Tracking Charge Transfer to Residual Metal Clusters in Conjugated Polymers for Photocatalytic Hydrogen Evolution DOI Creative Commons
Michael Sachs, Hyojung Cha, Ján Koščo

et al.

Journal of the American Chemical Society, Journal Year: 2020, Volume and Issue: 142(34), P. 14574 - 14587

Published: July 28, 2020

Semiconducting polymers are versatile materials for solar energy conversion and have gained popularity as photocatalysts sunlight-driven hydrogen production. Organic often contain residual metal impurities such palladium (Pd) clusters that formed during the polymerization reaction, there is increasing evidence a catalytic role of in polymer photocatalysts. Using transient operando optical spectroscopy on nanoparticles F8BT, P3HT, dibenzo[b,d]thiophene sulfone homopolymer P10, we demonstrate how differences time scale electron transfer to Pd translate into evolution activity optima at different concentrations. For F8BT with common concentrations >1000 ppm (>0.1 wt %), find quench photogenerated excitons via femto-nanosecond scale, thus outcompeting reductive quenching. We spectroscopically identify reduced our from microsecond onward show predominant location long-lived electrons gradually shifts when content lowered. While low yield limits P10 exhibits substantially higher activity, which results yields due more efficient Surprisingly, despite performance reside rather than particles, even very high 27000 (2.7 %). In contrast, already before typical evolution. This comparison shows quenching but slow clusters, whereas opposite case F8BT. These findings suggest development must target combine both rapid charge metal-based cocatalyst.

Language: Английский

Polymer photocatalysts for solar-to-chemical energy conversion DOI
Tanmay Banerjee, Filip Podjaski, Julia Kröger

et al.

Nature Reviews Materials, Journal Year: 2020, Volume and Issue: 6(2), P. 168 - 190

Published: Nov. 5, 2020

Language: Английский

Citations

556

Design, Fabrication, and Mechanism of Nitrogen‐Doped Graphene‐Based Photocatalyst DOI
Chuanbiao Bie, Huogen Yu, Bei Cheng

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 33(9)

Published: Jan. 18, 2021

Solving energy and environmental problems through solar-driven photocatalysis is an attractive challenging topic. Hence, various types of photocatalysts have been developed successively to address the demands photocatalysis. Graphene-based materials elicited considerable attention since discovery graphene. As a derivative graphene, nitrogen-doped graphene (NG) particularly stands out. Nitrogen atoms can break undifferentiated structure open bandgap while endowing with uneven electron density distribution. Therefore, NG retains nearly all advantages original equipped several novel properties, ensuring infinite possibilities for NG-based This review introduces atomic band structures NG, summarizes in situ ex synthesis methods, highlights mechanism photocatalysis, outlines its applications different directions (primarily hydrogen production, CO2 reduction, pollutant degradation, as photoactive ingredient). Lastly, central challenges possible improvements future are presented. study expected learn from past achieve progress toward

Language: Английский

Citations

442

Updates on the Roadmap for Photocatalysis DOI Creative Commons
Michele Melchionna, Paolo Fornasiero

