等离激元热点介导的C-C偶联驱动CO2向C2H6的高选择性光还原

doi:10.1016/S1872-2067(26)65262-X

催化学报 ›› 2027, Vol. 92: 237-247.DOI: 10.1016/S1872-2067(26)65262-X

等离激元热点介导的C-C偶联驱动CO₂向C₂H₆的高选择性光还原

刘小磊^a^,¹, 梁尹蓝^a^,¹, 李金雨^a, 李慧亮^b^,^*(), 郑昭科^c, 王泽岩^c, 罗建民^d, 李娟^a, 蒋保江^e^,^*(), 李宝军^a^,^*(), 娄在祝^a^,^*()

^a 暨南大学物理与光电工程学院, 广东省纳米光学操控重点实验室, 广东广州 511443
^b 河北农业大学理学院, 化学系, 河北保定 071001
^c 山东大学晶体材料全国重点实验室, 山东济南 250100
^d 韶关学院化学与土木工程学院, 广东韶关 512005
^e 广东工业大学材料与能源学院, 广东广州 510006

收稿日期:2026-03-24 接受日期:2026-05-08 出版日期:2027-01-02 发布日期:2026-10-30
通讯作者: *电子信箱: lxlhl@hebau.edu.cn (李慧亮),
jbj@gdut.edu.cn (蒋保江),
baojunli@jnu.edu.cn (李宝军),
zzlou@jnu.edu.cn (娄在祝).
作者简介:第一联系人：
¹共同第一作者.
基金资助:
国家自然科学基金(U23A20136);国家自然科学基金(22672081);国家自然科学基金(22175076);广州市科技计划项目(2025A04J0232);中央高校基本科研业务费.

Plasmonic hotspots-mediated C-C coupling drives selective CO₂-to-C₂H₆ photoreduction

Xiaolei Liu^a^,¹, Yinlan Liang^a^,¹, Jinyu Li^a, Huiliang Li^b^,^*(), Zhaoke Zheng^c, Zeyan Wang^c, Jianmin Luo^d, Juan Li^a, Baojiang Jiang^e^,^*(), Baojun Li^a^,^*(), Zaizhu Lou^a^,^*()

^a Guangdong Provincial Key Laboratory of Nanophotonic Manipulation, Institute of Nanophotonics, College of Physics & Optoelectronic Engineering, Jinan University, Guangzhou 511443, Guangdong, China
^b Department of Chemistry, College of Science, Hebei Agricultural University, Baoding 071001, Hebei, China
^c State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100, Shandong, China
^d School of Chemistry and Civil Engineering, Shaoguan University, Shaoguan 512005, Guangdong, China
^e School of Materials and Energy, Guangdong University of Technology, Guangzhou 510006, Guangdong, China

Received:2026-03-24 Accepted:2026-05-08 Online:2027-01-02 Published:2026-10-30
Contact: *E-mail: lxlhl@hebau.edu.cn (H. Li),
jbj@gdut.edu.cn (B. Jiang),
baojunli@jnu.edu.cn (B. Li),
zzlou@jnu.edu.cn (Z. Lou).
About author:First author contact:
¹ Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(U23A20136);National Natural Science Foundation of China(22672081);National Natural Science Foundation of China(22175076);Science and Technology Program of Guangzhou(2025A04J0232);Fundamental Research Funds for the Central Universities.

摘要/Abstract

摘要：

光催化CO₂还原技术能够利用太阳能将CO₂和H₂O转化为高附加值化学品, 是实现碳循环闭合和可持续发展的重要途径. 然而, 光催化CO₂还原到高值多碳(C₂₊)产物仍面临巨大挑战, 其核心瓶颈在于C-C偶联动力学缓慢、光生载流子密度低以及关键C₁中间体的吸附与转化效率不足. 等离激元材料凭借其表面等离激元共振效应(SPR), 可将入射光能量局域在纳米尺度, 显著增强局域电磁场并产生高能热载流子, 为突破上述瓶颈提供了新机遇. 然而, 传统等离激元材料仍存在热载流子密度低、表面活性位点匮乏等问题, 严重制约了C₂₊产物的生成. 因此, 亟需开发高性能等离激元光催化剂以实现高效高选择性的C₂₊产物生成.

