Molecular Engineering of Conjugated Polybenzothiadiazoles for Enhanced Hydrogen Production by Photosynthesis

Yang, Can; Chiyin, Beatriz; Zhang, Linzhu; Lin, Sen; Ghasimi, Saman; Landfester, Katharina; Zhang, Kai A. I.; Wang, Xinchen

doi:10.1002/anie.201603532

Cited by 354 publications

(286 citation statements)

References 28 publications

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“…Indeed, several linear or planarized, thus noncrosslinked and non-porous conjugated polymers have been recently shown to exhibit comparable or even better photocatalytic activities than their microporous network counterparts. 151,156,157 It is thus slightly surprising that so far no single paper on gas phase photocatalysis, e.g. CO 2 reduction has appeared as CMPs seem to be ideal candidates for such reactions.…”

Section: Cmps For Photocatalytic Hydrogen Evolutionmentioning

confidence: 99%

Trends and challenges for microporous polymers

et al. 2017

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Section: Cmps For Photocatalytic Hydrogen Evolutionmentioning

confidence: 99%

Trends and challenges for microporous polymers

et al. 2017

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“…[9] Compared to inorganic semiconductors,s oft hollow conjugated polymer spheres are more similar to biological membranes,b ut retain the added-value of light-harvesting functions and organic features for chemical modification. [10] If well developed, hollow conjugated polymers are expected to act as an ideal host scaffold for assembling dual cocatalysts to create complex nanostructures for cascade catalysis by shuttling energy and charge transfer. Theo rganic feature of the polymeric hollow structure could also enable further chemical modification of the reactive inner/outer surface.…”

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confidence: 99%

Precise Formation of a Hollow Carbon Nitride Structure with a Janus Surface To Promote Water Splitting by Photoredox Catalysis

2016

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The precise modification of redoxs pecies on the inner and outer surfaces of hollownanostructures is relevant in catalysis,surface science,and nanotechnology,but has proven difficult to achieve.H erein, we develop af acile approach to specifically fabricate Pt and Co 3 O 4 nanoparticles (NPs) onto the interior and exterior surface of hollowc arbon nitride spheres (HCNS), respectively,t op romote the surface redox functions of the polymer semiconductors.T he photocatalytic water splitting activities of HCNS with spatially separated oxidation and reduction centers at their nanodomains were enhanced. The origin of the enhanced activity was attributed to the spatially separated reactive sites for the evolution of H 2 and O 2 and also to the unidirectional migration of the electron and hole on the Janus surfaces,t hereby preventing the unwanted reverse reaction of water splitting and decreasing charge recombination.

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“…S2) [33]. A C=O stretching mode at 1,688 cm −1 is observed, and the signals at 3,426 and 1,193 cm −1 can be assigned to the -OH and C-O-C stretching modes, respectively.…”

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confidence: 93%

Fluorescein supramolecular nanosheets: A novel organic photocatalyst for visible-light-driven H2 evolution from water

Zhang

2018

Sci. China Mater.

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Photocatalytic water splitting for hydrogen evolution is one of the most promising approaches to address energy and environmental issues [1][2][3][4]. Metal-free photocatalysts, usually containing low cost and earth-abundant C, N and O elements, are more advantageous than the traditional metal-based photocatalysts and have attracted considerable interest for many years [5][6][7][8][9][10]. In the reported metal-free photocatalysts, polymer carbon nitride (PCN) is extensively studied, but the relatively large band gap (~2.7 eV) and the low activity limit its photocatalytic applications [11][12][13][14][15][16][17]. Therefore, to develop a novel wide light range and high-efficiency metal-free photocatalysts for H 2 production is very essential.Supramolecule usually refers to the molecular aggregates assembled by intermolecular interactions (hydrogen bonds) or constructed with other hybrid structures and has been used directly for energy harvesting and transformation, such as water splitting, pollutant degradation and sensor [18][19][20]. The supramolecules withflexible skeletal structure through the different molecular self-assembly patterns have larger conjugated structure, more efficient charge transfer and separation, and broader absorption range than single molecule and polymer [21,22]. Among very few supramolecular photocatalysts, although the widely reported metal-contained porphyrin hybrids have good photocatalytic performance for H 2 production, metal-free porphyrin systems present a relatively poor activity, the metal composition confines their further applications due to high cost, metals toxicity and complicated preparation process [23,24]. Recently, Zhu and co-workers [25] reported a non-covalent selfassembled perylene-3,4,9,10-tetracarboxylic diimide (PDINH) supramolecular composed of metal-free organic molecules, working as a visible-light photocatalyst for O 2 production and photodegradation. However, the conduction band (CB) of PDINH supra-molecular is (−0.049 V versus normal hydrogen electrode (NHE)); thus crippled in the application of H 2 production from water. Therefore, it is very significant to develop the easy obtained and novel metal-free supramolecular photocatalysts for H 2 production from water. The fluorescein, first synthesized in 1871, has been widely used in labelling and sensing biomolecules, as well as ophthalmology because of its high absorption in the visible region and low toxicity [26][27][28][29]. Herein, we demonstrate that the fluorescein supramolecular crystal self-assembled by single molecule is highly efficient for H 2 production from water under visible light. The morphology can be easily selfassembled into nanosheets via a simple dissolution-recrystallization process. To date, this is the first report on H 2 production under visible light over fluorescein supramolecular crystal, which extends the family of organic supramolecular photocatalytic materials. This study may open up new insights into the search of other metal-free and organic photocatalysts.We applied Gaussia...

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Molecular Engineering of Conjugated Polybenzothiadiazoles for Enhanced Hydrogen Production by Photosynthesis

Cited by 354 publications

References 28 publications

Trends and challenges for microporous polymers

Trends and challenges for microporous polymers

Precise Formation of a Hollow Carbon Nitride Structure with a Janus Surface To Promote Water Splitting by Photoredox Catalysis

Fluorescein supramolecular nanosheets: A novel organic photocatalyst for visible-light-driven H2 evolution from water

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