Tandem Electroreduction of CO2 to Programmable Acetate and Syngas via Single-Nickel-Atom-Encapsulated Copper Nanocatalysts,ACS Materials Letters

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Tandem Electroreduction of CO2 to Programmable Acetate and Syngas via Single-Nickel-Atom-Encapsulated Copper Nanocatalysts
ACS Materials Letters ( IF 9.6 ) Pub Date : 2022-12-01 , DOI: 10.1021/acsmaterialslett.2c00922
Xiaosong Hu _{1,

2,

3} , Jiye Li _{1,

2} , Ziqian Zhou _{1,

2} , Liaoyong Wen _{1,

2,

3}

Affiliation

The development of electrocatalysts for converting CO₂ to controllable chemicals would meet the strategic requirements, yet remains a great challenge. Herein, a cost-effective tandem catalyst based on Ni single-atom-encapsulated Cu NPs is developed for efficient electroreduction of CO₂ (CO₂RR) to acetate and syngas in a programmable manner. The operando infrared spectra and density functional theory calculations reveal that the high CO coverage constructed by Ni single atoms could provide favorable conditions for the C–C coupling on the adjacent Cu NPs dominated by the (111) facet and further facilitate the generation of acetate. Moreover, the as-prepared tandem catalyst can also facilitate the formation of syngas (H₂/CO) in a wide range from 0.06:1 to 19.5:1 for different application scenarios. Our tandem strategy is expected to contribute to promoting the high single-C₂ selectivity liquid fuel output, and facilitating the potential adaption of CO₂RR to syngas-mediated thermocatalytic processes for the industrial production.

中文翻译：

通过单镍原子包封铜纳米催化剂将 CO2 串联电还原为可编程乙酸盐和合成气

开发用于将CO ₂转化为可控化学品的电催化剂将满足战略需求，但仍然是一个巨大的挑战。在此，开发了一种基于 Ni 单原子包封 Cu NP 的经济高效的串联催化剂，用于以可编程方式将 CO ₂ (CO ₂ RR) 高效电还原为乙酸盐和合成气。原位红外光谱和密度泛函理论计算表明，由 Ni 单原子构成的高 CO 覆盖率可以为以 (111) 面为主的相邻 Cu NPs 上的 C-C 偶联提供有利条件，并进一步促进醋酸盐的生成。此外，所制备的串联催化剂还可以促进合成气（H ₂/CO) 在从 0.06:1 到 19.5:1 的广泛范围内适用于不同的应用场景。我们的串联策略有望有助于促进高单 C ₂选择性液体燃料输出，并促进 CO ₂ RR 对工业生产中合成气介导的热催化过程的潜在适应。

更新日期：2022-12-01

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