Structural Sensitivities in Bimetallic Catalysts for Electrochemical CO2 Reduction Revealed by Ag–Cu Nanodimers

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Jianfeng Huang, Mounir Mensi, Emad Oveisi, Valeria Mantella, Raffaella Buonsanti*
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引用次数: 277

Abstract

Understanding the structural and compositional sensitivities of the electrochemical CO2 reduction reaction (CO2RR) is fundamentally important for developing highly efficient and selective electrocatalysts. Here, we use Ag/Cu nanocrystals to uncover the key role played by the Ag/Cu interface in promoting CO2RR. Nanodimers including the two constituent metals as segregated domains sharing a tunable interface are obtained by developing a seeded growth synthesis, wherein preformed Ag nanoparticles are used as nucleation seeds for the Cu domain. We find that the type of metal precursor and the strength of the reducing agent play a key role in achieving the desired chemical and structural control. We show that tandem catalysis and electronic effects, both enabled by the addition of Ag to Cu in the form of segregated nanodomain within the same catalyst, synergistically account for an enhancement in the Faradaic efficiency for C2H4 by 3.4-fold and in the partial current density for CO2 reduction by 2-fold compared with the pure Cu counterpart. The insights gained from this work may be beneficial for designing efficient multicomponent catalysts for electrochemical CO2 reduction.

Abstract Image

Ag-Cu纳米二聚体揭示的电化学CO2还原双金属催化剂的结构敏感性
了解电化学CO2还原反应(CO2RR)的结构和组成敏感性对于开发高效、选择性的电催化剂至关重要。在这里,我们使用Ag/Cu纳米晶体来揭示Ag/Cu界面在促进CO2RR中所起的关键作用。纳米二聚体包括两种组成金属作为分离域共享可调界面,通过开发种子生长合成,其中预形成的银纳米粒子被用作铜域的成核种子。我们发现,金属前驱体的类型和还原剂的强度在实现所需的化学和结构控制方面起着关键作用。我们发现,串联催化和电子效应,都是通过在同一催化剂中以分离纳米结构域的形式向Cu中添加Ag而实现的,协同作用导致C2H4的法拉第效率提高了3.4倍,二氧化碳还原的分电流密度提高了2倍。本研究结果对设计高效的电化学CO2还原多组分催化剂具有重要的指导意义。
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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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