Publications

@article{matthews2016synthesis,

title = {Synthesis and extensive characterisation of phosphorus doped graphite},

author = {Peter D Matthews and Timothy C King and Hugh Glass and Pieter CMM Magusin and Gary J Tustin and Philip AC Brown and Jonathan A Cormack and Ra{'u}l Garc{'i}a-Rodr{'i}guez and Michal Leskes and Si{^a}n E Dutton and others},

url = {https://pubs.rsc.org/am/content/articlelanding/2016/ra/c6ra08639j/unauth#!divAbstract},

year  = {2016},

date = {2016-01-01},

journal = {RSC advances},

volume = {6},

number = {67},

pages = {62140--62145},

publisher = {Royal Society of Chemistry},

abstract = {The pyrolysis of 1,2-diphosphinobenzene at 800 °C gives a phosphorus-doped graphite (P-DG) with an unprecedented high phosphorus content, ca. 20 at%. In contrast with previously studied boron and nitrogen doped graphite materials, thorough characterisation and analysis of this material demonstrates that it is extensively disordered and contains substitutional P-atoms along with P[double bond, length as m-dash]O units in the host graphitic lattice, as well as P4 molecules trapped between the graphitic sheets. This represents a stabilised form of P4, which has been shown to covalently bind to lithium as Li3P in this material.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{keyzer2016mg,

title = {Mg (PF6) 2-based electrolyte systems: understanding electrolyte--electrode interactions for the development of mg-ion batteries},

author = {Evan N Keyzer and Hugh FJ Glass and Zigeng Liu and Paul M Bayley and Siân E Dutton and Clare P Grey and Dominic S Wright},

url = {https://pubs.acs.org/doi/abs/10.1021/jacs.6b04319},

year  = {2016},

date = {2016-01-01},

journal = {Journal of the American Chemical Society},

volume = {138},

number = {28},

pages = {8682--8685},

publisher = {American Chemical Society},

abstract = {Mg(PF6)2-based electrolytes for Mg-ion batteries have not received the same attention as the analogous LiPF6-based electrolytes used in most Li-ion cells owing to the perception that the PF6– anion decomposes on and passivates Mg electrodes. No synthesis of the Mg(PF6)2 salt has been reported, nor have its solutions been studied electrochemically. Here, we report the synthesis of the complex Mg(PF6)2(CH3CN)6 and its solution-state electrochemistry. Solutions of Mg(PF6)2(CH3CN)6 in CH3CN and CH3CN/THF mixtures exhibit high conductivities (up to 28 mS·cm–1) and electrochemical stability up to at least 4 V vs Mg on Al electrodes. Contrary to established perceptions, Mg electrodes are observed to remain electrochemically active when cycled in the presence of these Mg(PF6)2-based electrolytes, with no fluoride (i.e., MgF2) formed on the Mg surface. Stainless steel electrodes are found to corrode when cycled in the presence of Mg(PF6)2 solutions, but Al electrodes are passivated. The electrolytes have been used in a prototype Mg battery with a Mg anode and Chevrel (Mo3S4)-phase cathode.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{brooks2016polarisation,

title = {Polarisation-selective hotspots in metallic ring stack arrays},

author = {Laura J Brooks and Jan Mertens and Richard W Bowman and Rohit Chikkaraddy and Alan Sanders and Jeremy J Baumberg},

url = {https://www.osapublishing.org/oe/fulltext.cfm?uri=oe-24-4-3663},

year  = {2016},

date = {2016-01-01},

journal = {Optics express},

volume = {24},

number = {4},

pages = {3663--3671},

publisher = {Optical Society of America},

abstract = {We demonstrate a simple, scalable fabrication method for producing large-area arrays of vertically stacked metallic micro-rings, embedded in a deformable polymer sheet. Unusual polarisation-dependent hotspots are found to dominate the reflection images. To understand their origin, the arrays are characterized using point-scanning optical spectroscopy and directly compared to numerical simulations. Individual ring stacks act as microlenses, while polarisation-dependent hotspots arise at the connections between neighbouring stacks, which are comprised of parabolically-arranged parallel gold nanowires. The elastomeric properties of the polymer host opens the door to active control of the optics of this photonic material, through dynamic tuning of the nanowire spacings and array geometry.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{boughey2016research,

title = {Research Data Supporting "Vertically aligned zinc oxide nanowires electrodeposited within porous polycarbonate templates for vibrational energy harvesting"},

author = {Francesca L Boughey and Timothy Davies and Anuja Datta and Richard A Whiter and Suman-Lata Sahonta and Sohini Kar-Narayan},

url = {https://www.repository.cam.ac.uk/handle/1810/255931},

year  = {2016},

date = {2016-01-01},

publisher = {University of Cambridge},

abstract = {The data provided is all of the raw data presented in each graph contained in all of the figures in the paper. It is all contained in one excel spreadsheet file with a new sheet relating to each figure. The individual image files are also included for the figures that contain images.



