Molecularly Engineered Covalent Organic Frameworks for Hydrogen Peroxide Photosynthesis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(19)

Published: Feb. 15, 2022

Synthesizing H

Language: Английский

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Metal‐Organic Frameworks for Photocatalytic Water Splitting and CO₂Reduction

Angewandte Chemie International Edition, Journal Year: 2023, Volume and Issue: 62(15)

Published: Jan. 23, 2023

Abstract Photocatalytic water splitting and carbon dioxide (CO 2 ) reduction provide promising solutions to global energy environmental issues. In recent years, metal‐organic frameworks (MOFs), a class of crystalline porous solids featuring well‐defined tailorable structures as well high surface areas, have captured great interest toward photocatalytic CO reduction. this review, the semiconductor‐like behavior MOFs is first discussed. We then summarize advances in over MOF‐based materials focus on unique advantage for clarifying structure‐property relationship photocatalysis. addition, some representative characterization techniques been presented unveil kinetics reaction intermediates systems. Finally, challenges, perspectives future directions are proposed.

Language: Английский

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Porous materials for capture and catalytic conversion of CO2 at low concentration

Coordination Chemistry Reviews, Journal Year: 2022, Volume and Issue: 465, P. 214576 - 214576

Published: April 29, 2022

Language: Английский

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Reticular framework materials for photocatalytic organic reactions

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(22), P. 7949 - 8004

Published: Jan. 1, 2023

Photocatalytic organic reactions, harvesting solar energy to produce high value-added chemicals, have attracted increasing attention as a sustainable approach address the global crisis and environmental issues. Reticular framework materials, including metal-organic frameworks (MOFs) covalent (COFs), are widely considered promising candidates for photocatalysis owing their crystallinity, tailorable pore environment extensive structural diversity. Although design synthesis of MOFs COFs been intensively developed in last 20 years, applications photocatalytic transformations still preliminary stage, making systematic summary necessary. Thus, this review aims provide comprehensive understanding useful guidelines exploration suitable MOF COF photocatalysts towards appropriate reactions. The commonly used reactions categorized facilitate identification reaction types. From practical viewpoint, fundamentals experimental design, active species, performance evaluation external conditions, discussed detail easy experimentation. Furthermore, latest advances COFs, composites, comprehensively summarized according actual sites, together with discussion structure-property relationship. We believe that study will be helpful researchers novel reticular various synthetic applications.

Language: Английский

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Metal–Organic Framework‐Based Photocatalysis for Solar Fuel Production

Small Methods, Journal Year: 2022, Volume and Issue: 7(1)

Published: Dec. 1, 2022

Abstract Metal–organic frameworks (MOFs) represent a novel class of crystalline inorganic–organic hybrid materials with tunable semiconducting behavior. MOFs have potential for application in photocatalysis to produce sustainable solar fuels, owing their unique structural advantages (such as clarity and modifiability) that can facilitate deeper understanding the structure–activity relationship photocatalysis. This review takes photocatalytic active sites particular perspective, summarizing progress MOF‐based fuel production; mainly including three categories solar‐chemical conversions, water splitting hydrogen fuel, carbon dioxide reduction hydrocarbon nitrogen fixation high‐energy carriers such ammonia. focuses on types photocatalysts discusses enhanced activity based well‐defined structure MOFs, offering deep insights into

Language: Английский

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In-situ formation of Ag2O in metal-organic framework for light-driven upcycling of microplastics coupled with hydrogen production

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 319, P. 121940 - 121940

Published: Sept. 6, 2022

The release of microplastics (MPs) into the environment has engendered considerable ecosystem and human health concerns. Herein, we propose light-driven photocatalytic upcycling MPs using heterojunction photocatalysts. A novel synthesis method was developed through in-situ conversion unstable metal sites on bimetallic metal-organic frameworks (MOF), resulting in nanometer-sized particles with semiconductor properties which are confined framework MOFs to prevent agglomeration. These modified MOF can be used for along hydrogen (H2) production. As a proof concept, FeAg-MOF selected as precursor fabricate Ag2O/Fe-MOF Light illumination induced formation Ag2O particle size ∼6 nm structure. displays broad solar light-harvesting range exposed active sites. Furthermore, band-matching enable value-added chemicals, accompanied by H2 present work provides an insight designing advanced photocatalysts converting coupled clean energy

Language: Английский

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Switching Excited State Distribution of Metal–Organic Framework for Dramatically Boosting Photocatalysis

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(30)

Published: May 14, 2022

Photosensitization associated with electron/energy transfer represents the central science of natural photosynthesis. Herein, we proposed a protocol to dramatically improve sensitizing ability metal-organic frameworks (MOFs) by switching their excited state distribution from 3 MLCT (metal-to-ligand charge transfer) IL (intraligand). The hierarchical organization MOFs and Co/Cu catalysts facilitates electron for efficient photocatalytic H2 evolution yield 26 844.6 μmol g-1 CO2 photoreduction record HCOOH 4807.6 among all MOF photocatalysts. Systematic investigations demonstrate that strong visible-light-absorption, long-lived ingenious multi-component synergy in can facilitate both interface intra-framework boost photocatalysis. This work opens up an avenue solar-energy conversion engineering centers at molecular level.

