Mn‐Doped Perovskite Nanocrystals for Photocatalytic CO<sub>2</sub> Reduction: Insight into the Role of the Charge Carriers with Prolonged Lifetime

Wang, Jin; Xiong, Li; Bai, Yu; Chen, Zhoujie; Zheng, Qi; Shi, Yangyi; Zhang, Chao; Jiang, Guocan; Li, Zhengquan

doi:10.1002/solr.202270086

Cited by 10 publications

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“…[ 3,4 ] As an emerging candidate photocatalyst, perovskite nanocrystals (PNCs) have attracted enormous interests because they are featured by high extinction coefficient, low exciton binding energy, defect tolerance, and tunable band edges. [ 5–11 ] However, the pristine PNCs only exhibit low activities mainly due to the serious charge recombination. [ 4,12 ] To solve this problem, various PNC heterojunctions, such as schottky‐junction, [ 6,13 ] type II, [ 7,12,14,15 ] and Z‐scheme, [ 16–21 ] have been designed and prepared for photocatalytic CO 2 reduction.…”

Section: Introductionmentioning

confidence: 99%

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO₂ Reduction

Wang

Zhang

et al. 2023

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Perovskite nanocrystals (PNCs) are promising candidates for solar‐to‐fuel conversions yet exhibit low photocatalytic activities mainly due to serious recombination of photogenerated charge carriers. Constructing heterojunction is regarded as an effective method to promote the separation of charge carriers in PNCs. However, the low interfacial quality and non‐directional charge transfer in heterojunction lead to low charge transfer efficiency. Herein, a CsPbBr3–CdZnS heterojunction is designed and prepared via an in situ hot‐injection method for photocatalytic CO2 reduction. It is found that the high‐quality interface in heterojunction and anisotropic charge transfer of CdZnS nanorods (NRs) enable efficient spatial separation of charge carriers in CsPbBr3–CdZnS heterojunction. The CsPbBr3–CdZnS heterojunction achieves a higher CO yield (55.8 µmol g−1 h−1) than that of the pristine CsPbBr3 NCs (13.9 µmol g−1 h−1). Furthermore, spectroscopic experiments and density functional theory (DFT) simulations further confirm that the suppressed recombination of charge carriers and lowered energy barrier for CO2 reduction contribute to the improved photocatalytic activity of the CsPbBr3–CdZnS heterojunction. This work demonstrates a valid method to construct high‐quality heterojunction with directional charge transfer for photocatalytic CO2 reduction. This study is expected to pave a new avenue to design perovskite–chalcogenide heterojunction.

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Section: Introductionmentioning

confidence: 99%

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO₂ Reduction

Wang

Zhang

et al. 2023

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“…Atomic substitution is a well-established approach for band gap engineering, in which the B(III) site can be replaced with over 34 choices of trivalent metals . Doping can also potentially regulate the path of charge transfer as some dopants (e.g., Mn, Cu, and Cd) have the ability to generate additional electronic states within the energy levels of the semiconductor hosts, therefore customizing the charge transfer dynamics. − For instance, Tl 3+ , In 3+ , Sb 3+ , and Fe 3+ have been reported to alloy with Bi 3+ in Cs 2 AgBiBr 6 . − Among these trivalent elements, Fe 3+ , Tl 3+ and Sb 3+ can effectively extend the light absorption range of Cs 2 AgBiBr 6 . Considering the high toxicity of Tl and the variable valencies of transition metals, Sb substitution is more suitable for photocatalytic application.…”

Section: Introductionmentioning

confidence: 99%

Sb-Substituted Cs₂AgBiBr₆/g-C₃N₄ Composite for Photocatalytic C(sp³)–H Bond Activation in Toluene

Mai

Cox

et al. 2023

Chem. Mater.

