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

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

Abstract

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

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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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(25)64914-X

https://www.cjcatal.com/EN/Y2026/V83/I4/183

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

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