DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Enhanced visible light photocatalytic water reduction from a g-C3N4/SrTa2O6 heterojunction

Abstract

In this paper, a new g-C3N4/SrTa2O6 heterojunction photocatalyst was designed and prepared by chimie douce (soft chemistry) method where carbon nitride (g-C3N4) was deposited over the metastable perovskite phase of SrTa2O6. The morphological study of the heterojunction using SEM and STEM revealed that g-C3N4 nanofibers are dispersed uniformly on the surface of SrTa2O6 plates leading to the intimate contact between them. The heterojunction could achieve a high and stable visible light photocatalytic H2 generation of 137 mmol/h/mole of g-C3N4, which is much larger than the amount of hydrogen generated by one mole of pristine g-C3N4. Finally, a plausible mechanism for the observed enhanced photocatalytic activity for the heterojunction is proposed on the basis of effective charge separation of photogenerated electron-hole pairs, supported by band position calculations and photo-physical properties of g-C3N4 and SrTa2O6.

Authors:
 [1];  [2];  [3];  [4];  [5];  [5];  [6];  [4];  [4];  [5];  [1]
  1. Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Chemistry. Center for Energy, Environment and Sustainability (CEES)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences; Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences; Univ. of Louisville, KY (United States). Dept. of Mechanical Engineering. Conn Center for Renewable Energy Research
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences
  5. Wake Forest Univ., Winston-Salem, NC (United States). Dept. of Chemistry
  6. Georgia Inst. of Technology, Atlanta, GA (United States). School of Chemistry and Biochemistry
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); Wake Forest Univ. (United States)
Contributing Org.:
Univ. of Louisville, KY (United States)
OSTI Identifier:
1376489
Grant/Contract Number:  
AC05-00OR22725; MRI1040264; DGE-1148903
Resource Type:
Accepted Manuscript
Journal Name:
Applied Catalysis. B, Environmental
Additional Journal Information:
Journal Volume: 217; Journal ID: ISSN 0926-3373
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Photocatalysis; Semiconductor; Heterojunction; Perovskite; Hydrogen

Citation Formats

Adhikari, Shiba P., Hood, Zachary D., Wang, Hui, Peng, Rui, Krall, Alex, Li, Hui, Chen, Vincent W., More, Karren L., Wu, Zili, Geyer, Scott, and Lachgar, Abdou. Enhanced visible light photocatalytic water reduction from a g-C3N4/SrTa2O6 heterojunction. United States: N. p., 2017. Web. doi:10.1016/j.apcatb.2017.05.092.
Adhikari, Shiba P., Hood, Zachary D., Wang, Hui, Peng, Rui, Krall, Alex, Li, Hui, Chen, Vincent W., More, Karren L., Wu, Zili, Geyer, Scott, & Lachgar, Abdou. Enhanced visible light photocatalytic water reduction from a g-C3N4/SrTa2O6 heterojunction. United States. https://doi.org/10.1016/j.apcatb.2017.05.092
Adhikari, Shiba P., Hood, Zachary D., Wang, Hui, Peng, Rui, Krall, Alex, Li, Hui, Chen, Vincent W., More, Karren L., Wu, Zili, Geyer, Scott, and Lachgar, Abdou. Fri . "Enhanced visible light photocatalytic water reduction from a g-C3N4/SrTa2O6 heterojunction". United States. https://doi.org/10.1016/j.apcatb.2017.05.092. https://www.osti.gov/servlets/purl/1376489.
@article{osti_1376489,
title = {Enhanced visible light photocatalytic water reduction from a g-C3N4/SrTa2O6 heterojunction},
author = {Adhikari, Shiba P. and Hood, Zachary D. and Wang, Hui and Peng, Rui and Krall, Alex and Li, Hui and Chen, Vincent W. and More, Karren L. and Wu, Zili and Geyer, Scott and Lachgar, Abdou},
abstractNote = {In this paper, a new g-C3N4/SrTa2O6 heterojunction photocatalyst was designed and prepared by chimie douce (soft chemistry) method where carbon nitride (g-C3N4) was deposited over the metastable perovskite phase of SrTa2O6. The morphological study of the heterojunction using SEM and STEM revealed that g-C3N4 nanofibers are dispersed uniformly on the surface of SrTa2O6 plates leading to the intimate contact between them. The heterojunction could achieve a high and stable visible light photocatalytic H2 generation of 137 mmol/h/mole of g-C3N4, which is much larger than the amount of hydrogen generated by one mole of pristine g-C3N4. Finally, a plausible mechanism for the observed enhanced photocatalytic activity for the heterojunction is proposed on the basis of effective charge separation of photogenerated electron-hole pairs, supported by band position calculations and photo-physical properties of g-C3N4 and SrTa2O6.},
doi = {10.1016/j.apcatb.2017.05.092},
journal = {Applied Catalysis. B, Environmental},
number = ,
volume = 217,
place = {United States},
year = {Fri Jun 02 00:00:00 EDT 2017},
month = {Fri Jun 02 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 54 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Electrochemical Photolysis of Water at a Semiconductor Electrode
journal, July 1972

