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2. Reconstructed covalent organic frameworks

Author

Zhang, Weiwei, Chen, Linjiang, Dai, Sheng, Zhao, Chengxi, Ma, Cheng, Wei, Lei, Zhu, Minghui, Chong, Samantha Y., Yang, Haofan, Liu, Lunjie, Bai, Yang, Yu, Miaojie, Xu, Yongjie, Zhu, Xiao-Wei, Zhu, Qiang, An, Shuhao, Sprick, Reiner Sebastian, Little, Marc A., Wu, Xiaofeng, Jiang, Shan, Wu, Yongzhen, Zhang, Yue-Biao, Tian, He, Zhu, Wei-Hong, and Cooper, Andrew I.

Published
2022
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6. Non-conventional bulk heterojunction nanoparticle photocatalysts for sacrificial hydrogen evolution from water.

Author

Mistry, Jai-Ram, McQueen, Ewan, Nudelman, Fabio, Sprick, Reiner Sebastian, and Wright, Iain A.

Abstract

Photocatalyst systems combining donor polymers with acceptor molecules have shown the highest evolution rates for sacrificial hydrogen production from water for organic systems to date. Here, new donor molecules have been designed and synthesised taking inspiration from the structure–performance relationships which have been established in the development of non-fullerene acceptors. While a conventional bulk heterojunction (BHJ) pairing consists of a donor polymer and acceptor small molecule, here we have successfully reversed this approach by using new p-type small molecules in combination with a n-type conjugated polymer to produce non-conventional BHJ (ncBHJ) nanoparticles. We have applied these ncBHJs as photocatalysts in the sacrificial hydrogen evolution from water, and the best performing heterojunction displayed high activity for sacrificial hydrogen production from water with a hydrogen evolution rate of 22 321 μmol h−1 g−1 which compares well with the state-of-the-art for conventional BHJ photocatalyst systems. [ABSTRACT FROM AUTHOR]

Published
2024
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9. A mobile robotic chemist

Author

Burger, Benjamin, Maffettone, Phillip M., Gusev, Vladimir V., Aitchison, Catherine M., Bai, Yang, Wang, Xiaoyan, Li, Xiaobo, Alston, Ben M., Li, Buyi, Clowes, Rob, Rankin, Nicola, Harris, Brandon, Sprick, Reiner Sebastian, and Cooper, Andrew I.

Published
2020
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10. Polytriarylamines containing fused ring and heterocyclic structures prepared using N-heterocyclic carbene complexes of palladium

Author

Sprick, Reiner Sebastian and Turner, Michael

Subjects
547, Semiconducting polymer, Buchwald-Hartwig coupling, N-heterocyclic carbene, polytriarylamine
Abstract

For the preparation of semiconducting polymers often ‘standard’ catalytic systems are used without further optimisation. New ligands, such as N-heterocyclic carbenes have shown excellent activity in cross-coupling reactions (e.g. Suzuki-Miyaura reaction, or Hartwig-Buchwald amination). These systems show excellent conversions under mild conditions and even allow the use of aryl chlorides as reagents. Nevertheless, previously no system has been reported for the synthesis of conjugated polymers, e.g. the Suzuki polycondensation or Buchwald-Hartwig type polycondensation using these catalysts. A NHC-Pd based catalytic system was optimised for a polyamination reaction and the catalyst [(IPr)Pd(allyl)Cl] was found to be the most active. Polytriarylamines were synthesised using the optimised catalytic system and tested in organic field-effect transistors. Mobilities found were low which was found to be attributed to the presence of high molecular weight fractions. Molecular weights were controlled using an in situ end-capping approach and polymers tested in the semiconducting layer of OFETs gave similar mobilities tothose reported earlier. Several polytriarylamines, which have not been reported previously, were synthesised using NHC-chemistry and the in situ end-cappingapproach, as well as polytriarylamines that have been reported previously using Pd/phosphine catalysts. One library containing polymers based on biphenyles andbridged biphenyles and another library containing polymers with bridged oligoarenes were synthesised. Suzuki polycondensation was also studied besides the polyamination protocol and low catalyst loadings and reaction temperatures could be realised using a NHC-Pd catalyst. Sulfur containing monomers that could not be polymerised using the polyamination were polymerised successfully. All polymers were fully characterised and studied as the active layer in organic field-effect transistors. The highest mobilities determined for these polymers (~10-2 cm2/Vs) is close to the highest reported for this class of polymer reported to date.

Published
2013

12. Conjugated Polymer/Recombinant Escherichia coliBiohybrid Systems for Photobiocatalytic Hydrogen Production

Author

Yang, Ying, Zwijnenburg, Martijn A., Gardner, Adrian M., Adamczyk, Sylwia, Yang, Jing, Sun, Yaqi, Jiang, Qiuyao, Cowan, Alexander J., Sprick, Reiner Sebastian, Liu, Lu-Ning, and Cooper, Andrew I.

