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1.
J Environ Manage ; 269: 110758, 2020 Sep 01.
Artigo em Inglês | MEDLINE | ID: mdl-32560988

RESUMO

Membrane separation technology is recognized as a competitive approach to remove Pb2+ from water system due to its high efficiency and low operating cost. In present study, a simple and facile approach was developed to fabricate covalent organic framework (COF) modified PVDF ultrafiltration membranes with comprehensive antifouling property and superior Pb2+ removal ability. Herein, COF was synthesised in a homogenous PVDF/DMAc solution to fabricate hydrophilic COF modified PVDF ultrafiltration membranes with the Pb2+ removal property. The filtration test demonstrated that the COF modified PVDF ultrafiltration membranes exhibited excellent antifouling property and high water flux. Moreover, the membranes showed remarkable potential for treating Pb2+-containing water. The removal efficiency was determined at 92.4%, and its removal efficiency was 87.5% at the fourth treatment cycle with Pb2+-containing water. The present work provides a valuable platform for further development of efficient composite membranes for the treatment of Pb2+-containing water.


Assuntos
Estruturas Metalorgânicas , Ultrafiltração , Chumbo , Membranas Artificiais , Polivinil
2.
Chemphyschem ; 19(20): 2717-2723, 2018 10 19.
Artigo em Inglês | MEDLINE | ID: mdl-30088324

RESUMO

Photoelectrochemical (PEC) water splitting has been demonstrated as a promising way to acquire clean hydrogen energy. However, the efficiency has been limited by the high recombination rate of photogenerated electron-hole pairs. Herein, we provided a simple approach to construct a novel SnO2 quantum dots (QDs) modified TiO2 nanorod arrays (NAs) by the calcination of SnCl2 -adsorbed TiO2 NAs. The photocurrent density of SnO2 QDs/TiO2 NAs exhibits about 5 times higher than that of parent TiO2 NAs at a bias of 0.4 V vs. Ag/AgCl. SnO2 QDs/TiO2 NAs also show a high photoelectrocatalytic activity for overall water splitting with an actual yield of H2 and O2 to be 27.85 and 11.87 µmol cm-2 h-1 , respectively. The excellent performance of photoanode for PEC water splitting could be attributed to its Z-scheme heterostructure for good separation efficiency and transport rate of photogenerated charge carries.

3.
Phys Chem Chem Phys ; 18(14): 9636-44, 2016 Apr 14.
Artigo em Inglês | MEDLINE | ID: mdl-26996319

RESUMO

This paper mainly focuses on the synergistic effect of Sn and N dopants to enhance the photocatalytic performance of anatase TiO2 under visible light or simulated solar light irradiation. The Sn and N co-doped TiO2 (SNT-x) photocatalysts were successfully prepared by the facile sol-gel method and the post-nitridation route in the temperature range of 400-550 °C. All the as-prepared samples were characterized in detail by X-ray diffraction, UV-vis diffuse reflectance spectroscopy, transmission electron microscopy, X-ray photoelectron and electron spin resonance spectroscopy and photoelectrochemical measurements. The characterization results reveal that the co-incorporation of Sn and N atoms remarkably modifies the electronic structure of TiO2, which gives rise to a prominent separation of photogenerated charge carriers and more efficient interfacial charge-transfer reactions in a photocatalytic process. The enhanced photocatalytic activity is attributed to the intensified active oxygen species including hydroxyl radicals (˙OH) and superoxide anion radicals (O2˙(-)) for degradation of organic pollutants. And the result of photocatalytic hydrogen production further confirms the existence of the synergistic effect in the SNT-x samples, because they exhibit higher photocatalytic activity than the sum of N/TiO2 and Sn/TiO2. This work provides a paradigm to consolidate the understanding of the synergistic effect of metal and non-metal co-doped TiO2 in domains of photocatalysis and photoelectrochemistry.

4.
Chemphyschem ; 16(7): 1352-5, 2015 May 18.
Artigo em Inglês | MEDLINE | ID: mdl-25712145

RESUMO

Ternary core-shell heterostructured rutile@anatase@Crx Oy nanorod arrays were elaborately designed as photoanodes for efficient photoelectrochemical water splitting under visible-light illumination. The four-fold enhanced and stabilized visible-light photocurrent highlights the unique role of the interim anatase layer in accelerating the interfacial charge transfer from the Crx Oy chromophore to rutile nanorods.