  • Fujishima, Akira; Honda, Kenichi
  • Nature, Vol. 238, Issue 5358, p. 37-38
  • DOI: 10.1038/238037a0

Heterogeneous Photocatalysis: Recent Advances and Applications
journal, March 2013


An overview of semiconductor photocatalysis
journal, July 1997


Inorganic nanostructures for photoelectrochemical and photocatalytic water splitting
journal, January 2013


Photocatalytic water splitting using semiconductor particles: History and recent developments
journal, December 2011


Hydrogen Production from Semiconductor-based Photocatalysis via Water Splitting
journal, October 2012

  • Liao, Chi-Hung; Huang, Chao-Wei; Wu, Jeffrey C. S.
  • Catalysts, Vol. 2, Issue 4
  • DOI: 10.3390/catal2040490

Heterogeneous photocatalyst materials for water splitting
journal, January 2009

  • Kudo, Akihiko; Miseki, Yugo
  • Chem. Soc. Rev., Vol. 38, Issue 1
  • DOI: 10.1039/B800489G

Doped-TiO2: A Review
journal, November 2008


A review and recent developments in photocatalytic water-splitting using TiO2 for hydrogen production
journal, April 2007

  • Ni, Meng; Leung, Michael K. H.; Leung, Dennis Y. C.
  • Renewable and Sustainable Energy Reviews, Vol. 11, Issue 3
  • DOI: 10.1016/j.rser.2005.01.009

Semiconductor Composites: Strategies for Enhancing Charge Carrier Separation to Improve Photocatalytic Activity
journal, December 2013


Visible-light driven heterojunction photocatalysts for water splitting – a critical review
journal, January 2015

  • Moniz, Savio J. A.; Shevlin, Stephen A.; Martin, David James
  • Energy & Environmental Science, Vol. 8, Issue 3
  • DOI: 10.1039/C4EE03271C

Semiconductor heterojunction photocatalysts: design, construction, and photocatalytic performances
journal, January 2014

  • Wang, Huanli; Zhang, Lisha; Chen, Zhigang
  • Chemical Society Reviews, Vol. 43, Issue 15
  • DOI: 10.1039/C4CS00126E

Visible-light-driven Bi 2 O 3 /WO 3 composites with enhanced photocatalytic activity
journal, January 2015

  • Adhikari, Shiba P.; Dean, Hunter; Hood, Zachary D.
  • RSC Advances, Vol. 5, Issue 111
  • DOI: 10.1039/C5RA13579F

Visible light assisted photocatalytic hydrogen generation by Ta 2 O 5 /Bi 2 O 3 , TaON/Bi 2 O 3 , and Ta 3 N 5 /Bi 2 O 3 composites
journal, January 2015

  • Adhikari, Shiba P.; Hood, Zachary D.; More, Karren L.
  • RSC Advances, Vol. 5, Issue 68
  • DOI: 10.1039/C5RA06563A

Anchoring Tailored Low-Index Faceted BiOBr Nanoplates onto TiO 2 Nanorods to Enhance the Stability and Visible-Light-Driven Catalytic Activity
journal, May 2017

  • Xue, Chao; Zhang, Tianxi; Ding, Shujiang
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 19
  • DOI: 10.1021/acsami.7b00433

Synthesis and Photocatalytic Property of Layered Perovskite Tantalates, RbLnTa 2 O 7 (Ln = La, Pr, Nd, and Sm)
journal, March 2000

  • Machida, Masato; Yabunaka, Jun-ichi; Kijima, Tsuyoshi
  • Chemistry of Materials, Vol. 12, Issue 3
  • DOI: 10.1021/cm990577j

