Accelerated optochemical engineering solutions to CO2 photocatalysis for a sustainable future

Ozin, Geoffrey A.

doi:10.1016/j.matt.2022.07.033

Cited by 45 publications

(26 citation statements)

References 16 publications

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“…Meanwhile, the thermal effect is manifested through an increase in system temperature, which may be attributed to non-radiative relaxation of semiconductors, , localized heating induced by plasma, − thermal vibration of molecules, as summarized in our previous work . It is noteworthy to distinguish the subtle differences from the definitions of “photochemistry” and “thermochemistry,” “photochemical” and “photophysical” effects, and “photochemical” and “photothermal” effects in other studies. ,− Obviously, there is currently growing evidence that synergistic mechanisms in non-thermal and thermal effect are of particular interest. Some people started from photocatalytic reactions and tried to elevate the reaction temperature, which has beneficial effects such as enhancing reaction kinetics, improving mass transfer, and promoting the desorption of products or harmful species .…”

Section: Introductionmentioning

confidence: 89%

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In₂O₃

Zhang,

et al. 2023

ACS Appl. Mater. Interfaces

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To promote the solar-energy cascade utilization, it is necessary to increase the thermal effect of irradiation in the catalytic reactions, while simultaneously augmenting the nonthermal effect, so as to fulfill photothermal coupling. Herein, the non-thermal and thermal effect of light radiation on the surface of In 2 O 3 -based catalysts are explored and enhanced by the modification of transition metals Fe and Cu. Optical characterizations combined with water-splitting experiments show that Fe doping greatly broadens the radiation response range and enhances the absorption intensity of semiconductors' intrinsic portion, and Cu doping facilitates the absorption of visible-infrared light. The concurrent incorporation of Fe and Cu offers synergistic benefits, resulting in improved radiation response range, carrier separation and migration, as well as higher photothermal temperature upon photoexcitation. Collectively, these advantages comprehensively enhance the photothermal synergistic water-splitting reactivity. The characterizations under variable temperature conditions have demonstrated that the reaction temperature exerts a significant influence on the process of radiation absorption and conversion, ultimately impacting the non-thermal effect. The results of DFT calculations have revealed that the increasing temperature directly impacts the chemical reaction by reducing the energy barrier associated with the rate-determining step. These findings shine new light on the fundamental mechanisms underlying non-thermal and thermal effect, while also imparting significant insights for photo-thermal-coupled catalyst designing.

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Section: Introductionmentioning

confidence: 89%

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In₂O₃

Zhang,

et al. 2023

ACS Appl. Mater. Interfaces

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“…Using non-noble metal plasmonic nanostructures can reduce the material cost, , offering feasibility for the large-scale application of plasmonic photocatalysis in chemical manufacturing. To this end, rational reactor design should also be considered to enhance the photon utilization efficiency and reactor productivity, promoting the potential economic viability of the catalytic process. , Atomically precise active site design allows the plasmonic photocatalyst to have uniform active sites on its surface, avoiding the occurrence of undesirable side reactions. Furthermore, the hybrid catalyst with a clear structure also provides an ideal platform for investigating the complex interactions between plasmonic nanostructures, active sites, and surface reactants.…”

