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金-铜双面纳米结构的籽晶生长作为一种串联催化剂用于将CO高效电还原为C产物

Seeded Growth of Gold-Copper Janus Nanostructures as a Tandem Catalyst for Efficient Electroreduction of CO to C Products.

作者信息

Zheng Yiqun, Zhang Jiawei, Ma Zesong, Zhang Gongguo, Zhang Haifeng, Fu Xiaowei, Ma Yanyun, Liu Feng, Liu Maochang, Huang Hongwen

机构信息

School of Chemistry, Chemical Engineering, and Materials, Jining University, Qufu, Shandong, 273155, China.

School of Materials Science and Engineering, Hunan University, Changsha, Hunan, 410082, China.

出版信息

Small. 2022 May;18(19):e2201695. doi: 10.1002/smll.202201695. Epub 2022 Apr 10.

Abstract

Gold-copper (Au-Cu) Janus nanostructures (Au-Cu Janus NSs) are successfully prepared using N-oleyl-1,3-propanediamine as capping agent and Cu(acac) as the precursor in a typical seeded growth strategy. By preferably depositing Cu atoms on one side of concave cubic Au seeds, the Cu part gradually grows larger as more Cu precursors are added, making the size tuning feasible in the range of 74-156 nm. When employed as an electrocatalyst for electrochemical CO reduction (CO RR), the Au-Cu Janus NSs display superior performance to Au@Cu core-shell NSs and Cu NPs in terms of C products selectivity (67%) and C partial current density (-0.29 A cm ). Combined experimental verification and theoretical simulations reveal that CO spillover from Au sites to the nearby Cu counterparts would enhance CO coverage and thus promote C-C coupling, highlighting the unique structural advantages of the Au-Cu Janus NSs toward deep reduction of CO . The current work provides a facile strategy to fabricate tandem catalyst with a Janus structure and validates its structural advantages toward CO RR, which are of critical importance for the rational design of efficient CO RR catalyst.

摘要

采用典型的种子生长策略,以N-油基-1,3-丙二胺为封端剂、Cu(acac)为前驱体,成功制备了金铜(Au-Cu)Janus纳米结构(Au-Cu Janus NSs)。通过优先在凹面立方Au种子的一侧沉积Cu原子,随着加入更多的Cu前驱体,Cu部分逐渐变大,使得尺寸在74-156nm范围内可调。当用作电化学CO还原(CO RR)的电催化剂时,Au-Cu Janus NSs在C产物选择性(67%)和C分电流密度(-0.29A cm)方面表现出优于Au@Cu核壳NSs和Cu NPs的性能。结合实验验证和理论模拟表明,CO从Au位点溢流到附近的Cu位点会增加CO覆盖率,从而促进C-C偶联,突出了Au-Cu Janus NSs在CO深度还原方面的独特结构优势。当前工作提供了一种制备具有Janus结构的串联催化剂的简便策略,并验证了其在CO RR方面的结构优势,这对于高效CO RR催化剂的合理设计至关重要。

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