Liu Juzhe, Nai Jianwei, You Tingting, An Pengfei, Zhang Jing, Ma Guanshui, Niu Xiaogang, Liang Chaoying, Yang Shihe, Guo Lin
School of Chemistry and Beijing Advanced Innovation Center for Biomedical Engineering, Beihang University, Beijing, 100191, China.
School of Chemical and Biomedical Engineering, Nanyang Technological University, Singapore, 637459, Singapore.
Small. 2018 Apr;14(17):e1703514. doi: 10.1002/smll.201703514. Epub 2018 Apr 3.
Structural flexibility can be a desirable trait of an operating catalyst because it adapts itself to a given catalytic process for enhanced activity. Here, amorphous cobalt hydroxide nanocages are demonstrated to be a promising electrocatalyst with an overpotential of 0.28 V at 10 mA cm , far outperforming the crystalline counterparts and being in the top rank of the catalysts of their kind, under the condition of electrocatalytic oxygen evolution reaction. From the direct experimental in situ and ex situ results, this enhanced activity is attributed to its high structural flexibility in terms of 1) facile and holistic transformation into catalytic active phase; 2) hosting oxygen vacancies; and 3) structure self-regulation in a real-time process. Significantly, based on plausible catalytic mechanism and computational simulation results, it is disclosed how this structural flexibility facilitates the kinetics of oxygen evolution reaction. This work deepens the understanding of the structure-activity relationship of the Co-based catalysts in electrochemical catalysis, and it inspires more applications that require flexible structures enabled by such amorphous nanomaterials.
结构灵活性可能是一种理想的操作催化剂特性,因为它能使自身适应特定的催化过程以提高活性。在此,非晶态氢氧化钴纳米笼被证明是一种有前景的电催化剂,在电催化析氧反应条件下,在10 mA cm 时过电位为0.28 V,远远优于晶体对应物,在同类催化剂中名列前茅。从直接的原位和非原位实验结果来看,这种增强的活性归因于其在以下方面的高结构灵活性:1)轻松且整体地转变为催化活性相;2)容纳氧空位;3)在实时过程中进行结构自我调节。值得注意的是,基于合理的催化机理和计算模拟结果,揭示了这种结构灵活性如何促进析氧反应的动力学。这项工作加深了对钴基催化剂在电化学催化中结构 - 活性关系的理解,并激发了更多需要此类非晶态纳米材料实现灵活结构的应用。