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将惰性CeO负载到活性CoO上实现翻转负载,以显著提高类芬顿反应中的催化活性。

Overturned Loading of Inert CeO to Active Co O for Unusually Improved Catalytic Activity in Fenton-Like Reactions.

作者信息

Song Chunli, Zhan Qing, Liu Fei, Wang Chuan, Li Hongchao, Wang Xuan, Guo Xuefeng, Cheng Yingchun, Sun Wei, Wang Li, Qian Jieshu, Pan Bingcai

机构信息

Jiangsu Key Laboratory of Chemical Pollution Control and Resources Reuse, School of Environmental and Biological Engineering, Nanjing University of Science and Technology, 200 Xiao Ling Wei, Nanjing, 210094, China.

Key Laboratory of Flexible Electronics & Institute of Advanced Materials, Jiangsu National Synergetic Innovation Center for Advanced Materials, Nanjing Tech University, Nanjing, 211816, China.

出版信息

Angew Chem Int Ed Engl. 2022 Apr 11;61(16):e202200406. doi: 10.1002/anie.202200406. Epub 2022 Feb 21.

Abstract

In the past decades, numerous efforts have been devoted to improving the catalytic activity of nanocomposites by either exposing more active sites or regulating the interaction between the support and nanoparticles while keeping the structure of the active sites unchanged. Here, we report the fabrication of a Co O -CeO nanocomposite via overturning the loading direction, i.e., loading an inert CeO support onto active Co O nanoparticles. The resultant catalyst exhibits unexpectedly higher activity and stability in peroxymonosulfate-based Fenton-like reactions than its analog prepared by the traditional impregnation method. Abundant oxygen vacancies (O with a Co⋅⋅⋅O ⋅⋅⋅Ce structure instead of Co⋅⋅⋅O ) are generated as new active sites to facilitate the cleavage of the peroxide bond to produce SO and accelerate the rate-limiting step, i.e., the desorption of SO , affording improved activity. This strategy is a new direction for boosting the catalytic activity of nanocomposite catalysts in various scenarios, including environmental remediation and energy applications.

摘要

在过去几十年中,人们通过暴露更多活性位点或调节载体与纳米颗粒之间的相互作用,同时保持活性位点结构不变,致力于提高纳米复合材料的催化活性。在此,我们报道了一种通过颠倒负载方向制备CoO-CeO纳米复合材料的方法,即将惰性CeO载体负载到活性CoO纳米颗粒上。所得催化剂在基于过一硫酸盐的类芬顿反应中表现出比传统浸渍法制备的类似物更高的活性和稳定性。大量氧空位(具有Co⋅⋅⋅O ⋅⋅⋅Ce结构而非Co⋅⋅⋅O的O)作为新的活性位点生成,以促进过氧化物键的断裂产生SO 并加速限速步骤,即SO 的解吸,从而提高活性。该策略是在包括环境修复和能源应用等各种场景中提高纳米复合催化剂催化活性的新方向。

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