Search Menu
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information
Search Scholarly Publications

Title: Photocatalytic degradation of organic pollutants coupled with simultaneous photocatalytic H2 evolution over graphene quantum dots/Mn-N-TiO2/g-C3N4 composite catalysts: Performance and mechanism

Abstract

Graphene quantum dots/Mn-N-TiO2/g-C3N4 (GQDs/TCN) composite photocatalysts have been designed, synthesized and characterized by XRD, SEM, TEM, Raman, BET, and XPS. The photodegradation of organic pollutants (p-nitrophenol, diethyl phthalate and ciprofloxacin, called as 4-NP, CIP and DEP, respectively) coupled with simultaneous photocatalytic production of hydrogen was successfully achieved using the GQDs/TCN catalysts. The 5%GQDs/TCN-0.4 sample shows the best photocatalytic hydrogen production and organic pollutant degradation rate under simulated solar irradiation in the simultaneous photocatalytic oxidation and reduction system. Furthermore, the photocatalytic H2 evolution rates in the solution of 4-NP, CIP and DEP are all larger than that in pure water system over the 5%GQDs/TCN-0.4 catalyst. And the H2 evolution rate in the solution of 4-NP is smaller than that in the solutions of CIP and DEP. Accordingly, the photodegradation rate of 4-NP is larger than that of CIP and DEP. The analyses of density functional theory and liquid chromatography mass spectrometry indicate that some photogenerated electrons were used in the photodegradation process of 4-NP but not in that of CIP and DEP. And it leads to the photocatalytic rate of H2 evolution in the 4-NP solution smaller than that in the solution of CIP and DEP. For the first time, themore » present work illuminates the photocatalytic enhancement of the GQDs/TCN-0.4 catalyst and the mechanism of the effect of different organic pollutants on photocatalytic H2 evolution.« less

Authors:
 [1];  [1];  [1];  [1];  [2];  [2];  [1];  [1];  [3];  [4]
+ Show Author Affiliations
  1. Nanchang Hangkong Univ., Nanchang (China). Key Lab. of Jiangxi Province for Persistent Pollutants Control and Resources Recycle
  2. Xiangtan Univ. (China). Key Lab. of Environmentally Friendly Chemistry and Applications of Ministry of Education
  3. East China Univ. of Science and Technology, Shanghai (China). School of Chemistry & Molecular Engineering
  4. Univ. of Connecticut, Storrs, CT (United States)
Publication Date:
Research Org.:
Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
OSTI Identifier:
1597843
Grant/Contract Number:  
FG02-86ER-13622
Resource Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 227; Journal Issue: C; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 54 ENVIRONMENTAL SCIENCES; Degradation; Graphitic carbon nitride; Hydrogen evolution; Organic pollutants; Photocatalysis

