Electrochemically accessing ultrathin Co (oxy)-hydroxide nanosheets and operando identifying their active phase for the oxygen evolution reaction
Electrochemically accessing ultrathin Co (oxy)-hydroxide nanosheets and operando identifying their active phase for the oxygen evolution reaction
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电化学获取超薄 Co（氧）-氢氧化物纳米片并确定其析氧反应的活性相
DOI：
10.1039/c8ee03208d
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发表时间：
2019-02
影响因子：
32.5
通讯作者：
Zhang Shuo
中科院分区：
文献类型：
--
作者：
Zhou Jing;Wang Yu;Su Xiaozhi;Gu Songqi;Liu Renduo;Huang Yibo;Yan Shuai;Li Jiong;Zhang Shuo
近年来，钴(氧)-氢氧化物(CoOOH)被认为是电催化析氧反应(OER)的理想活性物种，在多种能量转换技术中起着关键作用。因此，寻找一种高产量的方法来制备先进的纳米结构并了解其反应活性是具有挑战性的但紧迫的任务。在这里，我们报告了一种可能大规模生产超薄CoOOH纳米片的电化学方法，而不是传统的液体剥离法，这种方法具有非常高的OER活性。这种几乎全表面的材料为研究电催化活性的表面化学提供了一个很好的平台。结合OPANDO X-射线能谱和理论计算，证明了在外加电势作用下，Co3+OH3+发生了与电位有关的去质子化反应，即Co3+OH3+转变为Co3+/4+OOH1Co3+/4+OH1型−x相。综合分析认为，降低去质子化能是提高OER活性的关键，氧化氧离子可能是OER的亲电中心。
Cobalt (oxy)-hydroxide (CoOOH) has recently been identified as a realistic active species under operando conditions for the electrocatalytic oxygen evolution reaction (OER), which plays a pivotal role in multiple energy conversion technologies. Therefore, searching for a high-yield method to fabricate advanced nanostructures and understanding their reactivity are challenging but urgent tasks. Here, rather than conventional liquid exfoliation, we report an electrochemical route for potentially large-scale production of ultrathin CoOOH nanosheets, which deliver exceptionally high OER activity. This “nearly-all-surface” material provides an excellent platform to study the surface chemistry for electrocatalytic activity. Combining operando X-ray spectroscopy and theoretical calculations demonstrated a potential-dependent deprotonation reaction, i.e., Co3+OOH is transformed into an active Co3+/4+OOH1−x phase for water oxidation under the applied potential. Comprehensive analysis suggested that reducing the deprotonation energy is the key to enhance the OER activity, and oxidized oxygen ions might act as electrophilic centers for the OER.
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