针对上述挑战, 本文设计并构建了一种由Au纳米粒子与Ni单原子掺杂W₁₈O₄₉纳米线组成的双等离激元异质结构, 旨在通过等离激元热点效应与双活性位点协同作用, 实现CO₂和H₂O向乙烷(C₂H₆)的高效高选择性光还原. X射线吸收光谱和透射电镜表明, Ni以单原子形式均匀掺杂于W₁₈O₄₉晶格中, 且Au纳米粒子紧密锚定于Ni-W₁₈O₄₉纳米线表面, 形成紧密接触的异质界面. 时域有限差分模拟结果显示, Au/Ni-W₁₈O₄₉界面处产生的等离激元热点能够显著增强局域电磁场, 大幅促进热载流子的产生与富集. 原位X射线光电子能谱和原位漫反射光谱证实, Ni_0.32-W₁₈O₄₉带间激发产生的光生电子可增强其自由电子密度和SPR响应, 且部分热电子会进一步由Ni_0.32-W₁₈O₄₉向Au纳米颗粒迁移. 在反应机理方面, 原位红外光谱和密度泛函理论计算结果表明, Ni掺杂位点促进CO₂还原生成*CHO中间体, 而相邻的Au位点则有利于*CO物种的生成与稳定, 增加了C₁中间体在催化剂表面的覆盖度; 等离激元热点增强了Ni与Au双活性位点之间的协同作用, 通过在Au位点优先形成关键的*COCHO中间体驱动高效的C-C偶联, 最终实现C₂H₆的高选择性生成. 光催化CO₂还原性能测试结果显示, 最优的Au_1.2/Ni_0.32-W₁₈O₄₉催化剂在模拟太阳光(AM 1.5G, 300 mW cm^-2)照射下, C₂H₆产率达到25.41 μmol g^-1 h^-1, 选择性高达72.13%, 而纯Ni_0.32-W₁₈O₄₉无法生成C₂H₆. 此外, 不同波长光照实验与表观量子效率结果表明, 全光谱激发同时激活Au的SPR和Ni-W₁₈O₄₉的带隙跃迁是实现高效C₂H₆生成的必要条件, 且Au的SPR效应在促进C₂H₆生成中发挥了决定性作用.

综上, 本工作通过将等离激元热点工程与原子级活性位点设计相结合, 成功实现了等离激元热载流子与表面活性位点的协同调控, 为高效、高选择性光催化CO₂还原制C₂₊产物提供了全新的设计思路. 这一策略为等离激元光催化CO₂还原向多碳产物合成的理性设计指明了方向.

关键词: 光催化CO₂还原, 表面等离子体共振, 等离激元热点, C₂H₆生成, C-C偶联

Abstract:

Photocatalytic CO₂ reduction to C₂₊ products remains challenging due to inefficient C-C coupling. Herein, we design a plasmonic heterostructure comprising Au nanoparticles (NPs) and Ni-doped W₁₈O₄₉ (Ni-W₁₈O₄₉) nanowires for selective CO₂-to-C₂H₆ photoreduction with H₂O. Plasmonic hotspots generated at the Au/Ni-W₁₈O₄₉ interface concentrate optical energy via localized electromagnetic field enhancement, greatly boosting hot-electron generation and enrichment at the active sites. Meanwhile, Ni dopants in W₁₈O₄₉ promote the formation of *CHO intermediates, while adjacent Au NPs favor the generation and stabilization of *CO species. Crucially, these plasmonic hotspots mediate the synergy between the dual active sites, driving efficient C-C coupling by forming the critical *COCHO intermediate and enabling selective C₂H₆ formation. Therefore, the optimized Au_1.2/Ni_0.32-W₁₈O₄₉ catalyst attains a C₂H₆ yield of 25.41 μmol g^-1 h^-1 with 72.13% selectivity, a performance unattainable with bare Ni-W₁₈O₄₉. This work establishes engineered plasmonic hotspots as a potent strategy to advance CO₂-to-C₂₊ photosynthesis.

Key words: Photocatalytic CO₂ reduction, Surface plasmon resonance, Plasmonic hotspots, C₂H₆ production, C-C coupling

刘小磊, 梁尹蓝, 李金雨, 李慧亮, 郑昭科, 王泽岩, 罗建民, 李娟, 蒋保江, 李宝军, 娄在祝. 等离激元热点介导的C-C偶联驱动CO₂向C₂H₆的高选择性光还原[J]. 催化学报, 2027, 92: 237-247.

Xiaolei Liu, Yinlan Liang, Jinyu Li, Huiliang Li, Zhaoke Zheng, Zeyan Wang, Jianmin Luo, Juan Li, Baojiang Jiang, Baojun Li, Zaizhu Lou. Plasmonic hotspots-mediated C-C coupling drives selective CO₂-to-C₂H₆ photoreduction[J]. Chinese Journal of Catalysis, 2027, 92: 237-247.