Abstract

Biohybrid photocatalysts are composite materials that combine the efficient light-absorbing properties of synthetic materials with the highly evolved metabolic pathways and self-repair mechanisms of biological systems. Here, we show the potential of conjugated polymers as photosensitizers in biohybrid systems by combining a series of polymer nanoparticles with engineered Escherichia colicells. Under simulated solar light irradiation, the biohybrid system consisting of fluorene/dibenzo [b,d]thiophene sulfone copolymer (LP41) and recombinant E. coli(i.e., a LP41/HydA BL21 biohybrid) shows a sacrificial hydrogen evolution rate of 3.442 mmol g–1h–1(normalized to polymer amount). It is over 30 times higher than the polymer photocatalyst alone (0.105 mmol g–1h–1), while no detectable hydrogen was generated from the E. colicells alone, demonstrating the strong synergy between the polymer nanoparticles and bacterial cells. The differences in the physical interactions between synthetic materials and microorganisms, as well as redox energy level alignment, elucidate the trends in photochemical activity. Our results suggest that organic semiconductors may offer advantages, such as solution processability, low toxicity, and more tunable surface interactions with the biological components over inorganic materials.

Published
2024
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17. Making the connections : physical and electric interactions in biohybrid photosynthetic systems

Author

Yang, Ying, Liu, Lu-Ning, Tian, Haining, Cooper, Andrew I., Sprick, Reiner Sebastian, Yang, Ying, Liu, Lu-Ning, Tian, Haining, Cooper, Andrew I., and Sprick, Reiner Sebastian

Abstract

Biohybrid photosynthesis systems, which combine biological and non-biological materials, have attracted recent interest in solar-to-chemical energy conversion. However, the solar efficiencies of such systems remain low, despite advances in both artificial photosynthesis and synthetic biology. Here we discuss the potential of conjugated organic materials as photosensitisers for biological hybrid systems compared to traditional inorganic semiconductors. Organic materials offer the ability to tune both photophysical properties and the specific physicochemical interactions between the photosensitiser and biological cells, thus improving stability and charge transfer. We highlight the state-of-the-art and opportunities for new approaches in designing new biohybrid systems. This perspective also summarises the current understanding of the underlying electron transport process and highlights the research areas that need to be pursued to underpin the development of hybrid photosynthesis systems. Biohybrid systems of synthetic materials and microorganisms can be obtained using a range of assembly strategies based on their interactions. This influences charge transfer between the components and their efficiency for solar fuels generation.

Published
2023
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24. Photocatalytic Overall Water Splitting Under Visible Light Enabled by a Particulate Conjugated Polymer Loaded with Palladium and Iridium**

Author

Bai, Yang, primary, Li, Chao, additional, Liu, Lunjie, additional, Yamaguchi, Yuichi, additional, Bahri, Mounib, additional, Yang, Haofan, additional, Gardner, Adrian, additional, Zwijnenburg, Martijn A., additional, Browning, Nigel D., additional, Cowan, Alexander J., additional, Kudo, Akihiko, additional, Cooper, Andrew I., additional, and Sprick, Reiner Sebastian, additional

Published
2022
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27. Photocatalytic overall water splitting under visible light enabled by a particulate conjugated polymer loaded with iridium

Author

Bai, Yang, primary, Li, Chao, additional, Liu, Lunjie, additional, Yamaguchi, Yuichi, additional, Mounib, Bahri, additional, Yang, Haofan, additional, Gardner, Adrian, additional, Zwijnenburg, Martijn, additional, Browning, Nigel, additional, Cowan, Alexander, additional, Kudo, Akihiko, additional, Cooper, Andrew, additional, and Sprick, Reiner Sebastian, additional

Published
2022
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32. Time-Resolved Raman Spectroscopy of Polaron Formation in a Polymer Photocatalyst

Author

Piercy, Verity L., primary, Saeed, Khezar H., additional, Prentice, Andrew W., additional, Neri, Gaia, additional, Li, Chao, additional, Gardner, Adrian M., additional, Bai, Yang, additional, Sprick, Reiner Sebastian, additional, Sazanovich, Igor V., additional, Cooper, Andrew I., additional, Rosseinsky, Matthew J., additional, Zwijnenburg, Martijn A., additional, and Cowan, Alexander J., additional

Published
2021
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33. A stable covalent organic framework for photocatalytic carbon dioxide reduction† †Electronic supplementary information (ESI) available. See DOI: 10.1039/c9sc03800k

Author

Fu, Zhiwei, Wang, Xiaoyan, Gardner, Adrian M., Wang, Xue, Chong, Samantha Y., Neri, Gaia, Cowan, Alexander J., Liu, Lunjie, Li, Xiaobo, Vogel, Anastasia, Clowes, Rob, Bilton, Matthew, Chen, Linjiang, Sprick, Reiner Sebastian, and Cooper, Andrew I.