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(10), P. 5493 - 5501

Published: April 14, 2020

ADVERTISEMENT RETURN TO ISSUEPREVViewpointNEXTUpdates on the Roadmap for PhotocatalysisMichele MelchionnaMichele MelchionnaChemistry Department, INSTM and ICCOM-CNR Trieste Research Unit, University of Trieste, Via L. Giorgieri 1, 34127, ItalyMore by Michele Melchionnahttp://orcid.org/0000-0001-9813-9753 Paolo Fornasiero*Paolo FornasieroChemistry Italy*Email P.F.: [email protected]More Fornasierohttp://orcid.org/0000-0003-1082-9157Cite this: ACS Catal. 2020, 10, 5493–5501Publication Date (Web):April 14, 2020Publication History Received13 March 2020Published online14 April inissue 15 May 2020https://doi.org/10.1021/acscatal.0c01204Copyright © 2020 American Chemical SocietyRIGHTS & PERMISSIONSACS AuthorChoiceCC: Creative CommonsBY: Credit must be given to creatorArticle Views16419Altmetric-Citations196LEARN ABOUT THESE METRICSArticle Views are COUNTER-compliant sum full text article downloads since November 2008 (both PDF HTML) across all institutions individuals. These metrics regularly updated reflect usage leading up last few days.Citations number other articles citing this article, calculated Crossref daily. Find more information about citation counts.The Altmetric Attention Score is a quantitative measure attention that research has received online. Clicking donut icon will load page at altmetric.com with additional details score social media presence article. how calculated. Share Add toView InAdd Full Text ReferenceAdd Description ExportRISCitationCitation abstractCitation referencesMore Options onFacebookTwitterWechatLinked InReddit (4 MB) Get e-AlertsSUBJECTS:Catalysts,Materials,Metals,Photocatalysis,Photocatalysts e-Alerts

Language: Английский

Citations

393

Protonated Imine‐Linked Covalent Organic Frameworks for Photocatalytic Hydrogen Evolution DOI Creative Commons
Jin Yang, Amitava Acharjya,

Mengyang Ye

et al.

Angewandte Chemie International Edition, Journal Year: 2021, Volume and Issue: 60(36), P. 19797 - 19803

Published: May 27, 2021

Abstract Covalent organic frameworks (COFs) have emerged as an important class of semiconductors and photocatalysts for the hydrogen evolution reaction (HER)from water. To optimize their photocatalytic activity, typically moieties constituting are considered most suitable combinations them searched for. However, effect covalent linkage between these on performance has rarely been studied. Herein, we demonstrate that donor‐acceptor (D‐A) type imine‐linked COFs can produce with a rate high 20.7 mmol g −1 h under visible light irradiation, upon protonation imine linkages. A significant red‐shift in absorbance, largely improved charge separation efficiency, increase hydrophilicity triggered by Schiff‐base COFs, responsible performance.

Language: Английский

Citations

285

Generation of long-lived charges in organic semiconductor heterojunction nanoparticles for efficient photocatalytic hydrogen evolution DOI
Ján Koščo, Soranyel González‐Carrero, Calvyn T. Howells

et al.

Nature Energy, Journal Year: 2022, Volume and Issue: 7(4), P. 340 - 351

Published: March 14, 2022

Language: Английский

Citations

285

Emerging applications of porous organic polymers in visible-light photocatalysis DOI
Tianxiong Wang, Hai‐Peng Liang, Dejene Assefa Anito

et al.

Journal of Materials Chemistry A, Journal Year: 2020, Volume and Issue: 8(15), P. 7003 - 7034

Published: Jan. 1, 2020

Porous organic polymers are efficient photocatalysts in synthesis, hydrogen evolution, CO2 reduction, and degradation of pollutants.

Language: Английский

Citations

264

Rational Design of Covalent Heptazine Frameworks with Spatially Separated Redox Centers for High‐Efficiency Photocatalytic Hydrogen Peroxide Production DOI
Hao Cheng, Haifeng Lv, Jun Cheng

et al.

Advanced Materials, Journal Year: 2021, Volume and Issue: 34(7)

Published: Nov. 24, 2021

The redox reaction centers in natural organisms conducting oxygenic photosynthesis are well arranged a physically separated manner to convert sunlight into chemical energy efficiently. Mimicking via precisely constructing oxidative and reductive within photocatalysts is ideal for enhancing catalytic performances artificial photosynthesis. In this study, new covalent heptazine frameworks (CHFs) with spatially rationally designed photocatalytic production of H2 O2 from water oxygen without using any sacrificial agents. Both experimental computational investigations indicate that the two-electron reduction occurs on moiety, whereas oxidation acetylene or diacetylene bond CHFs. This unique spatial separation feature critical charge achieving efficient production. Meanwhile, measured exciton binding diacetylene-containing polymer merely 24 meV. Under simulated solar irradiation, CHFs can achieve solar-to-chemical conversion efficiency 0.78%, surpassing previously reported materials. study establishes molecular engineering approach construct periodically single-component photocatalysts, representing hallmark create more exciting structures photocatalysis moving forward.

