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1.
J Colloid Interface Sci ; 651: 264-272, 2023 Dec.
Artigo em Inglês | MEDLINE | ID: mdl-37542901

RESUMO

Developing new and highly stable efficient photocatalysts is crucial for achieving high performance and selective photocatalytic CO2 conversion. In this paper, we designed a one-dimensional oxygen-deficient blue TiO2(B) (BT) catalyst for improved electron mobility and visible light accessibility. In addition, hexagonal ZnIn2S4 (ZIS) nanosheets with a low bandgap and great visible light accessibility are employed to produce effective heterostructures with BT. The synthesized materials are tested for photocatalytic conversion of CO2 into solar fuels (H2, CO and CH4). The optimized composite yields 71.6 and 10.3 µmol g-1h-1 of CO and CH4, three and ten times greater than ZIS, respectively. When ZIS nanosheets are combined with a one-dimensional oxygen-deficient BT catalyst, improved electron mobility and visible light accessibility are achieved, charge carriers are effectively segregated, and the transfer process is accelerated, resulting in efficient CO2 reduction. The photocatalytic CO2 conversion activity of the constructed BT/ZIS heterostructures is very stable over a 10-day (240-hour) period, and CO and CH4 production rates increase linearly with time; however, as time goes on, the rates of H2 production decrease. Further, a five-time recycling test confirmed this, revealing essentially equal activity and selectivity throughout the experiment. As a result, CO2 to CO and CH4 conversion has high selectivity and longer durability. The band structure of the BT/ZIS composite is determined using Mott-Schottky measurement, diffuse reflectance spectroscopy, and valence band X-ray photoelectron spectroscopy. This research demonstrates a novel approach to investigating effective, stable, and selective photocatalytic CO2 reduction systems for solar-to-chemical energy conversion.

2.
Environ Sci Pollut Res Int ; 30(3): 8280-8296, 2023 Jan.
Artigo em Inglês | MEDLINE | ID: mdl-36050554

RESUMO

Considering the ever-increasing need for efficient wastewater treatment, this study focused on the development of new kraft lignin-based carbon xerogel/zinc oxide (XCL/ZnO w) photocatalysts. The inclusion of the carbon xerogel is expected to cause an improvement in charge transfer throughout the photoactivation process, consequently enhancing its overall photocatalytic efficiency. Characterization shows that the materials developed are composed of both zinc oxide and carbon xerogel. The addition of the lignin-based carbon xerogel caused a significant morphological modification to the composite materials, resulting in a greater specific surface area. Regarding the photocatalytic efficiency, the optimized composite (XCL/ZnO 1.0) displayed superior efficiency to the pure zinc oxide, especially when calcined at 700 °C, with an increase of 20% in the overall photodegradation capacity for the 4-chlorophenol (4CP) molecule. The XCL/ZnO 1.0 also displayed better performance than its tannin counterpart, previously reported in the literature, obtaining a 60% increase in the apparent reaction rate constant. The XCL/ZnO 1.0 also displayed better performance for the simultaneous hexavalent chrome (Cr (VI)) reduction/4CP oxidation reaction. Salinity and system pH had a significant influence on the efficiency of the 4CP photodegradation, as higher values of salinity and lower pHs caused a decrease in the overall efficiency of the process. At last, chronoamperometry and open-circuit potential tests confirmed the superiority of the XCL/ZnO 1.0 over the pure ZnO, highlighting the beneficial impact of the carbon xerogel on the charge transport dynamics of the composite.


Assuntos
Óxido de Zinco , Óxido de Zinco/química , Lignina , Carbono , Salinidade , Catálise
3.
ACS Appl Mater Interfaces ; 10(31): 26153-26161, 2018 Aug 08.
Artigo em Inglês | MEDLINE | ID: mdl-30004215

RESUMO

Transition-metal dichalcogenide materials play a major role in the state-of-the-art innovations for energy conversion because of potential applications resulting from their unique properties. These materials additionally show inordinate potential toward the progress of hygienic power sources to deal with increasing environmental disputes at the time of skyrocketing energy demands. Herein, we report earth-abundant, few-layered, MoSe2-bridged MoS2/cadmium sulfide (CdS) nanocomposites, which reduce photogenerated electron and hole recombination by effectively separating charge carriers to achieve a high photocatalytic efficiency. Accordingly, the MoSe2-bridged MoS2/CdS system produced effective hydrogen (193 µmol·h-1) as that of water using lactic acid as a hole scavenger with the irradiation of solar light. The presence of few-layered MoSe2 bridges in MoS2/CdS successfully separates photogenerated charge carriers, thereby enhancing the shuttling of electrons on the surface to active edge sites. To the best of our knowledge, this few-layered MoSe2-bridged MoS2/CdS system exhibits the most effective concert among altogether-reported MoS2-based CdS composites. Notably, these findings with ample prospective for the development of enormously real photocatalytic systems are due to their economically viable and extraordinary efficiency.