Section: Conclusion and Future Perspectivesmentioning

confidence: 99%

Active Site Engineering on Plasmonic Nanostructures for Efficient Photocatalysis

et al. 2023

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Plasmonic nanostructures have shown immense potential in photocatalysis because of their distinct photochemical properties associated with tunable photoresponses and strong light−matter interactions. The introduction of highly active sites is essential to fully exploit the potential of plasmonic nanostructures in photocatalysis, considering the inferior intrinsic activities of typical plasmonic metals. This review focuses on active site-engineered plasmonic nanostructures with enhanced photocatalytic performance, wherein the active sites are classified into four types (i.e., metallic sites, defect sites, ligand-grafted sites, and interface sites). The synergy between active sites and plasmonic nanostructures in photocatalysis is discussed in detail after briefly introducing the material synthesis and characterization methods. Active sites can promote the coupling of solar energy harvested by plasmonic metal to catalytic reactions in the form of local electromagnetic fields, hot carriers, and photothermal heating. Moreover, efficient energy coupling potentially regulates the reaction pathway by facilitating the excited state formation of reactants, changing the status of active sites, and creating additional active sites using photoexcited plasmonic metals. Afterward, the application of active site-engineered plasmonic nanostructures in emerging photocatalytic reactions is summarized. Finally, a summary and perspective of the existing challenges and future opportunities are presented. This review aims to deliver some insights into plasmonic photocatalysis from the perspective of active sites, expediting the discovery of high-performance plasmonic photocatalysts.

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“…Photocatalytic carbon dioxide reduction reaction (CO 2 RR) for high value-added chemical production has evolved into a research hotspot owing to its attractive potential for producing renewable energy and mitigating the greenhouse effect. [1,2] However, as of today, the energy efficiency of solar-driven CO 2 conversion of currently developed catalysts is still far from satisfactory. [3][4][5][6][7] Photocatalysts generate electron-hole pairs under irradiation, which are then separated and transferred to varied sites for redox reactions.…”

Section: Introductionmentioning

confidence: 99%

Modulating Charge Separation of Oxygen‐Doped Boron Nitride with Isolated Co Atoms for Enhancing CO₂‐to‐CO Photoreduction

Liang,

Zhang,

Song

et al. 2023

Advanced Materials

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To alleviate the greenhouse effect and address the related energy crisis, solar‐driven reduction of CO2 to value‐added products has been considered as a sustainable strategy. However, the insufficient separation and rapid recombination of photogenerated charge carriers during photocatalysis greatly limit their reduction efficiency and practical application potential. Here, isolated Co atoms have been successfully decorated into oxygen‐doped BN via an in‐situ pyrolysis method, achieving greatly improved catalytic activity and selectivity to the CO product. X‐ray absorption fine spectroscopy demonstrates that the isolated Co atoms have been stabilized by the O and N atoms with an unsaturated CoO2N1 configuration. Further experimental investigation and theoretical simulations confirm that the decorated Co atoms not only work as the real active center during the CO2 reduction process but also perform as the electron pump to promote the electron/hole separation and transfer, resulting in greatly accelerated reaction kinetics and improved activity. In addition, the CoO2N1 coordination geometry is favorable to the conversion from *CO2 to *COOH, which should be considered as a selectivity‐determining step for the evolution of the CO products. The surface modulation strategy at the atomic level opens a new avenue for regulating the reaction kinetics for photocatalytic CO2 reduction.This article is protected by copyright. All rights reserved

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Accelerated optochemical engineering solutions to CO2 photocatalysis for a sustainable future

Cited by 45 publications

References 16 publications

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In₂O₃

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In₂O₃

Active Site Engineering on Plasmonic Nanostructures for Efficient Photocatalysis

Modulating Charge Separation of Oxygen‐Doped Boron Nitride with Isolated Co Atoms for Enhancing CO₂‐to‐CO Photoreduction

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Accelerated optochemical engineering solutions to CO2 photocatalysis for a sustainable future

Cited by 45 publications

References 16 publications

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In2O3

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In2O3

Active Site Engineering on Plasmonic Nanostructures for Efficient Photocatalysis

Modulating Charge Separation of Oxygen‐Doped Boron Nitride with Isolated Co Atoms for Enhancing CO2‐to‐CO Photoreduction

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Product

Resources

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Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In₂O₃

Synergistic Modulation between Non-thermal and Thermal Effects in Photothermal Catalysis based on Modified In₂O₃

Modulating Charge Separation of Oxygen‐Doped Boron Nitride with Isolated Co Atoms for Enhancing CO₂‐to‐CO Photoreduction