Boosting Cascade Electron Transfer for Highly Efficient CO<sub>2</sub> Photoreduction

Li, Na; Zhai, Xin-Ping; Yan, Wen-Kai; Zhang, Yajun; Zhang, Zhengtao; Xiao, Mingjun; Zhang, Xiaodong; Wang, Qiang; Zhang, Hao‐Li

doi:10.1002/solr.202100558

Cited by 14 publications

(19 citation statements)

References 57 publications

(58 reference statements)

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“…In addition, τ2 and τ3 represented the relaxation process from the S1 to the S0 state and the intersystem crossing from the S1 to the excited triplet (T1) state, respectively. [49] Notably, the relaxation time of Cu2 was much longer than that of Cu1 in each channel owing to the increase in the coordination numbers leading to an increase in the charge transfer, which was consistent with the results obtained from the first-principles analysis. In addition, Figure 6a,b reveals that the normalized decay curves of Cu1 and Cu2 at different wavelengths maintain a plateau with different normalized intensities after ≈1000 ps owing to the extremely slow recombination of carriers from the T1 to S0 state.…”

Section: Ultrafast Carrier Dynamicssupporting

confidence: 89%

Switchable Nonlinear Optical Absorption of Metal–Organic Frameworks

Liang

Xue

et al. 2022

Advanced Optical Materials

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Metal–organic frameworks (MOFs) are widely explored owing to their excellent nonlinear optical (NLO) properties. However, researchers have mainly focused on designing new structures of MOF crystals to adjust the NLO response while ignoring the influence of the number of metal–ligand coordination bonds on the NLO properties of MOFs. In this study, the influence of the coordination numbers of MOFs on their NLO properties is studied for the first time. Herein, MOFs with different coordination numbers, using trifluoroacetic acid as an auxiliary agent, are synthesized and their NLO properties are tested using the Z‐scan technique. The results reveal that the NLO absorption properties of MOFs with high coordination numbers can be effectively modulated from saturable absorption to reverse saturable absorption by increasing the excitation intensity. First‐principles calculations show that a change in the coordination numbers leads to a change in the charge transfer from metal to ligand, thereby resulting in different NLO responses. The MOFs with a high coordination number have potential applications in novel optical switches or logic gates. These results provide a reference for the precise adjustment of the NLO properties of MOFs.

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Section: Ultrafast Carrier Dynamicssupporting

confidence: 89%

Switchable Nonlinear Optical Absorption of Metal–Organic Frameworks

Liang

Xue

et al. 2022

Advanced Optical Materials

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“…Li and co‐workers built the “cascade electron transfer” by combining CsPbBr 3 QDs and 2D Cu‐based porphyrin MOF nanosheets (CsPbBr 3 /CuTCPP MOF) to spur both interfacial and inner electron transfer (Figure 9f). [ 83 ] The optimized CsPbBr 3 /CuTCPP MOF (0.1 wt% Cu) achieved the yield of 11.8 and 2.95 μmol g −1 h −1 for CO and CH 4 , respectively.…”

Section: Methods To Improve Photoelectrochemical Performancementioning

confidence: 99%

“…Combining with CsPbBr 3 nanomaterials, Ni-based and Cu-based 2D MOF materials also showed superior photocatalytic performance, and were reported by Xi et al and Li et al respectively. [82,83] In Xi's work, they compared the properties of CsPbBr 3 nanocubes, nanorods, and nanowires, and found that the charge carrier dynamics is depend on the aspect ratio of the PVK. [82] As shown in Figure 9e, the Ni-based MOF/ CsPbBr 3 nanowires (NMF/CPB-NWs) exhibited the highest CO production rate of 81.0 μmol g À1 h À1 .…”

Section: Type-ii Heterojunctionsmentioning

confidence: 99%

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Tailoring Inorganic Halide Perovskite Photocatalysts toward Carbon Dioxide Reduction

Zhang

Tang

et al. 2022

Solar RRL

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In recent years, photocatalytic carbon dioxide reduction has emerged as an attractive strategy to settle the global warming and energy crisis by converting CO2 into valuable chemicals utilizing solar energy. All‐inorganic halide perovskites (PVKs), as a class of promising light‐harvesting materials with outstanding optoelectronic properties and considerable stabilities, have received dramatic attention in the field of photocatalytic CO2 reduction reaction (CO2RR). In this review, the recent progress of PVK catalysts for CO2RR is systematically summarized and evaluated according to the modification strategies and their mechanisms. The working principles of CO2RR are first introduced. The main strategies for improving the photoelectrochemical performance are then discussed and their recent developments are summarized. Finally, the current challenges, including instability, charge recombination, and insufficient active sites, and future research opportunities for further development are addressed.