4.
ChemSusChem ; 11(1): 245-253, 2018 01 10.
Artigo em Inglês | MEDLINE | ID: mdl-28972688

RESUMO

Designing porous nanostructures with unprecedented functionalities and an effective ability to harvest the maximum energy region of the solar spectrum and suppress the charge-carrier recombination rate offers promising potential for sustainable energy production. Although several functional porous nanostructures have been developed, high-efficiency materials are still needed. Herein, we report a new, highly active, noble-metal-free, and redox-mediator-free Z-scheme photocatalyst, CdS/Co-C@Co9 S8 , for H2 production through water splitting under solar irradiation. The designed photocatalytic system contains open 3 D CdS mesopores as a light absorber for wider solar-light harvesting. Metal-organicframework-derived cobalt nanocrystal-embedded few-layered carbon@Co9 S8 double-shelled nanocages were used as a co-semiconductor to hamper the photo charge-carrier recombination by accelerating the photogenerated electrons and holes from the other semiconductor. The optimized catalyst shows a H2 evolution rate of 26.69 mmol g-1 h-1 under simulated solar irradiation, which is 46 times higher than that of the as-synthesized CdS mesoporous nanostructures. The apparent quantum yield reached 7.82 % at λ=425 nm in 5 h. The outstanding photocatalytic activity of CdS/Co-C@Co9S8 reflects the favorable suppression of the charge-carrier recombination rate, as determined by photoluminescence, photocurrent, and impedance analyses. We believe that the findings reported here may inspire the design of new noble-metal-free porous nanohybrids for sustainable H2 production.


Assuntos
Compostos de Cádmio/química , Cobalto/química , Nanoestruturas , Processos Fotoquímicos , Sulfetos/química , Catálise , Hidrogênio/química , Microscopia Eletrônica de Transmissão , Compostos Orgânicos/química , Oxirredução , Espectroscopia Fotoeletrônica , Porosidade
5.
Chemistry ; 23(53): 13112-13119, 2017 Sep 21.
Artigo em Inglês | MEDLINE | ID: mdl-28654722

RESUMO

It is imperative to suppress the rate of recombination of photogenerated carriers to improve the semiconductor-catalyzed solar-driven production of hydrogen. To this end, photocatalysts comprising active sunlight-harvesting photo-absorbers and stable metal co-catalysts have attracted significant attention. However, the size, clean surface, and highly dispersed nature of the metal co-catalysts are crucial factors affecting catalyst performance and reaction rate. Nevertheless, most of the available metal nanocrystals have been synthesized by complex procedures using harmful organic templates and stabilizers, affording high-purity compounds with difficulty and high cost. To overcome these problems, in this study, the pulsed laser ablation in liquid approach was utilized to generate palladium and bimetallic palladium-platinum nanoparticles with an average size and distribution by adjusting the laser wavelength and fluence. A high rate of evolution of hydrogen of 130.33 mmol g-1 h-1 was obtained by using the optimized CdS-PdPt catalyst under simulated sunlight irradiation. This value is 51.31 times greater than that observed for bare CdS nanostructures. Furthermore, the amount of hydrogen evolved was significantly better than that obtained by using several other noble-metal co-catalysts deposited on CdS. This proposed strategy is thought to open new avenues for the design of advanced photocatalytic materials for efficient solar-driven production of hydrogen.

6.
ChemSusChem ; 10(7): 1563-1570, 2017 04 10.
Artigo em Inglês | MEDLINE | ID: mdl-28121391

RESUMO

Solar-driven photocatalytic hydrogen evolution is important to bring solar-energy-to-fuel energy-conversion processes to reality. However, there is a lack of highly efficient, stable, and non-precious photocatalysts, and catalysts not designed completely with expensive noble metals have remained elusive, which hampers their large-scale industrial application. Herein, for the first time, a highly efficient and stable noble-metal-free CdS/WS2 -MoS2 nanocomposite was designed through a facile hydrothermal approach. When assessed as a photocatalyst for water splitting, the CdS/WS2 -MoS2 nanostructures exhibited remarkable photocatalytic hydrogen-evolution performance and impressive durability. An excellent hydrogen evolution rate of 209.79 mmol g-1 h-1 was achieved under simulated sunlight irradiation, which is higher than the values for CdS/MoS2 (123.31 mmol g-1 h-1 ) and CdS/WS2 nanostructures (169.82 mmol g-1 h-1 ) and the expensive CdS/Pt benchmark catalyst (34.98 mmol g-1 h-1 ). The apparent quantum yield reached 51.4 % at λ=425 nm in 5 h. Furthermore, the obtained hydrogen evolution rate was better than those of several noble-metal-free catalysts reported previously. The observed high rate of hydrogen evolution and remarkable stability may be a result of the ultrafast separation of photogenerated charge carriers and transport between the CdS nanorods and the WS2 -MoS2 nanosheets, which thus increases the number of electrons involved in hydrogen production. The proposed designed strategy is believed to potentially open a door to the design of advanced noble-metal-free photocatalytic materials for efficient solar-driven hydrogen production.


Assuntos
Compostos de Cádmio/química , Dissulfetos/química , Hidrogênio/química , Molibdênio/química , Nanotubos/química , Processos Fotoquímicos , Sulfetos/química , Luz Solar , Catálise , Transporte de Elétrons , Água/química
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