Covalent grafting of molecular photosensitizer and catalyst on MOF-808: effect of pore confinement toward visible light-driven CO₂ reduction in water

Energy & Environmental Science, Journal Year: 2021, Volume and Issue: 14(4), P. 2429 - 2440

Published: Jan. 1, 2021

We have fabricated Zr-MBA-Ru/Re-MOFvia post-synthetic modification of MOF-808. The integrated catalyst assembly was used to mimic natural photosynthesis for sunlight-driven CO₂ reduction produce CO in aqueous medium without external sacrificial electron donor.

Language: Английский

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Engineering graphitic carbon nitride (g-C₃N₄) for catalytic reduction of CO₂to fuels and chemicals: strategy and mechanism

Green Chemistry, Journal Year: 2021, Volume and Issue: 23(15), P. 5394 - 5428

Published: Jan. 1, 2021

This review summarises the structural-compositional engineering of carbon nitride (g-C₃N₄) for electrocatalytic and photocatalytic CO₂reduction to chemicals fuels experimentally theoretically.

Language: Английский

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Best practices for experiments and reporting in photocatalytic CO2 reduction

Nature Catalysis, Journal Year: 2023, Volume and Issue: 6(8), P. 657 - 665

Published: Aug. 10, 2023

Language: Английский

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Synthesis and modification strategies of g-C3N4 nanosheets for photocatalytic applications

Advanced Powder Materials, Journal Year: 2023, Volume and Issue: 3(1), P. 100150 - 100150

Published: July 5, 2023

Graphitic carbon nitride nanosheets (CNNs) become the most promising member in family benefitted from their two-dimensional structural features. Recently, great endeavors have been made synthesis and modification of CNNs to improve photocatalytic properties, many exciting progresses gained. In order elucidate fundamentals based catalysts provide insights into rational design photocatalysis system, we describe recent progress preparation strategies applications this review. Firstly, physicochemical properties are briefly introduced. Secondly, approaches reviewed, including top-down stripping (thermal, gas, liquid, composite stripping) bottom-up precursor molecules (solvothermal, template, supramolecular self-assembly method). Subsequently, on years discussed, crystal structure design, doping, surface functionalization, constructing 2D heterojunction, anchoring single-atom. Then multifunctional g-C3N4 nanosheet materials H2 evolution, O2 overall water splitting, H2O2 production, CO2 reduction, N2 fixation, pollutant removal, organic synthesis, sensing highlighted. Finally, opportunities challenges for development high-performance systems also promising.

Language: Английский

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P‐Mediated Cu–N₄ Sites in Carbon Nitride Realizing CO₂ Photoreduction to C₂H₄ with Selectivity Modulation

Advanced Materials, Journal Year: 2022, Volume and Issue: 35(3)

Published: Nov. 4, 2022

Photocatalytic CO2 reduction to high value-added C2 products (e.g., H4 ) is of considerable interest but challenging. The product selectivity strongly hinges on the intermediate energy levels in pathway. Herein, Cu-N4 sites anchored phosphorus-modulated carbon nitride (CuACs/PCN) designed as a photocatalyst tailor formation reaction pathway for realizing its production with tunable selectivity. Theoretical calculations combined experimental data demonstrate that C-C coupling intermediates can be realized and surrounding doped P facilitates . Thus, CuACs/PCN exhibits 53.2% yielding rate 30.51 µmol g-1 findings reveal significant role coordination environment microenvironment Cu single atoms offer an effective approach highly selective photoreduction produce

Language: Английский

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Construction of Core–Shell MOF@COF Hybrids with Controllable Morphology Adjustment of COF Shell as a Novel Platform for Photocatalytic Cascade Reactions

Advanced Science, Journal Year: 2021, Volume and Issue: 8(19)

