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

Title: Biomimetic Catalysts Based on Au@ZnO–Graphene Composites for the Generation of Hydrogen by Water Splitting

Abstract

For some decades, the scientific community has been looking for alternatives to the use of fossil fuels that allow for the planet’s sustainable and environmentally-friendly development. To do this, attempts have been made to mimic some processes that occur in nature, among which the photosystem-II stands out, which allows water splitting operating with different steps to generate oxygen and hydrogen. This research presents promising results using synthetic catalysts, which try to simulate some natural processes, and which are based on Au@ZnO–graphene compounds. These catalysts were prepared by incorporating different amounts of gold nanoparticles (1 wt.%, 3 wt.%, 5 wt.%, 10 wt.%) and graphene (1 wt.%) on the surface of synthesized zinc oxide nanowires (ZnO NWs), and zinc oxide nanoparticles (ZnO NPs), along with a commercial form (commercial ZnO) for comparison purposes. The highest amount of hydrogen (1127 μmol/hg) was reported by ZnO NWs with a gold and graphene loadings of 10 wt.% and 1 wt.%, respectively, under irradiation at 400 nm. Quantities of 759 μmol/hg and 709 μmol/hg were obtained with catalysts based on ZnO NPs and commercial ZnO, respectively. The photocatalytic activity of all composites increased with respect to the bare semiconductors, being 2.5 times higher in ZnO NWs,more » 8.8 times higher for ZnO NPs, and 7.5 times higher for commercial ZnO. The high photocatalytic activity of the catalysts is attributed, mainly, to the synergism between the different amount of gold and graphene incorporated, and the surface area of the composites.« less

Authors:
ORCiD logo; ORCiD logo; ; ; ; ; ; ORCiD logo; ; ORCiD logo
Publication Date:
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1650224
Grant/Contract Number:  
Massie Chair Project at Universidad del Turabo
Resource Type:
Published Article
Journal Name:
Biomimetics
Additional Journal Information:
Journal Name: Biomimetics Journal Volume: 5 Journal Issue: 3; Journal ID: ISSN 2313-7673
Publisher:
MDPI AG
Country of Publication:
Switzerland
Language:
English

Citation Formats

Machín, Abniel, Arango, Juan C., Fontánez, Kenneth, Cotto, María, Duconge, José, Soto-Vázquez, Loraine, Resto, Edgar, Petrescu, Florian Ion Tiberiu, Morant, Carmen, and Márquez, Francisco. Biomimetic Catalysts Based on Au@ZnO–Graphene Composites for the Generation of Hydrogen by Water Splitting. Switzerland: N. p., 2020. Web. doi:10.3390/biomimetics5030039.
Machín, Abniel, Arango, Juan C., Fontánez, Kenneth, Cotto, María, Duconge, José, Soto-Vázquez, Loraine, Resto, Edgar, Petrescu, Florian Ion Tiberiu, Morant, Carmen, & Márquez, Francisco. Biomimetic Catalysts Based on Au@ZnO–Graphene Composites for the Generation of Hydrogen by Water Splitting. Switzerland. https://doi.org/10.3390/biomimetics5030039
Machín, Abniel, Arango, Juan C., Fontánez, Kenneth, Cotto, María, Duconge, José, Soto-Vázquez, Loraine, Resto, Edgar, Petrescu, Florian Ion Tiberiu, Morant, Carmen, and Márquez, Francisco. Fri . "Biomimetic Catalysts Based on Au@ZnO–Graphene Composites for the Generation of Hydrogen by Water Splitting". Switzerland. https://doi.org/10.3390/biomimetics5030039.
@article{osti_1650224,
title = {Biomimetic Catalysts Based on Au@ZnO–Graphene Composites for the Generation of Hydrogen by Water Splitting},
author = {Machín, Abniel and Arango, Juan C. and Fontánez, Kenneth and Cotto, María and Duconge, José and Soto-Vázquez, Loraine and Resto, Edgar and Petrescu, Florian Ion Tiberiu and Morant, Carmen and Márquez, Francisco},
abstractNote = {For some decades, the scientific community has been looking for alternatives to the use of fossil fuels that allow for the planet’s sustainable and environmentally-friendly development. To do this, attempts have been made to mimic some processes that occur in nature, among which the photosystem-II stands out, which allows water splitting operating with different steps to generate oxygen and hydrogen. This research presents promising results using synthetic catalysts, which try to simulate some natural processes, and which are based on Au@ZnO–graphene compounds. These catalysts were prepared by incorporating different amounts of gold nanoparticles (1 wt.%, 3 wt.%, 5 wt.%, 10 wt.%) and graphene (1 wt.%) on the surface of synthesized zinc oxide nanowires (ZnO NWs), and zinc oxide nanoparticles (ZnO NPs), along with a commercial form (commercial ZnO) for comparison purposes. The highest amount of hydrogen (1127 μmol/hg) was reported by ZnO NWs with a gold and graphene loadings of 10 wt.% and 1 wt.%, respectively, under irradiation at 400 nm. Quantities of 759 μmol/hg and 709 μmol/hg were obtained with catalysts based on ZnO NPs and commercial ZnO, respectively. The photocatalytic activity of all composites increased with respect to the bare semiconductors, being 2.5 times higher in ZnO NWs, 8.8 times higher for ZnO NPs, and 7.5 times higher for commercial ZnO. The high photocatalytic activity of the catalysts is attributed, mainly, to the synergism between the different amount of gold and graphene incorporated, and the surface area of the composites.},
doi = {10.3390/biomimetics5030039},
journal = {Biomimetics},
number = 3,
volume = 5,
place = {Switzerland},
year = {Fri Aug 21 00:00:00 EDT 2020},
month = {Fri Aug 21 00:00:00 EDT 2020}
}