Chemical Structures and Performance of Perovskite Oxides
journal, July 2001

  • Pena, M.; Fierro, J.
  • Chemical Reviews, Vol. 101, Issue 7, p. 1981-2018
  • DOI: 10.1021/cr980129f

Water Splitting into H 2 and O 2 on New Sr 2 M 2 O 7 (M = Nb and Ta) Photocatalysts with Layered Perovskite Structures:  Factors Affecting the Photocatalytic Activity
journal, January 2000

  • Kudo, Akihiko; Kato, Hideki; Nakagawa, Seira
  • The Journal of Physical Chemistry B, Vol. 104, Issue 3
  • DOI: 10.1021/jp9919056

Perovskite-like crystals of the Ruddlesden-Popper series
journal, September 2000

  • Beznosikov, B. V.; Aleksandrov, K. S.
  • Crystallography Reports, Vol. 45, Issue 5
  • DOI: 10.1134/1.1312923

Synthesis and structure of a double-layered perovskite and its hydrate, K2SrTa2O7·mH2O (m = 0, 2)
journal, July 2000


The layered perovskite K2SrTa2O7: hydration and K+/H+ ion exchange
journal, January 2001

  • Crosnier-Lopez, Marie-Pierre; Le Berre, Françoise; Fourquet, Jean-Louis
  • Journal of Materials Chemistry, Vol. 11, Issue 4
  • DOI: 10.1039/b005755j

Synthesis and structure of novel layered perovskite oxides: Li2La1.78Nb0.66Ti2.34O10, and a new family, Li2[A0.5nBnO3n + 1]
journal, January 1999

  • Bhuvanesh, N. S. P.; Crosnier‐Lopez, M. P.; Duroy, H.
  • Journal of Materials Chemistry, Vol. 9, Issue 12
  • DOI: 10.1039/a903720i

Polymeric Carbon Nitrides: Semiconducting Properties and Emerging Applications in Photocatalysis and Photoelectrochemical Energy Conversion
journal, February 2012

  • Zhang, Yuanjian; Mori, Toshiyuki; Ye, Jinhua
  • Science of Advanced Materials, Vol. 4, Issue 2
  • DOI: 10.1166/sam.2012.1283

g-C 3 N 4 -Based Photocatalysts for Hydrogen Generation
journal, June 2014

  • Cao, Shaowen; Yu, Jiaguo
  • The Journal of Physical Chemistry Letters, Vol. 5, Issue 12
  • DOI: 10.1021/jz500546b

Mesoporous Carbon Nitride-Tungsten Oxide Composites for Enhanced Photocatalytic Hydrogen Evolution
journal, March 2015

  • Kailasam, Kamalakannan; Fischer, Anna; Zhang, Guigang
  • ChemSusChem, Vol. 8, Issue 8
  • DOI: 10.1002/cssc.201403278

Graphitic carbon nitride (g-C3N4)–Pt-TiO2 nanocomposite as an efficient photocatalyst for hydrogen production under visible light irradiation
journal, January 2012

  • Chai, Bo; Peng, Tianyou; Mao, Jing
  • Physical Chemistry Chemical Physics, Vol. 14, Issue 48
  • DOI: 10.1039/c2cp42484c

Mesoporous Phosphorus-Doped g-C 3 N 4 Nanostructured Flowers with Superior Photocatalytic Hydrogen Evolution Performance
journal, July 2015

  • Zhu, Yun-Pei; Ren, Tie-Zhen; Yuan, Zhong-Yong
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 30
  • DOI: 10.1021/acsami.5b04947

Phosphorus-Doped Carbon Nitride Tubes with a Layered Micro-nanostructure for Enhanced Visible-Light Photocatalytic Hydrogen Evolution
journal, December 2015

  • Guo, Shien; Deng, Zhaopeng; Li, Mingxia
  • Angewandte Chemie International Edition, Vol. 55, Issue 5
  • DOI: 10.1002/anie.201508505

A review on g-C3N4 for photocatalytic water splitting and CO2 reduction
journal, December 2015


Construction of novel three dimensionally ordered macroporous carbon nitride for highly efficient photocatalytic activity
journal, December 2016


