Three-Motif Molecular Junction Type Covalent Organic Frameworks for Efficient Photocatalytic Aerobic Oxidation DOI
Mingyi Yang, Shuai‐Bing Zhang, Mi Zhang

et al.

Journal of the American Chemical Society, Journal Year: 2024, Volume and Issue: 146(5), P. 3396 - 3404

Published: Jan. 24, 2024

Covalent organic frameworks (COFs), with the features of flexible structure regulation and easy introduction functional groups, have aroused broad interest in field photocatalysis. However, due to low light absorption intensity, photoelectron conversion efficiency, lack suitable active sites, it remains a great challenge achieve efficient photocatalytic aerobic oxidation reactions. Herein, based on reticular chemistry, we rationally designed series three-motif molecular junction type COFs, which formed dual photosensitizer coupled redox junctions containing multifunctional COF photocatalysts. Significantly, strong adsorption ability units integrated reduction features, PY-BT exhibited highest activity for oxidation. Especially, achieved benzylamine efficiency 99.9% 2.5 h, is much higher than that two-motif only one or unit lacking COFs. The mechanism selective was studied through comprehensive experiments density theory calculations. results showed photoinduced electron transfer occurred from PY then triphenylamine BT. Furthermore, thermodynamics energy lower others, confirmed synergistic effect This work provided new strategy design COFs also represented insight into catalytic

Language: Английский

Synergy of Pd atoms and oxygen vacancies on In2O3 for methane conversion under visible light DOI Creative Commons
Lei Luo, Lei Fu, Huifen Liu

et al.

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

Published: May 25, 2022

Methane (CH4) oxidation to high value chemicals under mild conditions through photocatalysis is a sustainable and appealing pathway, nevertheless confronting the critical issues regarding both conversion selectivity. Herein, visible irradiation (420 nm), synergy of palladium (Pd) atom cocatalyst oxygen vacancies (OVs) on In2O3 nanorods enables superior photocatalytic CH4 activation by O2. The optimized catalyst reaches ca. 100 μmol h-1 C1 oxygenates, with selectivity primary products (CH3OH CH3OOH) up 82.5%. Mechanism investigation elucidates that such induced dedicated function Pd single atoms boosting hole electron transfer, respectively. O2 proven be only source for CH3OH production, while H2O acts as promoter efficient ·OH production facilitates product desorption indicated DFT modeling. This work thus provides new understandings simultaneous regulation activity cocatalysts vacancies.

Language: Английский

Citations

213
Cocatalyst decorated ZnIn2S4 composites for cooperative alcohol conversion and H2 evolution DOI
Chang‐Long Tan, Ming–Yu Qi, Zi‐Rong Tang

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2021, Volume and Issue: 298, P. 120541 - 120541

Published: July 19, 2021

Language: Английский

Citations

185
Binary Au–Cu Reaction Sites Decorated ZnO for Selective Methane Oxidation to C1 Oxygenates with Nearly 100% Selectivity at Room Temperature DOI
Lei Luo,

Zhuyu Gong,

Youxun Xu

et al.

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 144(2), P. 740 - 750

Published: Dec. 20, 2021

Direct and efficient oxidation of methane to methanol the related liquid oxygenates provides a promising pathway for sustainable chemical industry, while still remaining an ongoing challenge owing dilemma between activation overoxidation. Here, ZnO with highly dispersed dual Au Cu species as cocatalysts enables selective photocatalytic conversion one-carbon (C1) using O2 oxidant operated at ambient temperature. The optimized AuCu-ZnO photocatalyst achieves up 11225 μmol·g-1·h-1 primary products (CH3OH CH3OOH) HCHO nearly 100% selectivity, resulting in 14.1% apparent quantum yield 365 nm, much higher than previous best photocatalysts reported oxygenates. In situ EPR XPS disclose that serve photoinduced electron mediators promote •OOH, simultaneously is hole acceptor enhance H2O •OH, thus synergistically promoting charge separation transformation. This work highlights significances co-modification suitable on simultaneous regulation activity selectivity.

Language: Английский

Citations

176
POM-incorporated ZnIn2S4 Z-scheme dual-functional photocatalysts for cooperative benzyl alcohol oxidation and H2 evolution in aqueous solution DOI

Fangshu Xing,

Renyou Zeng,

Chuchu Cheng

et al.

Applied Catalysis B Environment and Energy, Journal Year: 2022, Volume and Issue: 306, P. 121087 - 121087

Published: Jan. 7, 2022

Language: Английский

Citations

154
Carbon nitride based materials: more than just a support for single-atom catalysis DOI
Guilherme F. S. R. Rocha, Marcos A. R. da Silva, Andrea Rogolino

et al.

