Photocatalytic Selective Oxidation of HMF Coupled with H2 Evolution on Flexible Ultrathin g-C3N4 Nanosheets with Enhanced N–H Interaction DOI
Xiaolei Bao, Mu Liu, Zeyan Wang

et al.

ACS Catalysis, Journal Year: 2022, Volume and Issue: 12(3), P. 1919 - 1929

Published: Jan. 20, 2022

Solar-driven catalytic oxidation of 5-hydroxymethylfurfural (HMF) into 2,5-diformylfuran (DFF) coupled with H2 evolution has been considered a promising approach. The exploration an active and stable photocatalyst still remains challenging work. Herein, we found that the flexible ultrathin graphitic carbon nitride (UCNT) could be ideal candidate. UCNT exhibits photocatalytic performance in selective HMF DFF activities 95.0 92.0 μmol g–1 h–1 under visible light irradiation. Importantly, also demonstrates high selectivity (95%) good cycling stability. activity may ascribed to strong specific interaction between UCNT. Solid-state nuclear magnetic resonance (NMR) density functional theory (DFT) results reveal twisted structure molecules form UCNT, reducing dehydrogenation energy barrier for oxidation. In addition, mechanistic studies •C6H4O3 is key radical intermediate during process by situ electron spin (ESR) trapping test. Our work clarifies complex biomass on catalyst surface provides views further development heterogeneous conversion.

Language: Английский

Perovskite Oxide Based Materials for Energy and Environment-Oriented Photocatalysis DOI
Ashish Kumar, Ajay Kumar, Venkata Krishnan

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 10(17), P. 10253 - 10315

Published: Aug. 27, 2020

The use of solar energy to catalyze the photo-driven processes has attracted tremendous attention from scientific community because its great potential address and environmental issues. In this regard, several attempts have been made by researchers design develop different materials with enhanced photocatalytic efficiencies. This Review comprehensively summarizes recent reports on perovskite oxide based photocatalysts for organic pollutant degradation, water splitting, carbon dioxide conversion, nitrogen fixation along basic understanding involved mechanisms, current trends advances in field. design, synthesis, development strategies discussed detail provide a comprehensive view materials' fabrication that influences their properties. Subsequently, insights materials, including simple oxides, mixed layered are provided above-mentioned applications detailed manner. Finally, summary perspective future research direction discussed. Based progress field, it is highly anticipated systems, comprising groundbreaking technologies large-scale realization these processes, can be established near environment-oriented challenges.

Language: Английский

Citations

524

Recent advances in application of graphitic carbon nitride-based catalysts for degrading organic contaminants in water through advanced oxidation processes beyond photocatalysis: A critical review DOI
Yang Yang, Xin Li, Chengyun Zhou

et al.

Water Research, Journal Year: 2020, Volume and Issue: 184, P. 116200 - 116200

Published: July 18, 2020

Language: Английский

Citations

461

Facile fabrication of TaON/Bi2MoO6 core–shell S-scheme heterojunction nanofibers for boosting visible-light catalytic levofloxacin degradation and Cr(VI) reduction DOI
Shijie Li, Chunchun Wang, Mingjie Cai

et al.

Chemical Engineering Journal, Journal Year: 2021, Volume and Issue: 428, P. 131158 - 131158

Published: July 7, 2021

Language: Английский

Citations

456

Ta3N5/CdS Core–Shell S-scheme Heterojunction Nanofibers for Efficient Photocatalytic Removal of Antibiotic Tetracycline and Cr(VI): Performance and Mechanism Insights DOI
Shijie Li, Mingjie Cai, Chunchun Wang

et al.

Advanced Fiber Materials, Journal Year: 2023, Volume and Issue: 5(3), P. 994 - 1007

Published: Feb. 16, 2023

Language: Английский

Citations

367

A metal-free photocatalyst for highly efficient hydrogen peroxide photoproduction in real seawater DOI Creative Commons

Qingyao Wu,

Jingjing Cao, Xiao Wang

et al.

Nature Communications, Journal Year: 2021, Volume and Issue: 12(1)

Published: Jan. 20, 2021

Abstract Artificial photosynthesis of H 2 O from and , as a spotless method, has aroused widespread interest. Up to date, most photocatalysts still suffer serious salt-deactivated effects with huge consumption photogenerated charges, which severely limit their wide application. Herein, by using phenolic condensation approach, carbon dots, organic dye molecule procyanidins 4-methoxybenzaldehyde are composed into metal-free photocatalyst for the photosynthetic production in seawater. This catalyst exhibits high photocatalytic ability produce yield 1776 μmol g −1 h ( λ ≥ 420 nm; 34.8 mW cm −2 ) real seawater, about 4.8 times higher than pure polymer. Combining in-situ photoelectrochemical transient photovoltage analysis, active site catalytic mechanism this composite seawater also clearly clarified. work opens up an avenue highly efficient practical, available photoproduction

Language: Английский

Citations

328

Embedding CdS@Au into Ultrathin Ti3–xC2Ty to Build Dual Schottky Barriers for Photocatalytic H2 Production DOI
Zhipeng Li, Weixin Huang, Jiaxing Liu