This research data supports "Vertically aligned zinc oxide nanowires electrodeposited within porous polycarbonate templates for vibrational energy harvesting" which is published in "Nanotechnology".},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{boughey2016vertically,

title = {Vertically aligned zinc oxide nanowires electrodeposited within porous polycarbonate templates for vibrational energy harvesting},

author = {Francesca L Boughey and Timothy Davies and Anuja Datta and Richard A Whiter and Suman-Lata Sahonta and Sohini Kar-Narayan},

url = {https://iopscience.iop.org/article/10.1088/0957-4484/27/28/28LT02/meta},

year  = {2016},

date = {2016-01-01},

journal = {Nanotechnology},

volume = {27},

number = {28},

pages = {28LT02},

publisher = {IOP Publishing},

abstract = {A piezoelectric nanogenerator has been fabricated using a simple, fast and scalable template-assisted electrodeposition process, by which vertically aligned zinc oxide (ZnO) nanowires were directly grown within a nanoporous polycarbonate (PC) template. The nanowires, having average diameter 184 nm and length 12 μm, are polycrystalline and have a preferred orientation of the [100] axis parallel to the long axis. The output power density of a nanogenerator fabricated from the as-grown ZnO nanowires still embedded within the PC template was found to be 151 ± 25 mW m−3 at an impedance-matched load, when subjected to a low-level periodic (5 Hz) impacting force akin to gentle finger tapping. An energy conversion efficiency of ~4.2% was evaluated for the electrodeposited ZnO nanowires, and the ZnO–PC composite nanogenerator was found to maintain good energy harvesting performance through 24 h of continuous fatigue testing. This is particularly significant given that ZnO-based nanostructures typically suffer from mechanical and/or environmental degradation that otherwise limits their applicability in vibrational energy harvesting. Our template-assisted synthesis of ZnO nanowires embedded within a protective polymer matrix through a single growth process is thus attractive for the fabrication of low-cost, robust and stable nanogenerators.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{khan2016homologous,

title = {Homologous binary mixtures and improved hole conduction of self-assembled discotic liquid crystals},

author = {Ammar A Khan and Girish Rughoobur and Muhammad A Kamarudin and Alessandro Sepe and James A Dolan and Andrew J Flewitt and Malik M Qasim and Timothy D Wilkinson},

url = {https://www.sciencedirect.com/science/article/pii/S1566119916302233},

year  = {2016},

date = {2016-01-01},

journal = {Organic Electronics},

volume = {36},

pages = {35--44},

publisher = {North-Holland},

abstract = {Discotic liquid crystals (DLCs) are considered promising materials for organo-electronic applications. Columnar alignment of DLCs leads to anisotropic charge transport with high charge carrier mobility. However, pure DLCs exhibit low intrinsic charge carrier density which limits bulk conductivity. This research studies the alignment and conductivity properties of small molecule triphenylene-based DLCs to develop hole transport layers for potential applications in organic semiconductor devices. Binary mixtures of homologous DLCs of the hexakis(n-alkyloxy)triphenylene series (HAT6 and HAT10) are formulated. Mesophase characteristics and columnar alignment of these mixtures are characterized using polarizing optical microscopy (POM) and differential scanning calorimetry (DSC). Alignment, orientation and order of columnar packing in the mixtures is studied using X-ray diffraction (XRD) and grazing incidence wide angle X-ray scattering (GIWAXS) measurements. It is identified that binary mixture formation strongly effects the columnar alignment in solution processed films. Furthermore, to increase charge carrier density in the DLC films a strong electron acceptor 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) is added as a p-type dopant, followed by an extensive characterization of its doping effect. POM, DSC thermal scans, UV–visible spectroscopy, photo-luminescence spectroscopy (PL) and I-V measurements are utilized to characterize and establish the improvement of hole conduction in the doped films. It is observed that F4TCNQ-doped triphenylene DLC films exhibit two-fold increase in hole conductivity, making the materials highly relevant for charge transport applications.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{ou2016template,