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The visible-light-driven photocatalytic selective aromatic C(sp3)–H bond activation utilizing all-inorganic halide perovskites as photocatalysts is a sustainable and green approach to obtain value-added oxygenates. These catalysts, however, are restricted by low activity due to undesirable charge recombination and inefficient light absorption. In this research, we developed a Sb-substituted Cs2AgBiBr6/g-C3N4 composite to enhance the photocatalytic performance for toluene oxidation. The introduction of the Sb dopant extended the visible light absorbance to 650 nm, and the formation of the heterointerface and the staggered band structure between the two components substantially suppressed the charge recombination. This composite features a 2.3-fold and 72.5-fold higher visible light photocatalytic toluene oxidation rate toward benzaldehyde than that of either Sb-substituted Cs2AgBiBr6 or g-C3N4 alone, respectively, with a high selectivity of over 96%. The development of all-inorganic lead-free halide perovskite-based heterostructures for visible light photocatalytic organic transformations is expected to have wide-reaching application.

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“…Furthermore, the time for charge recombination in QDs is typically at the nanosecond scale, which is faster than the surface CO 2 reduction reaction (ranging from nanosecond to microsecond). , Hence, the photogenerated charge carriers would be largely eliminated before reaching the surface for subsequent photocatalytic reactions (Scheme ). In order to enhance the photocatalytic performance of QDs, it is crucial to minimize the undesired charge recombination processes (e.g., radiative recombination) and prolong the lifetime of charge carriers . Provided that the charge recombination can be slowed to match the rate of surface reactions, the photogenerated charge carriers are more likely to engage in redox reactions.…”

Section: Introductionmentioning

confidence: 99%

Generating Long-Lived Charge Carriers in CdS Quantum Dots by Cu-Doping for Photocatalytic CO₂ Reduction

Zhang,

Liu,

Wang

et al. 2024

Inorg. Chem.

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Converting CO 2 into high-value-added chemicals has been recognized as a promising way to tackle the fossil fuel crisis. Quantum dots (QDs) have been extensively studied for photocatalytic CO 2 reduction due to their excellent optoelectronic properties. However, most of the photogenerated charge carriers recombine before they participate in the photocatalytic reaction. It is crucial to regulate the charge carriers to minimize undesired charge recombination, thus, promoting surface photocatalysis. Herein, we report a copperdoped CdS (Cu:CdS) QD photocatalyst for CO 2 reduction. Density functional theory simulations and experimental results demonstrate that Cu dopants create intermediate energy levels in CdS QDs that can extend the lifetime of exciton charge carriers. Furthermore, the long-lived charge carriers can be harnessed for the photocatalytic reaction on Cu:CdS QDs. The resultant Cu:CdS QDs exhibited a significantly enhanced photocatalytic activity toward CO 2 reduction compared to the pristine CdS QDs. This work highlights the importance of charge regulation in photocatalysts and opens new pathways for the exploration of efficient QD photocatalysts.

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Mn‐Doped Perovskite Nanocrystals for Photocatalytic CO₂ Reduction: Insight into the Role of the Charge Carriers with Prolonged Lifetime

Cited by 10 publications

References 0 publications

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO₂ Reduction

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO₂ Reduction

Sb-Substituted Cs₂AgBiBr₆/g-C₃N₄ Composite for Photocatalytic C(sp³)–H Bond Activation in Toluene

Generating Long-Lived Charge Carriers in CdS Quantum Dots by Cu-Doping for Photocatalytic CO₂ Reduction

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Mn‐Doped Perovskite Nanocrystals for Photocatalytic CO2 Reduction: Insight into the Role of the Charge Carriers with Prolonged Lifetime

Cited by 10 publications

References 0 publications

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO2 Reduction

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO2 Reduction

Sb-Substituted Cs2AgBiBr6/g-C3N4 Composite for Photocatalytic C(sp3)–H Bond Activation in Toluene

Generating Long-Lived Charge Carriers in CdS Quantum Dots by Cu-Doping for Photocatalytic CO2 Reduction

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Product

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Mn‐Doped Perovskite Nanocrystals for Photocatalytic CO₂ Reduction: Insight into the Role of the Charge Carriers with Prolonged Lifetime

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO₂ Reduction

In Situ Constructed Perovskite–Chalcogenide Heterojunction for Photocatalytic CO₂ Reduction

Sb-Substituted Cs₂AgBiBr₆/g-C₃N₄ Composite for Photocatalytic C(sp³)–H Bond Activation in Toluene

Generating Long-Lived Charge Carriers in CdS Quantum Dots by Cu-Doping for Photocatalytic CO₂ Reduction