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Enhanced Photocatalytic Hydrogen Production Activity by Constructing a Robust Organic-Inorganic Hybrid Material Based Fulvalene and TiO₂.

ABSTRACT: A novel redox-active organic-inorganic hybrid material (denoted as H₄TTFTB-TiO₂) based on tetrathiafulvalene derivatives and titanium dioxide with a micro/mesoporous nanomaterial structure has been synthesized via a facile sol-gel method. In this study, tetrathiafulvalene-3,4,5,6-tetrakis(4-benzoic acid) (H₄TTFTB) is an ideal electron-rich organic material and has been introduced into TiO₂ for promoting photocatalytic H₂ production under visible light irradiation. Notably, the optimized composites demonstrate remarkably enhanced photocatalytic H₂ evolution performance with a maximum H₂ evolution rate of 1452 μmol g^-1 h^-1, which is much higher than the prototypical counterparts, the common dye-sensitized sample (denoted as H₄TTFTB-5.0/TiO₂) (390.8 μmol g^-1 h^-1) and pure TiO₂ (18.87 μmol g^-1 h^-1). Moreover, the composites perform with excellent stability even after being used for seven time cycles. A series of characterizations of the morphological structure, the photoelectric physics performance and the photocatalytic activity of the hybrid reveal that the donor-acceptor structural H₄TTFTB and TiO₂ have been combined robustly by covalent titanium ester during the synthesis process, which improves the stability of the hybrid nanomaterials, extends visible-light adsorption range and stimulates the separation of photogenerated charges. This work provides new insight for regulating precisely the structure of the fulvalene-based composite at the molecule level and enhances our in-depth fundamental understanding of the photocatalytic mechanism.

SUBMITTER: Wang M

PROVIDER: S-EPMC9182102 | biostudies-literature | 2022 Jun

REPOSITORIES: biostudies-literature

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Enhanced Photocatalytic Hydrogen Production Activity by Constructing a Robust Organic-Inorganic Hybrid Material Based Fulvalene and TiO2.

Wang Mengyuan M Su Shizhuo S Zhong Xin X Kong Derui D Li Bo B Song Yujie Y Jia Chunman C Chen Yifan Y

Nanomaterials (Basel, Switzerland) 20220603 11

A novel redox-active organic-inorganic hybrid material (denoted as H4TTFTB-TiO2) based on tetrathiafulvalene derivatives and titanium dioxide with a micro/mesoporous nanomaterial structure has been synthesized via a facile sol-gel method. In this study, tetrathiafulvalene-3,4,5,6-tetrakis(4-benzoic acid) (H4TTFTB) is an ideal electron-rich organic material and has been introduced into TiO2 for promoting photocatalytic H2 production under vis ...[more]

PMID: 35683773

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Project description:The photocatalytic production of hydrogen using biopolymer-immobilized titanium dioxide (TiO2) is an innovative and sustainable approach to renewable energy generation. TiO2, a well-known photocatalyst, benefits from immobilization on biopolymers due to its environmental friendliness, abundance, and biodegradability. In another way, to boost the efficiency of TiO2, its surface properties can be modified by incorporating co-catalysts like platinum (Pt) to improve charge separation. In this work, the surface of commercial TiO2 PC500 was modified with Pt nanoparticles (Pt1%@PC500) and then immobilized on glass surfaces using polyhydroxyalkanoate biopolymer poly(hydroxybutyrate-co-hydroxyhexanoate) (PHBH). The as-prepared immobilized Pt-modified TiO2 photocatalysts were fully characterized using various physicochemical techniques. The photocatalytic activity of the photocatalyst film was investigated for photocatalytic hydrogen production through water reduction using ethanol as a sacrificial donor. The impact of the film preparation conditions, e.g., PHBH concentration, PHBH:catalyst ratio, and temperature, on activity and stability was studied in detail. The application of biopolymer PHBH as a binder provides a green alternative to conventional immobilization methods, and with the application of PHBH, a stable and active photocatalyst film that showed lower activity compared to that of the suspended photocatalyst but good recyclability in six runs was prepared. A long-term photocatalytic hydrogen production experiment was carried out. In 98 h of operation, 12 mmol of hydrogen was produced in three consecutive runs with a PHBH/Pt1%@PC500 film having an area of ∼5.3 cm2. A significantly lower hydrogen productivity was observed after the first run, possibly due to a change in film structure, but thereafter, the productivity remained almost constant for the second and third runs. Hydrogen was the main product in the gas phase (90%), but carbon dioxide (4-5%) and methane (4-5%) were obtained as important byproducts. The byproducts are a consequence of the use of the sacrificial reagent ethanol. The results of the film performance are very promising, with regard to large-scale continuous hydrogen production.

Dataset Information

Enhanced Photocatalytic Hydrogen Production Activity by Constructing a Robust Organic-Inorganic Hybrid Material Based Fulvalene and TiO₂.

Publications

Enhanced Photocatalytic Hydrogen Production Activity by Constructing a Robust Organic-Inorganic Hybrid Material Based Fulvalene and TiO<sub>2</sub>.

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