title = {Template-assisted hydrothermal growth of aligned zinc oxide nanowires for piezoelectric energy harvesting applications},

author = {Canlin Ou and Pedro E Sanchez-Jimenez and Anuja Datta and Francesca L Boughey and Richard A Whiter and Suman-Lata Sahonta and Sohini Kar-Narayan},

url = {https://pubs.acs.org/doi/abs/10.1021/acsami.6b04041},

year  = {2016},

date = {2016-01-01},

journal = {ACS applied materials & interfaces},

volume = {8},

number = {22},

pages = {13678--13683},

publisher = {American Chemical Society},

abstract = {A flexible and robust piezoelectric nanogenerator (NG) based on a polymer-ceramic nanocomposite structure has been successfully fabricated via a cost-effective and scalable template-assisted hydrothermal synthesis method. Vertically aligned arrays of dense and uniform zinc oxide (ZnO) nanowires (NWs) with high aspect ratio (diameter ∼250 nm, length ∼12 μm) were grown within nanoporous polycarbonate (PC) templates. The energy conversion efficiency was found to be ∼4.2%, which is comparable to previously reported values for ZnO NWs. The resulting NG is found to have excellent fatigue performance, being relatively immune to detrimental environmental factors and mechanical failure, as the constituent ZnO NWs remain embedded and protected inside the polymer matrix.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{offeddu2016structural,

title = {Structural determinants of hydration, mechanics and fluid flow in freeze-dried collagen scaffolds},

author = {‪Giovanni S. Offeddu, JC Ashworth, Ruth Elizabeth Cameron and Michelle Oyen},

url = {https://www.sciencedirect.com/science/article/pii/S1742706116302422},

year  = {2016},

date = {2016-01-01},

journal = {Acta biomaterialia},

volume = {41},

pages = {193--203},

publisher = {Elsevier},

abstract = {Freeze-dried scaffolds provide regeneration templates for a wide range of tissues, due to their flexibility in physical and biological properties. Control of structure is crucial for tuning such properties, and therefore scaffold functionality. However, the common approach of modeling these scaffolds as open-cell foams does not fully account for their structural complexity. Here, the validity of the open-cell model is examined across a range of physical characteristics, rigorously linking morphology to hydration and mechanical properties. Collagen scaffolds with systematic changes in relative density were characterized using Scanning Electron Microscopy, X-ray Micro-Computed Tomography and spherical indentation analyzed in a time-dependent poroelastic framework. Morphologically, all scaffolds were mid-way between the open- and closed-cell models, approaching the closed-cell model as relative density increased. Although pore size remained constant, transport pathway diameter decreased. Larger collagen fractions also produced greater volume swelling on hydration, although the change in pore diameter was constant, and relatively small at ∼6%. Mechanically, the dry and hydrated scaffold moduli varied quadratically with relative density, as expected of open-cell materials. However, the increasing pore wall closure was found to determine the time-dependent nature of the hydrated scaffold response, with a decrease in permeability producing increasingly elastic rather than viscoelastic behavior. These results demonstrate that characterizing the deviation from the open-cell model is vital to gain a full understanding of scaffold biophysical properties, and provide a template for structural studies of other freeze-dried biomaterials.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{gross2016photoelectrochemical,

title = {Photoelectrochemical hydrogen production in water using a layer-by-layer assembly of a Ru dye and Ni catalyst on NiO},

author = {Manuela A Gross and Charles E Creissen and Katherine L Orchard and Erwin Reisner},

