School of Chemistry - Research Publications

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    Pyridine End-Capped Polymer to Stabilize Organic Nanoparticle Dispersions for Solar Cell Fabrication through Reversible Pyridinium Salt Formation
    Saxena, S ; Marlow, P ; Subbiah, J ; Colsmann, A ; Wong, WWH ; Jones, DJ (AMER CHEMICAL SOC, 2021-08-04)
    Bulk-heterojunction nanoparticle dispersions in water or alcohol can be employed as eco-friendly inks for the fabrication of organic solar cells by printing or coating. However, one major drawback is the need for stabilizing surfactants, which facilitate nanoparticle formation but later hamper device performance. When surfactant-free dispersions are formulated, a strong limitation is imposed by the dispersion concentration due to the tendency of nanoparticles to aggregate. In this work, pyridine end-capped poly(3-hexylthiophene) (P3HT-Py) is synthesized and included as an additive for the stabilization of P3HT:indene-C60 bis-adduct (ICBA) nanoparticle dispersions. In the presence of acetic acid (AcOH), a surface-active pyridinium acetate end-capped P3HT ion pair, P3HT-PyH+AcO-, is formed which effectively stabilizes the dispersion and hence allows the formation of dispersions with smaller nanoparticle sizes and higher concentrations of up to 30 mg/mL in methanol. The dispersions exhibit an enhanced shelf-lifetime of at least 60 days at room temperature. After the deposition of light-harvesting layers from the nanoparticle dispersions, the ion-pair formation is reversed at elevated temperatures leading to regeneration of P3HT-Py and AcOH. The AcOH evaporates from the active layer, while the performance of the corresponding solar cells is not affected by the residual P3HT-Py in the devices. Enhanced nanoparticle stability is achieved with only 0.017 wt % pyridine in the P3HT/ICBA formulation.
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    Controlled synthesis of poly(3-hexylthiophene) in continuous flow
    Seyler, H ; Subbiah, J ; Jones, DJ ; Holmes, AB ; Wong, WWH (BEILSTEIN-INSTITUT, 2013-07-25)
    There is an increasing demand for organic semiconducting materials with the emergence of organic electronic devices. In particular, large-area devices such as organic thin-film photovoltaics will require significant quantities of materials for device optimization, lifetime testing and commercialization. Sourcing large quantities of materials required for the optimization of large area devices is costly and often impossible to achieve. Continuous-flow synthesis enables straight-forward scale-up of materials compared to conventional batch reactions. In this study, poly(3-hexylthiophene), P3HT, was synthesized in a bench-top continuous-flow reactor. Precise control of the molecular weight was demonstrated for the first time in flow for conjugated polymers by accurate addition of catalyst to the monomer solution. The P3HT samples synthesized in flow showed comparable performance to commercial P3HT samples in bulk heterojunction solar cell devices.
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    Bulk Heterojunction Nanomorphology of Fluorenyl Hexa-peri-hexabenzocoronene-Fullerene Blend Films
    Pfaff, M ; Mueller, P ; Bockstaller, P ; Mueller, E ; Subbiah, J ; Wong, WWH ; Klein, MFG ; Kiersnowski, A ; Puniredd, SR ; Pisula, W ; Colsmann, A ; Gerthsen, D ; Jones, DJ (AMER CHEMICAL SOC, 2013-11-27)
    In this study, the nanomorphology of fluorenyl hexa-peri-hexabenzocoronene:[6,6]-phenyl C61-butyric acid methyl ester (FHBC:PC61BM) absorber layers of organic solar cells was investigated. Different electron microscopical techniques, atomic force microscopy, and grazing incidence wide-angle X-ray scattering were applied for a comprehensive nanomorphology analysis. The development of the nanomorphology upon sample annealing and the associated change of the device performance were investigated. It was shown that the annealing process enhances the phase separation and therefore the bulk heterojunction structure. Due to π-π stacking, the FHBC molecules assemble into columnar stacks, which are already present before annealing. While the nonannealed sample consists of a mixture of homogeneously distributed PC61BM molecules and FHBC stacks with a preferential in-plane stack orientation, crystalline FHBC precipitates occur in the annealed samples. These crystals, which consist of hexagonal arranged FHBC stacks, grow with increased annealing time. They are distributed homogeneously over the whole volume of the absorber layer as revealed by electron tomography. The FHBC stacks, whether in the two phase mixture or in the pure crystalline precipitates, exhibit an edge-on orientation, according to results from grazing incidence wide-angle X-ray scattering (GIWAXS), dark-field transmission electron microscopy (DF TEM) imaging and selective area electron diffraction (SAED). The best solar cell efficiencies were obtained after 20 or 40 s sample annealing. These annealing times induce an optimized degree of phase separation between donor and acceptor material.
