Photosynthetic H2 generation and organic transformations with CdSe@CdS-Pt nanorods for highly efficient solar-to-chemical energy conversion

Agosti, Amedeo; Nakibli, Yifat; Amirav, Lilac; Bergamini, Giacomo

doi:10.1016/j.nanoen.2020.104510

Cited by 39 publications

(32 citation statements)

References 51 publications

(11 reference statements)

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“…The selective oxidation of alcohols to carbonyls represents one of the most important reactions in both the fine chemical industry and laboratory research ( Shibuya et al, 2011 ; Yang and Xu, 2013 ; Sharma et al, 2016 ; Xue Yang et al, 2017 ; Liu et al, 2018a ; Huang et al, 2018 ; Li et al, 2020 ; Shang et al, 2021 ); the carbonyl products are widely used intermediates and precursors for the manufacture of perfumes, pharmaceuticals, and dyes ( Liu et al, 2015 ; Agosti et al, 2020 ; Xia et al, 2020 ; Shang et al, 2021 ). Generally, the oxidative dehydrogenation of alcohols is carried out in the presence of chemical oxidants such as iodine, manganese, chromium oxide, or molecular oxygen.…”

Section: Introductionmentioning

confidence: 99%

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Chen

Roeffaers

et al. 2022

Front. Chem.

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Metal halide perovskites (MHPs) have been widely investigated for various photocatalytic applications. However, the dual-functional reaction system integrated selective organic oxidation with H2 production over MHPs is rarely reported. Here, we demonstrate for the first time the selective oxidation of aromatic alcohols to aldehydes integrated with hydrogen (H2) evolution over Pt-decorated CsPbBr3. Especially, the functionalization of CsPbBr3 with graphene oxide (GO) further improves the photoactivity of the perovskite catalyst. The optimal amount of CsPbBr3/GO-Pt exhibits an H2 evolution rate of 1,060 μmol g−1 h−1 along with high selectivity (>99%) for benzyl aldehyde generation (1,050 μmol g−1 h−1) under visible light (λ > 400 nm), which is about five times higher than the CsPbBr3-Pt sample. The enhanced activity has been ascribed to two effects induced by the introduction of GO: 1) GO displays a structure-directing role, decreasing the particle size of CsPbBr3 and 2) GO and Pt act as electron reservoirs, extracting the photogenerated electrons and prohibiting the recombination of the electron–hole pairs. This study opens new avenues to utilize metal halide perovskites as dual-functional photocatalysts to perform selective organic transformations and solar fuel production.

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Section: Introductionmentioning

confidence: 99%

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Chen

Roeffaers

et al. 2022

Front. Chem.

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“…115,116 Moreover, a novel Pt-tipped CdSe@CdS rods photocatalysts were reported to produce hydrogen with 69% photon-to-hydrogen conversion efficiency, along with simultaneous benzylamine (BnNH2) oxidation to benzylidenebenzylamine and benzaldehyde under the illumination of visible light. 117 The detailed mechanism study showed that the BnNH2 can firstly be converted into benzylidenebenzylamine, which could be further hydrolyzed to form benzaldehyde and BnNH2 with water. The newly formed BnNH2 was further oxidized under continuous light irradiation and shifted the latter reaction out of equilibrium toward the accumulation of benzaldehyde.…”

Section: Photocatalytic Oxidation Of Various Alcohols Coupled With Hydrogen Evolutionmentioning

confidence: 99%

Synergistic Redox Reaction for Value-Added Organic Transformation via Dual-Functional Photocatalytic Systems

Shang

Huang

et al. 2021

ACS Catal.