Subjects
Chemistry
Abstract

A metal-decorated alkene-linked covalent organic framework is a robust, selective photocatalyst for CO2 reduction., Photocatalytic conversion of CO2 into fuels is an important challenge for clean energy research and has attracted considerable interest. Here we show that tethering molecular catalysts—a rhenium complex, [Re(bpy)(CO)3Cl]—together in the form of a crystalline covalent organic framework (COF) affords a heterogeneous photocatalyst with a strong visible light absorption, a high CO2 binding affinity, and ultimately an improved catalytic performance over its homogeneous Re counterpart. The COF incorporates bipyridine sites, allowing for ligation of the Re complex, into a fully π-conjugated backbone that is chemically robust and promotes light-harvesting. A maximum rate of 1040 μmol g–1 h–1 for CO production with 81% selectivity was measured. CO production rates were further increased up to 1400 μmol g–1 h–1, with an improved selectivity of 86%, when a photosensitizer was added. Addition of platinum resulted in production of syngas, hence, the co-formation of H2 and CO, the chemical composition of which could be adjusted by varying the ratio of COF to platinum. An amorphous analog of the COF showed significantly lower CO production rates, suggesting that crystallinity of the COF is beneficial to its photocatalytic performance in CO2 reduction.

Published
2019

34. Mapping binary copolymer property space with neural networks† †Electronic supplementary information (ESI) available: Training data (before and after calibration), co-polymer optoelectronic property space data and associated SMILES for all copolymer compositions, machine learning model and training parameters, Python module (pychemlp, ref. 61) for recreating fingerprints, model and data. Raw data can be accessed freely via a GitHub repository (https://github.com/ZwijnenburgGroup/2019-polymer-neural-network). See DOI: 10.1039/c8sc05710a

Author

Wilbraham, Liam, Sprick, Reiner Sebastian, Jelfs, Kim E., and Zwijnenburg, Martijn A.

Subjects
Condensed Matter::Soft Condensed Matter, Quantitative Biology::Biomolecules, Chemistry, Computer Science::Emerging Technologies, Computer Science::Databases
Abstract

We map the property space of binary copolymers to understand how copolymerisation can be used to tune the optoelectronic properties of polymers., The extremely large number of unique polymer compositions that can be achieved through copolymerisation makes it an attractive strategy for tuning their optoelectronic properties. However, this same attribute also makes it challenging to explore the resulting property space and understand the range of properties that can be realised. In an effort to enable the rapid exploration of this space in the case of binary copolymers, we train a neural network using a tiered data generation strategy to accurately predict the optical and electronic properties of 350 000 binary copolymers that are, in principle, synthesizable from their dihalogen monomers via Yamamoto, or Suzuki–Miyaura and Stille coupling after one-step functionalisation. By extracting general features of this property space that would otherwise be obscured in smaller datasets, we identify simple models that effectively relate the properties of these copolymers to the homopolymers of their constituent monomers, and challenge common ideas behind copolymer design. We find that binary copolymerisation does not appear to allow access to regions of the optoelectronic property space that are not already sampled by the homopolymers, although it conceptually allows for more fine-grained property control. Using the large volume of data available, we test the hypothesis that copolymerisation of ‘donor’ and ‘acceptor’ monomers can result in copolymers with a lower optical gap than their related homopolymers. Overall, despite the prevalence of this concept in the literature, we observe that this phenomenon is relatively rare, and propose conditions that greatly enhance the likelihood of its experimental realisation. Finally, through a ‘topographical’ analysis of the co-polymer property space, we show how this large volume of data can be used to identify dominant monomers in specific regions of property space that may be amenable to a variety of applications, such as organic photovoltaics, light emitting diodes, and thermoelectrics.

Published
2019

35. Integrated Covalent Organic Framework/Carbon Nanotube Composite as Li‐Ion Positive Electrode with Ultra‐High Rate Performance

Author

Gao, Hui, primary, Zhu, Qiang, additional, Neale, Alex R., additional, Bahri, Mounib, additional, Wang, Xue, additional, Yang, Haofan, additional, Liu, Lunjie, additional, Clowes, Rob, additional, Browning, Nigel D., additional, Sprick, Reiner Sebastian, additional, Little, Marc A., additional, Hardwick, Laurence J., additional, and Cooper, Andrew I., additional

Published
2021
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46. Correction to “Tracking Charge Transfer to Residual Metal Clusters in Conjugated Polymers for Photocatalytic Hydrogen Evolution”

Author

Sachs, Michael, primary, Cha, Hyojung, additional, Kosco, Jan, additional, Aitchison, Catherine M., additional, Francàs, Laia, additional, Corby, Sacha, additional, Chiang, Chao-Lung, additional, Wilson, Anna A., additional, Godin, Robert, additional, Fahey-Williams, Alexander, additional, Cooper, Andrew I., additional, Sprick, Reiner Sebastian, additional, McCulloch, Iain, additional, and Durrant, James R., additional

Published
2020
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48. Covalent Organic Framework Nanosheets Embedding Single Cobalt Sites for Photocatalytic Reduction of Carbon Dioxide

Author

Wang, Xiaoyan, primary, Fu, Zhiwei, additional, Zheng, Lirong, additional, Zhao, Chengxi, additional, Wang, Xue, additional, Chong, Samantha Y., additional, McBride, Fiona, additional, Raval, Rasmita, additional, Bilton, Matthew, additional, Liu, Lunjie, additional, Wu, Xiaofeng, additional, Chen, Linjiang, additional, Sprick, Reiner Sebastian, additional, and Cooper, Andrew I., additional

Published
2020
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