Synthesis of donor-acceptor-type conjugated polymer dots as organic photocatalysts for dye degradation and hydrogen evolution

Polymer ◽  
2021 ◽  
pp. 124004
Author(s):  
Yougjin Gwon ◽  
Seonyoung Jo ◽  
Hyun-Jun Lee ◽  
Soo Young Park ◽  
Taek Seung Lee
Author(s):  
Haofan Yang ◽  
Xiaobo Li ◽  
Reiner Sebastian Sprick ◽  
Andrew I. Cooper

A library of 237 organic binary/ternary nanohybrids consisting of conjugated polymers donors and both fullerene and non-fullerene molecular acceptors was prepared and screened for sacrificial photocatalytic hydrogen evolution. These donor-acceptor nanohybrids (DANHs) showed significantly enhanced hydrogen evolution rates compared with the parent donor or acceptor compounds. DANHs of <a></a><a>a polycarbazole</a>-based donor combined with a methanofullerene acceptor (PCDTBT/PC<sub>60</sub>BM) showed a high hydrogen evolution rate of 105.2 mmol g<sup>-1</sup> h<sup>-1</sup> under visible light (λ > 420 nm). This DANH photocatalyst produced 5.9 times more hydrogen than a sulfone-containing polymer (P10) under the same conditions, which is one of the most efficient organic photocatalysts reported so far. An apparent quantum yield of hydrogen evolution of 3.0 % at 595 nm was measured for this DANH. The photocatalytic activity of the DANHs, which in optimized cases reached 179.0 mmol g<sup>-1</sup> h<sup>-1</sup>, is attributed to efficient charge transfer at the polymer donor/molecular acceptor interface. We also show that ternary donor<sub>A</sub>-donor<sub>B</sub>-acceptor nanohybrids can give higher activities than binary donor-acceptor hybrids in some cases.


2019 ◽  
Author(s):  
Haofan Yang ◽  
Xiaobo Li ◽  
Reiner Sebastian Sprick ◽  
Andrew I. Cooper

A library of 237 organic binary/ternary nanohybrids consisting of conjugated polymers donors and both fullerene and non-fullerene molecular acceptors was prepared and screened for sacrificial photocatalytic hydrogen evolution. These donor-acceptor nanohybrids (DANHs) showed significantly enhanced hydrogen evolution rates compared with the parent donor or acceptor compounds. DANHs of <a></a><a>a polycarbazole</a>-based donor combined with a methanofullerene acceptor (PCDTBT/PC<sub>60</sub>BM) showed a high hydrogen evolution rate of 105.2 mmol g<sup>-1</sup> h<sup>-1</sup> under visible light (λ > 420 nm). This DANH photocatalyst produced 5.9 times more hydrogen than a sulfone-containing polymer (P10) under the same conditions, which is one of the most efficient organic photocatalysts reported so far. An apparent quantum yield of hydrogen evolution of 3.0 % at 595 nm was measured for this DANH. The photocatalytic activity of the DANHs, which in optimized cases reached 179.0 mmol g<sup>-1</sup> h<sup>-1</sup>, is attributed to efficient charge transfer at the polymer donor/molecular acceptor interface. We also show that ternary donor<sub>A</sub>-donor<sub>B</sub>-acceptor nanohybrids can give higher activities than binary donor-acceptor hybrids in some cases.


2018 ◽  
Vol 9 (18) ◽  
pp. 5296-5302 ◽  
Author(s):  
Ziyu Wang ◽  
Yaqiang Feng ◽  
Ningning Wang ◽  
Yixiang Cheng ◽  
Yiwu Quan ◽  
...  

2019 ◽  
Vol 7 (1) ◽  
pp. 303-311 ◽  
Author(s):  
Wei Zhou ◽  
Tao Jia ◽  
Haixian Shi ◽  
Dingshan Yu ◽  
Wei Hong ◽  
...  

Pdot/g-C3N4 heterojunctions exhibit an HER of 929.3 μmol h−1 g−1 and AQE of 5.7% at 420 nm without a metallic catalyst.


2020 ◽  
Vol 10 (20) ◽  
pp. 7017
Author(s):  
Yves Ira A. Reyes ◽  
Li-Yu Ting ◽  
Xin Tu ◽  
Hsin-Yi Tiffany Chen ◽  
Ho-Hsiu Chou ◽  
...  

The application of donor-acceptor (D-A) conjugated polymer catalysts for hydrogen evolution reaction (HER) has shown great promise because of the tunability of such catalysts to have desired properties. Herein, we synthesized two polymer catalysts: poly[4,4′-(9-(4-aminophenyl)-9H-carbazole-3,6-diamine-alt-5-oxido-5-phenylbenzo[b]phosphindole-3,7-diyl)dibenzaldehyde] (PCzPO) and poly[N1,N1-bis(4-amino-2-fluorophenyl)-2-fluorobenzene-1,4-diamine-alt-5-oxido-5-phenylbenzo[b]phosphindole-3,7-diyl)dibenzaldehyde] (PNoFPO). The UV-vis absorption spectra showed that the less planar structure and the presence of electronegative fluorine atoms in the donor group of PNoFPO led to a higher optical gap compared to PCzPO, leading to almost five times faster HER rate using PCzPO compared to PNoFPO. However, density functional theory (DFT) calculations show that the frontier orbitals and the highest occupied molecular orbitals – lowest unoccupied molecular orbitals (HOMO-LUMO) gaps of PCzPO and PNoFPO D-A moiety models are very similar, such that, during light absorption, electrons move from donor to acceptor group where proton binding is preferred to happen thereafter. For both PCzPO and PNoFPO D-A moieties, H2 formation through an intramolecular reaction with a barrier of 0.6–0.7 eV, likely occurs at the acceptor group atoms where protons bind through electrostatic interaction. The intermolecular reaction has nearly zero activation energy but is expected to occur only when the repulsion is low between separate polymers chains. Finally, experimental and DFT results reveal the importance of extended configurations of D-A polymers on HER rate.


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