Graphitic carbon nitride based nanocomposites: a review
journal, January 2015

  • Zhao, Zaiwang; Sun, Yanjuan; Dong, Fan
  • Nanoscale, Vol. 7, Issue 1
  • DOI: 10.1039/C4NR03008G

A ball-in-ball g-C 3 N 4 @SiO 2 nano-photoreactor for highly efficient H 2 generation and NO removal
journal, January 2017


A Visible-Light-Active Heterojunction with Enhanced Photocatalytic Hydrogen Generation
journal, June 2016

  • Adhikari, Shiba P.; Hood, Zachary D.; More, Karren L.
  • ChemSusChem, Vol. 9, Issue 14
  • DOI: 10.1002/cssc.201600424

A “Chimie Douce” Sythesis of Perovskite-Type SrTa 2 O 6 and SrTa 2-x Nb x O 6 1
journal, October 1998

  • Ollivier, Patricia J.; Mallouk, Thomas E.
  • Chemistry of Materials, Vol. 10, Issue 10
  • DOI: 10.1021/cm9802144

Photocatalytic Water Splitting over Spontaneously Hydrated Layered Tantalate A 2 SrTa 2 O 7 · n H 2 O (A=H, K, Rb)
journal, November 2002

  • Shimizu, Ken-ichi; Tsuji, Yoshihiro; Kawakami, Masato
  • Chemistry Letters, Vol. 31, Issue 11
  • DOI: 10.1246/cl.2002.1158

Proton-Conducting Films of Nanoscale Ribbons Formed by Exfoliation of the Layer Perovskite H 2 SrTa 2 O 7
journal, December 2007

  • Schottenfeld, Joshua A.; Kobayashi, Yoji; Wang, Jinguo
  • Chemistry of Materials, Vol. 20, Issue 1
  • DOI: 10.1021/cm702593m

Polymeric Graphitic Carbon Nitride as a Heterogeneous Organocatalyst: From Photochemistry to Multipurpose Catalysis to Sustainable Chemistry
journal, November 2011

  • Wang, Yong; Wang, Xinchen; Antonietti, Markus
  • Angewandte Chemie International Edition, Vol. 51, Issue 1
  • DOI: 10.1002/anie.201101182

A New Metastable Thin-Film Strontium Tantalate Perovskite
journal, August 1999


Synthesis of a g-C 3 N 4 -sensitized and NaNbO 3 -substrated II-type heterojunction with enhanced photocatalytic degradation activity
journal, January 2015

  • Chengjie, Song; Mingshan, Fan; Bo, Hu
  • CrystEngComm, Vol. 17, Issue 24
  • DOI: 10.1039/C5CE00622H

Morphology-controlled synthesis and efficient photocatalytic performances of a new promising photocatalyst Sr0.25H1.5Ta2O6·H2O
journal, January 2011

  • Liang, Shijing; Shen, Lijuan; Zhu, Jia
  • RSC Advances, Vol. 1, Issue 3
  • DOI: 10.1039/c1ra00233c

Nature of the use of adventitious carbon as a binding energy standard
journal, May 1995

  • Barr, Tery L.; Seal, Sudipta
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 13, Issue 3
  • DOI: 10.1116/1.579868

Polymeric g-C 3 N 4 Coupled with NaNbO 3 Nanowires toward Enhanced Photocatalytic Reduction of CO 2 into Renewable Fuel
journal, September 2014

  • Shi, Haifeng; Chen, Guoqing; Zhang, Chengliang
  • ACS Catalysis, Vol. 4, Issue 10
  • DOI: 10.1021/cs500848f

Visible-light-induced WO3/g-C3N4 composites with enhanced photocatalytic activity
journal, January 2013

  • Huang, Liying; Xu, Hui; Li, Yeping
  • Dalton Transactions, Vol. 42, Issue 24
  • DOI: 10.1039/c3dt00115f

Roles of Cocatalysts in Photocatalysis and Photoelectrocatalysis
journal, March 2013

  • Yang, Jinhui; Wang, Donge; Han, Hongxian
  • Accounts of Chemical Research, Vol. 46, Issue 8
  • DOI: 10.1021/ar300227e

Solar-to-fuels conversion over In2O3/g-C3N4 hybrid photocatalysts
journal, April 2014


TiO2–g-C3N4 composite materials for photocatalytic H2 evolution under visible light irradiation
journal, January 2011


Prediction of Flatband Potentials at Semiconductor-Electrolyte Interfaces from Atomic Electronegativities
journal, January 1978

