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Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation

Yassine Cherif, Hajer Azzi, Kishore Sridharan Orcid Logo, Seulgi Ji, Heechae Choi Orcid Logo, Michael G. Allan, Sihem Benaissa, Karima Saidi-Bendahou, Lois Damptey, Camila Silva Ribeiro, Satheesh Krishnamurthy Orcid Logo, Sanjay Nagarajan Orcid Logo, M. Mercedes Maroto-Valer, Moritz Kuehnel, Sudhagar Pitchaimuthu Orcid Logo

ACS Omega, Volume: 8, Issue: 1, Pages: 1249 - 1261

Swansea University Authors: Moritz Kuehnel, Sudhagar Pitchaimuthu Orcid Logo

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Abstract

This work demonstrates a two-step gram-scale synthesis of presynthesized silver (Ag) nanoparticles impregnated with mesoporous TiO2 and evaluates their feasibility for wastewater treatment and hydrogen gas generation under natural sunlight. Paracetamol was chosen as the model pharmaceutical pollutan...

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Published in: ACS Omega
ISSN: 2470-1343 2470-1343
Published: American Chemical Society (ACS) 2023
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Paracetamol was chosen as the model pharmaceutical pollutant for evaluating photocatalytic performance. A systematic material analysis (morphology, chemical environment, optical bandgap energy) of the Ag/TiO2 photocatalyst powder was carried out, and the influence of material properties on the performance is discussed in detail. The experimental results showed that the decoration of anatase TiO2 nanoparticles (size between 80 and 100 nm) with 5 nm Ag nanoparticles (1 wt %) induced visible-light absorption and enhanced charge carrier separation. As a result, 0.01 g/L Ag/TiO2 effectively removed 99% of 0.01 g/L paracetamol in 120 min and exhibited 60% higher photocatalytic removal than pristine TiO2. Alongside paracetamol degradation, Ag/TiO2 led to the generation of 1729 μmol H2 g–1 h–1. This proof-of-concept approach for tandem pollutant degradation and hydrogen generation was further evaluated with rare earth metal (lanthanum)- and nonmetal (nitrogen)-doped TiO2, which also showed a positive response. Using a combination of ab initio calculations and our new theory model, we revealed that the enhanced photocatalytic performance of Ag/TiO2 was due to the surface Fermi-level change of TiO2 and lowered surface reaction energy barrier for water pollutant oxidation. 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spelling v2 65137 2023-11-28 Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation 210dbad181ce095d6f8bf2bd1d616d4e Moritz Kuehnel Moritz Kuehnel true false 2fdbee02f4bfc5a1b174c8bd04afbd2b 0000-0001-9098-8806 Sudhagar Pitchaimuthu Sudhagar Pitchaimuthu true false 2023-11-28 FGSEN This work demonstrates a two-step gram-scale synthesis of presynthesized silver (Ag) nanoparticles impregnated with mesoporous TiO2 and evaluates their feasibility for wastewater treatment and hydrogen gas generation under natural sunlight. Paracetamol was chosen as the model pharmaceutical pollutant for evaluating photocatalytic performance. A systematic material analysis (morphology, chemical environment, optical bandgap energy) of the Ag/TiO2 photocatalyst powder was carried out, and the influence of material properties on the performance is discussed in detail. The experimental results showed that the decoration of anatase TiO2 nanoparticles (size between 80 and 100 nm) with 5 nm Ag nanoparticles (1 wt %) induced visible-light absorption and enhanced charge carrier separation. As a result, 0.01 g/L Ag/TiO2 effectively removed 99% of 0.01 g/L paracetamol in 120 min and exhibited 60% higher photocatalytic removal than pristine TiO2. Alongside paracetamol degradation, Ag/TiO2 led to the generation of 1729 μmol H2 g–1 h–1. This proof-of-concept approach for tandem pollutant degradation and hydrogen generation was further evaluated with rare earth metal (lanthanum)- and nonmetal (nitrogen)-doped TiO2, which also showed a positive response. Using a combination of ab initio calculations and our new theory model, we revealed that the enhanced photocatalytic performance of Ag/TiO2 was due to the surface Fermi-level change of TiO2 and lowered surface reaction energy barrier for water pollutant oxidation. This work opens new opportunities for exploiting tandem photocatalytic routes beyond water splitting and understanding the simultaneous reactions in metal-doped metal oxide photocatalyst systems under natural sunlight. Journal Article ACS Omega 8 1 1249 1261 American Chemical Society (ACS) 2470-1343 2470-1343 Degradation, Environmental pollution, Hydrogen, Oxides, Photocatalysts 10 1 2023 2023-01-10 10.1021/acsomega.2c06657 COLLEGE NANME Science and Engineering - Faculty COLLEGE CODE FGSEN Swansea University Other The authorsY.C. and H.J. wouldlike to thankthe AlgerianDGRST-MESRSand the Universityof Tlemcenfor financialsupport.SP thanksHeriot-WattUniversityfor the Seed Grantsupport.S.J. and H.C. thankthe Universityof Cologneand theExcellenceCluster“QuantumMatterand Materials”for theinfrastructuralsupport.S.K. acknowledgesthe RoyalAcademyof EngineeringNewtonFundand EuropeanCommissionprojectid: 958491�Smartinnovativesystemfor recyclingwastewaterand creatingclosedloopsin textilemanufacturingindustrialprocesses. 