Highly Selective Photoconversion of CO2 to CH4 over SnO2/Cs3Bi2Br9 Heterojunctions Assisted by S-Scheme Charge Separation

Hu, Peiyu; Liang, Guijie; Zhu, Bicheng; Macyk, Wojciech; Yu, Jiaguo; Xu, Feiyan

doi:10.1021/acscatal.3c03095

Cited by 63 publications

(13 citation statements)

References 65 publications

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“…It is apparent from Figure 5b that m/z of CO from 13 C labelled 13 CO 2 gas is 29, while the m/z of CO coming from 12 CO 2 is 28, indicating that the carbon of CO comes from CO 2 gas, therefore validating the reliability of the above photoreduction performance. [ 50 ] On the other hand, the existence of 16 O 18 O and 18 O 2 has confirmed that water oxidation occurred as the other half reaction to consume the photo‐generated holes (Figure 5b). In addition, liquid 1 H NMR results indicate that there is no obvious peak associated with liquid product (Figure S24, Supporting Information).…”

Section: Resultsmentioning

confidence: 86%

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO₂ Photoreduction

Zhang,

Li,

Gao

et al. 2024

Advanced Energy Materials

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The inclusion of colloidal particles into 3D porous constructs to realize heterostructure ensembles enhances surface interactions and energy transfer that can transform the catalytic properties of conventional catalysts. However, assembling hydrophobic colloidal nanoparticles within hydrophilic 3D porous matrices to create tailored heterostructures and catalytic properties is particularly challenging. Here, a modified ligand grafting method is presented to spontaneously assemble CdS inorganic colloidal quantum dots within a metal‐organic framework (MOF) derived porous framework for efficient photocatalytic CO2 reduction. The grafted long chain molecular ligands effectively suppress phase separation and endow a molecular‐recognition effect to form ordered assembly microstructures. The proof‐of‐concept assembly of CdS and Prussian blue analogues (PBA) derived Co3O4 facilitates a high density of heterojunctions formation, improving charge transfer and extended lifetimes of photo‐induced electrons. Consequently, CdS/Co3O4 assembly exhibits exceptionally active and stable photocatalytic CO2 reduction activity, with a CO production rate of 73.9 µmol g−1 h−1 and CO selectivity of 98.9%. Importantly, the ligand grafting method can be generalized to achieve spontaneous assembly of quantum dots within various metal organic framework derived porous scaffolds. This work provides a rational strategy for precise self‐assembly of colloidal nanoparticles within porous microstructures, allowing tailored heterointerfaces for functional materials and applications.

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Section: Resultsmentioning

confidence: 86%

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO₂ Photoreduction

Zhang,

Li,

Gao

et al. 2024

Advanced Energy Materials

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“…The presence of absorption peaks of monodentate carbonate (m-CO 3 2– , 1507, 1484, and 1310 cm –1 ), bidentate carbonate (b-CO 3 2– , 1587 cm –1 ), bicarbonate (HCO 3 – , 1422 and 1354 cm –1 ), and CO 2 – (1612 and 1244 cm –1 ) suggests the chemisorption of CO 2 on the COF/QDs heterojunction (Figure S20). − Under light irradiation, new adsorption signals corresponding to *COOH (1705 cm –1 ), *CO (2078 cm –1 ), *CHO (1008 cm –1 ), *CH 2 O (967 cm –1 ), and *CH 3 O (1103 and 1187 cm –1 ) are observed, which are critical intermediates in the formation of CO and CH 4 . − During CO 2 photoreduction, the *CO*H intermediate on the catalyst can undergo three processes: the desorption of CO (Pathway I), the release of H from the interface (Pathway II), and continuous protonation to form the *CHO species and generate CH 4 (Pathway III). DFT calculations reveal that the Δ G values for the three pathways are −0.21, – 0.22, and −0.91 eV, respectively (Figure d), providing a reasonable explanation for the production of CO and CH 4 over the COF/QDs heterojunctions.…”

Section: Resultsmentioning

confidence: 99%

Boosting Artificial Photosynthesis: CO₂ Chemisorption and S-Scheme Charge Separation via Anchoring Inorganic QDs on COFs

He,

Hu,

Zhang

et al. 2024

ACS Catal.