Works referenced in this record:

Preparation and Photocatalytic Hydrogen Production of Pt-Graphene/TiO 2 Composites from Water Splitting
journal, January 2018

  • Nguyen, Nhat-Thien; Zheng, Dan-Dan; Chen, Shiao-Shing
  • Journal of Nanoscience and Nanotechnology, Vol. 18, Issue 1
  • DOI: 10.1166/jnn.2018.14556

Hydrogen production via water splitting using different Au@ZnO catalysts under UV–vis irradiation
journal, February 2018


One-pot synthesis of a reduced graphene oxide–zinc oxide sphere composite and its use as a visible light photocatalyst
journal, August 2013


Reduced TiO 2 -Graphene Oxide Heterostructure As Broad Spectrum-Driven Efficient Water-Splitting Photocatalysts
journal, March 2016

  • Li, Lihua; Yu, Lili; Lin, Zhaoyong
  • ACS Applied Materials & Interfaces, Vol. 8, Issue 13
  • DOI: 10.1021/acsami.6b00966

Enhancing Efficiency and Stability of Photovoltaic Cells by Using Perovskite/Zr-MOF Heterojunction Including Bilayer and Hybrid Structures
journal, January 2019


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

Photocatalytic Hydrogen Production from Glycerol-water over Metal Loaded and Non-metal Doped Titanium Oxide
journal, October 2015

  • Slamet, Slamet; Kusrini, Eny; Salim Afrozi, Agus
  • International Journal of Technology, Vol. 6, Issue 4
  • DOI: 10.14716/ijtech.v6i4.2176

Development of Sulfonic-Acid-Functionalized Mesoporous Materials: Synthesis and Catalytic Applications
journal, November 2018

  • Doustkhah, Esmail; Lin, Jianjian; Rostamnia, Sadegh
  • Chemistry - A European Journal, Vol. 25, Issue 7
  • DOI: 10.1002/chem.201802183

Importance of Plasmonic Heating on Visible Light Driven Photocatalysis of Gold Nanoparticle Decorated Zinc Oxide Nanorods
journal, May 2016

  • Bora, Tanujjal; Zoepfl, David; Dutta, Joydeep
  • Scientific Reports, Vol. 6, Issue 1
  • DOI: 10.1038/srep26913

Influence of Excitation Wavelength (UV or Visible Light) on the Photocatalytic Activity of Titania Containing Gold Nanoparticles for the Generation of Hydrogen or Oxygen from Water
journal, January 2011

  • Gomes Silva, Cláudia; Juárez, Raquel; Marino, Tiziana
  • Journal of the American Chemical Society, Vol. 133, Issue 3
  • DOI: 10.1021/ja1086358

