Photoreduction of CO2 into sustainable and green solar fuels is generally believed to be an appealing solution to simultaneously overcome both environmental problems and energy crisis. The low selectivity of challenging multi-electron CO2 photoreduction reactions makes it one of the holy grails in heterogeneous photocatalysis. This Review highlights the important roles of cocatalysts in selective photocatalytic CO2 reduction into solar fuels using semiconductor catalysts. A special emphasis in this review is placed on the key role, design considerations and modification strategies of cocatalysts for CO2 photoreduction. Various cocatalysts, such as the biomimetic, metal-based, metal-free, and multifunctional ones, and their selectivity for CO2 photoreduction are summarized and discussed, along with the recent advances in this area. This Review provides useful information for the design of highly selective cocatalysts for photo(electro)reduction and electroreduction of CO2 and complements the existing reviews on various semiconductor photocatalysts.

Cocatalysts for Selective Photoreduction of CO2 into Solar Fuels.

Photocatalysts and Photoelectrodes James L. White,† Maor F. Baruch,† James E. Pander III,† Yuan Hu,† Ivy C. Fortmeyer,† James Eujin Park,† Tao Zhang,† Kuo Liao,† Jing Gu,‡ Yong Yan,‡ Travis W. Shaw,† Esta Abelev,† and Andrew B. Bocarsly*,† †Department of Chemistry, Princeton University, Princeton, New Jersey 08544, United States ‡Chemical and Materials Science Center, National Renewable Energy Laboratory, Golden, Colorado 80401, United States

Light-Driven Heterogeneous Reduction of Carbon Dioxide: Photocatalysts and Photoelectrodes

Photocatalytic reduction of CO2 into hydrocarbon fuels, an artificial photosynthesis, is based on the simulation of natural photosynthesis in green plants, whereby O2 and carbohydrates are produced from H2 O and CO2 using sunlight as an energy source. It couples the reductive half-reaction of CO2 fixation with a matched oxidative half-reaction such as water oxidation, to achieve a carbon neutral cycle, which is like killing two birds with one stone in terms of saving the environment and supplying future energy. The present review provides an overview and highlights recent state-of-the-art accomplishments of overcoming the drawback of low photoconversion efficiency and selectivity through the design of highly active photocatalysts from the point of adsorption of reactants, charge separation and transport, light harvesting, and CO2 activation. It specifically includes: i) band-structure engineering, ii) nanostructuralization, iii) surface oxygen vacancy engineering, iv) macro-/meso-/microporous structuralization, v) exposed facet engineering, vi) co-catalysts, vii) the development of a Z-scheme system. The challenges and prospects for future development of this field are also present.

Photocatalytic Conversion of CO 2 into Renewable Hydrocarbon Fuels: State‐of‐the‐Art Accomplishment, Challenges, and Prospects

Ever-increasing fossil-fuel combustion along with massive CO2 emissions has aroused a global energy crisis and climate change. Photocatalytic CO2 reduction represents a promising strategy for clean, cost-effective, and environmentally friendly conversion of CO2 into hydrocarbon fuels by utilizing solar energy. This strategy combines the reductive half-reaction of CO2 conversion with an oxidative half reaction, e.g., H2 O oxidation, to create a carbon-neutral cycle, presenting a viable solution to global energy and environmental problems. There are three pivotal processes in photocatalytic CO2 conversion: (i) solar-light absorption, (ii) charge separation/migration, and (iii) catalytic CO2 reduction and H2 O oxidation. While significant progress is made in optimizing the first two processes, much less research is conducted toward enhancing the efficiency of the third step, which requires the presence of cocatalysts. In general, cocatalysts play four important roles: (i) boosting charge separation/transfer, (ii) improving the activity and selectivity of CO2 reduction, (iii) enhancing the stability of photocatalysts, and (iv) suppressing side or back reactions. Herein, for the first time, all the developed CO2 -reduction cocatalysts for semiconductor-based photocatalytic CO2 conversion are summarized, and their functions and mechanisms are discussed. Finally, perspectives in this emerging area are provided.

Cocatalysts in Semiconductor-based Photocatalytic CO2 Reduction: Achievements, Challenges, and Opportunities.

The shortage of fossil fuels and the disastrous pollution of the environment have led to an increasing interest in artificial photosynthesis. The photocatalytic conversion of CO2 into solar fuel is believed to be one of the best methods to overcome both the energy crisis and environmental problems. It is of significant importance to efficiently manage the surface reactions and the photo-generated charge carriers to maximize the activity and selectivity of semiconductor photocatalysts for photoconversion of CO2 and H2O to solar fuel. To date, a variety of strategies have been developed to boost their photocatalytic activity and selectivity for CO2 photoreduction. Based on the analysis of limited factors in improving the photocatalytic efficiency and selectivity, this review attempts to summarize these strategies and their corresponding design principles, including increased visible-light excitation, promoted charge transfer and separation, enhanced adsorption and activation of CO2, accelerated CO2 reduction kinetics and suppressed undesirable reaction. Furthermore, we not only provide a summary of the recent progress in the rational design and fabrication of highly active and selective photocatalysts for the photoreduction of CO2, but also offer some fundamental insights into designing highly efficient photocatalysts for water splitting or pollutant degradation.

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Design and fabrication of semiconductor photocatalyst for photocatalytic reduction of CO 2 to solar fuel

Carbon dioxide (CO2) photoreduction by gaseous water over silica-pillared lamellar niobic acid, viz. HNb3O8, was studied in this work. The physicochemical characteristics of samples were examined b...

Photocatalytic Reduction of Carbon Dioxide to Methane over SiO2-Pillared HNb3O8

Efficient photocatalytic degradation of rhodamine B over CdS sensitized SiO2–HNb3O8 under visible light

The effects of NaNbO3 particle size on the photocatalytic activity were investigated by taking gaseous 2-propanol photodegradation as a model reaction. By varying the loading amount of precursors onto mesoporous SBA-15, nanocrystalline NaNbO3 samples with particle sizes ranging from 3 to 50 nm were successfully synthesized. The particle size and surface area value of templated NaNbO3 change systematically with the change in loading amount of the precursors. The physicochemical characteristics of the samples were examined by techniques such as XRD, SEM, TEM, Raman spectroscopy, and UV-visible diffuse reflectance spectroscopy. The optimum NaNbO3 particle size for the highest photocatalytic activity was found to be 30 nm. The current study also revealed that the NaNbO3 photocatalyst is structure sensitive for 2-propanol photodegradation. The density of active sites on the sample surface decreases as the particle size decreases. Competing effects of factors such as the surface area, changes in electronic structure, defect density, and concentration of reaction active sites determine the optimum particle size of NaNbO3.

The effects of NaNbO3 particle size on the photocatalytic activity for 2-propanol photodegradation.

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Photocatalytic Reduction of Carbon Dioxide to Methane over SiO2-Pillared HNb3O8

Efficient photocatalytic degradation of rhodamine B over CdS sensitized SiO2–HNb3O8 under visible light

The effects of NaNbO3 particle size on the photocatalytic activity for 2-propanol photodegradation.