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- ItemTowards on-site testing of Phytophthora species(Cambridge : RSC Publ., 2014) Schwenkbier, Lydia; Pollok, Sibyll; König, Stephan; Urban, Matthias; Werres, Sabine; Cialla-May, Dana; Weber, Karina; Popp, JürgenRapid detection and accurate identification of plant pathogens in the field is an ongoing challenge. In this study, we report for the first time on the development of a helicase-dependent isothermal amplification (HDA) in combination with on-chip hybridization for the detection of selected Phytophthora species. The HDA approach allows efficient amplification of the yeast GTP-binding protein (Ypt1) target gene region at one constant temperature in a miniaturized heating device. The assay's specificity was determined by on-chip DNA hybridization and subsequent silver nanoparticle deposition. The silver deposits serve as stable endpoint signals that enable the visual as well as the electrical readout. Our promising results point to the direction of a near future on-site application of the combined techniques for a reliable detection of Phytophthora species.
- ItemPatterning and control of the nanostructure in plasma thin films with acoustic waves: mechanical vs. electrical polarization effects(Cambridge : RSC Publ., 2021) GarcÃa-Valenzuela, Aurelio; Fakhfouri, Armaghan; Oliva-RamÃrez, Manuel; Rico-Gavira, Victor; Rojas, Teresa Cristina; Alvarez, Rafael; Menzel, Siegfried B.; Palmero, Alberto; Winkler, Andreas; González-Elipe, AgustÃn R.Nanostructuration and 2D patterning of thin films are common strategies to fabricate biomimetic surfaces and components for microfluidic, microelectronic or photonic applications. This work presents the fundamentals of a surface nanotechnology procedure for laterally tailoring the nanostructure and crystalline structure of thin films that are plasma deposited onto acoustically excited piezoelectric substrates. Using magnetron sputtering as plasma technique and TiO2 as case example, it is demonstrated that the deposited films depict a sub-millimetre 2D pattern that, characterized by large lateral differences in nanostructure, density (up to 50%), thickness, and physical properties between porous and dense zones, reproduces the wave features distribution of the generated acoustic waves (AW). Simulation modelling of the AW propagation and deposition experiments carried out without plasma and under alternative experimental conditions reveal that patterning is not driven by the collision of ad-species with mechanically excited lattice atoms of the substrate, but emerges from their interaction with plasma sheath ions locally accelerated by the AW-induced electrical polarization field developed at the substrate surface and growing film. The possibilities of the AW activation as a general approach for the tailored control of nanostructure, pattern size, and properties of thin films are demonstrated through the systematic variation of deposition conditions and the adjustment of AW operating parameters.
- ItemColloidal PbS nanoplatelets synthesized via cation exchange for electronic applications(Cambridge : RSC Publ., 2019) Sonntag, Luisa; Shamraienko, Volodymyr; Fan, Xuelin; Samadi Khoshkhoo, Mahdi; Kneppe, David; Koitzsch, Andreas; Gemming, Thomas; Hiekel, Karl; Leo, Karl; Lesnyak, Vladimir; Eychmüller, AlexanderIn this work, we present a new synthetic approach to colloidal PbS nanoplatelets (NPLs) utilizing a cation exchange (CE) strategy starting from CuS NPLs synthesized via the hot-injection method. Whereas the thickness of the resulting CuS NPLs was fixed at approx. 5 nm, the lateral size could be tuned by varying the reaction conditions, such as time from 6 to 16 h, the reaction temperature (120 °C, 140 °C), and the amount of copper precursor. In a second step, Cu+ cations were replaced with Pb2+ ions within the crystal lattice via CE. While the shape and the size of parental CuS platelets were preserved, the crystal structure was rearranged from hexagonal covellite to PbS galena, accompanied by the fragmentation of the monocrystalline phase into polycrystalline one. Afterwards a halide mediated ligand exchange (LE) was carried out in order to remove insulating oleic acid residues from the PbS NPL surface and to form stable dispersions in polar organic solvents enabling thin-film fabrication. Both CE and LE processes were monitored by several characterization techniques. Furthermore, we measured the electrical conductivity of the resulting PbS NPL-based films before and after LE and compared the processing in ambient to inert atmosphere. Finally, we fabricated field-effect transistors with an on/off ratio of up to 60 and linear charge carrier mobility for holes of 0.02 cm2 V−1 s−1.
