Seeded Growth of Gold–Copper Janus Nanostructures as a Tandem Catalyst for Efficient Electroreduction of CO2 to C2+ Products

• Published in: Small (Weinheim an der Bergstrasse, Germany) Vol. 18; no. 19; pp. e2201695 - n/a
• Main Authors: Zheng, Yiqun, Zhang, Jiawei, Ma, Zesong, Zhang, Gongguo, Zhang, Haifeng, Fu, Xiaowei, Ma, Yanyun, Liu, Feng, Liu, Maochang, Huang, Hongwen
• Format: Journal Article
• Language: English
• Published: Weinheim Wiley Subscription Services, Inc 01.05.2022
• Subjects: bimetallic Janus nanocrystals; Carbon dioxide; Catalysts; CO 2 electroreduction; Copper; Electrocatalysts; Gold; Janus structures; nanocrystals; Nanostructure; Nanotechnology; Precursors; Reduction; Selectivity; tandem catalysts
• ISSN: 1613-6810; 1613-6829
• DOI: 10.1002/smll.202201695

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)2 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 CO2 reduction (CO2RR), the Au‐Cu Janus NSs display superior performance to Au@Cu core‐shell NSs and Cu NPs in terms of C2+ products selectivity (67%) and C2+ partial current density (−0.29 A cm–2). 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 CO2. The current work provides a facile strategy to fabricate tandem catalyst with a Janus structure and validates its structural advantages toward CO2RR, which are of critical importance for the rational design of efficient CO2RR catalyst. Gold–copper (Au‐Cu) Janus nanostructure is successfully crafted and employed as an efficient tandem catalyst to enable deep electrochemical CO2 reduction (CO2RR) by capitalizing on the unique carbon monoxide (CO) spillover from Au concave cubic to the Cu nanoparticle. The as crafted Au‐Cu Janus NSs exhibit outstanding CO2RR activity (C2+ partial Faraday Efficiency (FEC2+) = 67% and C2+ partial current density (jC2+) = −0.29 A cm‐2), placing it among state‐of‐the‐art CO2RR catalysts.