Ru单原子与Ni团簇双位点协同构筑CeO2纳米棒实现高效太阳能驱动CO2甲烷化

doi:10.1016/S1872-2067(25)64914-X

催化学报 ›› 2026, Vol. 83: 183-197.DOI: 10.1016/S1872-2067(25)64914-X

Ru单原子与Ni团簇双位点协同构筑CeO₂纳米棒实现高效太阳能驱动CO₂甲烷化

尤长君^a^,¹, 任宇奇^a^,¹, 贺红斌^a^,¹, 彭若轩^a, 朱元皓^a, 程淼^a^,^*(), 丁培根^b, 张刘娜^b, 兰盛楠^a, 张虹扬^a, 章毅琴^a, 朱丰帆^a^,^*(), 李敬^c^,^*(), 周建成^a^,^*()

^a东南大学化学化工学院, 江苏南京 211189
^b延安大学化学与化工学院, 陕北低阶煤清洁高效利用协同创新中心, 陕西省化学反应工程重点实验室, 陕西延安 716000
^c中国科学院理化技术研究所, 光化学转换与功能材料重点实验室, 北京 100190

收稿日期:2025-08-03 接受日期:2025-09-24 出版日期:2026-04-18 发布日期:2026-03-04
通讯作者: * 电子信箱: cmiao@seu.edu.cn (程淼), fengfanzhu@outlook.com (朱丰帆), lijingsp@mail.ipc.ac.cn (李敬), jczhou@seu.edu.cn (周建成).
作者简介:¹共同第一作者.
基金资助:
东南大学博士研究生创新能力提升计划(CXJH_SEU 25169)

Dual-site atomic engineering of Ru Single-atoms and Ni clusters on CeO₂ nanorods for solar-driven CO₂ methanation

Changjun You^a^,¹, Yuqi Ren^a^,¹, Hongbin He^a^,¹, Ruoxuan Peng^a, Yuan-Hao Zhu^a, Miao Cheng^a^,^*(), Peigen Ding^b, Liuna Zhang^b, Shengnan Lan^a, Hongyang Zhang^a, Yiqin Zhang^a, Fengfan Zhu^a^,^*(), Jing Li^c^,^*(), Jiancheng Zhou^a^,^*()

^aSchool of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189, Jiangsu, China
^bDepartment of Chemistry and Chemical Engineering, Shaanxi Modern Industrial College of Green and Efficient Utilization of Energy Resources, Shaanxi Collaborative Innovation Center of Clean Utilization of Low Rank Coal, Yan’an University, Yan’an 716000, Shaanxi, China
^cKey Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy ofSciences, Beijing 100190, China

Received:2025-08-03 Accepted:2025-09-24 Online:2026-04-18 Published:2026-03-04
Contact: * E-mail: cmiao@seu.edu.cn (M. Cheng), fengfanzhu@outlook.com (F. Zhu),lijingsp@mail.ipc.ac.cn (J. Li), jczhou@seu.edu.cn (J. Zhou).
About author:¹Contributed equally to this work.
Supported by:
SEU Innovation Capability Enhancement Plan for Doctoral Students(CXJH_SEU 25169)

摘要/Abstract

摘要：

化石燃料燃烧导致的二氧化碳(CO₂)过度排放引发全球气候变化与能源危机, 发展太阳能驱动CO₂转化技术对实现“双碳”目标具有重要意义. 然而, 该过程面临光捕获效率低与CO₂甲烷化高活化能壁垒的双重瓶颈, 限制了反应速率和能量转化效率. 针对该挑战, 开发具备高效光吸收、活性位点精准调控和协同催化功能的新型光催化剂, 成为该领域的研究焦点. 本工作致力于通过构建原子尺度活性位点解耦的光催化剂, 协同利用光、电、热多物理场效应, 显著提升太阳能驱动CO₂转化的性能与效率, 为开发高效太阳能-化学品转换路径提供新策略.
本文采用溶剂热-湿化学还原法成功制备了一种单原子钌(Ru)与镍(Ni)团簇共负载的多孔二氧化铈(CeO₂)纳米棒催化剂. 创新设计思路在于利用原子分散的Ru位点取代CeO₂晶格Ce原子, 构成强金属-载体相互作用, 优化其局部电子结构. 同时, 在邻近区域构筑Ni团簇, 利用其局域表面等离子体共振(LSPR)效应拓宽可见光至近红外光吸收范围, 从而实现两种活性位点的空间分离、功能解耦与协同互作. 实验内容包括催化剂的精准合成、结构表征、光热催化性能评价以及原位/瞬态光谱机制研究. 在聚集太阳能辐照条件下, 该催化剂展现出优异的性能, 甲烷(CH₄)产率达133.1 μmol·cm⁻²·h⁻¹, 是非聚集太阳能辐照条件下的31倍, 同时, 太阳能转化为化学能的直接效率达到0.423%. 反应机理揭示Ru单原子位点可以显著加速H₂O解离产生大量高活性氢物种(^*H), 为还原反应提供充足质子源. Ni团簇通过LSPR高效捕获宽谱段太阳光产生热电子, 不仅优化了CO₂吸附, 还有效降低C=O键断裂能垒. 通过氢溢流效应, ^*H在Ru与Ni位点间高效传递, 从而解决了质子供给与碳源活化/加氢之间的时空失配问题. 飞秒/纳秒瞬态吸收光谱证明双位点结构实现光生载流子的空间分离、定向传输与快速利用, 显著延长了热载流子寿命. 聚焦强光场诱导的强烈光-电-热协同效应, 同步提升了载流子浓度与反应体系温度, 从而协同驱动反应动力学显著加速.
综上, 本文为通过精准设计原子级组装的多功能位点与有效耦合光、电、热多物理场构建高效光热协同催化系统提供了创新范式, 其深入的反应机制解析对未来太阳能燃料合成及其他相关光催化反应体系的设计与优化具有重要指导意义.