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    Benzotriazole-based donor-acceptor conjugated polymers with a broad absorption in the visible range
    Wong, WWH ; Subbiah, J ; Puniredd, SR ; Pisula, W ; Jones, DJ ; Holmes, AB (ROYAL SOC CHEMISTRY, 2014-02-21)
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    Thiazolyl substituted benzodithiophene copolymers: synthesis, properties and photovoltaic applications
    Xiao, Z ; Subbiah, J ; Sun, K ; Ji, S ; Jones, DJ ; Holmes, AB ; Wong, WWH (Royal Society of Chemistry, 2014)
    Three new conjugated polymers based on 5-decylthiazol-2-yl substituted benzodithiophene have been synthesized by Stille cross-coupling polymerization. 1,3-Dibromo-5-octylthieno[3,4-c]pyrrole-4,6-dione (M1), 2,5-diethylhexyl-3,6-bis(5-bromothiophen-2-yl)pyrrolo[3,4-c]-pyrrole-1,4-dione (M2) and 4,6-dibromo-thieno[3,4-b]thiophene-2-dodecyl carboxylate (M3) were used as acceptor building blocks for the synthesis of conjugated donor-acceptor polymers. The thermal, optical, electrochemical, and photovoltaic properties of the synthesized polymers were studied.
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    Single Isomer of Indene-C70 Bisadduct-Isolation and Performance in Bulk Heterojunction Solar Cells
    Wong, WWH ; Subbiah, J ; White, JM ; Seyler, H ; Zhang, B ; Jones, DJ ; Holmes, AB (AMER CHEMICAL SOC, 2014-02-25)
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    Organic Solar Cells Using a High-Molecular-Weight Benzodithiophene-Benzothiadiazole Copolymer with an Efficiency of 9.4%
    Subbiah, J ; Purushothaman, B ; Chen, M ; Qin, T ; Gao, M ; Vak, D ; Scholes, FH ; Chen, X ; Watkins, SE ; Wilson, GJ ; Holmes, AB ; Wong, WWH ; Jones, DJ (WILEY-V C H VERLAG GMBH, 2015-01-27)
    A high molecular weight donor-acceptor conjugated polymer is synthesized using the Suzuki polycondensation method. Using this polymer, a single-junction bulk-heterojunction solar cell is fabricated giving a power conversion efficiency of 9.4% using a fullerene-modified ZnO interlayer at the cathode contact.
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    Fullerene peapod nanoparticles as an organic semiconductor-electrode interface layer
    Ren, JM ; Subbiah, J ; Zhang, B ; Ishitake, K ; Satoh, K ; Kamigaito, M ; Qiao, GG ; Wong, EHH ; Wong, WWH (ROYAL SOC CHEMISTRY, 2016)
    A syndiotactic poly(methyl methacrylate) bottlebrush polymer has been shown to complex with C60 fullerene and assemble into nanoparticles that can be dispersed in polar organic solvents. This composite material was used as an electrode interlayer in organic solar cell (OSC) devices leading to enhanced device performance.
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    Plasma deposition of organic polymer films for solar cell applications
    Wong, WWH ; Rudd, S ; Ostrikov, K ; Ramiasa-MacGregor, M ; Subbiah, J ; Vasilev, K (ELSEVIER SCIENCE BV, 2016-05)
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    Development of a High-Performance Donor Acceptor Conjugated Polymer: Synergy in Materials and Device Optimization
    Gao, M ; Subbiah, J ; Geraghty, PB ; Chen, M ; Purushothaman, B ; Chen, X ; Qin, T ; Vak, D ; Scholes, FH ; Watkins, SE ; Skidmore, M ; Wilson, GJ ; Holmes, AB ; Jones, DJ ; Wong, WWH (AMER CHEMICAL SOC, 2016-05-24)