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“…Another key hurdle in the formation of the highly reactive charge-separated state is the ease of photoinduced electron transfer, also called charge transfer, from either the singlet or triplet states, in MOFs ,, and COFs . These processes generally occur in the picosecond (10 –12 s) time scale. − …”

Section: Excited-state Properties Of Porphyrin-containing Mofs and Cofsmentioning

confidence: 99%

Visible-Light-Driven Production of Solar Fuels Catalyzed by Nanosized Porphyrin-Based Metal–Organic Frameworks and Covalent–Organic Frameworks: A Review

Asselin

Harvey

2022

ACS Appl. Nano Mater.

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Porphyrin-based materials are excellent chromophores because they strongly absorb visible light and their relatively low-energy lowest unoccupied molecular orbitals thermodynamically favor photoinduced electron transfer. They can generate charge-transfer excited states with and without cocatalyst(s) and ease energy transfer and ultrafast excitation energy migration. Combined with synthetic accessibility, these qualities make them ideal building blocks for porous metal− organic framework (MOF)-and covalent−organic framework (COF)-based photocatalysts to produce solar fuels. This review first describes the structures of the most common porphyrinic MOFs and COFs and their excited-state properties and semiconducting behavior as well as that of derived composites. The generally accepted mechanisms of formation of H 2 , CH 4 and derivatives, and N 2 are then reviewed, followed by the detailed examples of nano-MOFs and nano-COFs used for the said purpose: characteristic parameters such as rates of production, turnover numbers (TONs), turnover frequencies (TOFs), and apparent quantum efficiencies are described and compared. This shows that porphyrin-based MOFs and COFs are efficient solar-fuelproducing photocatalysts, with characteristics comparable to those of nonporphyrinic MOF and COF photocatalysts, although, on some occasions, the rates of production fall short of record values. Conversely, porphyrinic MOFs and COFs exhibit the greatest TONs and TOFs of any solar-fuel-producing MOFs or COFs but still face shortcomings concerning selectivity in CH 4 production because of the many possible side products. Importantly, while the best rate of photoproduction of solar fuels has been observed from nanoscale photocatalysts, there seem to be no drastic differences in the rate (within μmol −1 h −1 and mmol g −1 h −1 ) between nanoscale and microscale heterogeneous photocatalysts. This observation suggests that the more active sites are mostly located at or near the surface of the particles. Overall, nanosized porphyrin-based MOFs and COFs show rich and promising photocatalytic properties for generating solar fuels but still have room for improvement.

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Boosting Cascade Electron Transfer for Highly Efficient CO₂ Photoreduction

Cited by 14 publications

References 57 publications

Switchable Nonlinear Optical Absorption of Metal–Organic Frameworks

Switchable Nonlinear Optical Absorption of Metal–Organic Frameworks

Tailoring Inorganic Halide Perovskite Photocatalysts toward Carbon Dioxide Reduction

Visible-Light-Driven Production of Solar Fuels Catalyzed by Nanosized Porphyrin-Based Metal–Organic Frameworks and Covalent–Organic Frameworks: A Review

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Boosting Cascade Electron Transfer for Highly Efficient CO2 Photoreduction

Cited by 14 publications

References 57 publications

Switchable Nonlinear Optical Absorption of Metal–Organic Frameworks

Switchable Nonlinear Optical Absorption of Metal–Organic Frameworks

Tailoring Inorganic Halide Perovskite Photocatalysts toward Carbon Dioxide Reduction

Visible-Light-Driven Production of Solar Fuels Catalyzed by Nanosized Porphyrin-Based Metal–Organic Frameworks and Covalent–Organic Frameworks: A Review

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Boosting Cascade Electron Transfer for Highly Efficient CO₂ Photoreduction