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Ultra-small Cu nanoparticles embedded in N-doped carbon arrays for electrocatalytic CO2 reduction reaction in dimethylformamide
Nano Research ( IF 9.9 ) Pub Date : 2018-08-02 , DOI: 10.1007/s12274-017-1936-1
Xiaolong Zhang , Ying Zhang , Fengwang Li , Christopher D. Easton , Alan M. Bond , Jie Zhang

The development of heterogeneous catalysts with a well-defined micro structure to promote their activity and stability for electrocatalytic CO2 reduction has been shown to be a promising strategy. In this work, Cu nanoparticles (∼ 4 nm in diameter) embedded in N-doped carbon (Cu@NC) arrays were fabricated by thermal decomposition of copper tetracyanoquinodimethane (CuTCNQ) under N2. Compared to polycrystalline copper electrodes, the Cu@NC arrays provide a significantly improved number of catalytically active sites. This resulted in a 0.7 V positive shift in onset potential, producing a catalytic current density an order magnitude larger at a potential of–2.7 V vs. Fc/Fc+ (Fc = ferrocene) in dimethylformamide (DMF). By controlling the water content in the DMF solvent, the CO2 reduction product distribution can be tuned. Under optimal conditions (0.5 vol% water), 64% HCOO, 20% CO, and 13% H2 were obtained. The Cu@NC arrays exhibited excellent catalytic stability with only a 0.5% decrease in the steady-state catalytic current during 6 h of electrolysis. The three-dimensional (3D) array structure of the Cu@NC was demonstrated to be effective for improving the catalytic activity of copper based catalysts while maintaining long-term catalytic stability.

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中文翻译:

嵌入N掺杂碳阵列中的超小Cu纳米颗粒用于电催化CO2个 二甲基甲酰胺中的还原反应

已经开发出具有明确定义的微观结构以提高其活性和电催化还原CO 2稳定性的非均相催化剂是一种有前途的策略。在这项工作中,通过在N 2下对四氰基喹甲烷铜(CuTCNQ)进行热分解,制备了嵌入N掺杂碳(Cu @ NC)阵列中的Cu纳米粒子(直径约4 nm)。与多晶铜电极相比,Cu @ NC阵列可显着提高催化活性位的数量。这导致起始电势有0.7 V的正移,在–2.7 V的电势下,与Fc / Fc +相比,产生的催化电流密度大一个数量级。(Fc =二茂铁)在二甲基甲酰胺(DMF)中。通过控制DMF溶剂中的水含量,可以调整CO 2还原产物的分布。在最佳条件下(0.5%的水),可获得64%的HCOO ,20%的CO和13%的H 2。Cu @ NC阵列表现出出色的催化稳定性,在电解6小时期间,稳态催化电流仅降低了0.5%。事实证明,Cu @ NC的三维(3D)阵列结构可有效提高铜基催化剂的催化活性,同时保持长期的催化稳定性。

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更新日期:2018-08-02
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