  • Butler, M. A.
  • Journal of The Electrochemical Society, Vol. 125, Issue 2
  • DOI: 10.1149/1.2131419

Photophysical and Photocatalytic Properties of AgInW 2 O 8
journal, December 2003

  • Tang, Junwang; Zou, Zhigang; Ye, Jinhua
  • The Journal of Physical Chemistry B, Vol. 107, Issue 51
  • DOI: 10.1021/jp0359891

Roles of TaON and Ta3N5 in the visible-Fenton-like degradation of atrazine
journal, February 2014


Hematite/Si Nanowire Dual-Absorber System for Photoelectrochemical Water Splitting at Low Applied Potentials
journal, July 2012

  • Mayer, Matthew T.; Du, Chun; Wang, Dunwei
  • Journal of the American Chemical Society, Vol. 134, Issue 30
  • DOI: 10.1021/ja3051734

Graphene-Like Carbon Nitride Nanosheets for Improved Photocatalytic Activities
journal, July 2012

  • Niu, Ping; Zhang, Lili; Liu, Gang
  • Advanced Functional Materials, Vol. 22, Issue 22
  • DOI: 10.1002/adfm.201200922

Visible light-driven novel g-C 3 N 4 /NiFe-LDH composite photocatalyst with enhanced photocatalytic activity towards water oxidation and reduction reaction
journal, January 2015

  • Nayak, Susanginee; Mohapatra, Lagnamayee; Parida, Kulamani
  • Journal of Materials Chemistry A, Vol. 3, Issue 36
  • DOI: 10.1039/C5TA05002B

Extraordinarily efficient photocatalytic hydrogen evolution in water using semiconductor nanorods integrated with crystalline Ni 2 P cocatalysts
journal, January 2015

  • Sun, Zijun; Zheng, Huafei; Li, Jingshi
  • Energy & Environmental Science, Vol. 8, Issue 9
  • DOI: 10.1039/C5EE01310K

Fabrication of High Conductivity TiO 2 /Ag Fibrous Electrode by the Electrophoretic Deposition Method
journal, November 2008

  • Hosseini, Z.; Taghavinia, N.; Sharifi, N.
  • The Journal of Physical Chemistry C, Vol. 112, Issue 47
  • DOI: 10.1021/jp8046054

Visible Photocatalytic Activity Enhancement of ZnWO 4 by Graphene Hybridization
journal, November 2012

  • Bai, Xiaojuan; Wang, Li; Zhu, Yongfa
  • ACS Catalysis, Vol. 2, Issue 12
  • DOI: 10.1021/cs3005852

Hydrothermal Synthesis g-C 3 N 4 /Nano-InVO 4 Nanocomposites and Enhanced Photocatalytic Activity for Hydrogen Production under Visible Light Irradiation
journal, August 2015

  • Hu, Bo; Cai, Fanpeng; Chen, Tianjun
  • ACS Applied Materials & Interfaces, Vol. 7, Issue 33
  • DOI: 10.1021/acsami.5b05715

Works referencing / citing this record:

A highly stable metal–organic framework derived phosphorus doped carbon/Cu 2 O structure for efficient photocatalytic phenol degradation and hydrogen production
journal, January 2019

  • Dubale, Amare Aregahegn; Ahmed, Ibrahim Nasser; Chen, Xia-Hui
  • Journal of Materials Chemistry A, Vol. 7, Issue 11
  • DOI: 10.1039/c8ta12544a

A Review on Quantum Dots Modified g-C3N4-Based Photocatalysts with Improved Photocatalytic Activity
journal, January 2020


Interstitial N-doped SrSnO 3 perovskite: structural design, modification and photocatalytic degradation of dyes
journal, January 2019

  • Zhang, Xinhua; Liu, Anjie; Cao, Yali
  • New Journal of Chemistry, Vol. 43, Issue 27
  • DOI: 10.1039/c9nj02087j

Visible-light-active g-C 3 N 4 /N-doped Sr 2 Nb 2 O 7 heterojunctions as photocatalysts for the hydrogen evolution reaction
journal, January 2018

  • Adhikari, Shiba P.; Hood, Zachary D.; Chen, Vincent W.
  • Sustainable Energy & Fuels, Vol. 2, Issue 11
  • DOI: 10.1039/c8se00319j