url = {https://pubs.rsc.org/fi/content/articlehtml/2016/sc/c6sc00715e},

year  = {2016},

date = {2016-01-01},

journal = {Chemical science},

volume = {7},

number = {8},

pages = {5537--5546},

publisher = {Royal Society of Chemistry},

abstract = {Capture and conversion of sunlight into the storable energy carrier H2 can be achieved through photoelectrochemical water splitting using light-absorbing cathodes and anodes bearing H2 and O2 evolving catalysts. Here, we report on the development of a dye-sensitised p-type nickel oxide (NiO) photocathode with a hexaphosphonated Ru(2,2′-bipyridine)3 based dye (RuP3) and a tetraphosphonated molecular [Ni(P2N2)2]2+ type proton reduction catalyst (NiP) for the photoreduction of aqueous protons to H2. A layer-by-layer deposition approach was employed, using Zr4+ ions to link the phosphonate units in RuP3 and NiP in a supramolecular assembly on the NiO photocathode. This approach keeps the dye in close proximity to the catalyst and semiconductor surface, but spatially separates NiP from NiO for advantageous electron transfer dynamics. The NiO|RuP3–Zr4+–NiP electrodes generate higher photocurrents and are more stable than photocathodes with RuP3 and NiP co-immobilised on the NiO surface in the absence of Zr4+ cations linking dye and catalyst. The generation of H2 with the NiO|RuP3–Zr4+–NiP hybrid electrode in pH 3 aqueous electrolyte solution during irradiation with a UV-filtered solar light simulator (λ > 400 nm, 100 mW cm−2, AM1.5G) has been confirmed by gas chromatography at an underpotential of 300 mV (Eappl = +0.3 V vs. RHE), demonstrating the potential of these electrodes to store solar energy in the chemical bond of H2.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{holtzmann2016brain,

title = {Brain tissue stiffness is a sensitive marker for acidosis},

author = {Kathrin Holtzmann and Hél{`e}ne OB Gautier and Andreas F Christ and Jochen Guck and Ragnhildur Thóra Káradóttir and Kristian Franze},

url = {https://www.sciencedirect.com/science/article/pii/S0165027016301558},

year  = {2016},

date = {2016-01-01},

journal = {Journal of neuroscience methods},

volume = {271},

pages = {50--54},

publisher = {Elsevier},

abstract = {Carbon dioxide overdose is frequently used to cull rodents for tissue harvesting. However, this treatment may lead to respiratory acidosis, which potentially could change the properties of the investigated tissue.

},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{tait2016simulation,

title = {Simulation of electron energy loss spectra of nanomaterials with linear-scaling density functional theory},

author = {Edward Tait, ‪Laura E Ratcliff‬, Mike Payne, Peter D Haynes and ‪Nicholas D M Hine},

url = {https://iopscience.iop.org/article/10.1088/0953-8984/28/19/195202/meta},

year  = {2016},

date = {2016-01-01},

journal = {Journal of Physics: Condensed Matter},

volume = {28},

number = {19},

pages = {195202},

publisher = {IOP Publishing},

abstract = {Experimental techniques for electron energy loss spectroscopy (EELS) combine high energy resolution with high spatial resolution. They are therefore powerful tools for investigating the local electronic structure of complex systems such as nanostructures, interfaces and even individual defects. Interpretation of experimental electron energy loss spectra is often challenging and can require theoretical modelling of candidate structures, which themselves may be large and complex, beyond the capabilities of traditional cubic-scaling density functional theory. In this work, we present functionality to compute electron energy loss spectra within the onetep linear-scaling density functional theory code. We first demonstrate that simulated spectra agree with those computed using conventional plane wave pseudopotential methods to a high degree of precision. The ability of onetep to tackle large problems is then exploited to investigate convergence of spectra with respect to supercell size. Finally, we apply the novel functionality to a study of the electron energy loss spectra of defects on the (1 0 1) surface of an anatase slab and determine concentrations of defects which might be experimentally detectable.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{michan2016solid,

title = {Solid electrolyte interphase growth and capacity loss in silicon electrodes},

author = {Alison L Michan and Giorgio Divitini and Andrew J Pell and Michal Leskes and Caterina Ducati and Clare P Grey},

