Solar Energy Catalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(29)

Published: April 26, 2022

When it comes to using solar energy promote catalytic reactions, photocatalysis technology is the first choice. However, sunlight can not only be directly converted into chemical through a photocatalytic process, also different energy-transfer pathways. Using as source, reactions proceed independently, and coupled with other technologies enhance overall efficiency. Therefore, sunlight-driven are diverse, need given specific definition. We propose timely perspective for driven by give them definition, namely "solar catalysis". The concept of types catalysis, such photocatalysis, photothermal cell powered electrocatalysis, pyroelectric highlighted. Finally, their limitations future research directions discussed.

Language: Английский

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Boosted Inner Surface Charge Transfer in Perovskite Nanodots@Mesoporous Titania Frameworks for Efficient and Selective Photocatalytic CO₂ Reduction to Methane

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(20)

Published: Feb. 22, 2022

Exploring high-efficiency and stable halide perovskite-based photocatalysts for the selective reduction of CO2 to methane is a challenge because intrinsic photo- chemical instability perovskites. In this study, perovskites (Cs3 Bi2 Br9 Cs2 AgBiBr6 ) were grown in situ mesoporous TiO2 frameworks an efficient reduction. Benchmarked CH4 production rates 32.9 24.2 μmol g-1 h-1 with selectivities 88.7 % 84.2 %, achieved, respectively, which are better than most reported perovskite photocatalysts. Focused ion-beam sliced-imaging techniques used directly image hyperdispersed nanodots confined mesopores tunable sizes ranging from 3.8 9.9 nm. X-ray photoelectronic spectroscopy Kelvin probe force microscopy showed that built-in electric field between titania channels efficiently promoted photo-induced charge transfer. Density functional theory calculations indicate high selectivity was attributed Bi-adsorption-mediated hydrogenation *CO *HCO dominates CO desorption.

Language: Английский

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Advances of MOFs and COFs for photocatalytic CO2 reduction, H2 evolution and organic redox transformations

Coordination Chemistry Reviews, Journal Year: 2023, Volume and Issue: 490, P. 215210 - 215210

Published: May 21, 2023

Language: Английский

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Rational design of donor-acceptor conjugated polymers with high performance on peroxydisulfate activation for pollutants degradation

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 316, P. 121611 - 121611

Published: June 9, 2022

Language: Английский

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Synergistic promotions between CO2 capture and in-situ conversion on Ni-CaO composite catalyst

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: Feb. 22, 2023

The integrated CO2 capture and conversion (iCCC) technology has been booming as a promising cost-effective approach for Carbon Neutrality. However, the lack of long-sought molecular consensus about synergistic effect between adsorption in-situ catalytic reaction hinders its development. Herein, we illustrate promotions through constructing consecutive high-temperature Calcium-looping dry reforming methane processes. With systematic experimental measurements density functional theory calculations, reveal that pathways reduction carbonate dehydrogenation CH4 can be interactively facilitated by participation intermediates produced in each process on supported Ni-CaO composite catalyst. Specifically, adsorptive/catalytic interface, which is controlled balancing loading size Ni nanoparticles porous CaO, plays an essential role ultra-high conversions 96.5% 96.0% at 650 °C, respectively.

Language: Английский

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Encapsulated CdSe/CdS nanorods in double-shelled porous nanocomposites for efficient photocatalytic CO2 reduction

Nature Communications, Journal Year: 2022, Volume and Issue: 13(1)

Published: Oct. 29, 2022

Colloidal quantum dots have been emerging as promising photocatalysts to convert CO2 into fuels by using solar energy. However, the above usually suffer from low adsorption capacity because of their nonporous structures, which principally reduces catalytic efficiency. Here, we show that synchronizing imine polycondensation reaction self-assembly colloidal CdSe/CdS nanorods can produce micro-meso hierarchically porous nanocomposites with double-shelled nanocomposites. Owing hierarchical pores and ability separate photoexcited electrons, self-assembled exhibit remarkably higher activity (≈ 64.6 μmol g-1 h-1) toward CO in solid-gas regime than solids under identical conditions. Importantly, length is demonstrated be crucial correlate long-distance separation photogenerated electrons holes along axial direction. Overall, this approach provides a rational strategy optimize conversion integrating inorganic organic semiconductors.