- ItemHuman spermbots for patient-representative 3D ovarian cancer cell treatment(Cambridge : RSC Publ., 2020) Xu, Haifeng; Medina-Sánchez, Mariana; Zhang, Wunan; Seaton, Melanie P. H.; Brison, Daniel R.; Edmondson, Richard J.; Taylor, Stephen S.; Nelson, Louisa; Zeng, Kang; Bagley, Steven; Ribeiro, Carla; Restrepo, Lina P.; Lucena, Elkin; Schmidt, Christine K.; Schmidt, Oliver G.Cellular micromotors are attractive for locally delivering high concentrations of drug, and targeting hard-to-reach disease sites such as cervical cancer and early ovarian cancer lesions by non-invasive means. Spermatozoa are highly efficient micromotors perfectly adapted to traveling up the female reproductive system. Indeed, bovine sperm-based micromotors have shown potential to carry drugs toward gynecological cancers. However, due to major differences in the molecular make-up of bovine and human sperm, a key translational bottleneck for bringing this technology closer to the clinic is to transfer this concept to human material. Here, we successfully load human sperm with Doxorubicin (DOX) and perform treatment of 3D cervical cancer and patient-representative ovarian cancer cell cultures, resulting in strong anticancer cell effects. Additionally, we define the subcellular localization of the chemotherapeutic drug within human sperm, using high-resolution optical microscopy. We also assess drug effects on sperm motility and viability over time, employing sperm samples from healthy donors as well as assisted reproduction patients. Finally, we demonstrate guidance and release of human drug-loaded sperm onto cancer tissues using magnetic microcaps, and show the sperm microcap loaded with a second anticancer drug, camptothecin (CPT), which unlike DOX is not suitable for directly loading into sperm due to its hydrophobic nature. This co-drug delivery approach opens up novel targeted combinatorial drug therapies for future applications. © 2020 The Royal Society of Chemistry.
- ItemTin/vanadium redox electrolyte for battery-like energy storage capacity combined with supercapacitor-like power handling(Cambridge : RSC Publ., 2016) Lee, Juhan; Krüner, Benjamin; Tolosa, Aura; Sathyamoorthi, Sethuraman; Kim, Daekyu; Choudhury, Soumyadip; Seo, Kum-Hee; Presser, VolkerWe introduce a high performance hybrid electrochemical energy storage system based on an aqueous electrolyte containing tin sulfate (SnSO4) and vanadyl sulfate (VOSO4) with nanoporous activated carbon. The energy storage mechanism of this system benefits from the unique synergy of concurrent electric double-layer formation, reversible tin redox reactions, and three-step redox reactions of vanadium. The hybrid system showed excellent electrochemical properties such as a promising energy capacity (ca. 75 W h kg−1, 30 W h L−1) and a maximum power of up to 1.5 kW kg−1 (600 W L−1, 250 W m−2), exhibiting capacitor-like galvanostatic cycling stability and a low level of self-discharging rate.
- ItemThe mutual dependence of negative emission technologies and energy systems(Cambridge : RSC Publ., 2019) Creutzig, Felix; Breyer, Christian; Hilaire, Jérôme; Minx, Jan; Peters, Glen P.; Socolow, RobertWhile a rapid decommissioning of fossil fuel technologies deserves priority, most climate stabilization scenarios suggest that negative emission technologies (NETs) are required to keep global warming well below 2 °C. Yet, current discussions on NETs are lacking a distinct energy perspective. Prominent NETs, such as bioenergy with carbon capture and storage (BECCS) and direct air carbon capture and storage (DACCS), will integrate differently into the future energy system, requiring a concerted research effort to determine adequate means of deployment. In this perspective, we discuss the importance of energy per carbon metrics, factors of future cost development, and the dynamic response of NETs in intermittent energy systems. The energy implications of NETs deployed at scale are massive, and NETs may conceivably impact future energy systems substantially. DACCS outperform BECCS in terms of primary energy required per ton of carbon sequestered. For different assumptions, DACCS displays a sequestration efficiency of 75–100%, whereas BECCS displays a sequestration efficiency of 50–90% or less if indirect land use change is included. Carbon dioxide removal costs of DACCS are considerably higher than BECCS, but if DACCS modularity and granularity helps to foster technological learning to <100$ per tCO2, DACCS may remove CO2 at gigaton scale. DACCS also requires two magnitudes less land than BECCS. Designing NET systems that match intermittent renewable energies will be key for stringent climate change mitigation. Our results contribute to an emerging understanding of NETs that is notably different to that derived from scenario modelling.
