析氧
塔菲尔方程
化学
电子转移
光致变色
电解质
光化学
过电位
光系统II
氧气
电化学
电极
物理化学
光合作用
生物化学
有机化学
作者
Dahuan Li,Xiaoyue Zhang,Jiangquan Lv,Pingwei Cai,Yan‐Qiong Sun,Cai Sun,Shou‐Tian Zheng
标识
DOI:10.1002/anie.202312706
摘要
Inspired by the metal-oxo cluster structural feature and charge separation behaviour of the oxygen evolving center (OEC) in photosystem II (PS-II) under photoirradiation, a new crystalline photochromic polyoxomolybdate, MV2 [β-Mo8 O26 ] (1, MV=methyl viologen cation), is designed as a biomimetic oxygen evolution reaction (OER) catalyst in neutral electrolytes. After photoinduced electron transfer (PIET) with colour change from colourless to grey, it remains in an ultra-stable charge-separated state over a year under ambient conditions. The observed overpotential at 10 mA ⋅ cm-2 and Tafel slope decrease by 49 mV and 62.8 mV ⋅ dec-1 after coloration, respectively. The outstanding OER performance of the coloured state in neutral electrolytes even outperforms the commercial RuO2 benchmark. Experimental and theoretical studies show that oxygen holes within polyanions after irradiation serve as sites for enhancing direct O-O coupling, thus effectively promoting OER. This is the first successful application of electron-transfer photochromism to realize OER activity gain.
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