Citation Formats

Nie, Yu-Chun, Yu, Fan, Wang, Lai-Chun, Xing, Qiu-Ju, Liu, Xia, Pei, Yong, Zou, Jian-Ping, Dai, Wei-Li, Li, Yan, and Suib, Steven L. Photocatalytic degradation of organic pollutants coupled with simultaneous photocatalytic H2 evolution over graphene quantum dots/Mn-N-TiO2/g-C3N4 composite catalysts: Performance and mechanism. United States: N. p., 2018. Web. doi:10.1016/j.apcatb.2018.01.033.
Copy to clipboard
Nie, Yu-Chun, Yu, Fan, Wang, Lai-Chun, Xing, Qiu-Ju, Liu, Xia, Pei, Yong, Zou, Jian-Ping, Dai, Wei-Li, Li, Yan, & Suib, Steven L. Photocatalytic degradation of organic pollutants coupled with simultaneous photocatalytic H2 evolution over graphene quantum dots/Mn-N-TiO2/g-C3N4 composite catalysts: Performance and mechanism. United States. https://doi.org/10.1016/j.apcatb.2018.01.033
Copy to clipboard
Nie, Yu-Chun, Yu, Fan, Wang, Lai-Chun, Xing, Qiu-Ju, Liu, Xia, Pei, Yong, Zou, Jian-Ping, Dai, Wei-Li, Li, Yan, and Suib, Steven L. Sun . "Photocatalytic degradation of organic pollutants coupled with simultaneous photocatalytic H2 evolution over graphene quantum dots/Mn-N-TiO2/g-C3N4 composite catalysts: Performance and mechanism". United States. https://doi.org/10.1016/j.apcatb.2018.01.033. https://www.osti.gov/servlets/purl/1597843.
Copy to clipboard
@article{osti_1597843,
title = {Photocatalytic degradation of organic pollutants coupled with simultaneous photocatalytic H2 evolution over graphene quantum dots/Mn-N-TiO2/g-C3N4 composite catalysts: Performance and mechanism},
author = {Nie, Yu-Chun and Yu, Fan and Wang, Lai-Chun and Xing, Qiu-Ju and Liu, Xia and Pei, Yong and Zou, Jian-Ping and Dai, Wei-Li and Li, Yan and Suib, Steven L.},
abstractNote = {Graphene quantum dots/Mn-N-TiO2/g-C3N4 (GQDs/TCN) composite photocatalysts have been designed, synthesized and characterized by XRD, SEM, TEM, Raman, BET, and XPS. The photodegradation of organic pollutants (p-nitrophenol, diethyl phthalate and ciprofloxacin, called as 4-NP, CIP and DEP, respectively) coupled with simultaneous photocatalytic production of hydrogen was successfully achieved using the GQDs/TCN catalysts. The 5%GQDs/TCN-0.4 sample shows the best photocatalytic hydrogen production and organic pollutant degradation rate under simulated solar irradiation in the simultaneous photocatalytic oxidation and reduction system. Furthermore, the photocatalytic H2 evolution rates in the solution of 4-NP, CIP and DEP are all larger than that in pure water system over the 5%GQDs/TCN-0.4 catalyst. And the H2 evolution rate in the solution of 4-NP is smaller than that in the solutions of CIP and DEP. Accordingly, the photodegradation rate of 4-NP is larger than that of CIP and DEP. The analyses of density functional theory and liquid chromatography mass spectrometry indicate that some photogenerated electrons were used in the photodegradation process of 4-NP but not in that of CIP and DEP. And it leads to the photocatalytic rate of H2 evolution in the 4-NP solution smaller than that in the solution of CIP and DEP. For the first time, the present work illuminates the photocatalytic enhancement of the GQDs/TCN-0.4 catalyst and the mechanism of the effect of different organic pollutants on photocatalytic H2 evolution.},
doi = {10.1016/j.apcatb.2018.01.033},
journal = {Applied Catalysis. B, Environmental},
number = C,
volume = 227,
place = {United States},
year = {Sun Jul 01 00:00:00 EDT 2018},
month = {Sun Jul 01 00:00:00 EDT 2018}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1016/j.apcatb.2018.01.033
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 186 works
Citation information provided by
Web of Science
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Acute and chronic toxicity of veterinary antibiotics to Daphnia magna
journal, April 2000

Environmental pollution by antibiotics and by antibiotic resistance determinants
journal, November 2009

CdSe QDs@UIO-66 composite with enhanced photocatalytic activity towards RhB degradation under visible-light irradiation
journal, January 2016

  • Gan, Haijun; Wang, Zhen; Li, Huimin
  • RSC Advances, Vol. 6, Issue 7
  • DOI: 10.1039/C5RA23565K

CdS/Pt photocatalytic activity boosted by high-energetic photons based on efficient triplet–triplet annihilation upconversion
journal, November 2017

Pesticides: Seeking answers amid a toxic debate
journal, May 2015

Electrochemically enhanced removal of perfluorinated compounds (PFCs) from aqueous solution by CNTs-graphene composite electrode
journal, November 2017

Advanced Nanoarchitectures for Solar Photocatalytic Applications
journal, November 2011

  • Kubacka, Anna; Fernández-García, Marcos; Colón, Gerardo
  • Chemical Reviews, Vol. 112, Issue 3
  • DOI: 10.1021/cr100454n

Semiconductor-based Photocatalytic Hydrogen Generation
journal, November 2010

  • Chen, Xiaobo; Shen, Shaohua; Guo, Liejin
  • Chemical Reviews, Vol. 110, Issue 11
  • DOI: 10.1021/cr1001645

