铜表面的氢氧化镨纳米棒通过相互作用和几何变形产生不对称的活性中心用于CO2电还原反应

doi:10.1016/S1872-2067(26)65193-5

催化学报 ›› 2026, Vol. 90: 158-168.DOI: 10.1016/S1872-2067(26)65193-5

铜表面的氢氧化镨纳米棒通过相互作用和几何变形产生不对称的活性中心用于CO₂电还原反应

张恒^a^,¹, 张泽宇^a^,¹, 侯坤明^a, 贾霖^a, 郭颖昕^a^,^*(), 李昊润^a, 邹梦波^a, 孙宪虎^b^,^*(), 曾尚红^a^,^*()

^a 内蒙古大学化学化工学院, 内蒙古呼和浩特 010021
^b 中国科学院大学化学科学学院, 北京 101408

收稿日期:2026-02-10 接受日期:2026-04-11 出版日期:2026-11-18 发布日期:2026-09-09
通讯作者: *电子信箱: yingxin.guo@imu.edu.cn (郭颖昕),
sunxianhu@ucas.ac.cn (孙宪虎),
zengshanghong@imu.edu.cn (曾尚红).
作者简介:
¹共同第一作者.
基金资助:
国家自然科学基金(22468034);鄂尔多斯重点研发项目(YF20240062)

Pr(OH)₃ nanorods on Cu generates asymmetric active sites through interplay and geometric deformation for CO₂ electroreduction

Heng Zhang^a^,¹, Zeyu Zhang^a^,¹, Kunming Hou^a, Lin Jia^a, Yingxin Guo^a^,^*(), Haorun Li^a, Mengbo Zou^a, Xianhu Sun^b^,^*(), Shanghong Zeng^a^,^*()

^a College of Chemistry and Chemical Engineering, Inner Mongolia University, Hohhot 010021, Inner Mongolia, China
^b School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 101408, China

Received:2026-02-10 Accepted:2026-04-11 Online:2026-11-18 Published:2026-09-09
Contact: *E-mail:yingxin.guo@imu.edu.cn(Y. Guo),sunxianhu@ucas.ac.cn(X. Sun),zengshanghong@imu.edu.cn(S. Zeng).
About author:
¹Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(22468034);Key Research and Development Project of Ordos(YF20240062)

摘要/Abstract

摘要：

利用可再生电力驱动的二氧化碳电化学还原(CO₂RR)是一种极具前景的途径, 不仅有助于降低大气中CO₂浓度, 还能生产高附加值化学品或燃料. 在各种产物中, 乙烯和乙醇因其经济潜力与实际应用价值而备受关注. 然而, 目标C₂₊产物的选择性仍不理想, 稳定Cu⁺物种对于提升Cu⁰/Cu⁺界面处的C₂₊产物选择性具有关键作用. 通过组分间的协同作用来稳定所需的Cu⁰/Cu⁺界面, 是提升CO₂催化转化性能的可行策略. 稀土元素因其独特的电子结构, 常作为掺杂剂用于提升多相催化反应的性能, 但其作用机制以及反应过程中与Cu物种之间的相互作用与结构重构尚不明确.

本文采用水热法合成了一系列Pr(OH)₃/CuO预催化剂, 在CO₂RR中原位转变为Pr(OH)₃/Cu催化剂, 借助组分间协同作用与几何形变诱导生成不对称活性位点. 结构表征结果显示, Pr(OH)₃纳米棒均匀分布在Cu纳米片表面, 形成稳定的Pr(OH)₃/Cu⁺/Cu异质界面, 可有效抑制Cu⁺过度还原, 显著提升表面Cu⁺物种占比; X-射线光电子能谱与X-射线吸收光谱结果证实, 催化剂中存在Pr³⁺/Pr⁴⁺与Cu⁺/Cu不对称活性位点, 加快界面电荷传输. 电催化性能测试表明, Pr(OH)₃有效地增强了催化剂CO₂RR到C₂H₄的催化活性. 在250 mA cm^-2时, 12.7% Pr(OH)₃/Cu催化剂可以实现50.2%的FE_C2H4, 同时, 其C₂产物也可以达到69.6%, 且可连续稳定运行25 h性能无明显衰减. 而纯Cu催化剂C₂H₄的选择性为36.1%. 原位拉曼光谱证实, Pr(OH)₃有助于CO₂在催化剂表面的吸附, 同时提升*CO中间体在催化剂表面覆盖率进而促进C-C耦合. 原位红外光谱结果表明, Pr(OH)₃促进了H₂O分子的解离, 有助于*CO质子化生成*COH和随后的*CO和*COH耦合. 更强的*OCCOH关键中间体信号强度表明, 反应遵循CO→*COH→*OCCOH的不对称C-C耦合路径. 由此可见, 稀土氢氧化物的引入可以激活铜上的不对称活性位点, 为有效的CO₂到C₂的转化提供了可持续的途径.

