用于 pH 通用 CO2 电还原的原子分散 Ni-Cu 催化剂,Advanced Materials

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用于 pH 通用 CO2 电还原的原子分散 Ni-Cu 催化剂
Advanced Materials ( IF 27.4 ) Pub Date : 2023-01-10 , DOI: 10.1002/adma.202209590
Libing Zhang _{1,

2} , Jiaqi Feng ₁ , Shoujie Liu ₃ , Xingxing Tan _{1,

2} , Limin Wu _{1,

2} , Shunhan Jia _{1,

2} , Liang Xu ₁ , Xiaodong Ma _{1,

2} , Xinning Song _{1,

2} , Jun Ma ₁ , Xiaofu Sun _{1,

2} , Buxing Han _{1,

2,

4}

Affiliation

CO _{2电还原对于减少CO}₂排放和完成碳循环具有重要意义。然而，在中性或碱性电解质中不可避免的碳酸盐形成和低CO ₂利用率阻碍了其在商业规模上的应用。在酸性条件下开发CO ₂还原提供了一个有前途的策略，但抑制析氢反应是困难的。在此，首次报道了设计负载在空心氮掺杂碳上的 Ni-Cu 双原子催化剂用于 pH 通用 CO ₂电还原为CO。催化剂在酸性、中性和碱性电解质中显示出≈99%的高CO法拉第效率，CO的分电流密度达到190±11、225±10和489±14mA cm ^-2，分别。特别是酸性条件下CO _{2 的}利用效率达到64.3%，是碱性条件下的2倍。详细研究表明Ni和Cu原子之间存在电子相互作用。Cu 原子将 Ni d 带中心进一步推向费米能级，从而加速 *COOH 的形成。此外，操作数表征和密度泛函理论计算用于阐明在酸性和碱性电解质下CO ₂生成CO的可能反应机理。

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Atomically Dispersed Ni–Cu Catalysts for pH-Universal CO2 Electroreduction

CO₂ electroreduction is of great significance to reduce CO₂ emissions and complete the carbon cycle. However, the unavoidable carbonate formation and low CO₂ utilization efficiency in neutral or alkaline electrolytes hinder its application at commercial scale. The development of CO₂ reduction under acidic conditions provides a promising strategy, but the inhibition of the hydrogen evolution reaction is difficult. Herein, the first work to design a Ni–Cu dual atom catalyst supported on hollow nitrogen-doped carbon is reported for pH-universal CO₂ electroreduction to CO. The catalyst shows a high CO Faradaic efficiency of ≈99% in acidic, neutral, and alkaline electrolytes, and the partial current densities of CO reach 190 ± 11, 225 ± 10, and 489 ± 14 mA cm⁻², respectively. In particular, the CO₂ utilization efficiency under acidic conditions reaches 64.3%, which is twice as high as that of alkaline conditions. Detailed study indicates the existence of electronic interaction between Ni and Cu atoms. The Cu atoms push the Ni d-band center further toward the Fermi level, thereby accelerating the formation of *COOH. In addition, operando characterizations and density functional theory calculation are used to elucidate the possible reaction mechanism of CO₂ to CO under acidic and alkaline electrolytes.

更新日期：2023-01-10

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