url = {https://pubs.acs.org/doi/abs/10.1021/jacs.6b02882},

year  = {2016},

date = {2016-01-01},

journal = {Journal of the American Chemical Society},

volume = {138},

number = {25},

pages = {7918--7931},

publisher = {American Chemical Society},

abstract = {The solid electrolyte interphase (SEI) of the high capacity anode material Si is monitored over multiple electrochemical cycles by 7Li, 19F, and 13C solid-state nuclear magnetic resonance spectroscopies, with the organics dominating the SEI. Homonuclear correlation experiments are used to identify the organic fragments −OCH2CH2O–, −OCH2CH2–, −OCH2CH3, and −CH2CH3 contained in both oligomeric species and lithium semicarbonates ROCO2Li, RCO2Li. The SEI growth is correlated with increasing electrode tortuosity by using focused ion beam and scanning electron microscopy. A two-stage model for lithiation capacity loss is developed: initially, the lithiation capacity steadily decreases, Li+ is irreversibly consumed at a steady rate, and pronounced SEI growth is seen. Later, below 50% of the initial lithiation capacity, less Si is (de)lithiated resulting in less volume expansion and contraction; the rate of Li+ being irreversibly consumed declines, and the Si SEI thickness stabilizes. The decreasing lithiation capacity is primarily attributed to kinetics, the increased electrode tortuousity severely limiting Li+ ion diffusion through the bulk of the electrode. The resulting changes in the lithiation processes seen in the electrochemical capacity curves are ascribed to non-uniform lithiation, the reaction commencing near the separator/on the surface of the particles.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{zhu2016quantum,

title = {Quantum mechanical effects in plasmonic structures with subnanometre gaps},

author = {Wenqi Zhu and Ruben Esteban and Andrei G Borisov and Jeremy J Baumberg and Peter Nordlander and Henri J Lezec and Javier Aizpurua and Kenneth B Crozier},

url = {https://www.nature.com/articles/ncomms11495/briefing/signup/},

year  = {2016},

date = {2016-01-01},

journal = {Nature communications},

volume = {7},

number = {1},

pages = {1--14},

publisher = {Nature Publishing Group},

abstract = {Metallic structures with nanogap features have proven highly effective as building blocks for plasmonic systems, as they can provide a wide tuning range of operating frequencies and large near-field enhancements. Recent work has shown that quantum mechanical effects such as electron tunnelling and nonlocal screening become important as the gap distances approach the subnanometre length-scale. Such quantum effects challenge the classical picture of nanogap plasmons and have stimulated a number of theoretical and experimental studies. This review outlines the findings of many groups into quantum mechanical effects in nanogap plasmons, and discusses outstanding challenges and future directions.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{li2016research,

title = {Research data supporting "Highly-Efficient Perovskite Nanocrystal Light-Emitting Diodes Enabled by a Universal Cross-linking Method"},

author = {Guangru Li and Florencia Wisnivesky-Rocca-Rivarola and Nathaniel JLK Davis and Sai Bai and Tom C Jellicoe and Francisco de la Pe{~n}a and Shaocong Hou and Caterina Ducati and Feng Gao and Richard H Friend and others},

url = {https://aspace.repository.cam.ac.uk/handle/1810/253968},

year  = {2016},

date = {2016-01-01},

publisher = {University of Cambridge},

abstract = {The data corresponds to the images in the paper, the user need to have a power point and an origin software, and then open the data by clicking the images in the powerpoint.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{khan2016research,

title = {Research data supporting "Homologous binary mixtures and improved hole conduction of self-assembled discotic liquid crystals"},

author = {Ammar A Khan and Girish Rughoobur and Muhammad A Kamarudin and Alessandro Sepe and James A Dolan and Andrew J Flewitt and Malik M Qasim and Timothy D Wilkinson},

url = {https://www.repository.cam.ac.uk/handle/1810/256563},

year  = {2016},

date = {2016-01-01},

publisher = {University of Cambridge},

abstract = {Raw data, corresponding to each figure in the paper has been included. This includes data of all the various characterizations that were performed during the research. Excel files summarizing each figure have been included.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{li2016highly,

title = {Highly efficient perovskite nanocrystal light-emitting diodes enabled by a universal crosslinking method},

author = {Guangru Li and Florencia Wisnivesky Rocca Rivarola and Nathaniel JLK Davis and Sai Bai and Tom C Jellicoe and Francisco de la Pe{~n}a and Shaocong Hou and Caterina Ducati and Feng Gao and Richard H Friend and others},

url = {https://onlinelibrary.wiley.com/doi/full/10.1002/adma.201600064},

year  = {2016},

date = {2016-01-01},

journal = {Advanced materials},

volume = {28},

number = {18},

pages = {3528--3534},

abstract = {The preparation of highly efficient perovskite nanocrystal light‐emitting diodes is shown. A new trimethylaluminum vapor‐based crosslinking method to render the nanocrystal films insoluble is applied. The resulting near‐complete nanocrystal film coverage, coupled with the natural confinement of injected charges within the perovskite crystals, facilitates electron–hole capture and give rise to a remarkable electroluminescence yield of 5.7%.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{zhao2016nanoassembly,

title = {Nanoassembly of polydisperse photonic crystals based on binary and ternary polymer opal alloys},