综上, 本文揭示Pr(OH)₃的引入诱导了不对称Pr³⁺/Pr⁴⁺和Cu⁺/Cu不对称活性位点的生成, 有效地增强了Cu催化剂CO₂RR到C₂H₄的催化活性. 通过系统的结构表征与原位光谱分析, 我们从分子层面深入探讨了可能的反应机制.

关键词: 氢氧化镨, 铜纳米片, 不对称活性位点, 催化机理, 二氧化碳电还原

Abstract:

Leveraging the asymmetric active motifs with high precision holds potential and presents substantial challenge due to design constraints and complex interphase. Herein, Pr(OH)₃ nanorods are introduced onto Cu nanosheets to spontaneously regulate the interplay aiming to prevent Cu over-reduction during the CO₂ electroreduction. Specifically, the 12.7% Pr(OH)₃/Cu catalyst achieves a 50.2% Faradaic efficiency of C₂H₄ at industrially relevant current density of 250 mA cm^-2. Complementary structural characterizations combined with in-situ/operando spectroscopy studies prove that Pr(OH)₃ incorporation facilitates the generation of asymmetric Pr³⁺/Pr⁴⁺ and Cu⁺/Cu motifs, synergizing the formation of C₂ products-related intermediates through increasing the number of active sites on the Pr(OH)₃/Cu⁺/Cu heterogeneous interphase. This work demonstrates that the introduction of rare earth hydroxide can activate the asymmetric active sites on Cu, providing a sustainable pathway for efficient CO₂-to-C₂ conversion.

Key words: Pr(OH)₃, Cu nanosheets, Asymmetric active sites, Catalytic mechanism, CO₂ electroreduction

张恒, 张泽宇, 侯坤明, 贾霖, 郭颖昕, 李昊润, 邹梦波, 孙宪虎, 曾尚红. 铜表面的氢氧化镨纳米棒通过相互作用和几何变形产生不对称的活性中心用于CO₂电还原反应[J]. 催化学报, 2026, 90: 158-168.

Heng Zhang, Zeyu Zhang, Kunming Hou, Lin Jia, Yingxin Guo, Haorun Li, Mengbo Zou, Xianhu Sun, Shanghong Zeng. Pr(OH)₃ nanorods on Cu generates asymmetric active sites through interplay and geometric deformation for CO₂ electroreduction[J]. Chinese Journal of Catalysis, 2026, 90: 158-168.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65193-5

https://www.cjcatal.com/CN/Y2026/V90/I11/158

图/表 5

Fig. 1. Structural and microscopic characterizations of CuO, Pr(OH)3/CuO and Pr(OH)3/Cu. (a) Schematic diagram for the preparation of Pr(OH)3/CuO and Pr(OH)3/Cu. Representative TEM (b) and AFM (c) images of the CuO. Representative TEM (d,e), HRTEM (f,g), HAADF-STEM images and corresponding EDS mappings (h) of the 12.7% Pr(OH)3/CuO pre-catalyst. Representative TEM (i) and HRTEM (j,k) images of the12.7% Pr(OH)3/Cu catalyst.

Fig. 2. Normalized Cu k-edge XANES spectra (a) and the corresponding FT-EXAFS spectra (b) of 12.7% Pr(OH)3/Cu, Cu nanosheet and references in R space. (c) WT plots for the k3-weighted EXAFS signal of 12.7% Pr(OH)3/Cu, Cu nanosheet and Cu foil. (d) Pr L3-edge XANES spectra of the 12.7% Pr(OH)3/Cu, 12.7% Pr(OH)3/CuO, Pr(OH)3 and Pr2O3. (e) FT EXAFS spectra of 12.7% Pr(OH)3/Cu, 12.7% Pr(OH)3/CuO, Pr(OH)3 and Pr2O3 at R space. (f) WT plots for the k3-weighted EXAFS signal of 12.7% Pr(OH)3/CuO, 12.7% Pr(OH)3/Cu and Pr2O3.

Fig. 3. (a) LSV curves of Cu and Pr(OH)3/Cu catalysts in 1 mol L-1 KOH in a flow cell. FE of Cu (b) and 12.7% Pr(OH)3/Cu (c) catalyst at applied current density in the range from 100 to 300 mA cm-2. (d) Relationship between Pr(OH)3 content and FE. (e) Stability test results for the 12.7% Pr(OH)3/Cu catalyst at 250 mA cm-2.

Fig. 4. In-situ potential-dependent surface-enhanced Raman spectra of 12.7% Pr(OH)3/CuO catalyst (a) and CuO nanosheet (b) in the regions of 200-1200 and 1600-2200 cm-1.

Fig. 5. Operando ATR-SEIRAS spectra of 12.7% Pr(OH)3/Cu (a,c) and Cu nanosheet (b,d) with 0.1 V interval from -0.6 to -1.4 V in a CO2-saturated 0.1 mol L-1 KHCO3 electrolyte.

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铜表面的氢氧化镨纳米棒通过相互作用和几何变形产生不对称的活性中心用于CO₂电还原反应

Pr(OH)₃ nanorods on Cu generates asymmetric active sites through interplay and geometric deformation for CO₂ electroreduction

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