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Photocatalytic selective organic transformations provide an efficient synthetic alternative for several industrially relevant chemicals using solar rather than thermal energy. However, in most cases, photocatalytic organic reaction systems involve only reductive or oxidative pathways with the aid of sacrificial reagents as efficient electron acceptors or donors, thus limiting the economic added value. Recently, merging selective organic reductions and oxidations in a dual-functional photocatalytic reaction system has been put forward to tackle this limitation. In this coupled reaction system, both the photogenerated electrons and holes can be simultaneously utilized to generate value-added products, make the overall process more valuable from the economic perspective. In this review, the development of dualfunctional photocatalytic organic synthesis is systemically summarized. Particular emphasis is paid to merging selective organic oxidation and reduction reactions and coupling selective organic transformations with chemical fuel generation (e.g., H2, CO). Also, a personal perspective on future developments in this field is provided. Although still in its infancy, it is expected that this dual-functional technology offers opportunities to develop the next-generation selective organic transformation processes that meet the stringent economic, societal, and ecological expectations.

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“…In contrast, the integration of photocatalytic water splitting into H 2 with the selective oxidation of organics represents a more efficient solar energy conversion system that can achieve the simultaneous productions of solar fuel and value‐added organic chemicals, where the products are naturally separated in two phases of gas and liquid, avoiding the additional procedure and cost for separation. [ 8–12 ] However, compared with those for the photocatalytic H 2 evolution with sacrificial regents, the available high‐efficiency photocatalysts for synchronous productions of H 2 and high value‐added chemicals as well as understanding their structure‐performance relationships are still in short supply, requiring more efforts to explore.…”

Section: Introductionmentioning

confidence: 99%

Synergistic Pd Single Atoms, Clusters, and Oxygen Vacancies on TiO₂ for Photocatalytic Hydrogen Evolution Coupled with Selective Organic Oxidation

Wang

Tao

et al. 2020

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120

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Developing efficient photocatalysts for synchronously producing H2 and high value‐added chemicals holds great promise to enhance solar energy conversion. Herein, a facile strategy of simultaneously engineering Pd cocatalyst and oxygen vacancies (VOs) on TiO2 to promote H2 production coupled with selective oxidation of benzylamine is demonstrated. The optimized PdSA+C/TiO2‐VO photocatalyst containing Pd single atoms (SAs), clusters (C), and VOs exhibits much superior performance to those of TiO2‐VO and PdSA/TiO2‐VO counterparts. The production rates of H2 and N‐benzylidenebenzylamine over PdSA+C/TiO2‐VO are 52.7 and 1.5 times those over TiO2‐VO, respectively. Both experimental and theoretical studies have elucidated the synergistic effect of Pd SAs, clusters, and VOs on TiO2 in boosting the photocatalytic reaction. The presence of Pd SAs facilitates the generation and stabilization of abundant VOs by the formation of PdOTi3+ atomic interface, while Pd clusters promote the photogenerated charge separation and afford the optimum active sites for H2 evolution. Surface VOs of TiO2 guarantee the efficient adsorption and dissociation/activation of reactant molecules. This study reveals the effect of active‐site engineering on the photocatalysis and is expected to shed substantial light on future structure design and modulation of semiconductor photocatalysts.

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Photosynthetic H2 generation and organic transformations with CdSe@CdS-Pt nanorods for highly efficient solar-to-chemical energy conversion

Cited by 39 publications

References 51 publications

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Synergistic Redox Reaction for Value-Added Organic Transformation via Dual-Functional Photocatalytic Systems

Synergistic Pd Single Atoms, Clusters, and Oxygen Vacancies on TiO₂ for Photocatalytic Hydrogen Evolution Coupled with Selective Organic Oxidation

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Photosynthetic H2 generation and organic transformations with CdSe@CdS-Pt nanorods for highly efficient solar-to-chemical energy conversion

Cited by 39 publications

References 51 publications

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Photocatalytic Anaerobic Oxidation of Aromatic Alcohols Coupled With H2 Production Over CsPbBr3/GO-Pt Catalysts

Synergistic Redox Reaction for Value-Added Organic Transformation via Dual-Functional Photocatalytic Systems

Synergistic Pd Single Atoms, Clusters, and Oxygen Vacancies on TiO2 for Photocatalytic Hydrogen Evolution Coupled with Selective Organic Oxidation

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Product

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Synergistic Pd Single Atoms, Clusters, and Oxygen Vacancies on TiO₂ for Photocatalytic Hydrogen Evolution Coupled with Selective Organic Oxidation