Journal
JOURNAL OF MATERIALS CHEMISTRY A
Volume 10, Issue 6, Pages 2800-2806Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta10273g
Keywords
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Funding
- National Natural Science Foundation of China [21902061, 52022037]
- Taishan Scholars Project Special Funds [tsqn201812083]
- Natural Science Foundation of Shandong Province [ZR2021QE011]
- China Postdoctoral Science Foundation [2021M701402]
- Postdoctoral Innovative Talents Support Program of Shandong Province [SDBX2020009]
- Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment [SKLPEE-KF202110, SKLPEE-KF202010]
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This work presents a strategy for efficient NRR through integrating Ni3+ and oxygen vacancies on NiO@TiO2 via magnetron sputtering. The resulting material exhibits excellent pi back-donation behavior and shows high NH3 yield and faradaic efficiency in neutral media, indicating great potential for TMO-based electrocatalysts.
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 pi 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 pi back-donation behavior. Accordingly, NiO@TiO2 exhibited NH3 yield (similar to 10.75 mu g h(-1) cm(cat.)(-2)) and faradaic efficiency (similar to 9.83%), which are nearly 10-fold higher relative to those of TiO2 in neutral media. This work provides an efficient strategy for engineering pi back-donation sites, and holds great potential in exploring new TMO-based electrocatalysts.
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