Solar fuels: research and development strategies to accelerate photocatalytic CO<sub>2</sub> conversion into hydrocarbon fuels

Gong, Eunhee; Ali, Shahzad; Hiragond, Chaitanya B.; Kim, Hong Soo; Powar, Niket S.; Kim, Dongyun; Kim, Hwapyong; In, Su‐Il

doi:10.1039/d1ee02714j

Cited by 362 publications

(218 citation statements)

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“…Coupling CO 2 reduction and H 2 O oxidation over photocatalysts using solar energy is an appealing strategy to alleviate the greenhouse effect and simultaneously produce value-added chemicals or fuels 1 , 2 . In recent decades, photocatalytic studies have almost exclusively focused on semiconductors, which provide an opportunity for reducing CO 2 with H 2 O at room temperature 3 , 4 .…”

Section: Introductionmentioning

confidence: 99%

Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

et al. 2022

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Achieving CO2 reduction with H2O on metal photocatalysts and understanding the corresponding mechanisms at the molecular level are challenging. Herein, we report that quantum-sized Au nanoparticles can photocatalytically reduce CO2 to CO with the help of H2O by electron-hole pairs mainly originating from interband transitions. Notably, the Au photocatalyst shows a CO production rate of 4.73 mmol g−1 h−1 (~100% selectivity), ~2.5 times the rate during CO2 reduction with H2 under the same experimental conditions, under low-intensity irradiation at 420 nm. Theoretical and experimental studies reveal that the increased activity is induced by surface Au–O species formed from H2O decomposition, which synchronously optimizes the rate-determining steps in the CO2 reduction and H2O oxidation reactions, lowers the energy barriers for the *CO desorption and *OOH formation, and facilitates CO and O2 production. Our findings provide an in-depth mechanistic understanding for designing active metal photocatalysts for efficient CO2 reduction with H2O.

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Section: Introductionmentioning

confidence: 99%

Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

et al. 2022

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“…Finally, the Pb-free halide double perovskites and 2D layered perovskites are also promising in the field of photocatalysis due to their large electronic bandgap and stability. 211 For instance, Zhou et al synthesized Cs 2 AgBiBr 6 nanocrystals that were shown to be stable for more than three weeks in a low polarity medium under light-soaking and 55% relative humidity. 242 Double perovskites with B = Bi and B ′ = Ag have the highest rate of H 2 evolution that reaches 380 μmol g −1 h −1 when supported on carbon doped with nitrogen.…”

Section: Discussionmentioning

confidence: 99%

“…The main requirements for a promising photocatalytic material are suitable band alignments and bandgaps, strong light absorption, high chemical stability, efficient charge carrier transport, and good operation in strong acidity and/or alkali environments. [211][212][213] Over the past few years, the potential of Pb-based halide perovskites has been investigated as a catalyst for photocatalytic hydrogen (H 2 ) evolution, CO 2 reduction reaction, and various organic synthesis or chemical reactions. 212,214 The performance of a complete water splitting system can be evaluated by introducing the solar-to-hydrogen (STH) conversion efficiency.…”

Section: Photo-catalysismentioning

confidence: 99%

Pb-free halide perovskites for solar cells, light-emitting diodes, and photocatalysts

et al. 2022

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Metal halide perovskites have recently emerged as one of the most promising classes of semiconductors for various applications, especially in the field of optoelectronics. Lead-based halide perovskite materials, virtually unexploited for decades, have become prominent candidates due to their unique and intrinsic physicochemical and optical properties. Current challenges faced by the scientific community to capitalize on the properties of Pb-based perovskites are mainly associated with environmental concerns due to the toxicity of Pb and their poor stability. Under this context, over recent years, a number of new Pb-free halide perovskite (and perovskite-like) semiconductor classes have been introduced. This Perspective reviews recent developments in Pb-free halide perovskites, which specifically target their application in solar cells, light-emitting devices, and photocatalysts. Each type of Pb-free material is paired with a specific optoelectronic application, and the latest record performances are reported. Although these materials do not yet exhibit as attractive intrinsic optoelectronic properties as the Pb-based halide perovskites, their potential as alternatives for well-suited applications is discussed.