关键词: 光热催化, CO₂还原, 金属单原子, 团簇催化剂, 载流子传输动力学

Abstract:

Solar-driven CO₂ reduction is confronted with challenges of limited light absorption and elevated reaction energy barriers. To address these, a solvothermal-wet coupled chemical reduction method was developed to precisely construct a bifunctional catalyst comprising single-atom Ru and clustered Ni on porous CeO₂ nanorods, featuring efficient CO₂ methanation in H₂O vapor under concentrated solar irradiation (4.01 W·cm^-2). Through lattice substitution at Ce sites, Ru single atoms form a distinctive pentacoordinate configuration, largely accelerating H₂O dissociation to generate active hydrogen (^*H). Conversely, Ni clusters enhance visible-to-near-infrared light capture via localized surface plasmon resonance effects, optimizing the CO₂ adsorption configuration to reduce the activation energy barrier of the C=O bond. The synergistic interplay between these dual sites, mediated by the hydrogen spillover effect, resolves the spatiotemporal mismatch between proton supply and carbon source activation. Based on the evidence from femtosecond and nanosecond transient absorption spectroscopy, the Ru/Ni dual-active sites enable spatially decoupled directional transport of charge carriers, synergistically handling the photogenerated carrier transfer dynamics. Furthermore, the robust photoelectric and thermal effects induced by concentrated irradiation enhance photogenerated carrier concentrations and the reaction temperature, reducing the apparent activation energy for CH₄ formation to 14.61 kJ·mol^-1 (a 29.9% decrease compared to non-concentrated systems). This catalyst achieves a CH₄ production rate of 133.1 μmol·cm^-2·h^-1 (a 31-fold enhancement over non-concentrated systems) and a solar-to-chemical energy conversion efficiency of 0.423%, offering insights into the design of photothermal synergistic catalytic systems through atomic-scale active site decoupling and multi-physical field coupling.

Key words: Photothermal catalysis, CO₂ reduction, Metal single-atom, Cluster catalyst, Carrier transport dynamics

尤长君, 任宇奇, 贺红斌, 彭若轩, 朱元皓, 程淼, 丁培根, 张刘娜, 兰盛楠, 张虹扬, 章毅琴, 朱丰帆, 李敬, 周建成. Ru单原子与Ni团簇双位点协同构筑CeO₂纳米棒实现高效太阳能驱动CO₂甲烷化[J]. 催化学报, 2026, 83: 183-197.

Changjun You, Yuqi Ren, Hongbin He, Ruoxuan Peng, Yuan-Hao Zhu, Miao Cheng, Peigen Ding, Liuna Zhang, Shengnan Lan, Hongyang Zhang, Yiqin Zhang, Fengfan Zhu, Jing Li, Jiancheng Zhou. Dual-site atomic engineering of Ru Single-atoms and Ni clusters on CeO₂ nanorods for solar-driven CO₂ methanation[J]. Chinese Journal of Catalysis, 2026, 83: 183-197.

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图/表 7

Fig. 1. Schematic illustration of the thermodynamic state of artificial photosynthesis.