author = {Qibin Zhao and Chris E Finlayson and Christian G Schaefer and Peter Spahn and Markus Gallei and Lars Herrmann and Andrei V Petukhov and Jeremy J Baumberg},

url = {https://onlinelibrary.wiley.com/doi/abs/10.1002/adom.201600328},

year  = {2016},

date = {2016-01-01},

journal = {Advanced Optical Materials},

volume = {4},

number = {10},

pages = {1494--1500},

abstract = {Ordered binary and ternary photonic crystals, composed of different sized polymer‐composite spheres with diameter ratios up to 120%, are generated using bending‐induced oscillatory shearing. This viscoelastic system creates polydisperse equilibrium structures, producing mixed opaline colored films with greatly reduced requirements for particle monodispersity, and very different sphere size ratios compared to other methods of nanoassembly.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{cole2016conjugated,

title = {Conjugated polyelectrolyte nano field emission adlayers},

author = {Matthew T. Cole, Richard J. Parmee , A Kumar, Clare M Collins, MH Kang, James Xiao, Cinzia Cepek, X Yuan and William I. Milne },

url = {https://pubs.rsc.org/en/content/articlehtml/2016/nh/c6nh00071a},

year  = {2016},

date = {2016-01-01},

journal = {Nanoscale horizons},

volume = {1},

number = {4},

pages = {304--312},

publisher = {Royal Society of Chemistry},

abstract = {Here we report on a straightforward and rapid means of enhancing the field electron emission performance of nascent vertically aligned multi-walled carbon nanotubes by introducing a polar zwitterionic conjugated polyelectrolyte adlayer at the vacuum–emitter interface. We attribute the observed 66% decrease in turn-on electric field to the augmented emitter micro-morphology and shifted surface band structure. The composite emitters can be optically modulated by exploiting the absorption cross-section of the solution cast adlayer, which increases the local carrier concentration which broadens the effective electrostatic shape of the emitter during optical excitation. Assessment via scanning anode field emission microscopy reveals a 25% improvement in DC time stability, a significant reduction in long-term hysteresis shift, and a threefold increase in bandwidth during pulsed mode operation.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}

@article{sokol2016rational,

title = {Rational wiring of photosystem II to hierarchical indium tin oxide electrodes using redox polymers},

author = {Katarzyna P Sokol and Dirk Mersch and Volker Hartmann and Jenny Z Zhang and Marc M Nowaczyk and Matthias Rögner and Adrian Ruff and Wolfgang Schuhmann and Nicolas Plumeré and Erwin Reisner},

url = {https://pubs.rsc.org/ko/content/articlehtml/2016/ee/c6ee01363e},

year  = {2016},

date = {2016-01-01},

journal = {Energy & Environmental Science},

volume = {9},

number = {12},

pages = {3698--3709},

publisher = {Royal Society of Chemistry},

abstract = {Photosystem II (PSII) is a multi-subunit enzyme responsible for solar-driven water oxidation to release O2 and highly reducing electrons during photosynthesis. The study of PSII in protein film photoelectrochemistry sheds light into its biological function and provides a blueprint for artificial water-splitting systems. However, the integration of macromolecules, such as PSII, into hybrid bio-electrodes is often plagued by poor electrical wiring between the protein guest and the material host. Here, we report a new benchmark PSII–electrode system that combines the efficient wiring afforded by redox-active polymers with the high loading provided by hierarchically-structured inverse opal indium tin oxide (IO-ITO) electrodes. Compared to flat electrodes, the hierarchical IO-ITO electrodes enabled up to an approximately 50-fold increase in the immobilisation of an Os complex-modified and a phenothiazine-modified polymer. When the Os complex-modified polymer is co-adsorbed with PSII on the hierarchical electrodes, photocurrent densities of up to ∼410 μA cm−2 at 0.5 V vs. SHE were observed in the absence of diffusional mediators, demonstrating a substantially improved wiring of PSII to the IO-ITO electrode with the redox polymer. The high photocurrent density allowed for the quantification of O2 evolution, and a Faradaic efficiency of 85 ± 9% was measured. As such, we have demonstrated a high performing and fully integrated host–guest system with excellent electronic wiring and loading capacity. This assembly strategy may form the basis of all-integrated electrode designs for a wide range of biological and synthetic catalysts.},

keywords = {},

pubstate = {published},

tppubtype = {article}

}