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用于将稳定的 CO 还原为碳氢化合物的自清洁催化剂电极。

Self-Cleaning Catalyst Electrodes for Stabilized CO Reduction to Hydrocarbons.

机构信息

Department of Chemistry, Yale University, 225 Prospect Street, New Haven, CT, 06511, USA.

Energy Sciences Institute, Yale University, 810 West Campus Drive, West Haven, CT, 06516, USA.

出版信息

Angew Chem Int Ed Engl. 2017 Oct 9;56(42):13135-13139. doi: 10.1002/anie.201707478. Epub 2017 Sep 7.

Abstract

A surface-restructuring strategy is presented that involves self-cleaning Cu catalyst electrodes with unprecedented catalytic stability toward CO reduction. Under the working conditions, the Pd atoms pre-deposited on Cu surface induce continuous morphological and compositional restructuring of the Cu surface, which constantly refreshes the catalyst surface and thus maintains the catalytic properties for CO reduction to hydrocarbons. The Pd-decorated Cu electrode can catalyze CO reduction with relatively stable selectivity and current density for up to 16 h, which is one of the best catalytic durability performances among all Cu electrocatalysts for effective CO conversion to hydrocarbons. The generality of this approach of utilizing foreign metal atoms to induce surface restructuring toward stabilizing Cu catalyst electrodes against deactivation by carbonaceous species accumulation in CO reduction is further demonstrated by replacing Pd with Rh.

摘要

提出了一种表面重构策略,涉及具有空前 CO 还原催化稳定性的自清洁 Cu 催化剂电极。在工作条件下,预沉积在 Cu 表面上的 Pd 原子诱导 Cu 表面的连续形态和组成重构,不断更新催化剂表面,从而保持 CO 还原为碳氢化合物的催化性能。Pd 修饰的 Cu 电极可以催化 CO 还原,具有相对稳定的选择性和电流密度,长达 16 小时,这是所有有效将 CO 转化为碳氢化合物的 Cu 电催化剂中最好的催化耐久性性能之一。通过用 Rh 代替 Pd,进一步证明了利用外来金属原子诱导表面重构来稳定 Cu 催化剂电极,防止因 CO 还原中碳质物种积累而失活的这种方法具有普遍性。

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