Fig. 2. Morphological characterizations of the NF@Ru0.2/Ni2-CeO2 catalyst. (a) TEM image of NF@Ru0.2/Ni2-CeO2. (b-d) HAADF-STEM image of NF@Ru0.2/Ni2-CeO2. (e) EDS images of O, Ce, Ni, and Ru distribution of the NF@Ru0.2/Ni2-CeO2. (f) Ni K-edge XANES spectra of NF@Ru0.2/Ni2-CeO2, NiO, and Ni foil. (g) Ni K-edge FT-EXAFS spectra of NF@Ru0.2/Ni2-CeO2, NiO, and Ni foil. (h) XPS spectra of Ni 2p. (i) The normalized XANES at the Ru K-edge. (j) FT-EXAFS spectra of NF@Ru0.2/Ni2-CeO2 catalyst in reference to Ru foil and bulk RuO2. (k) Diagram of the model structure for NF@Ru0.2/Ni2-CeO2.

Fig. 3. Photocatalytic activity of NF@Ru0.2/Ni2-CeO2. (a) Photothermal catalytic CO/CH4 yields from NF@CeO2, NF@Ni/CeO2, NF@Ru/CeO2 and NF@Ru0.2/Ni2-CeO2 catalysts under different conditions (unconcentrated solar irradiation = 0.55 W·cm-2, and concentrated solar irradiation = 4.01 W·cm-2). (b) Yield of products under different circumstances. (c) 13CO2 isotopic tracing experiments of NF@Ru0.2/Ni2-CeO2. (d) Photothermal catalytic CO/CH4 yields at different temperatures under unconcentrated solar irradiation. (e) Photothermal catalytic CO/CH4 yields at different irradiation intensities. (f) Apparent activation energy under concentrated solar irradiation and unconcentrated solar irradiation of NF@Ru0.2/Ni2-CeO2. (g) UV-vis DRS of different catalysts. (h) Photothermal catalytic CO/CH4 yields from different catalysts under UV-vis-concentrated solar irradiation. (i) Photothermal catalytic CO/CH4 yields from different catalysts under NIR-concentrated solar irradiation. (j) Recycling photothermal CO2 tests of the NF@Ru0.2/Ni2-CeO2 catalyst. (k) Comparison of energy efficiency of a series of literature-reported catalysts under similar conditions.

Fig. 4. Two-dimensional pseudo-color maps of NF@CeO2 (a,g) and NF@Ru0.2/Ni2-CeO2 (d,j) in water, and the fs-TA and ns-TA spectra ofNF@CeO2 (b,c,h,i) and NF@Ru0.2/Ni2-CeO2 (e,f,k,l) under several representative probe delays. EtOH and GLY were the abbreviation of ethanol and glycerol, respectively.

Fig. 5. Light and thermal effects on carrier migration. (a) Steady-state PL spectra at different temperature. (b) TRPL at different temperature. (c) IMPS spectra at different irradiation intensities. (d) The plot of the rate constant charge transfer rate vs. potential at different irradiation intensities. (e) The plot of the rate constant of charge recombination vs. potential at different irradiation intensities. (f) LSV curves at different light intensity. (g) Open circuit potential at different light intensity. (h) Plot of the electron transfer mechanism under changing irradiation intensities.

Fig. 6. Chemisorption and activation of CO2/H2O over NF@Ru0.2/Ni2-CeO2 catalyst. (a) CO2-TPD spectra of different catalysts. (b) CO-TPD spectra of different catalysts. (c) H2O-TPD spectra of different catalysts. (d) Adsorption energy of CO2 molecules on different catalyst surfaces. (e) Adsorption energy of H2O molecules on different catalyst surfaces. (f) Differential charge density of NF@Ru0.2/Ni2-CeO2 catalyst adsorbed CO2. (g) Differential charge density of NF@Ru0.2/Ni2-CeO2 catalyst adsorbed H2O. Pink and green isosurfaces elucidate electron gain and electron loss, respectively. (h) ELF of NF@Ru0.2/Ni2-CeO2 catalyst adsorbed CO2. (i) ELF of NF@Ru0.2/Ni2-CeO2 catalyst adsorbed H2O.

Fig. 7. Investigation into the CO2 reduction mechanism by NF@Ru0.2/Ni2-CeO2 catalyst under concentrated solar irradiation. (a) In-situ DRIFTS spectra of CO2/H2O with 950-1650 cm-1 on NF@Ru0.2/Ni2-CeO2. (b) In-situ DRIFTS spectra of CO2/H2O with 3500-3900 cm-1 on NF@Ru0.2/Ni2-CeO2. (c) Possible CO2 conversion pathway to CO and CH4. (d,e) Free energy diagrams of CO2 reduction on the NF@Ni/CeO2 and NF@Ru0.2/Ni2-CeO2. (f) Schematic illustration of the photothermal coupling effect on NF@Ru0.2/Ni2-CeO2.

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Ru单原子与Ni团簇双位点协同构筑CeO₂纳米棒实现高效太阳能驱动CO₂甲烷化

Dual-site atomic engineering of Ru Single-atoms and Ni clusters on CeO₂ nanorods for solar-driven CO₂ methanation

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