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Photocatalytic conversion of CO 2 into valuable hydrocarbon fuels holds great promise in addressing emerging energy shortages and environmental crises while fulfilling pressing societal and national development demands. Nonetheless, its efficiency is hindered by restricted CO 2 chemisorption, rapid electron−hole recombination, and weak redox capability. Drawing inspiration from the distinctive characteristics of Schiff-based covalent organic frameworks (COFs), including substantial specific surface area, unique pore structure, and an abundance of weakly alkaline nitrogen elements, we employ the TPA-COF to enhance the chemisorption and activation of acidic CO 2 molecules, as validated by the CO 2 -temperature-programmed desorption analysis. Furthermore, anchoring CsPbBr 3 quantum dots (QDs) onto the COF facilitates the effective spatial separation of photoinduced charge carriers with strong redox capability, resulting from the formation of S-scheme heterojunctions between the COF and QDs as substantiated by in situ irradiation X-ray photoelectron spectroscopy, femtosecond transient absorption spectroscopy, and density functional theory simulations. As anticipated, the optimized COF/QDs heterostructures exhibit remarkable enhancements in CO 2 photoreduction performance in the absence of any molecule cocatalyst or scavenger, yielding CO and CH 4 at rates of 41.2 and 13.7 μmol g −1 , respectively. This work provides valuable insights into the development of novel organic/inorganic heterojunction photocatalysts with CO 2 chemisorption and S-scheme charge separation, offering great potential for sustainable artificial photosynthesis.

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“…65 For example, Xu et al reported an SnO 2 /Cs 3 Bi 2 Br 9 (SC4) S-scheme heterojunction via the electrostatic self-assembly of SnO 2 nanofibers and lead-free Cs 3 Bi 2 Br 9 quantum dots (QDs). 66 In situ XPS under light and dark conditions was performed to determine the charge transfer mechanism (Fig. 3).…”

Section: Methods For Identifying the S-scheme Charge Transfer Mechanismmentioning

confidence: 99%

Metal–organic framework-based S-scheme heterojunction photocatalysts

Yuan,

Du,

Yin

et al. 2024

Nanoscale

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Highly Selective Photoconversion of CO₂ to CH₄ over SnO₂/Cs₃Bi₂Br₉ Heterojunctions Assisted by S-Scheme Charge Separation

Cited by 63 publications

References 65 publications

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO₂ Photoreduction

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO₂ Photoreduction

Boosting Artificial Photosynthesis: CO₂ Chemisorption and S-Scheme Charge Separation via Anchoring Inorganic QDs on COFs

Metal–organic framework-based S-scheme heterojunction photocatalysts

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Highly Selective Photoconversion of CO2 to CH4 over SnO2/Cs3Bi2Br9 Heterojunctions Assisted by S-Scheme Charge Separation

Cited by 63 publications

References 65 publications

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO2 Photoreduction

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO2 Photoreduction

Boosting Artificial Photosynthesis: CO2 Chemisorption and S-Scheme Charge Separation via Anchoring Inorganic QDs on COFs

Metal–organic framework-based S-scheme heterojunction photocatalysts

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Product

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Highly Selective Photoconversion of CO₂ to CH₄ over SnO₂/Cs₃Bi₂Br₉ Heterojunctions Assisted by S-Scheme Charge Separation

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO₂ Photoreduction

Ligand Mediated Assembly of CdS Colloids in 3D Porous Metal–Organic Framework Derived Scaffold with Multi‐Sites Heterojunctions for Efficient CO₂ Photoreduction

Boosting Artificial Photosynthesis: CO₂ Chemisorption and S-Scheme Charge Separation via Anchoring Inorganic QDs on COFs