Waltzing with the Versatile Platform of Graphene to Synthesize Composite Photocatalysts
journal, August 2015

Titanium Dioxide-Based Nanomaterials for Photocatalytic Fuel Generations
journal, May 2014

  • Ma, Yi; Wang, Xiuli; Jia, Yushuai
  • Chemical Reviews, Vol. 114, Issue 19
  • DOI: 10.1021/cr500008u

Synthesis of Cu 2 O Nanotubes with Efficient Photocatalytic Activity by Electrochemical Corrosion Method
journal, September 2015

  • Wang, Qi; Jia, Yanlin; Wang, Mingpu
  • The Journal of Physical Chemistry C, Vol. 119, Issue 38
  • DOI: 10.1021/acs.jpcc.5b06213

Ordered Mesoporous Black TiO 2 as Highly Efficient Hydrogen Evolution Photocatalyst
journal, June 2014

  • Zhou, Wei; Li, Wei; Wang, Jian-Qiang
  • Journal of the American Chemical Society, Vol. 136, Issue 26
  • DOI: 10.1021/ja504802q

Visible-Light Photocatalysis in Nitrogen-Doped Titanium Oxides
journal, July 2001

The Role of Metal Ion Dopants in Quantum-Sized TiO 2 : Correlation between Photoreactivity and Charge Carrier Recombination Dynamics
journal, December 1994

  • Choi, Wonyong; Termin, Andreas; Hoffmann, Michael R.
  • The Journal of Physical Chemistry, Vol. 98, Issue 51
  • DOI: 10.1021/j100102a038

TiO2-assisted photocatalytic degradation of azo dyes in aqueous solution: kinetic and mechanistic investigations
journal, April 2004

  • Konstantinou, Ioannis K.; Albanis, Triantafyllos A.
  • Applied Catalysis B: Environmental, Vol. 49, Issue 1
  • DOI: 10.1016/j.apcatb.2003.11.010

Heterogeneous photocatalytic degradation of organic contaminants over titanium dioxide: A review of fundamentals, progress and problems
journal, March 2008

Facile in-situ design strategy to disperse TiO2 nanoparticles on graphene for the enhanced photocatalytic degradation of rhodamine 6G
journal, December 2017

Synergistic Effects of Sm and C Co-Doped Mixed Phase Crystalline TiO2 for Visible Light Photocatalytic Activity
journal, February 2017

  • Peng, Fuchang; Gao, Honglin; Zhang, Genlin
  • Materials, Vol. 10, Issue 2
  • DOI: 10.3390/ma10020209

Enhanced Photoactivity of V−N Codoped TiO 2 Derived from a Two-Step Hydrothermal Procedure for the Degradation of PCP−Na under Visible Light Irradiation
journal, February 2011

  • Liu, Jinwen; Han, Rong; Zhao, Yan
  • The Journal of Physical Chemistry C, Vol. 115, Issue 11
  • DOI: 10.1021/jp110814b

Enhanced photocatalytic degradation of dye under visible light on mesoporous microspheres by defects in manganese- and nitrogen-co-doped TiO2
journal, September 2016

One-Step “Green” Synthetic Approach for Mesoporous C-Doped Titanium Dioxide with Efficient Visible Light Photocatalytic Activity
journal, August 2009

  • Dong, Fan; Wang, Haiqiang; Wu, Zhongbiao
  • The Journal of Physical Chemistry C, Vol. 113, Issue 38
  • DOI: 10.1021/jp9049654

Kinetics of ethyl paraben degradation by simulated solar radiation in the presence of N-doped TiO 2 catalysts
journal, September 2015

Synthesis and characterization of N-doped TiO2 photocatalysts with tunable response to solar radiation
journal, June 2014

Effect of ceria doping on SO2 resistance of Mn/TiO2 for selective catalytic reduction of NO with NH3 at low temperature
journal, February 2009

A metal-free polymeric photocatalyst for hydrogen production from water under visible light
journal, November 2008

  • Wang, Xinchen; Maeda, Kazuhiko; Thomas, Arne
  • Nature Materials, Vol. 8, Issue 1
  • DOI: 10.1038/nmat2317