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“…The numbers of photogenerated electrons (e − ) and protons (H + ) available for photocatalytic CO 2 reduction affect product selectivity. [1] The reduction of CO 2 to a specific product requires a specific reduction potential, as shown in Table 1. The reduction capacity of photoexcited electrons must be sufficient to trigger the desired reduction reaction to preferentially generate a desired product.…”

Section: Product Selectivity Of Sacs For Co 2 Reductionmentioning

confidence: 99%

“…Recycling undesirable CO 2 into functional chemical compounds is recognized as an ambitious approach to addressing global environmental and energy issues. [1][2][3][4] However, the direct capture and conversion of CO 2 from the atmosphere is challenging since only four CO 2 molecules are available for every ten thousand air molecules. Fortunately, plants are effective at converting CO 2 into carbohydrates and oxygen; and researchers, inspired by natural photocatalysis, have explored numerous artificial ways of converting CO 2 into carbonaceous compounds.…”

Section: Introductionmentioning

confidence: 99%

Single‐Atom Catalysts (SACs) for Photocatalytic CO₂ Reduction with H₂O: Activity, Product Selectivity, Stability, and Surface Chemistry

Hiragond

Powar

Lee

et al. 2022

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electrochemical, [7][8][9] thermo-, [10,11] and biocatalysis. [12,13] Converting CO 2 using readily available sunlight and water is one of the most promising strategies due to the following advantages: i) it utilizes solar light, a renewable energy, to drive the reduction of CO 2 , ii) it can convert CO 2 into valuable carbonaceous products like CO, CH 4 , C 2 H 6 , and CH 3 OH, iii) it operates under atmospheric conditions, iv) it is a controllable process, and v) it is scalable for industrial application. [14,15] Thus, converting undesirable CO 2 into value-added chemicals using artificial photosynthesis is a plausible way to address the current environmental and energy issues associated with the burning of fossil fuels. [16] Given the significance of photocatalytic CO 2 conversion, researchers have extensively researched various catalysts, such as metal oxides, alloys, chalcogenides, carbon-based structures, organic polymers, inorganic complexes, and MXenes. [17][18][19][20][21][22][23][24][25][26] However, low productivity, poor product selectivity, poor long-term stability, sluggish mechanisms, and economic unviability limit the application of these conventional catalysts. Furthermore, the solar to fuel conversion efficiency of most reported catalysts is less than 1%, which is insufficient for large-scale applications. Accordingly, the need for high-performance and economically viable catalysts has prompted research organizations to design and synthesize a range of materials that can advance CO 2 reduction technology and its commercial viability.It has been recognized that the downsizing of nanoparticles (NPs) of a catalyst exposes more active sites, leading to the optimization of its electronic properties. [27] Recently, catalysts based on size-and shape-controlled, atomically dispersed metals have garnered the attention of the scientific community for various energy and environmental applications. [28,29] Single-atom (SA) catalysts (SACs) are obtained once the size and aggregation of metal particles are reduced to isolated metal atoms, which form low coordination states and enable the use of almost 100% of active metal sites; the electronic properties of metal SAs differ from those of corresponding bulk materials. [30,31] In nature, the magnesium porphyrin complex in chlorophyll has an SA-like structure necessary for photosynthesis; the iron porphyrin complex in cytochrome has a similar SA-like structure which plays a vital role in the molecular transfer of CO 2 . [32][33][34] In recent years, single-atom catalysts (SACs) have attracted the interest of researchers owing to their suitability for various catalytic applications. For instance, their optoelectronic features, site-specific activity, and costeffectiveness make SACs ideal for photocatalytic CO 2 reduction. The activity, product selectivity, and photostability of SACs depend on various factors such as the nature of the metal/support material, the interaction between the metal atoms and support, light-harvesting ability, charge separation behavior, ...

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Solar fuels: research and development strategies to accelerate photocatalytic CO₂ conversion into hydrocarbon fuels

Abstract: Photocatalytic CO2 conversion is vital technology to realize global carbon neutrality and generate future energy supplies. This review proposes fundamentals, challenges, strategies, and prospects for photocatalytic CO2 conversion research.

Cited by 362 publications

References 433 publications

Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

Pb-free halide perovskites for solar cells, light-emitting diodes, and photocatalysts

Single‐Atom Catalysts (SACs) for Photocatalytic CO₂ Reduction with H₂O: Activity, Product Selectivity, Stability, and Surface Chemistry

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Solar fuels: research and development strategies to accelerate photocatalytic CO2 conversion into hydrocarbon fuels

Abstract: Photocatalytic CO2 conversion is vital technology to realize global carbon neutrality and generate future energy supplies. This review proposes fundamentals, challenges, strategies, and prospects for photocatalytic CO2 conversion research.

Cited by 362 publications

References 433 publications

Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

Molecular-level insight into photocatalytic CO2 reduction with H2O over Au nanoparticles by interband transitions

Pb-free halide perovskites for solar cells, light-emitting diodes, and photocatalysts

Single‐Atom Catalysts (SACs) for Photocatalytic CO2 Reduction with H2O: Activity, Product Selectivity, Stability, and Surface Chemistry

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Product

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Solar fuels: research and development strategies to accelerate photocatalytic CO₂ conversion into hydrocarbon fuels

Single‐Atom Catalysts (SACs) for Photocatalytic CO₂ Reduction with H₂O: Activity, Product Selectivity, Stability, and Surface Chemistry