Language: Английский

Citations

257

Porous organic polymers for light-driven organic transformations DOI
Zhenwei Zhang,

Ji Jia,

Yongfeng Zhi

et al.

Chemical Society Reviews, Journal Year: 2022, Volume and Issue: 51(7), P. 2444 - 2490

Published: Jan. 1, 2022

As a new generation of porous materials, organic polymers (POPs), have recently emerged as powerful platform heterogeneous photocatalysis. POPs are constructed using extensive synthesis methodologies, with various functional units being connected via high-energy covalent bonds. This review systematically presents the recent advances in for visible-light driven transformations. Herein, we firstly summarize common construction strategies POP-based photocatalysts based on two major approaches: pre-design and post-modification; secondly, categorize methods reaction types constructing POPs. We then classify introduce specific reactions current light-driven POP-mediated Finally, outline state development problems faced transformations by POPs, present some perspectives to motivate reader explore solutions these confront challenges process.

Language: Английский

Citations

252

Metal-Free Catalysis: A Redox-Active Donor–Acceptor Conjugated Microporous Polymer for Selective Visible-Light-Driven CO2 Reduction to CH4 DOI
Soumitra Barman, Ashish Singh, Faruk Ahamed Rahimi

et al.

Journal of the American Chemical Society, Journal Year: 2021, Volume and Issue: 143(39), P. 16284 - 16292

Published: Sept. 21, 2021

Achieving more than a two-electron photochemical CO2 reduction process using metal-free system is quite exciting and challenging, as it needs proper channeling of electrons. In the present study, we report rational design synthesis redox-active conjugated microporous polymer (CMP), TPA-PQ, by assimilating an electron donor, tris(4-ethynylphenyl)amine (TPA), with acceptor, phenanthraquinone (PQ). The TPA-PQ shows intramolecular charge-transfer (ICT)-assisted catalytic activity for visible-light-driven photoreduction to CH4 (yield = 32.2 mmol g–1) impressive rate (2.15 h–1 high selectivity (>97%). Mechanistic analysis based on experimental results, in situ DRIFTS, computational studies reveals that potential catalyzing was energetically driven photoactivated ICT upon surface adsorption CO2, wherein adjacent keto groups PQ unit play pivotal role. critical role stimulating photocatalysis further illustrated synthesizing another CMP (TEB-PQ), bearing triethynylbenzene (TEB) PQ, 8-fold lesser toward 4.4 compared TPA-PQ. results demonstrate novel concept efficient, sustainable, recyclable robust organic photocatalyst.

Language: Английский

Citations

250

How to Build a Microplastics‐Free Environment: Strategies for Microplastics Degradation and Plastics Recycling DOI Creative Commons
Junliang Chen, Jing Wu, Peter C. Sherrell

et al.

Advanced Science, Journal Year: 2022, Volume and Issue: 9(6)

Published: Jan. 6, 2022

Microplastics are an emergent yet critical issue for the environment because of high degradation resistance and bioaccumulation. Unfortunately, current technologies to remove, recycle, or degrade microplastics insufficient complete elimination. In addition, fragmentation mismanaged plastic wastes in have recently been identified as a significant source microplastics. Thus, developments effective removal methods, well as, plastics recycling strategies crucial build microplastics-free environment. Herein, this review comprehensively summarizes eliminating from highlights two key aspects achieve goal: 1) Catalytic into environmentally friendly organics (carbon dioxide water); 2) catalytic upcycling monomers, fuels, valorized chemicals. The mechanisms, catalysts, feasibility, challenges these methods also discussed. Novel such photocatalysis, advanced oxidation process, biotechnology promising eco-friendly candidates transform benign valuable products. future, more effort is encouraged develop conversion products with efficiency, product selectivity, low cost under mild conditions.

Language: Английский

Citations

247