Overall water splitting by Pt/g-C 3 N 4 photocatalysts without using sacrificial agents
journal, January 2016

  • Zhang, Guigang; Lan, Zhi-An; Lin, Lihua
  • Chemical Science, Vol. 7, Issue 5
  • DOI: 10.1039/C5SC04572J

Role of Frontier Orbitals in Chemical Reactions
journal, November 1982

Sonolytic degradation of dimethoate: Kinetics, mechanisms and toxic intermediates controlling
journal, November 2011

Enhancing the H2 evolution from water–methanol solution using Mn2+–Mn+3–Mn4+ redox species of Mn-doped TiO2 sol–gel photocatalysts
journal, May 2016

  • Pérez-Larios, Alejandro; Hernández-Gordillo, Agileo; Morales-Mendoza, Getsemani
  • Catalysis Today, Vol. 266
  • DOI: 10.1016/j.cattod.2015.12.029

Crystalline Mixed Phase (Anatase/Rutile) Mesoporous Titanium Dioxides for Visible Light Photocatalytic Activity
journal, December 2014

  • Luo, Zhu; Poyraz, Altug S.; Kuo, Chung-Hao
  • Chemistry of Materials, Vol. 27, Issue 1
  • DOI: 10.1021/cm5035112

Photoelectrocatalytic degradation of phenol-containing wastewater by TiO2/g-C3N4 hybrid heterostructure thin film
journal, February 2017

Graphene quantum dots: emergent nanolights for bioimaging, sensors, catalysis and photovoltaic devices
journal, January 2012

  • Shen, Jianhua; Zhu, Yihua; Yang, Xiaoling
  • Chemical Communications, Vol. 48, Issue 31
  • DOI: 10.1039/c2cc00110a

Macroscopic 3D Porous Graphitic Carbon Nitride Monolith for Enhanced Photocatalytic Hydrogen Evolution
journal, July 2015

Graphene Quantum Dots Derived from Carbon Fibers
journal, January 2012

  • Peng, Juan; Gao, Wei; Gupta, Bipin Kumar
  • Nano Letters, Vol. 12, Issue 2
  • DOI: 10.1021/nl2038979

Characterization and photocatalytic mechanism of nanosized CdS coupled TiO2 nanocrystals under visible light irradiation
journal, February 2006

Heterogeneous photocatalytic degradation of nitrophenols
journal, February 2003

  • Di Paola, A.; Augugliaro, V.; Palmisano, L.
  • Journal of Photochemistry and Photobiology A: Chemistry, Vol. 155, Issue 1-3
  • DOI: 10.1016/S1010-6030(02)00390-8

An improved UV/Fe3+ process by combination with electrocatalysis for p-nitrophenol degradation
journal, May 2006

Determination of phthalates in fruit jellies by dispersive SPE coupled with HPLC-MS: Sample Preparation
journal, December 2009

  • Ma, Yuwei; Hashi, Yuki; Ji, Feng
  • Journal of Separation Science, Vol. 33, Issue 2
  • DOI: 10.1002/jssc.200900557

Photocatalytic degradation of dimethyl phthalate in an aqueous solution with Pt-doped TiO2-coated magnetic PMMA microspheres
journal, December 2009

Titanium dioxide mediated photocatalytic degradation of dibutyl phthalate in aqueous solution—kinetics, mineralization and reaction mechanism
journal, December 2006

  • Kaneco, Satoshi; Katsumata, Hideyuki; Suzuki, Tohru
  • Chemical Engineering Journal, Vol. 125, Issue 1
  • DOI: 10.1016/j.cej.2006.08.004
    Sort by:
    [ × clear filter / sort ]

    Works referencing / citing this record:

    The fabrication of a biomass carbon quantum dot-Bi 2 WO 6 hybrid photocatalyst with high performance for antibiotic degradation
    journal, January 2019

    • Tang, Xu; Yu, Yang; Ma, Changchang
    • New Journal of Chemistry, Vol. 43, Issue 47
    • DOI: 10.1039/c9nj04764f

    Highly Efficient Photo-Reduction of p -Nitrophenol by Protonated Graphitic Carbon Nitride Nanosheets
    journal, September 2018

    The Role of Surface Texture on the Photocatalytic H2 Production on TiO2
    journal, January 2019

