Magnetron sputtering tuned "π back-donation" sites over metal oxides for enhanced electrocatalytic nitrogen reduction

Yuan Tian; Bin Chang; Guihua Wang; Lili Li; Lianguo Gong; Bo Wang; Rusheng Yuan; Weijia Zhou

doi:10.1039/d1ta10273g

Magnetron sputtering tuned "π back-donation" sites over metal oxides for enhanced electrocatalytic nitrogen reduction

Yuan Tian, Bin Chang^*, Guihua Wang, Lili Li, Lianguo Gong, Bo Wang, Rusheng Yuan, Weijia Zhou

^*Corresponding author for this work

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

24 Scopus citations

Abstract

As an environmentally-benign and sustainable option for NH3 synthesis, the electrochemical nitrogen reduction reaction (NRR) is expected to replace the traditional Haber-Bosch process. Transition metals with empty d-orbitals achieve NRR activity via a "π back-donation"process. However, the problem in overcoming hydrogen evolution reaction (HER) competition makes the exploration of transition metal-based catalysts with relatively inferior HER activity worthwhile. The challenges lie in designing a rational structure for efficient NRR. Herein, Ni3+ and oxygen vacancies were synergistically integrated on NiO@TiO2 by magnetron sputtering, which provide this transition-metal oxide-based (TMO-based) material with "π back-donation"behavior. Accordingly, NiO@TiO2 exhibited NH3 yield (∼10.75 μg h-1 cmcat.-2) and faradaic efficiency (∼9.83%), which are nearly 10-fold higher relative to those of TiO2 in neutral media. This work provides an efficient strategy for engineering "π back-donation"sites, and holds great potential in exploring new TMO-based electrocatalysts.

Original language	English (US)
Pages (from-to)	2800-2806
Number of pages	7
Journal	JOURNAL OF MATERIALS CHEMISTRY A
Volume	10
Issue number	6
DOIs	https://doi.org/10.1039/d1ta10273g
State	Published - Feb 14 2022

ASJC Scopus subject areas

General Chemistry
Renewable Energy, Sustainability and the Environment
General Materials Science

UN SDGs

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

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10.1039/d1ta10273g

Cite this

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title = "Magnetron sputtering tuned {"}π back-donation{"} sites over metal oxides for enhanced electrocatalytic nitrogen reduction",

abstract = "As an environmentally-benign and sustainable option for NH3 synthesis, the electrochemical nitrogen reduction reaction (NRR) is expected to replace the traditional Haber-Bosch process. Transition metals with empty d-orbitals achieve NRR activity via a {"}π back-donation{"}process. However, the problem in overcoming hydrogen evolution reaction (HER) competition makes the exploration of transition metal-based catalysts with relatively inferior HER activity worthwhile. The challenges lie in designing a rational structure for efficient NRR. Herein, Ni3+ and oxygen vacancies were synergistically integrated on NiO@TiO2 by magnetron sputtering, which provide this transition-metal oxide-based (TMO-based) material with {"}π back-donation{"}behavior. Accordingly, NiO@TiO2 exhibited NH3 yield (∼10.75 μg h-1 cmcat.-2) and faradaic efficiency (∼9.83%), which are nearly 10-fold higher relative to those of TiO2 in neutral media. This work provides an efficient strategy for engineering {"}π back-donation{"}sites, and holds great potential in exploring new TMO-based electrocatalysts.",

author = "Yuan Tian and Bin Chang and Guihua Wang and Lili Li and Lianguo Gong and Bo Wang and Rusheng Yuan and Weijia Zhou",

note = "Funding Information: This work is supported by the National Natural Science Foundation of China (21902061, 52022037), Taishan Scholars Project Special Funds (tsqn201812083), the Natural Science Foundation of Shandong Province (ZR2021QE011), China Postdoctoral Science Foundation (2021M701402), Postdoctoral Innovative Talents Support Program of Shandong Province (SDBX2020009) and the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment (SKLPEE-KF202110, SKLPEE-KF202010). Publisher Copyright: {\textcopyright} 2022 The Royal Society of Chemistry.",

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T1 - Magnetron sputtering tuned "π back-donation" sites over metal oxides for enhanced electrocatalytic nitrogen reduction

AU - Tian, Yuan

AU - Chang, Bin

AU - Wang, Guihua

AU - Li, Lili

AU - Gong, Lianguo

AU - Wang, Bo

AU - Yuan, Rusheng

AU - Zhou, Weijia

N1 - Funding Information: This work is supported by the National Natural Science Foundation of China (21902061, 52022037), Taishan Scholars Project Special Funds (tsqn201812083), the Natural Science Foundation of Shandong Province (ZR2021QE011), China Postdoctoral Science Foundation (2021M701402), Postdoctoral Innovative Talents Support Program of Shandong Province (SDBX2020009) and the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment (SKLPEE-KF202110, SKLPEE-KF202010). Publisher Copyright: © 2022 The Royal Society of Chemistry.

PY - 2022/2/14

Y1 - 2022/2/14

N2 - As an environmentally-benign and sustainable option for NH3 synthesis, the electrochemical nitrogen reduction reaction (NRR) is expected to replace the traditional Haber-Bosch process. Transition metals with empty d-orbitals achieve NRR activity via a "π back-donation"process. However, the problem in overcoming hydrogen evolution reaction (HER) competition makes the exploration of transition metal-based catalysts with relatively inferior HER activity worthwhile. The challenges lie in designing a rational structure for efficient NRR. Herein, Ni3+ and oxygen vacancies were synergistically integrated on NiO@TiO2 by magnetron sputtering, which provide this transition-metal oxide-based (TMO-based) material with "π back-donation"behavior. Accordingly, NiO@TiO2 exhibited NH3 yield (∼10.75 μg h-1 cmcat.-2) and faradaic efficiency (∼9.83%), which are nearly 10-fold higher relative to those of TiO2 in neutral media. This work provides an efficient strategy for engineering "π back-donation"sites, and holds great potential in exploring new TMO-based electrocatalysts.

AB - As an environmentally-benign and sustainable option for NH3 synthesis, the electrochemical nitrogen reduction reaction (NRR) is expected to replace the traditional Haber-Bosch process. Transition metals with empty d-orbitals achieve NRR activity via a "π back-donation"process. However, the problem in overcoming hydrogen evolution reaction (HER) competition makes the exploration of transition metal-based catalysts with relatively inferior HER activity worthwhile. The challenges lie in designing a rational structure for efficient NRR. Herein, Ni3+ and oxygen vacancies were synergistically integrated on NiO@TiO2 by magnetron sputtering, which provide this transition-metal oxide-based (TMO-based) material with "π back-donation"behavior. Accordingly, NiO@TiO2 exhibited NH3 yield (∼10.75 μg h-1 cmcat.-2) and faradaic efficiency (∼9.83%), which are nearly 10-fold higher relative to those of TiO2 in neutral media. This work provides an efficient strategy for engineering "π back-donation"sites, and holds great potential in exploring new TMO-based electrocatalysts.

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Magnetron sputtering tuned "π back-donation" sites over metal oxides for enhanced electrocatalytic nitrogen reduction

Abstract

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