5.
Phys Chem Chem Phys ; 17(16): 10726-36, 2015 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-25811660

RESUMO

The role of polymers in artificial photosystems has been studied in detail. The photosystems were composed of tris(2,2'-bipyridyl) ruthenium(II) chloride as a photosensitizer (PS), colloidal Pt stabilized by polymer as a hydrogen-evolving catalyst and sodium ascorbate as an electron donor, without the addition of a traditional molecular electron mediator. Comprehensive insights into the production of hydrogen on irradiation with visible light were achieved. Several polymers, including neutral polyvinyl pyrrolidone, anionic poly(sodium 4-styrene sulfonate) and poly(acrylic acid) not only stabilized the nanoparticles, but were also effective in the production of hydrogen. Under the optimum conditions, an outstanding apparent quantum efficiency of 12.8% for the evolution of hydrogen was achieved. The formation of self-assembled and spatially separated donor-acceptor complexes via the non-covalent intermolecular interaction between PS and the polymer-Pt was pivotal in the efficient conversion of solar energy to hydrogen fuel. Important details of the photo-induced electron and energy transfer processes in the self-assembled artificial photosystems were determined by nanosecond transient absorption spectrometry and time-resolved fluorescence spectrometry. The initial step in the photo-catalytic production of hydrogen was a reductive quenching of the triplet excited state of the PS by sodium ascorbate, leading to a reduced form of PS, which could then be quickly quenched by the polymer. The rate-determining step was the electron transfer from PS to the catalyst via the polymer bridge.


Assuntos
2,2'-Dipiridil/análogos & derivados , Hidrogênio/química , Processos Fotoquímicos , Platina/química , Polímeros/química , 2,2'-Dipiridil/química , Ácido Ascórbico/química , Catálise , Complexos de Coordenação , Transporte de Elétrons , Nanopartículas/química , Tamanho da Partícula
6.
Phys Chem Chem Phys ; 16(24): 12521-34, 2014 Jun 28.
Artigo em Inglês | MEDLINE | ID: mdl-24830634

RESUMO

A variety of ternary nanoheterostructures composed of Pt nanoparticles (NPs), SnOx species, and anatase TiO2 are designed elaborately to explore the effect of interfacial electron transfer on photocatalytic H2 evolution from a biofuel-water solution. Among numerous factors controlling the H2 evolution, the significance of Pt sites for the H2 evolution is highlighted by tuning the loading procedure of Pt NPs and SnOx species over TiO2. A synergistic enhancement of H2 evolution can be achieved over the Pt/SnOx/TiO2 heterostructures formed by anchoring Pt NPs at atomically-isolated Sn-oxo sites, whereas the Pt/TiO2/SnOx counterparts prepared by grafting single-site Sn-oxo species on Pt/TiO2 show a marked decrease in the rate of H2 evolution. The characterization results clearly reveal that the synergy of Pt NPs and SnOx species originates from the vectorial electron transfer of TiO2 → SnOx → Pt occurring on the former, while the latter results from the competitive electron transfer from TiO2 to SnOx and to Pt NPs.


Assuntos
Hidrogênio/química , Platina/química , Compostos de Estanho/química , Titânio/química , Catálise , Microscopia Eletrônica de Transmissão , Difração de Raios X
7.
Sci Rep ; 5: 16947, 2015 Nov 19.
Artigo em Inglês | MEDLINE | ID: mdl-26582652

RESUMO

Herein, we reported a octahedral Cd3(C3N3S3)2 coordination polymer as a new noble metal-free photocatalyst for robust photocatalytic H2O2 production from methanol/water solution. The coordination polymer can give an unprecedented H2O2 yield of ca. 110.0 mmol • L(-1) • g(-1) at pH = 2.8 under visible light illumination. The characterization results clearly revealed that the photocatalytic H2O2 production proceeds by a pathway of two-electron reduction of O2 on the catalyst surface. This work showed the potential perspective of Mx(C3N3S3)y (M = transitional metals) coordination polymers as a series of new materials for solar energy storage and conversion.

8.
ChemSusChem ; 7(9): 2537-44, 2014 Sep.
Artigo em Inglês | MEDLINE | ID: mdl-25045039

RESUMO

In this work, CdS quantum dots (QDs) supported on Ga2O3 and In2O3 are applied for visible-light-driven H2 evolution from aqueous solutions that contain lactic acid. With Pt as the cocatalyst, the H2 evolution rates on CdS/Pt/Ga2O3 and CdS/Pt/In2O3 are as high as 995.8 and 1032.2 µmol h(-1), respectively, under visible light (λ>420 nm) with apparent quantum efficiencies of 43.6 and 45.3% obtained at 460 nm, respectively. These are much higher than those on Pt/CdS (108.09 µmol h(-1)), Pt/Ga2O3 (0.12 µmol h(-1)), and Pt/In2O3 (0.05 µmol h(-1)). The photocatalysts have been characterized thoroughly and their band structures and photocurrent responses have been measured. The band alignment between the CdS QDs and In2O3 can lead to interfacial charge separation, which cannot occur between the CdS QDs and Ga2O3. Among the various possible factors that contribute to the high H2 evolution rates on CdS/Pt/oxide, the surface properties of the metal oxides play important roles, which include (i) the anchoring of CdS QDs and Pt nanoparticles for favorable interactions and (ii) the efficient trapping of photogenerated electrons from the CdS QDs because of surface defects (such as oxygen defects) based on photoluminescence and photocurrent studies.


Assuntos
Compostos de Cádmio/química , Gálio/química , Hidrogênio/química , Índio/química , Luz , Pontos Quânticos/química , Sulfetos/química , Água/química , Processos Fotoquímicos
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