Published: Aug. 10, 2021

Recently, novel core-shell MOF@COF hybrids display excellent performance in various fields because of their inherited advantages from parent MOFs and/or COFs. However, it is still a grand challenge to adjust the morphology COFs for consequent improvement. Herein, Ti-MOF@TpTt hybrid coated with ultra-thin COF nanobelt, which different fibrillar-like COF, successfully synthesized through sequential growth strategy. The as-obtained Pd decorated catalyst exhibits much higher photocatalytic than those Ti-MOF, TpTt-COF, and shell cascade reactions ammonia borane (AB) hydrolysis nitroarenes hydrogenation. These can be attributed its high BET surface area, structure, type II heterojunction, offers more accessible active sites improves separation efficiency photo-generated carriers. Finally, possible mechanisms reaction are also proposed well explain improved this system. This work presents constructive route designing controllable adjustment shell, leading ability broaden applications MOF/COF materials.

Language: Английский

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Defects controlling, elements doping, and crystallinity improving triple-strategy modified carbon nitride for efficient photocatalytic diclofenac degradation and H2O2 production

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 321, P. 121941 - 121941

Published: Sept. 6, 2022

Language: Английский

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Engineering a Copper Single‐Atom Electron Bridge to Achieve Efficient Photocatalytic CO₂ Conversion

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(13)

Published: Feb. 7, 2023

Developing highly efficient and stable photocatalysts for the CO2 reduction reaction (CO2 RR) remains a great challenge. We designed Z-Scheme photocatalyst with N-Cu1 -S single-atom electron bridge (denoted as Cu-SAEB), which was used to mediate RR. The production of CO O2 over Cu-SAEB is high 236.0 120.1 μmol g-1 h-1 in absence sacrificial agents, respectively, outperforming most previously reported photocatalysts. Notably, as-designed throughout 30 cycles, totaling 300 h, owing strengthened contact interface Cu-SAEB, mediated by atomic structure. Experimental theoretical calculations indicated that SAEB greatly promoted Z-scheme interfacial charge-transport process, thus leading enhancement photocatalytic RR Cu-SAEB. This work represents promising platform development have potential conversion applications.

Language: Английский

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Quantum Dot-Sensitized Photoreduction of CO₂ in Water with Turnover Number > 80,000

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(43), P. 18131 - 18138

Published: Oct. 19, 2021

Climate change and global energy demands motivate the search for sustainable transformations of carbon dioxide (CO2) to storable liquid fuels. Photocatalysis is a pathway direct conversion CO2 CO, one step within light-powered reaction networks that could, if efficient enough, transform solar landscape. To date, best performing photocatalytic reduction systems operate in nonaqueous solvents, but technologically viable fuels will likely water. Here we demonstrate catalytic photoreduction CO pure water at pH 6-7 with an unprecedented combination performance parameters: turnover number (TON(CO)) = 72,484-84,101, quantum yield (QY) 0.96-3.39%, selectivity (SCO) > 99%, using CuInS2 colloidal dots (QDs) as photosensitizers Co-porphyrin catalyst. At higher catalyst concentration, system reaches QY 3.53-5.23%. The QD-driven greatly exceeds benchmark aqueous (926 turnovers 0.81% 82%), due primarily (i) electrostatic attraction QD catalyst, which promotes fast multielectron delivery colocalization protons, CO2, source photoelectrons, (ii) termination QD's ligand shell free amines, capture carbamic acid serves reservoir effectively increasing its solubility water, lowers onset potential by Co-porphyrin. breakthrough efficiency achieved this work represents nonincremental realization solar-to-fuel conversion.

Language: Английский

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Multifunctional carbon nitride nanoarchitectures for catalysis

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(21), P. 7602 - 7664

Published: Jan. 1, 2023

Carbon nitrides, with feasibility of tailored band gap via suitable nanoarchitectonics, are deemed as best catalysts amongst existing materials, especially for HER, OWS, COR, NRR, water oxidation, pollutant removal, and organocatalysis.

Language: Английский

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