting. Journal of Materials Chemistry A, 7(2), 827-833. https://dx.doi.org/10.1039/C8TA10162K 2050-7488 https://hdl.handle.net/10356/151596 10.1039/C8TA10162K 2 7 827 833 en Journal of Materials Chemistry A © 2019 The Royal Society of Chemistry. All rights reserved.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Chemistry
Highly Efficient
Oxygen Evolution
spellingShingle Science::Chemistry
Highly Efficient
Oxygen Evolution
Lai, Feili
Feng, Jianrui
Ye, Xiaobin
Zong, Wei
He, Guanjie
Miao, Yue-E
Han, Xuemei
Ling, Xing Yi
Parkin, Ivan P.
Pan, Bicai
Sun, Yongfu
Liu, Tianxi
Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
description Unraveling the role of transition-metal doping in affecting the native spinel-structured nanosheets' water splitting remains a grand challenge. In this work, a series of spinel-structured nanosheets wrapped hollow nitrogen-doped carbon polyhedrons were constructed, and doped transition-metal domains were deliberately introduced on the surface. Theoretical investigations show that their energy level can be finely tuned via direct transition-metal doping engineering. As a prototype, an Fe-doped NiCo₂O₄ nanosheets wrapped hollow nitrogen-doped carbon polyhedron (Fe–NiCo₂O₄@HNCP) exhibits outstanding bifunctional electrocatalytic performances with low overpotentials (η = 270 mV for OER, η = 84 mV for HER), low Tafel slopes (b = 42 mV dec⁻¹ for OER, b = 47 mV dec⁻¹ for HER), and high durability. The enhanced performance is attributed to the synergistic effects of energy level matching for electron transfer, and partial charge delocalization-induced rich active sites for reactant adsorption via thermodynamic and kinetic acceleration. This work may open a new pathway to design highly active and stable transition-metal doped electrocatalysts by manipulated energy levels for efficient overall water splitting.
author2 School of Physical and Mathematical Sciences
author_facet School of Physical and Mathematical Sciences
Lai, Feili
Feng, Jianrui
Ye, Xiaobin
Zong, Wei
He, Guanjie
Miao, Yue-E
Han, Xuemei
Ling, Xing Yi
Parkin, Ivan P.
Pan, Bicai
Sun, Yongfu
Liu, Tianxi
format Article
author Lai, Feili
Feng, Jianrui
Ye, Xiaobin
Zong, Wei
He, Guanjie
Miao, Yue-E
Han, Xuemei
Ling, Xing Yi
Parkin, Ivan P.
Pan, Bicai
Sun, Yongfu
Liu, Tianxi
author_sort Lai, Feili
title Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
title_short Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
title_full Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
title_fullStr Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
title_full_unstemmed Energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
title_sort energy level engineering in transition-metal doped spinel-structured nanosheets for efficient overall water splitting
publishDate 2021
url https://hdl.handle.net/10356/151596
_version_ 1707050409599696896