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链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(26)65262-X

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图/表 6

Fig. 1. (a) Schematic diagram of the fabrication for the Au/Ni-W18O49 heterostructures with different Au NP sizes. TEM images of Ni0.32-W18O49 (b) and Au1.2/Ni0.32-W18O49 (c). (d-g) EDS elemental mappings of Au1.2/Ni0.32-W18O49. (h) HRTEM images of Au1.2/Ni0.32-W18O49. (i) UV-Vis-NIR DRS of W18O49, Ni0.32-W18O49, and Au1.2/Ni0.32-W18O49. Normalized Ni K-edge XANES spectra (j) and FT-EXAFS spectra (k) of Ni0.32-W18O49, Ni foil, and NiO reference. WT-Ni K-edge EXAFS of Ni foil (l), NiO reference (m), and Ni0.32-W18O49 (n).

Fig. 2. (a) CH4 and CO production rates and CH4 selectivity of W18O49 and Nix-W18O49 (x = 0.15, 0.32, 0.44, and 0.59). CH4, CO, and C2H6 production rates and C2H6 selectivity of the Auy/Ni0.32-W18O49 heterostructures (y = 0.3, 0.6, 0.9, 1.2, 1.5, and 1.8) (b), and W18O49, Ni0.32-W18O49, Au1.2/Ni0.32-W18O49, and Au1.2/W18O49 (c). (d) Comparative activity of Au1.2/Ni0.32-W18O49 under different conditions. (e) Isotope-labeling MS analysis of products from photocatalytic 13CO2 reduction over Au1.2/Ni0.32-W18O49. (f) Stability test of Au1.2/Ni0.32-W18O49 over five consecutive reaction cycles.

Fig. 3. (a) CH4, CO, C2H4, and C2H6 production rates and C2H6 selectivity of Ni0.32-W18O49, Cu1.2/Ni0.32-W18O49, Ag1.2/Ni0.32-W18O49, and Au1.2/Ni0.32-W18O49. (b) Relation between the size of Au NPs and C2H6 production rate and selectivity over Auy/Ni0.32-W18O49. (c) CH4, CO, and C2H6 production rates and C2H6 selectivity of Au1.2/Ni0.32-W18O49 upon different light irradiations with the same intensity of 300 mW cm-2. (d) UV-Vis-NIR DRS and AQE of Au1.2/Ni0.32-W18O49.

Fig. 4. Spatial distributions of SPR-induced electric fields (a) and extinction spectra (b) of the single W18O49 nanowire (a length of 350 nm and a width of 10 nm), Au NP (55 nm), and 55 nm Au/W18O49 heterostructure from FDTD simulations. (c) Spatial distributions of SPR-induced electric fields of the Au/W18O49 heterostructures with different Au NP sizes of 30, 40, 50, 85, and 110 nm from FDTD simulations. Extinction spectra (d) and the ratio of absorbance to scattering (e) of the Au/W18O49 heterostructures with different Au NP sizes.

Fig. 5. W 4f (a), O 1s (b), Ni 2p (c), and Au 4f (d) XPS spectra of Au1.2/Ni0.32-W18O49 in the dark and under full-spectrum irradiation (OL: lattice oxygen, *OH: adsorbed hydroxyl species). (e) UV-Vis-NIR DRS of Ni0.32-W18O49 and Au1.2/Ni0.32-W18O49 before and after UV-irradiation for 25 s. (f) Schematic diagram of charge transfer in the Au1.2/Ni0.32-W18O49 heterostructure.

Fig. 6. In-situ FTIR spectroscopy of Ni0.32-W18O49 (a) and Au1.2/Ni0.32-W18O49 (b) under light irradiation in a CO2 and water vapor atmosphere. (c) Free energy diagrams for CO2 reduction to *CHO or CO on the W site of W18O49 and the Ni and Au sites of Au/Ni-W18O49. (d) Free energy diagrams for anchoring two C1 intermediates on different sites in Au/Ni-W18O49. (e) Free energy diagram for coupling of *CO and *CHO into *COCHO and its subsequent protonation to CH3CH3 over Au/Ni-W18O49. The structural models consist of W (gray), Ni (blue), Au (yellow), O (red), C (brown), and H (white) atoms. (f) Schematic diagram of PCR mechanism over plasmonic Au/Ni-W18O49 heterostructures.

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等离激元热点介导的C-C偶联驱动CO₂向C₂H₆的高选择性光还原

Plasmonic hotspots-mediated C-C coupling drives selective CO₂-to-C₂H₆ photoreduction

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