Li Fusheng, Yang Hao, Zhuo Qiming, Zhou Dinghua, Wu Xiujuan, Zhang PeiLi, Yao Zhaoyang, Sun Licheng
State Key Laboratory of Fine Chemicals, Institute of Artificial Photosynthesis, DUT-KTH Joint Education and Research Centre on Molecular Devices, Dalian University of Technology, 116024, Dalian, China.
Department of Chemistry, School of Engineering Sciences in Chemistry, Biotechnology and Health, KTH Royal Institute of Technology, 10044, Stockholm, Sweden.
Angew Chem Int Ed Engl. 2021 Jan 25;60(4):1976-1985. doi: 10.1002/anie.202011069. Epub 2020 Nov 24.
A host-guest complex self-assembled through Co and cucurbit[5]uril (Co@CB[5]) is used as a supramolecular catalyst on the surface of metal oxides including porous indium tin oxide (ITO) and porous BiVO for efficient electrochemical and photoelectrochemical water oxidation. When immobilized on ITO, Co@CB[5] exhibited a turnover frequency (TOF) of 9.9 s at overpotential η=550 mV in a pH 9.2 borate buffer. Meanwhile, when Co@CB[5] complex was immobilized onto the surface of BiVO semiconductor, the assembled Co@CB[5]/BiVO photoanode exhibited a low onset potential of 0.15 V (vs. RHE) and a high photocurrent of 4.8 mA cm at 1.23 V (vs. RHE) under 100 mW cm (AM 1.5) light illumination. Kinetic studies confirmed that Co@CB[5] acts as a supramolecular water oxidation catalyst, and can effectively accelerate interfacial charge transfer between BiVO and electrolyte. Surface charge recombination of BiVO can be also significantly suppressed by Co@CB[5].
一种通过钴与瓜环[5]（Co@CB[5]）自组装形成的主客体配合物被用作金属氧化物表面的超分子催化剂，这些金属氧化物包括多孔氧化铟锡（ITO）和多孔钒酸铋，用于高效的电化学和光电化学水氧化反应。当固定在ITO上时，在pH 9.2的硼酸盐缓冲液中，Co@CB[5]在过电位η = 550 mV时表现出9.9 s⁻¹的周转频率（TOF）。同时，当Co@CB[5]配合物固定在钒酸铋半导体表面时，组装后的Co@CB[5]/BiVO光阳极在100 mW cm⁻²（AM 1.5）光照下，在1.23 V（相对于可逆氢电极，RHE）时表现出0.15 V（相对于RHE）的低起始电位和4.8 mA cm⁻²的高光电流。动力学研究证实，Co@CB[5]作为超分子水氧化催化剂，能够有效地加速钒酸铋与电解质之间的界面电荷转移。Co@CB[5]还可以显著抑制钒酸铋的表面电荷复合。
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