KOH-Enabled Axial-Oxygen Coordinated Ni Single-Atom Catalyst for Efficient Electrocatalytic CO2 Reduction,Small Methods

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KOH-Enabled Axial-Oxygen Coordinated Ni Single-Atom Catalyst for Efficient Electrocatalytic CO2 Reduction
Small Methods ( IF 10.7 ) Pub Date : 2023-01-05 , DOI: 10.1002/smtd.202201311
Xuanyi Chen _{1,

2} , Wei Liu ₃ , Yuxia Sun ₂ , Ting Tan ₃ , Chen-Xia Du ₁ , Yuehui Li ₂

Affiliation

Precise control of the coordination structure of metal centers is an ideal approach to achieve reasonable selectivity, activity, and stability in the electrochemical reduction of CO₂. In this work, the KOH activation strategy for preparation of hierarchically porous material containing Ni single-atoms with axial-oxygen coordination is reported. Spectroscopic measurements reveal the multiple roles of KOH as oxygen source, pore-making reagent and promoter for the formation of key phthalocyanine structure. It exhibits superior surface area (1801 m² g⁻¹) and electrocatalytic performance (Faradaic efficiency of 94%, Turnover frequency of 11 362 h⁻¹). Notably, KOH-enabled architecture with abundant pores benefits the anchoring of Ni atoms and mass transfer for high activity and selectivity. Density functional theory calculations suggest that the axial-oxygen ligand can promote the electronic delocalization of the Ni site for facilitating the *COOH formation and *CO desorption to efficiently produce CO.

中文翻译：

KOH 赋能的轴向氧配位 Ni 单原子催化剂用于高效电催化 CO2 还原

_{精确控制金属中心的配位结构是在CO 2}的电化学还原中实现合理的选择性、活性和稳定性的理想途径。在这项工作中，报道了用于制备含 Ni 单原子轴向氧配位分级多孔材料的 KOH 活化策略。光谱测量揭示了 KOH 作为氧源、造孔剂和促进关键酞菁结构形成的多重作用。它表现出优异的表面积 (1801 m ² g ⁻¹ ) 和电催化性能（法拉第效率为 94%，转换频率为 11 362 h ⁻¹). 值得注意的是，具有丰富孔隙的 KOH 架构有利于 Ni 原子的锚定和传质，从而实现高活性和选择性。密度泛函理论计算表明，轴向氧配体可以促进 Ni 位点的电子离域，从而促进 *COOH 的形成和 *CO 的解吸，从而有效地产生 CO。

更新日期：2023-01-05

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