The role of hydrogen and fuel cells in the global energy system
journal, January 2019

  • Staffell, Iain; Scamman, Daniel; Velazquez Abad, Anthony
  • Energy & Environmental Science, Vol. 12, Issue 2
  • DOI: 10.1039/C8EE01157E

A technical and environmental comparison between hydrogen and some fossil fuels
journal, January 2015


Hydrothermal synthesis of PdAu nanocatalysts with variable atom ratio for methanol oxidation
journal, January 2018


TiO 2 -Based Nanomaterials for the Production of Hydrogen and the Development of Lithium-Ion Batteries
journal, November 2017

  • Pinilla, Sergio; Machín, Abniel; Park, Sang-Hoon
  • The Journal of Physical Chemistry B, Vol. 122, Issue 2
  • DOI: 10.1021/acs.jpcb.7b07130

Enhanced Daylight-Induced Photocatalytic Activity of Solvent Exfoliated Graphene (SEG)/ZnO Hybrid Nanocomposites toward Degradation of Reactive Black 5
journal, August 2014

  • Ong, Wee-Jun; Voon, Seen-Yee; Tan, Lling-Lling
  • Industrial & Engineering Chemistry Research, Vol. 53, Issue 44
  • DOI: 10.1021/ie5027088

Novel Au/TiO2 photocatalysts for hydrogen production in alcohol–water mixtures based on hydrogen titanate nanotube precursors
journal, October 2015


Preparation and visible light photocatalytic activity of Ag/TiO2/graphene nanocomposite
journal, January 2011

  • Wen, Yanyuan; Ding, Hanming; Shan, Yongkui
  • Nanoscale, Vol. 3, Issue 10
  • DOI: 10.1039/c1nr10604j

1D/0D WO3/CdS heterojunction photoanodes modified with dual co-catalysts for efficient photoelectrochemical water splitting
journal, June 2019


Chemical approaches to artificial photosynthesis: A molecular, dye-sensitized photoanode for O 2 production prepared by layer-by-layer self-assembly
journal, June 2020

  • Wang, Degao; Farnum, Byron H.; Dares, Christopher J.
  • The Journal of Chemical Physics, Vol. 152, Issue 24
  • DOI: 10.1063/5.0007383

Synthesis of Graphene-ZnO-Au Nanocomposites for Efficient Photocatalytic Reduction of Nitrobenzene
journal, May 2013

  • Roy, Prathik; Periasamy, Arun Prakash; Liang, Chi-Te
  • Environmental Science & Technology, Vol. 47, Issue 12
  • DOI: 10.1021/es400422k

Visible-light activation of TiO2 photocatalysts: Advances in theory and experiments
journal, December 2015

  • Etacheri, Vinodkumar; Di Valentin, Cristiana; Schneider, Jenny
  • Journal of Photochemistry and Photobiology C: Photochemistry Reviews, Vol. 25
  • DOI: 10.1016/j.jphotochemrev.2015.08.003

Microwave-assisted hydrothermal synthesis of graphene based Au–TiO 2 photocatalysts for efficient visible-light hydrogen production
journal, January 2014

  • Wang, Ying; Yu, Jiaguo; Xiao, Wei
  • J. Mater. Chem. A, Vol. 2, Issue 11
  • DOI: 10.1039/C3TA14908K

Pt and Au/TiO2 photocatalysts for methanol reforming: Role of metal nanoparticles in tuning charge trapping properties and photoefficiency
journal, February 2013

  • Naldoni, Alberto; D’Arienzo, Massimiliano; Altomare, Marco
  • Applied Catalysis B: Environmental, Vol. 130-131
  • DOI: 10.1016/j.apcatb.2012.11.006

Corrosion behavior of a positive graphite electrode in vanadium redox flow battery
journal, October 2011


Graphene based catalyst supports for high temperature PEM fuel cell application
journal, June 2018

  • Devrim, Yılser; Arıca, Elif Damla; Albostan, Ayhan
  • International Journal of Hydrogen Energy, Vol. 43, Issue 26
  • DOI: 10.1016/j.ijhydene.2018.03.047

Novel Green Biomimetic Approach for Preparation of Highly Stable Au-ZnO Heterojunctions with Enhanced Photocatalytic Activity
journal, March 2018

