Title Atomically targeting NiFe LDH to create multivacancies for OER catalysis with a small organic anchor
Authors Wang, Yaqiong
Tao, Shi
Lin, He
Wang, Gaopeng
Zhao, Kangning
Cai, Rongmin
Tao, Kewen
Zhang, Chengxu
Sun, Mingzi
Hu, Jue
Huang, Bolong
Yang, Shihe
Affiliation Peking Univ, Sch Chem Biol & Biotechnol, Guangdong Key Lab Nanomicro Mat Res, Shenzhen Grad Sch, Shenzhen 518055, Peoples R China
Hong Kong Univ Sci & Technol, Dept Chem, Kowloon, Clear Water Bay, Hong Kong, Peoples R China
Changshu Inst Technol, Sch Elect & Engn, Jiangsu Lab Adv Funct Mat, Changshu 215500, Jiangsu, Peoples R China
Shanghai Univ, Coll Sci, Shanghai 200444, Peoples R China
Shanghai Univ, Inst Sustainable Energy, Shanghai 200444, Peoples R China
Kunming Univ Sci & Technol, Fac Sci, Kunming 650093, Yunnan, Peoples R China
Hong Kong Polytech Univ, Dept Appl Biol & Chem Technol, Kowloon, Hung Hom, Hong Kong, Peoples R China
Hong Kong Polytech Univ, Res Inst Smart Energy RISE, Hung Hom, Kowloon, Hong Kong, Peoples R China
Issue Date Mar-2021
Publisher NANO ENERGY
Abstract 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.
URI http://hdl.handle.net/20.500.11897/605090
ISSN 2211-2855
DOI 10.1016/j.nanoen.2020.105606
Indexed SCI(E)
Appears in Collections: 化学生物学与生物技术学院
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