Language: Английский

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Trace to the Source: Self‐Tuning of MOF Photocatalysts

Advanced Energy Materials, Journal Year: 2023, Volume and Issue: 13(23)

Published: April 23, 2023

Abstract Benefitting from ultra‐high porosity, large specific surface area (SSA), and rich active sites, metal–organic frameworks (MOFs) have emerged as a star material in energy environment related applications, especially photocatalysis. In comparison with conventional photocatalysts, MOFs can be customized terms of electronic structure, photo‐responsiveness, morphological dimensions by rational design, which means that eliminate the need for other species to achieve enhanced photocatalytic performance, such metals, compounds, polymers, may introduce extra costs, time‐consuming, multi‐phase, or an unclear mechanism. Most previous review works MOF photocatalysis mixed self‐tuning assisted‐tuning, often gives incomplete understanding. this work, self‐tunning analyzing component (as clusters, ligands, inclusions), defect (defect engineering, linkers, oxygen vacancies (OVs), crystal facets, dimensions, amorphization) is summarized. Then, outstanding examples these strategies applied water redox, CO 2 /N reduction, organic conversion, environmental treatment are discussed. Finally, opportunities challenges faced analyzed different perspectives. This paper comprehensive systematic on enhance activity.

Language: Английский

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Incorporating Catalytic Units into Nanomaterials: Rational Design of Multipurpose Catalysts for CO₂ Valorization

Accounts of Chemical Research, Journal Year: 2023, Volume and Issue: 56(16), P. 2225 - 2240

Published: Aug. 3, 2023

ConspectusCO2 conversion to valuable chemicals is effective at reducing CO2 emissions. We previously proposed valorization strategies and developed efficient catalysts address thermodynamic stability kinetic inertness issues related conversion. Earlier, we molecular capture reagents integrate conversion, i.e., in situ transformation. Based on the mechanistic understanding of capture, activation, transformation a level, set out develop heterogeneous by incorporating catalytic units into nanomaterials via immobilization active onto designing with intrinsic sites.In thermocatalytic carbonaceous metal-organic framework (MOF)-based were for nonreductive reductive Novel Cu- Zn-based MOFs carbon-supported Cu prepared successfully applied cycloaddition, carboxylation, carboxylative cyclization reactions CO2, generating cyclic carbonates, carboxyl acids, oxazolidinones as respective target products. Reductive especially functionalization promising strategy produce chemicals, alleviating chemical production that relies petrochemistry. explored hierarchical using organocatalysts regulate reduction triggering catalyst investigation. Introducing multiple sites opens possibilities novel strategies. realized an N-doped Zn complex MOF materials adsorbents catalysts. These nanomaterial-based feature high excellent efficiency act shape-selective some cases due their unique pore structure.Nanomaterial-based are also appealing candidates photocatalytic (PCO2RR) electrocatalytic (ECO2RR), so series hybrid photo-/electrocatalysts metal complexes different matrixes such porous organic polymers (POPs), layers (MOLs), micelles, conducting polymers. By introducing Re-bipyridine Fe-porphyrin POPs regulating structure polymer chain, increased PCO2RR. PCO2RR aqueous solution was Re-bipyridine-containing amphiphilic form micelles nanoreactors. MOLs two metallic centers, Ni-bipyridine site Ni-O node, improve synergistic effect these centers. Sulfylphenoxy-decorated cobalt phthalocyanine (CoPc) cross-linked polypyrrole used cathode, achieving diluted benefiting from adsorption capability polypyrrole. fabricated immobilized 4-(t-butyl)-phenoxy Bi-MOF cathodes promote paired electrolysis 5-hydroxymethylfurfural (HMF) obtained products 2,5-furandicarboxylic acid (FDCA) efficiently.

Language: Английский

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Substoichiometric covalent organic frameworks with uncondensed aldehyde for highly efficient hydrogen peroxide photosynthesis in pure water

Applied Catalysis B Environment and Energy, Journal Year: 2023, Volume and Issue: 331, P. 122691 - 122691

Published: March 25, 2023

Language: Английский

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