    • Pellegrino, Francesco; Sordello, Fabrizio; Minella, Marco
    • Catalysts, Vol. 9, Issue 1
    • DOI: 10.3390/catal9010032

    Photocatalytic hydrogen energy evolution from antibiotic wastewater via metallic bi nanosphere doped g-C 3 N 4 : performances and mechanisms
    journal, January 2019

    • Wei, Zhidong; Liu, Junying; Fang, Wenjian
    • Catalysis Science & Technology, Vol. 9, Issue 19
    • DOI: 10.1039/c9cy01375j

    Facile design of F-doped TiO2/g-C3N4 heterojunction for enhanced visible-light photocatalytic activity
    journal, January 2020

    • Li, Chao; Zhong, Wan-Ling; Gou, Qian-Zhi
    • Journal of Materials Science: Materials in Electronics, Vol. 31, Issue 4
    • DOI: 10.1007/s10854-020-02927-5

    Tuning the Photocatalytic Performance of Tungsten Oxide by Incorporating Cu3V2O8 Nanoparticles for H2 Evolution Under Visible Light Irradiation
    journal, December 2019

    • Tahir, M. B.; Iqbal, T.; Zeba, I.
    • Journal of Electrochemical Energy Conversion and Storage, Vol. 17, Issue 1
    • DOI: 10.1115/1.4043491

    Photocatalytic Applications of Heterostructure Graphitic Carbon Nitride: Pollutant Degradation, Hydrogen Gas Production (water splitting), and CO2 Reduction
    journal, July 2019

    • Darkwah, Williams Kweku; Oswald, Kivyiro Adinas
    • Nanoscale Research Letters, Vol. 14, Issue 1
    • DOI: 10.1186/s11671-019-3070-3

    2D ultrathin CoP modified Mn x Cd 1−x S with controllable band structure and robust photocatalytic performance for hydrogen generation
    journal, January 2019

    • Chen, Ran; Ao, Yanhui; Wang, Chao
    • Dalton Transactions, Vol. 48, Issue 39
    • DOI: 10.1039/c9dt02849h

    Enhanced photocatalytic activity of g-C 3 N 4 /MnO composites for hydrogen evolution under visible light
    journal, January 2019

    • Mao, Na; Gao, Xiaomin; Zhang, Chong
    • Dalton Transactions, Vol. 48, Issue 39
    • DOI: 10.1039/c9dt02748c

    Nitrogen doped graphene quantum dot-decorated earth-abundant nanotubes for enhanced capacitive deionization
    journal, January 2020

    • Ganganboina, Akhilesh Babu; Doong, Ruey-An
    • Environmental Science: Nano, Vol. 7, Issue 1
    • DOI: 10.1039/c9en00852g

    Decolorization of Reactive Black 5 by Mesoporous Al 2 O 3 @TiO 2 Nanocomposites: RB5 decolorization by Al2O3@TiO2
    journal, September 2018

    • Deng, Hui; Zhang, Mingwei; Cao, Yuekun
    • Environmental Progress & Sustainable Energy, Vol. 38, Issue s1
    • DOI: 10.1002/ep.12976

    Prospects of biosynthesized nanomaterials for the remediation of organic and inorganic environmental contaminants
    journal, January 2018

    • Das, Surajit; Chakraborty, Jaya; Chatterjee, Shreosi
    • Environmental Science: Nano, Vol. 5, Issue 12
    • DOI: 10.1039/c8en00799c

    Manganese Complexes: Hydrogen Generation and Oxidation: Manganese Complexes: Hydrogen Generation and Oxidation
    journal, November 2019

    • Kaim, Vishakha; Kaur-Ghumaan, Sandeep
    • European Journal of Inorganic Chemistry, Vol. 2019, Issue 48
    • DOI: 10.1002/ejic.201900988

    Remediation of wastewater contaminated by antibiotics. A review
    journal, November 2019

    Photocatalytic Activation of Saturated C–H Bond Over the CdS Mixed-Phase Under Visible Light Irradiation
    journal, October 2018

      Sort by:
      [ × clear filter / sort ]

      Similar Records in DOE PAGES and OSTI.GOV collections: