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Photo‐thermal catalytic CO2 hydrogenation is currently extensively studied as one of the most promising approaches for the conversion of CO2 into value‐added chemicals under mild conditions; however, achieving desirable conversion efficiency and target product selectivity remains challenging. Herein, the fabrication of Ir‐CoO/Al2O3 catalysts derived from Ir/CoAl LDH composites is reported for photo‐thermal CO2 methanation, which consist of Ir‐CoO ensembles as active centers that are evenly anchored on amorphous Al2O3 nanosheets. A CH4 production rate of 128.9 mmol gcat⁻1 h⁻1  is achieved at 250 °C under ambient pressure and visible light irradiation, outperforming most reported metal‐based catalysts. Mechanism studies based on density functional theory (DFT) calculations and numerical simulations reveal that the CoO nanoparticles function as photocatalysts to donate electrons for Ir nanoparticles and meanwhile act as “nanoheaters” to effectively elevate the local temperature around Ir active sites, thus promoting the adsorption, activation, and conversion of reactant molecules. In situ diffuse reflectance infrared Fourier transform spectroscopy (in situ DRIFTS) demonstrates that illumination also efficiently boosts the conversion of formate intermediates. The mechanism of dual functions of photothermal semiconductors as photocatalysts for electron donation and as nano‐heaters for local temperature enhancement provides new insight in the exploration for efficient photo‐thermal catalysts. This work prepares Ir‐CoO/Al2O3 catalysts to realize the highly efficient photo‐thermal catalytic CO2 methanation under mild conditions. The CoO nanoparticles function as photocatalysts to donate electrons for Ir nanoparticles and meanwhile act as “nanoheaters” to effectively elevate the local temperature around Ir active sites, thus promoting the adsorption, activation, and conversion of reactant molecules.

Solar-driven photo-thermal catalytic CO 2 methanation reaction is a promising technology to alleviate the problems posed by greenhouse gases emissions. However, designing advanced photo-thermal catalysts remains a research challenge for CO 2 methanation reaction. In this work, a series of ABO 3 (A = lanthanide, B = transition metal) perovskite catalysts with Ce-substituted LaNiO 3 (La 1− x Ce x NiO 3 , x = 0, 0.2, 0.5, 0.8, 1) were synthesized for CO 2 methanation. The La 0.2 Ce 0.8 NiO 3 exhibited the highest CH 4 formation rate of 258.9 mmol·g −1 ·h cat −1 , CO 2 conversion of 55.4% and 97.2% CH 4 selectivity at 300 °C with the light intensity of 2.9 W·cm −2 . Then the catalysts were thoroughly analyzed by physicochemical structure and optical properties characterizations. The partial substitution of the A-site provided more active sites for the adsorption and activation of CO 2 /H 2 . The sources of the active sites were considered to be the oxygen vacancies (O v ) created by lattice distortions due to different species of ions (La 3+ , Ce 4+ , Ce 3+ ) and exsolved Ni 0 by H 2 reduction. The catalysts have excellent light absorption absorbance and low electron–hole (e − /h + ) recombination rate, which greatly contribute to the excellent performance in photo-thermal synergistic catalysis (PTC) CO 2 methanation. The results of in situ irradiated electron paramagnetic resonance spectrometer (ISI-EPR) and ISI-X-ray photoelectron spectroscopy (XPS) indicated that the aggregation of unpaired electrons near the defects and Ni metal (from La and Ce ions to O v and Ni 0 ) accelerated adsorption and activation of CO 2 /H 2 . At last, the catalyst properties and structure were correlated with the proposed reaction mechanism from the in situ diffuse reflection infrared Fourier transform spectrum (DRIFTS) measurements. The in situ precipitation of the B-site enhanced the dispersion of Ni, while its enriched photoelectrons upon illumination further promote hydrogen dissociation. More H* spillover accelerated the rate-determining step (RDS) of HCOO* hydrogenation. This work provides the theoretical basis for the development of catalysts and industrial application.

Hydrogen (H2) has emerged as a clean and versatile energy carrier to power a carbon‐neutral economy for the post‐fossil era. Hydrogen generation from low‐cost and renewable biomass by virtually inexhaustible solar energy presents an innovative strategy to process organic solid waste, combat the energy crisis, and achieve carbon neutrality. Herein, the progress and breakthroughs in solar‐powered H2 production from biomass are reviewed. The basic principles of solar‐driven H2 generation from biomass are first introduced for a better understanding of the reaction mechanism. Next, the merits and shortcomings of various semiconductors and cocatalysts are summarized, and the strategies for addressing the related issues are also elaborated. Then, various bio‐based feedstocks for solar‐driven H2 production are reviewed with an emphasis on the effect of photocatalysts and catalytic systems on performance. Of note, the concurrent generation of value‐added chemicals from biomass reforming is emphasized as well. Meanwhile, the emerging photo‐thermal coupling strategy that shows a grand prospect for maximally utilizing the entire solar energy spectrum is also discussed. Further, the direct utilization of hydrogen from biomass as a green reductant for producing value‐added chemicals via organic reactions is also highlighted. Finally, the challenges and perspectives of photoreforming biomass toward hydrogen are envisioned. The progress and breakthroughs in semiconductor‐based photocatalysts for hydrogen generation from solar‐driven reforming of biomass and its derivatives are reviewed.

Photo-thermal catalysis has recently emerged as a viable strategy to produce solar fuels or chemicals using sunlight. In particular, nanostructures featuring localized surface plasmon resonance (LSPR) hold great promise as photo-thermal catalysts given their ability to convert light into heat. In this regard, traditional plasmonic materials include gold (Au) or silver (Ag), but in the last years, transition metal nitrides have been proposed as a cost-efficient alternative. Herein, we demonstrate that titanium nitride (TiN) tubes derived from the nitridation of TiO2 precursor display excellent light absorption properties thanks to their intense LSPR band in the visible–IR regions. Upon deposition of Ru nanoparticles (NPs), Ru-TiN tubes exhibit high activity towards the photo-thermal CO2 reduction reaction, achieving remarkable methane (CH4) production rates up to 1200 mmol g−1 h−1. Mechanistic studies suggest that the reaction pathway is dominated by thermal effects thanks to the effective light-to-heat conversion of Ru-TiN tubes. This work will serve as a basis for future research on new plasmonic structures for photo-thermal applications in catalysis.

Solar fuel is one of the ideal energy sources in the future. The synergy of photo and thermal effects leads to a new approach to higher solar fuel production under relatively mild conditions. This paper reviews different approaches for solar fuel production from spectrum- selective photo-thermal synergetic catalysis. The review begins with the meaning of synergetic effects, and the mechanisms of spectrum-selectivity and photo-thermal catalysis. Then, from a technical perspective, a number of experimental or theoretical works are sorted by the chemical reactions and the sacrificial reagents applied. In addition, these works are summarized and tabulated based on the operating conditions, spectrum-selectivity, materi- als, and productivity. A discussion is finally presented concerning future development of photo-thermal catalytic reactions with spectrum-selectivity.

Defect engineering provides a promising strategy to design efficient photo-thermal catalysts for methane dry reforming reaction, addressing challenges of harsh reaction conditions, and ultimately achieve the reduction of carbon footprint. Here, a series of Ru-Ceria catalysts with different defect structures were synthesized by controlling the duration of hydrothermal self-assembly treatment, and their physicochemical properties were systematically characterized. The results revealed how the sensitivity of the surface defect engineering affected the optical and catalytic performance of the catalysts. Furthermore, by integrating the operando characterization and structural analysis, a linear correlation between structure (Defects concentration, Ru 0 content), intermediate species (CO * and CH x * species) and catalytic performance (Products formation rates and catalytic stability) was established. This work provided a theoretical foundation for the application of surface defect engineering in photothermal MDR catalysis. Highlights ▪ The influence of self-assembly duration on the defect structure of Ru-Ceria catalysts were elucidated. ▪ The influence of surface defect structures on electronic structure and charge carrier migration properties of Ru-Ceria catalysts is investigated. ▪ The linear correlation between surface defect structures and catalytic performance is established. ▪ The correlation for surface defect structures-specific intermediate species signals-catalytic performance was carry out.

