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Atmospheric-Temperature Chain Reaction towards Ultrathin Non-Crystal-Phase Construction for Highly Efficient Water Splitting

Journal 2022 · IF 5.02 · 28(51): e202200683 · 发表于 2022 年 6 月 20 日
作者: Yanling Qiu,Zhiqiang Liu,Qian Yang,Xinyue Zhang,Jingquan Liu,Mengyao Liu,Tianyi Bi,Xuqiang Ji
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摘要

Graphical A multistep chain reaction at atmospheric temperature restructures the surface of high-crystallinity cobalt carbonate hydroxides (CCHs). An ultrathin (∼5 nm) lattice-disorder layer of Fe(OH) 3 on the CCH appeared to form CCH−FeOH hetero-interfaces, which are of great benefit for nano-interface exposure. The microscopic surface morphology of the material (CCH−FeOH-D x ) can be controlled by adjusting the degree of chain reaction. The as-obtained CCH−FeOH with an ultrathin shell structure is conducive to mass transfer and ion migration, giving excellent HER/OER performance. Combining the self-sacrifice of a highly crystalline substance to design a multistep chain reaction towards ultrathin active-layer construction for high-performance water splitting with atmospheric-temperature conditions and an environmentally benign aqueous environment is extremely intriguing and full of challenges. Here, taking cobalt carbonate hydroxides (CCHs) as the initial crystalline material, we choose the Lewis acid metal salt of Fe(NO 3 ) 3 to induce an aqueous-phase chain reaction generating free CO 3 2− ions with subsequent instant FeCO 3 hydrolysis. The resultant ultrathin (∼5 nm) amorphous Fe-based hydroxide layer on CCH results in considerable activity in catalyzing the oxygen evolution reaction (OER) and hydrogen evolution reaction (HER), yielding 10/50 mA ⋅ cm −2 at overpotentials of 230/266.5 mV for OER and 72.5/197.5 mV for HER. The catalysts can operate constantly in 1.0 M KOH over 48 and 45 h for the OER and HER, respectively. For bifunctional catalysis for alkaline electrolyzer assembly, a cell voltage as low as 1.53 V was necessary to yield 10 mA cm −2 (1.7 V at 50 mA cm −2 ). This work rationally builds high-efficiency electrochemical bifunctional water-splitting catalysts and offers a trial in establishing a controllable nanolevel ultrathin lattice disorder layer through an atmospheric-temperature chemical route.