Transition metal (Fe, Co, Ni)-doped cuprous oxide nanowire arrays as self-supporting catalysts for electrocatalytic CO2 reduction reaction to ethylene

IF 6.3 2区材料科学 Q2 CHEMISTRY, PHYSICAL

Applied Surface Science Pub Date : 2024-04-23 DOI:10.1016/j.apsusc.2024.160150

Shihao Min , Zhuoyue Wang , Xiao Xu , Jiaxin He , Miao Sun , Wenlie Lin , Longtian Kang

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Abstract

The transition metal (Fe, Co, Ni)-doped cuprous oxide (Cu₂O) nanowire arrays on Cu mesh (CM) (M-Cu₂O@CM, M = Fe, Co, Ni) are successfully synthesized for the electrocatalytic CO₂ reduction reaction (CO₂RR) to ethylene (C₂H₄) through the simple calcination and impregnation-exchange methods. Systematic characterizations have demonstrated that the Ni/Co doping in Cu₂O@CM is conducive to stabilizing the Cu⁺ sites due to the electron transfer from Cu₂O to Ni/Co, while the Fe doping has the opposite effect. Consequently, they show the different electrocatalytic performances of Ni-Cu₂O@CM > Co-Cu₂O@CM > Cu₂O@CM > Fe-Cu₂O@CM for CO₂RR to C₂H₄ in an H-cell. Among them, Ni-Cu₂O@CM exhibits the ∼2.0-fold faradaic efficiency for C₂H₄ (58.2 % vs. 28.7 %) and the ∼2.5-fold current density (−37.6 vs. −15.0 mA·cm⁻²) at −1.1 V vs. RHE, as compared with Cu₂O@CM. Further experiments reveal that during the electrocatalytic CO₂RR, the Ni-Cu₂O@CM can generate more *CO, which promotes the C–C coupling reaction. The activity of Co-Cu₂O@CM is lower than Ni-Cu₂O@CM because of the strong adsorption of *COOH, while the Fe-Cu₂O@CM even exhibits a lower activity than Cu₂O@CM. This work provides an insight into the effect of transition metal-doped Cu₂O array on the electrocatalytic CO₂RR to C₂H₄ products.

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掺杂过渡金属（铁、钴、镍）的氧化亚铜纳米线阵列作为电催化二氧化碳还原乙烯反应的自支撑催化剂

通过简单的煅烧和浸渍-交换方法，成功合成了掺杂过渡金属（铁、钴、镍）的氧化亚铜（Cu2O）纳米线阵列（M-Cu2O@CM，M = 铁、钴、镍），用于电催化二氧化碳还原反应（CO2RR）制乙烯（C2H4）。系统表征表明，由于电子从 Cu2O 转移到 Ni/Co，Cu2O@CM 中的 Ni/Co 掺杂有利于稳定 Cu+ 位点，而 Fe 掺杂则具有相反的效果。因此，他们展示了 Ni-Cu2O@CM > Co-Cu2O@CM > Cu2O@CM > Fe-Cu2O@CM 在 H 细胞中将 CO2RR 转化为 C2H4 的不同电催化性能。其中，与 Cu2O@CM 相比，Ni-Cu2O@CM 在-1.1 V 对 RHE 条件下对 C2H4 的远动效率提高了 2.0 倍（58.2 % 对 28.7 %），电流密度提高了 2.5 倍（-37.6 对 -15.0 mA-cm-2）。进一步的实验表明，在电催化 CO2RR 的过程中，Ni-Cu2O@CM 可以生成更多的 *CO，从而促进 C-C 偶联反应。Co-Cu2O@CM 的活性比 Ni-Cu2O@CM 低，因为它吸附了较多的 *COOH，而 Fe-Cu2O@CM 的活性甚至低于 Cu2O@CM。这项研究深入探讨了掺杂过渡金属的 Cu2O 阵列对电催化 CO2RR 转化为 C2H4 产物的影响。

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来源期刊

Applied Surface Science 工程技术-材料科学：膜

CiteScore

12.50

自引率

7.50%

发文量

3393

审稿时长

67 days

期刊介绍： Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.