The use of metal–organic frameworks (MOFs) as templates or precursors in the manufacture of heterogeneous catalysts is highly attractive due to the transfer of MOFs’ inherent porosity and homogeneous metallic distribution to the derived structure. Herein, we report on the preparation of MOF-derived Ru@ZrO2 catalysts by controlled thermal treatment of zirconium-based MOF UiO-66 with ruthenium moieties. Ru3+ (3 or 10 mol%) precursor was added to UiO-66 synthesis and, subsequently, the as-synthesized hybrid structure was calcined in flowing air at different temperatures (400–600 °C) to obtain ZrO2-derived oxides doped with highly dispersed Ru metallic clusters. The materials were tested for the catalytic photo-thermal conversion of CO2 to CH4. Methanation experiments were conducted in a continuous flow (feed flow rate of 5 sccm and 1:4 CO2 to H2 molar ratio) reactor at temperatures from 80 to 300 °C. Ru0.10@ZrO2 catalyst calcined at 600 °C was able to hydrogenate CO2 to CH4 with production rates up to 65 mmolCH4·gcat.–1·h–1, CH4 yield of 80% and nearly 100% selectivity at 300 °C. The effect of the illumination was investigated with this catalyst using a high-power visible LED. A CO2 conversion enhancement from 18% to 38% was measured when 24 sun of visible LED radiation was applied, mainly due to the increase in the temperature as a result of the efficient absorption of the radiation received. MOF-derived Ru@ZrO2 catalysts have resulted to be noticeably active materials for the photo-thermal hydrogenation of CO2 for the purpose of the production of carbon-neutral methane. A remarkable effect of the ZrO2 crystalline phase on the CH4 selectivity has been found, with monoclinic zirconia being much more selective to CH4 than its cubic allotrope.

The oxidative dehydrogenation of propane (ODHP) catalyzed by oxygen offers several advantages, including resistance to carbon deposition and low energy consumption. However, achieving high propylene selectivity at industrially relevant conversions remains challenging, as existing catalysts typically require temperatures exceeding 500 °C, promoting over-oxidation to COx. In this study, we developed a NiO nanoparticle-decorated graphitic carbon nitride catalyst (NiO@CN-600) via thermal polymerization–oxidation for photo-thermal synergistic ODHP. At 430 °C, thermal catalysis achieved a propane conversion of 14%. Remarkably, introducing light irradiation boosted conversion to 24%, a 10% increase. Further experimental results reveal that the photo-thermal synergistic catalysis can be described by the following mechanism: initial thermal energy provides sufficient activation energy, enabling the reaction to overcome the energy barrier and proceed smoothly. Simultaneously, the introduction of light energy enhances the activity of lattice oxygen, making it more likely to detach from the lattice and form oxygen vacancies, which in turn boosts the efficiency of the oxidation reaction on the catalyst surface.

The climate crisis necessitates the development of non-fossil energy sources. Harnessing solar energy for fuel production shows promise and offers the potential to utilize existing energy infrastructure. However, solar fuel production is in its early stages of development, constrained by low conversion efficiency and challenges in scaling up production. Concentrated solar energy (CSE) technology has matured alongside the rapid growth of solar thermal power plants. This review provides an overview of current CSE methods and solar fuel production, analyzes their integration compatibility, and delves into the theoretical mechanisms by which CSE impacts solar energy conversion efficiency and product selectivity in the context of photo-electrochemistry, thermochemistry, and photo-thermal co-catalysis for solar fuel production. The review also summarizes approaches to studying the photoelectric and photothermal effects of CSE. Lastly, it explores emerging novel CSE technology methods in the field of solar fuel production. [Display omitted] •The concept of concentrating solar energy and solar fuel production are introduced.•Solar fuel production integrated with concentrating solar energy is reviewed.•Photoelectric and photothermal effects of concentrating solar energy are reviewed.•Novel devices for solar fuel production by concentrating light are discussed.

The exploration of a noble‐metal‐free photo‐thermal‐coupled catalytic architecture plays a vital role in solar‐driven conversion of carbon dioxide (CO2) into high‐value fuels and chemicals. In this study, FeNiCrMnCo multicomponent alloy (MCA) is integrated with GaN nanowires (NW's) for photo‐thermal‐coupled catalytic CO2 methanation. The MCA/GaN NW's nanohybrid demonstrates a considerable methane production rate of 199 mmol∙g−1∙h−1 with an impressive selectivity of 93% under white light irradiation of 3 W∙cm−2 at 290 °C by external heating. The turnover number approaches 20,160 mole CH4 per mole of MCA over a continuous operation period of 120 h, showcasing remarkable stability. Mechanistic investigations reveal that the unique MCA provides a flexible platform for tailoring the electronic and catalytic properties to optimize the adsorption and activation of CO₂ and H₂, thus leading to efficient and selective CO₂ methanation. This study presents an industry‐friendly architecture for photo‐thermal‐coupled CO2 hydrogenation into high‐value fuels and chemicals by coupling a noble‐metal‐free multicomponent alloy with GaN NWs, paving the way for advancements in sustainable energy conversion through CO2 utilization.