Chemical Society Reviews, Journal Year: 2023, Volume and Issue: 52(15), P. 4878 - 4932

Published: Jan. 1, 2023

Recently, the missing link between homogeneous and heterogeneous catalysis has been found it was named single-atom (SAC). However, SAC field still faces important challenges, one of which is controlling bonding/coordination single atoms support in order to compensate for increase surface energy when particle size reduced due atomic dispersion. Excellent candidates meet this requirement are carbon nitride (CN)-based materials. Metal can be firmly trapped nitrogen-rich coordination sites CN materials, makes them a unique class hosts preparing catalysts (SACs). As most promising two-dimensional supports stabilize isolated metal atoms, materials have increasingly employed SACs. Herein, we will cover recent advances single-atoms supported by In review, characterization techniques challenges faced topic discussed, commonly synthetic methods delineated different Finally, catalytic performance SACs based on nitrides reviewed with special focus their photocatalytic applications. particular, prove as non-innocent support. The relationship two-way, where change electronic properties support, while features matrix tune activity reactions. highlight frontiers field, including analytical method development, truly controlled methods, allowing fine control loading multi-element synthesis, how understanding two-way exchange behind push next level.

Language: Английский

Citations

145
Atomic‐Layered Cu5 Nanoclusters on FeS2 with Dual Catalytic Sites for Efficient and Selective H2O2 Activation DOI

Cancan Ling,

Xiufan Liu, Hao Li

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(21)

Published: March 3, 2022

Regulating the distribution of reactive oxygen species generated from H2 O2 activation is prerequisite to ensuring efficient and safe use in chemistry life science fields. Herein, we demonstrate that constructing a dual Cu-Fe site through self-assembly single-atomic-layered Cu5 nanoclusters onto FeS2 surface achieves selective with high efficiency. Unlike its unitary Cu or Fe counterpart, sites residing at perimeter zone /FeS2 interface facilitate adsorption barrierless decomposition into ⋅OH via forming bridging Cu-O-O-Fe complex. The robust situ formation governed by this atomic-layered catalyst enables effective oxidation several refractory toxic pollutants across broad pH range, including alachlor, sulfadimidine, p-nitrobenzoic acid, p-chlorophenol, p-chloronitrobenzene. This work highlights concept building catalytic manipulating on molecular level towards environmental control beyond.

Language: Английский

Citations

143
Recent advances in Metal-Organic Frameworks-based materials for photocatalytic selective oxidation DOI

Guilong Lu,

Feng Chu,

Xiubing Huang

et al.

Coordination Chemistry Reviews, Journal Year: 2021, Volume and Issue: 450, P. 214240 - 214240

Published: Oct. 13, 2021

Language: Английский

Citations

139
Photoreforming of Waste Polymers for Sustainable Hydrogen Fuel and Chemicals Feedstock: Waste to Energy DOI
Muhammad Ashraf, Nisar Ullah, Ibrahim Khan

et al.

Chemical Reviews, Journal Year: 2023, Volume and Issue: 123(8), P. 4443 - 4509

Published: April 17, 2023

Energy from renewable resources is central to environmental sustainability. Among the renewables, sunlight-driven fuel synthesis a sustainable and economical approach produce vectors such as hydrogen through water splitting. The photocatalytic splitting limited by oxidation half-reaction, which kinetically energetically demanding entails designer photocatalysts. Such challenges can be addressed employing alternative half-reactions. Photoreforming drive breakdown of waste plastics biomass into valuable organic products for production H2. We provide an overview photoreforming its underlying mechanisms that convert polymers H2 fuels fine chemicals. This paramount importance two complementary perspectives: (i) green energy harvesting (ii) sustainability decomposing valuables. Competitive results generation without hazards are being generated. process, mechanisms, critical assessment field scarce. address points focusing on concept up-to-date knowledge with key milestones achieved, uncovering concepts in photoreforming, (iii) design photocatalysts pathways use different polymer wastes substrates.

Language: Английский

Citations

124
A review on photo-, electro- and photoelectro- catalytic strategies for selective oxidation of alcohols DOI

Duoyue Tang,

Guilong Lu,

Zewen Shen

et al.

Journal of Energy Chemistry, Journal Year: 2022, Volume and Issue: 77, P. 80 - 118

Published: Nov. 1, 2022

Language: Английский

Citations

122
Chemically Bonded α‐Fe2O3/Bi4MO8Cl Dot‐on‐Plate Z‐Scheme Junction with Strong Internal Electric Field for Selective Photo‐oxidation of Aromatic Alcohols DOI
Zijian Zhu, Hongwei Huang,

Lizhen Liu

et al.

Angewandte Chemie International Edition, Journal Year: 2022, Volume and Issue: 61(26)

Published: April 5, 2022

Inferior contact interface and low charge transfer efficiency seriously restrict the performance of heterojunctions. Herein, chemically bonded α-Fe2 O3 /Bi4 MO8 Cl (M=Nb, Ta) dot-on-plate Z-scheme junctions with strong internal electric field are crafted by an in situ growth route. Experimental theoretical results demonstrate that provides a powerful driving force for vectorial migration photocharges between Bi4 , interfacial Fe-O bond not only serves as atomic-level flow highway but also lowers energy barrier, thereby accelerating realizing effective spatial separation. Impressively, manifests significantly improved photocatalytic activity selective oxidation aromatic alcohols into aldehydes (Con. ≥92 %, Sel. ≥96 %), improvement one to two orders magnitude. This work presents insight steering.

Language: Английский

Citations

112