Engineering atomic-scale synergy of Ni and Mn dual-atom catalysts for highly efficient CO2 electroreduction†

IF 9.5 2区 材料科学 Q1 CHEMISTRY, PHYSICAL
Xin Cui, Yang Chen, Xiaodong Sun, Ying Sun, Hui Li and Tianyi Ma
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引用次数: 0

Abstract

The electrochemical CO2 reduction into value-added products is a promising way to reduce CO2 emissions. However, the design of efficient dual-atom catalysts to improve electrochemical CO2 reduction performance remains a challenge. Herein, a novel Ni1Mn1–NC dual-atom catalyst with neighboring Ni and Mn atomic interactions is developed for CO2 reduction. The Ni1Mn1–NC catalyst with Ni and Mn atomic pairs exhibits excellent performance with a faradaic efficiency of CO (FECO) of up to 97% at −0.7 V vs. RHE, far outperforming the Ni1–NC and Mn1–NC single-atom catalysts. In addition, the CO partial current density achieves 9.0 mA cm−2 at −1.1 V vs. RHE, which is 2.3 and 45.0 times higher than that of Ni1–NC and Mn1–NC. Moreover, Ni1Mn1–NC demonstrated long-term stability with FECO above 90% for over 60 h. Structural characterization and kinetic analysis reveal that Mn atoms donate partial electrons to Ni via N-bridged interaction and facilitate the adsorption of CO2 and the formation of *COOH, thus boosting CO2 electroreduction. This work elucidates the importance of the cooperative effect between adjacent dual atoms and provides a new strategy for designing highly efficient metal–N–C catalysts for boosted catalysis.

Abstract Image

Ni和Mn双原子催化剂的工程原子级协同高效CO2电还原
电化学将二氧化碳还原为高附加值产品是一种很有前途的减少二氧化碳排放的方法。然而,设计高效的双原子催化剂来提高电化学CO2还原性能仍然是一个挑战。本文研究了一种具有相邻Ni和Mn原子相互作用的新型Ni1Mn1-NC双原子催化剂。具有Ni和Mn原子对的Ni1Mn1-NC催化剂表现出优异的性能,在-0.7 V vs. RHE下CO (FECO)的法拉第效率高达97%,远远优于Ni1-NC和Mn1-NC单原子催化剂。在-1.1 V时CO的偏电流密度达到9.0 mA cm-2,分别是Ni1-NC和Mn1-NC的2.3倍和45.0倍。此外,Ni1Mn1-NC在FECO高于90%的情况下表现出60 h以上的长期稳定性。结构表征和动力学分析表明,Mn原子通过n桥相互作用将部分电子给予Ni,促进了CO2的吸附和*COOH的形成,从而促进了CO2的电还原。这项工作阐明了相邻双原子之间的共通效应的重要性,并为设计高效的促进催化的金属- n - c催化剂提供了新的策略。
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来源期刊
Journal of Materials Chemistry A
Journal of Materials Chemistry A CHEMISTRY, PHYSICAL-ENERGY & FUELS
CiteScore
19.50
自引率
5.00%
发文量
1892
审稿时长
1.5 months
期刊介绍: The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.
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