期刊
NANO ENERGY
卷 81, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.nanoen.2020.105606
关键词
Layered double hydroxide; Methyl-isorhodanate; Targeted atoms; Multivacancies; Oxygen evolution reaction
类别
资金
- China Postdoctoral Fund [2019M660331]
- Shenzhen Peacock Plan Program [KQTD2016053015544057]
- Nanshan Pilot Plan [LHTD20170001]
- NFSC/Hong Kong RGC Research Scheme [N_HKUST610/14]
- RGC of Hong Kong (GRF) [16312216]
- HK Innovation and Technology Fund [GHP/079/17SZ]
- National Nature Science Foundation of China [21862011, 51864024, 21771156]
- Yunnan province [2019FI003]
- Early Career Scheme (ECS) fund from the Research Grant Council (RGC) in Hong Kong [PolyU 253026/16P]
- Research Institute for Smart Energy (RISE) of the Hong Kong Polytechnic University
Introducing small molecules successfully overcomes the difficulties in fabricating porous structures in ultrathin materials, improving the electrocatalytic performance of NiFe LDH layered double hydroxides, particularly excelling in the oxygen evolution reaction (OER).
The fabrication of porous structure in the ultrathin materials still faces high difficulties. In particular, the precise modulations in the porosity and size are highly challenging. In this work, we have introduced small molecules to overcome such a challenge. And this substantially contributes to the energy related applications, especially to the water-energy (WE) treatment. Electrocatalytic water-splitting is hindered by the sluggish kinetics of water oxidation, requiring efficient earth-abundant electrocatalysts for the oxygen evolution reaction (OER). Herein we demonstrate the robust OER activity by introducing metal and oxygen multivacancies in noble-metal-free layered double hydroxides (LDHs) through the specific electron-withdrawing organic molecule methyl-isorhodanate (CH3NCS). Our work reveals that the metal and oxygen vacancies endow NiFe LDH with enhanced electron transfer and modulate the H2O adsorption, thereby boosting the OER electrocatalytic properties. Remarkably, the best-performing laminar NiFe LDH nanosheets with metal and oxygen multivacancies (v-L-LDHs) show an ultra-low overpotential of 230 mV at 100 mA cm(2) and Tafel slope of 37.1 mV dec 1. Density functional theory (DFT) has revealed the improved OER performance is realized by the co-existence of metal and O vacancies in NiFe LDH, where the defective region activates the electroactivity of Ni sites and O sites to promote the electron transfer and intermediate transformation. The Fe sites play a key role to preserve the high electroactivity of the Ni sites in long-term applications. The superior OER performance underpins the high potential of the reported facile organic anchor strategy for designing and synthesizing advanced electrocatalysts in both LDH and other potential 2D layered materials.
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