RT Journal Article A1 Zhongyin Zhao,Qi Shao,Jiangyan Xue,Bolong Huang,Zheng Niu,Hongwei Gu,Xiaoqing Huang,Jianping Lang; AD 有机金属化学国家重点实验室, 中国 ; 化学工程与材料科学, 中国 ; 化学工程与材料科学, 中国 ; 化学工程与材料科学, 中国 ; 应用生物与化学技术系, 中国 ; 化学工程与材料科学, 中国 ; 化学工程与材料科学, 中国 ; 化学工程与材料科学, 中国 ; 有机金属化学国家重点实验室, 中国 ; 化学工程与材料科学, 中国 T1 Multiple structural defects in ultrathin NiFe-LDH nanosheets synergistically and remarkably boost water oxidation reaction YR 2022 IS 1 vo 15 OP 310-OP 316 K1 oxygen evolution reaction;layered double hydroxide;oxygen vacancies;holey structures;Ni3+ defects AB Modifying electrocatalysts nanostructures and tuning their electronic properties through defects-oriented synthetic strategies are essential to improve the oxygen evolution reaction (OER) performance of electrocatalysts. Current synthetic strategies about electrocatalysts mainly target the single or double structural defects, while the researches about the synergistic effect of multiple structural defects are rare. In this work, the ultrathin NiFe layered double hydroxide nanosheets with a holey structure, oxygen vacancies and Ni3+ defects on nickel foam (NiFe-LDH-NSs/NF) are prepared by employing a simple and green H2O2-assisted etching method. The synergistic effect of the above three defects leads to the exposure of more active sites and significant improvement of the intrinsic activity. The optimized catalyst exhibits an excellent OER performance with an extraordinarily low overpotential of 170 mV at 10 mA·cm−2 and a small Tafel slope of 39.3 mV·dec−1 in 1 M KOH solution. Density functional theory calculations reveal this OER performance arises from pseudo re-oxidized metal-stable Ni3+ near oxygen vacancies (Ovac), which suppresses 3d-eg of Ni-site and elevates d-band center towards the competitively low electron-transfer barrier. This work provides a new insight to fabricate advanced electrocatalysts for renewable energy conversion technologies. SN 1998-0124 LA EN