  • Choudhary, Manoj Kumar; Kataria, Jyoti; Sharma, Shweta
  • ACS Applied Nano Materials, Vol. 1, Issue 4
  • DOI: 10.1021/acsanm.8b00272

Electrified methane reforming: A compact approach to greener industrial hydrogen production
journal, May 2019

  • Wismann, Sebastian T.; Engbæk, Jakob S.; Vendelbo, Søren B.
  • Science, Vol. 364, Issue 6442
  • DOI: 10.1126/science.aaw8775

Zinc Oxide—From Synthesis to Application: A Review
journal, April 2014

  • Kołodziejczak-Radzimska, Agnieszka; Jesionowski, Teofil
  • Materials, Vol. 7, Issue 4
  • DOI: 10.3390/ma7042833

Synthesis of ZnO nanowires by thermal decomposition of zinc acetate dihydrate
journal, January 2009


Effect of seeded substrates on hydrothermally grown ZnO nanorods
journal, February 2009

  • Baruah, Sunandan; Dutta, Joydeep
  • Journal of Sol-Gel Science and Technology, Vol. 50, Issue 3
  • DOI: 10.1007/s10971-009-1917-2

Mo-doped ZnO nanoflakes on Ni-foam for asymmetric supercapacitor applications
journal, January 2019

  • Ali, Awais; Ammar, Muhammad; Ali, Muddassir
  • RSC Advances, Vol. 9, Issue 47
  • DOI: 10.1039/C9RA05051E

Harnessing MOF materials in photovoltaic devices: recent advances, challenges, and perspectives
journal, January 2019

  • Chueh, Chu-Chen; Chen, Chih-I; Su, Yu-An
  • Journal of Materials Chemistry A, Vol. 7, Issue 29
  • DOI: 10.1039/C9TA03595H

Synthesis of Silver-Doped Zinc Oxide Nanocomposite by Pulse Mode Ultrasonication and Its Characterization Studies
journal, January 2013

  • Siva Vijayakumar, T.; Karthikeyeni, S.; Vasanth, S.
  • Journal of Nanoscience, Vol. 2013
  • DOI: 10.1155/2013/785064

Recent biomedical applications of gold nanoparticles: A review
journal, July 2018


XPS determination of oxygen-containing functional groups on carbon-fibre surfaces and the cleaning of these surfaces
journal, October 1990

  • Desimoni, E.; Casella, G. I.; Morone, A.
  • Surface and Interface Analysis, Vol. 15, Issue 10
  • DOI: 10.1002/sia.740151011

ZnO nanorod arrays co-loaded with Au nanoparticles and reduced graphene oxide: Synthesis, characterization and photocatalytic application
journal, March 2016


Facile and green synthesis of titanate nanotube/graphene nanocomposites for photocatalytic H2 generation from water
journal, July 2013


Metal-organic framework (MOF)-derived catalysts for fine chemical production
journal, August 2020

  • Konnerth, Hannelore; Matsagar, Babasaheb M.; Chen, Season S.
  • Coordination Chemistry Reviews, Vol. 416
  • DOI: 10.1016/j.ccr.2020.213319

Fabrication of ZnO@C foam: A flexible free-standing electrode for energy storage devices
journal, April 2020


Preparation of multi-branched Au–ZnO hybrid nanocrystals on graphene for enhanced photocatalytic performance
journal, December 2015


ZnO nanospheres based simple hydrothermal route for photocatalytic degradation of azo dye
journal, March 2019

  • Saleh, Sayed M.
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 211
  • DOI: 10.1016/j.saa.2018.11.065

Fabrication of gold–calcium phosphate composite nanoparticles through coprecipitation mediated by amino-terminated polyethylene glycol
journal, October 2020


Enhanced visible light photocatalysis through fast crystallization of zinc oxide nanorods
journal, January 2010

  • Baruah, Sunandan; Mahmood, Mohammad Abbas; Myint, Myo Tay Zar
  • Beilstein Journal of Nanotechnology, Vol. 1
  • DOI: 10.3762/bjnano.1.3

Enhanced removal of various dyes from aqueous solutions by UV and simulated solar photocatalysis over TiO2/ZnO/rGO composites
journal, February 2020