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(14), P. 8510 - 8520

Published: June 29, 2021

One of the research hotspots in solar energy conversion is developing photocatalysts for visible-light-driven H2 production. In this study, a ternary CdS@Au/MXene composite was elaborately constructed by facile situ self-assembly strategy, where ultrathin Ti3–xC2Ty nanosheets with characteristic Ti vacancies were employed as support core–shell structured CdS@Au nanojunctions. presence 1.0 wt % MXene, merely 0.1 Au helped composites achieve high H2-production rate 5371 μmol·g–1·h–1 under visible-light irradiation, more than 26.6 times higher that bare CdS. Such an enhancement predominantly attributed to "dual Schottky barriers" formed at interface CdS@Au/MXene, which evidenced systematic characterizations including X-ray photoelectron spectroscopy and Kelvin probe measurements, conjunction density functional theory (DFT) calculations. This work not only highlights significant role MXene reducing dosage noble metal cocatalysts photocatalysis, but also opens avenues fabricate MXene-based beyond.

Language: Английский

Citations

256

Vacancy Engineering in Semiconductor Photocatalysts: Implications in Hydrogen Evolution and Nitrogen Fixation Applications DOI
Ashish Kumar, Venkata Krishnan

Advanced Functional Materials, Journal Year: 2021, Volume and Issue: 31(28)

Published: April 25, 2021

Abstract It is a well‐known fact that the pronounced photogenerated charge recombination and poor light absorption are main bottlenecks of photocatalysis applications. The conventional approaches to address these problems involve bandgap engineering suppression after irradiation, which results in an enhancement photocatalytic performance materials. However, most essential aspect surface modification engineer active sites on catalyst generally not given much importance. Contrary this, defect another approach by optical, separation, properties materials can be tuned. In this review article, effect introduction vacancies selected semiconductor materials, viz., metal oxides, perovskite sulfides, oxyhalides, nitrides comprehensively summarized. only improves their optical transfer but also affects properties, helpful adsorption reactants surface. Herein, hydrogen evolution nitrogen fixation applications vacancy engineered discussed detail along with current trends, scalability requirements, rigorous experimental protocols.

Language: Английский

Citations

251

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

Enhanced Photocatalytic CO2 Reduction Activity over NH2-MIL-125(Ti) by Facet Regulation DOI
Xiaomei Cheng,

Xiao‐Yao Dao,

Shiqing Wang

et al.

ACS Catalysis, Journal Year: 2020, Volume and Issue: 11(2), P. 650 - 658

Published: Dec. 30, 2020

Designation and optimization of facets photocatalysts is an effective strategy to address the issue facet-dependent photocatalytic reactions. However, studies regarding facet effect metal–organic frameworks (MOFs) on process are in infancy. In this study, NH2-MIL-125(Ti) with different ratios {001} {111} was exactly controlled synthesized, it found that activity photoreduction CO2 enhanced gradually increasing exposed proportion facets. The exhibit maximal CO CH4 yields 8.25 1.01 μmol g–1 h–1, which 9 5 times higher than those facets, respectively. Also, give highest quantum 0.14 0.07% for production, Steady-state time-resolved fluorescence spectra reveal importance inhibiting recombination photoinduced electrons holes sample Besides, TiIII formed during reaction exhibits strong reducibility CO2. Starting from NH2-MIL-125(Ti), performance can be by regulating This work not only provides a further enhancing tuning active MOFs, but also deep understanding factors improving reduction

Language: Английский

Citations

243

Platinum Single Atoms Anchored on a Covalent Organic Framework: Boosting Active Sites for Photocatalytic Hydrogen Evolution DOI
Pengyu Dong, Yan Wang,

Aicaijun Zhang

et al.

ACS Catalysis, Journal Year: 2021, Volume and Issue: 11(21), P. 13266 - 13279

Published: Oct. 18, 2021

It is of great importance to explore and achieve a more effective approach toward the controllable synthesis single-atom-based photocatalysts with high metal content long-term durability. Herein, single-atom platinum (Pt) loading anchored on pore walls two-dimensional β-ketoenamine-linked covalent organic frameworks (TpPa-1-COF) presented. Aided by advanced characterization techniques aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (AC HAADF-STEM) X-ray absorption fine structure (XAFS) spectroscopy, it has been demonstrated that atomically dispersed Pt formed TpPa-1-COF support through six-coordinated C3N–Pt–Cl2 species. The optimized Pt1@TpPa-1 catalyst exhibits photocatalytic H2 evolution rate 719 μmol g–1 h–1 under visible-light irradiation, actual 0.72 wt %, large turnover frequency (TOF) 19.5 h–1, activity equivalent 3.9 48 times higher than those nanoparticles/TpPa-1 bare TpPa-1, respectively. improved performance for ascribed photogenerated charge separation migration well-dispersed active sites Pt. Moreover, density functional theory (DFT) calculations further reveal role single atoms in enhanced evolution. Overall, this work provides some inspiration designing outstanding stability efficiency using COFs as support.

Language: Английский

Citations

242