Facile Synthesis of Gram-Scale Mesoporous Ag/TiO2 Photocatalysts for Pharmaceutical Water Pollutant Removal and Green Hydrogen Generation

被引:21
作者
Cherif, Yassine [1 ]
Azzi, Hajer [1 ,5 ]
Sridharan, Kishore [2 ]
Ji, Seulgi [3 ]
Choi, Heechae [3 ]
Allan, Michael G. [4 ]
Benaissa, Sihem [5 ,6 ]
Saidi-Bendahou, Karima [1 ]
Damptey, Lois [7 ]
Ribeiro, Camila Silva [7 ]
Krishnamurthy, Satheesh [7 ]
Nagarajan, Sanjay [8 ]
Maroto-Valer, M. Mercedes [9 ]
Kuehnel, Moritz F. [4 ,10 ]
Pitchaimuthu, Sudhagar [9 ]
机构
[1] Univ Tlemcen, Lab Catalyse & Synth Chim Organ, Tilimsen 13000, Algeria
[2] Univ Calicut, Sch Phys Sci, Dept Nanosci & Technol, PO Thenhipalam, Thenhipalam 673635, India
[3] Univ Cologne, Inst Inorgan Chem, Theoret Mat & Chem Grp, D-50939 Cologne, Germany
[4] Swansea Univ, Dept Chem, Swansea SA2 8PP, W Glam, Wales
[5] Univ Ain Temouchent, Inst Sci & La Technol, Ain Temouchent 46000, Algeria
[6] High Natl Sch Publ Works, BP 32 Rue Sidi Garidi, Kouba, Alger, Algeria
[7] Open Univ, Sch Engn & Innovat, Milton Keynes MK7 6AA, Bucks, England
[8] Univ Bath, Dept Chem Engn, Bath BA2 7AY, Avon, England
[9] Heriot Watt Univ, Res Ctr Carbon Solut, Sch Engn & Phys Sci, Inst Mech & Proc Engn, Edinburgh EH14 4AS, Midlothian, Scotland
[10] Fraunhofer Inst Wind Energy Syst IWES, D-06237 Leuna, Germany
来源
ACS OMEGA | 2023年 / 8卷 / 01期
基金
英国工程与自然科学研究理事会;
关键词
GENERALIZED GRADIENT APPROXIMATION; TOTAL-ENERGY CALCULATIONS; DOPED TIO2; WASTE-WATER; H-2; EVOLUTION; SURFACE-AREA; ANATASE TIO2; DEGRADATION; OXIDATION; NANOPARTICLES;
D O I
10.1021/acsomega.2c06657
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
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 smol 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.
引用
收藏
页码:1249 / 1261
页数:13
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