Language: Английский

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Confining charge-transfer complex in a metal-organic framework for photocatalytic CO2 reduction in water

Nature Communications, Journal Year: 2023, Volume and Issue: 14(1)

Published: July 26, 2023

In the quest for renewable fuel production, selective conversion of CO2 to CH4 under visible light in water is a leading-edge challenge considering involvement kinetically sluggish multiple elementary steps. Herein, 1-pyrenebutyric acid post-synthetically grafted defect-engineered Zr-based metal organic framework by replacing exchangeable formate. Then, methyl viologen incorporated confined space post-modified MOF achieve donor-acceptor complex, which acts as an antenna harvest light, and regulates electron transfer catalytic center (Zr-oxo cluster) enable visible-light-driven reduction reaction. The proximal presence charge complex enhances kinetics realized from transient absorption spectroscopy, facile helps produce CO2. reported material produces 7.3 mmol g-1 irradiation aqueous medium using sacrificial agents. Mechanistic information gleans paramagnetic resonance, situ diffuse reflectance FT-IR density functional theory calculation.

Language: Английский

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Thiadiazole-Based Covalent Organic Frameworks with a Donor–Acceptor Structure: Modulating Intermolecular Charge Transfer for Efficient Photocatalytic Degradation of Typical Emerging Contaminants

Environmental Science & Technology, Journal Year: 2022, Volume and Issue: 56(22), P. 16303 - 16314

Published: Oct. 28, 2022

As novel metal-free photocatalysts, covalent organic frameworks (COFs) have great potential to decontaminate pollutants in water. Fast charge recombination COFs yet inhibits their photocatalytic performance. We found that the intramolecular transfer within could be modulated via constructing a donor-acceptor (D-A) structure, leading improved performance of toward pollutant degradation. By integrating electron donor units (1,3,4-thiadiazole or 1,2,4-thiadiazole ring) and acceptor (quinone), two (COF-TD1 COF-TD2) with robust D-A characteristics were fabricated as visible-light-driven photocatalysts paracetamol. With readily excited electrons 1,3,4-thiadiazole rings, COF-TD1 exhibited efficient electron-hole separation through push-pull electronic effect, resulting superior paracetamol photodegradation (>98% degradation 60 min) than COF-TD2 (∼60% 120 min). efficiently photodegrade complicated water matrices even river water, lake sewage wastewater. Diclofenac, bisphenol A, naproxen, tetracycline hydrochloride also effectively degraded by COF-TD1. Efficient scaled-up reactor achieved either powder form immobilized onto glass slide (to further ease recovery reuse) under natural sunlight irradiation. Overall, this study provided an effective strategy for designing excellent COF-based degrade emerging contaminants.

Language: Английский

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Visible‐Light‐Driven Photocatalytic CO₂ Reduction to CO/CH₄ Using a Metal–Organic “Soft” Coordination Polymer Gel

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(16)

Published: Feb. 7, 2022

The self-assembly of a well-defined and astutely designed, low-molecular weight gelator (LMWG) based linker with suitable metal ion is promising method for preparing photocatalytically active coordination polymer gels. Here, we report the design, synthesis, gelation behaviour tetrapodal LMWG on porphyrin core connected to four terpyridine units (TPY-POR) through amide linkages. TPY-POR RuII ions results in Ru-TPY-POR gel (CPG), nanoscroll morphology. CPG exhibits efficient CO2 photoreduction CO (3.5 mmol g-1 h-1 ) >99 % selectivity presence triethylamine (TEA) as sacrificial electron donor. Interestingly, 1-benzyl-1,4-dihydronicotinamide (BNAH) TEA donor, 8e- /8H+ CH4 realized >95 (6.7 ). In CPG, acts photosensitizer covalently attached [Ru(TPY)2 ]2+ catalytic center demonstrated by femtosecond transient absorption (TA) spectroscopy. Further, combining information from situ DRIFT spectroscopy DFT calculation, possible reaction mechanism reduction was outlined.

Language: Английский

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Rational design of MoS2@COF hybrid composites promoting C-C coupling for photocatalytic CO2 reduction to ethane

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 325, P. 122393 - 122393

Published: Jan. 9, 2023

Language: Английский

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