2024-03-07T13:09:33.3529727 2023-11-28T14:56:36.2091883 Faculty of Science and Engineering School of Engineering and Applied Sciences - Chemical Engineering Yassine Cherif 1 Hajer Azzi 2 Kishore Sridharan 0000-0002-2099-2962 3 Seulgi Ji 4 Heechae Choi 0000-0002-9390-6607 5 Michael G. Allan 6 Sihem Benaissa 7 Karima Saidi-Bendahou 8 Lois Damptey 9 Camila Silva Ribeiro 10 Satheesh Krishnamurthy 0000-0001-7237-9206 11 Sanjay Nagarajan 0000-0003-2678-693x 12 M. Mercedes Maroto-Valer 13 Moritz Kuehnel 14 Sudhagar Pitchaimuthu 0000-0001-9098-8806 15 65137__29136__1c5aa61b63544373a46883f4ab879422.pdf 65137_MKuehnel.pdf 2023-11-28T15:00:08.6472290 Output 11632522 application/pdf Version of Record true © 2022 The Authors. Released under the terms of a Creative Commons Attribution License. true eng https:// creativecommons.org/licenses/by/ 4.0/
title Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
spellingShingle Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
Moritz Kuehnel
Sudhagar Pitchaimuthu
title_short Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
title_full Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
title_fullStr Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
title_full_unstemmed Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
title_sort Facile Synthesis of Gram-Scale Mesoporous Ag/TiO<sub>2</sub> Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation
author_id_str_mv 210dbad181ce095d6f8bf2bd1d616d4e
2fdbee02f4bfc5a1b174c8bd04afbd2b
author_id_fullname_str_mv 210dbad181ce095d6f8bf2bd1d616d4e_***_Moritz Kuehnel
2fdbee02f4bfc5a1b174c8bd04afbd2b_***_Sudhagar Pitchaimuthu
author Moritz Kuehnel
Sudhagar Pitchaimuthu
author2 Yassine Cherif
Hajer Azzi
Kishore Sridharan
Seulgi Ji
Heechae Choi
Michael G. Allan
Sihem Benaissa
Karima Saidi-Bendahou
Lois Damptey
Camila Silva Ribeiro
Satheesh Krishnamurthy
Sanjay Nagarajan
M. Mercedes Maroto-Valer
Moritz Kuehnel
Sudhagar Pitchaimuthu
format Journal article
container_title ACS Omega
container_volume 8
container_issue 1
container_start_page 1249
publishDate 2023
institution Swansea University
issn 2470-1343
2470-1343
doi_str_mv 10.1021/acsomega.2c06657
publisher American Chemical Society (ACS)
college_str Faculty of Science and Engineering
hierarchytype
hierarchy_top_id facultyofscienceandengineering
hierarchy_top_title Faculty of Science and Engineering
hierarchy_parent_id facultyofscienceandengineering
hierarchy_parent_title Faculty of Science and Engineering
department_str School of Engineering and Applied Sciences - Chemical Engineering{{{_:::_}}}Faculty of Science and Engineering{{{_:::_}}}School of Engineering and Applied Sciences - Chemical Engineering
document_store_str 1
active_str 0
description This work demonstrates a two-step gram-scale synthesis of presynthesized silver (Ag) nanoparticles impregnated with mesoporous TiO2 and evaluates their feasibility for wastewater treatment and hydrogen gas generation under natural sunlight. Paracetamol was chosen as the model pharmaceutical pollutant for evaluating photocatalytic performance. A systematic material analysis (morphology, chemical environment, optical bandgap energy) of the Ag/TiO2 photocatalyst powder was carried out, and the influence of material properties on the performance is discussed in detail. The experimental results showed that the decoration of anatase TiO2 nanoparticles (size between 80 and 100 nm) with 5 nm Ag nanoparticles (1 wt %) induced visible-light absorption and enhanced charge carrier separation. As a result, 0.01 g/L Ag/TiO2 effectively removed 99% of 0.01 g/L paracetamol in 120 min and exhibited 60% higher photocatalytic removal than pristine TiO2. Alongside paracetamol degradation, Ag/TiO2 led to the generation of 1729 μmol H2 g–1 h–1. This proof-of-concept approach for tandem pollutant degradation and hydrogen generation was further evaluated with rare earth metal (lanthanum)- and nonmetal (nitrogen)-doped TiO2, which also showed a positive response. Using a combination of ab initio calculations and our new theory model, we revealed that the enhanced photocatalytic performance of Ag/TiO2 was due to the surface Fermi-level change of TiO2 and lowered surface reaction energy barrier for water pollutant oxidation. This work opens new opportunities for exploiting tandem photocatalytic routes beyond water splitting and understanding the simultaneous reactions in metal-doped metal oxide photocatalyst systems under natural sunlight.
published_date 2023-01-10T13:09:30Z
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