- ItemTwo-photon, visible light water splitting at a molecular ruthenium complex(Cambridge : RSC Publ., 2021) Schneidewind, Jacob; Argüello Cordero, Miguel A.; Junge, Henrik; Lochbrunner, Stefan; Beller, MatthiasWater splitting to give molecular oxygen and hydrogen or the corresponding protons and electrons is a fundamental four-electron redox process, which forms the basis of photosynthesis and is a promising approach to convert solar into chemical energy. Artificial water splitting systems have struggled with orchestrating the kinetically complex absorption of four photons as well as the difficult utilization of visible light. Based on a detailed kinetic, spectroscopic and computational study of Milstein's ruthenium complex, we report a new mechanistic paradigm for water splitting, which requires only two photons and offers a new method to extend the range of usable wavelengths far into the visible region. We show that two-photon water splitting is enabled by absorption of the first, shorter wavelength photon, which produces an intermediate capable of absorbing the second, longer wavelength photon (up to 630 nm). The second absorption then causes O–O bond formation and liberation of O2. Theoretical modelling shows that two-photon water splitting can be used to achieve a maximum solar-to-hydrogen efficiency of 18.8%, which could be increased further to 28.6% through photochemical instead of thermal H2 release. It is therefore possible to exceed the maximum efficiency of dual absorber systems while only requiring a single catalyst. Due to the lower kinetic complexity, intrinsic utilization of a wide wavelength range and high-performance potential, we believe that this mechanism will inspire the development of a new class of water splitting systems that go beyond the reaction blueprint of photosynthesis.
- ItemHydrogen bonding in a mixture of protic ionic liquids: A molecular dynamics simulation study(Cambridge : RSC Publ., 2015) Paschek, Dietmar; Golub, Benjamin; Ludwig, RalfWe report results of molecular dynamics (MD) simulations characterising the hydrogen bonding in mixtures of two different protic ionic liquids sharing the same cation: triethylammonium-methylsulfonate (TEAMS) and triethylammonium-triflate (TEATF). The triethylammonium-cation acts as a hydrogen-bond donor, being able to donate a single hydrogen-bond. Both, the methylsulfonate- and the triflate-anions can act as hydrogen-bond acceptors, which can accept multiple hydrogen bonds via their respective SO3-groups. In addition, replacing a methyl-group in the methylsulfonate by a trifluoromethyl-group in the triflate significantly weakens the strength of a hydrogen bond from an adjacent triethylammonium cation to the oxygen-site in the SO3-group of the anion. Our MD simulations show that these subtle differences in hydrogen bond strength significantly affect the formation of differently-sized hydrogen-bonded aggregates in these mixtures as a function of the mixture-composition. Moreover, the reported hydrogen-bonded cluster sizes can be predicted and explained by a simple combinatorial lattice model, based on the approximate coordination number of the ions, and using statistical weights that mostly account for the fact that each anion can only accept three hydrogen bonds.
- ItemIn situ spectroelectrochemical and theoretical study on the oxidation of a 4H-imidazole-ruthenium dye adsorbed on nanocrystalline TiO2 thin film electrodes(Cambridge : RSC Publ., 2015) Zhang, Ying; Kupfer, Stephan; Zedler, Linda; Schindler, Julian; Bocklitz, Thomas; Guthmuller, Julien; Rau, Sven; Dietzek, BenjaminTerpyridine 4H-imidazole-ruthenium(II) complexes are considered promising candidates for use as sensitizers in dye sensitized solar cells (DSSCs) by displaying broad absorption in the visible range, where the dominant absorption features are due to metal-to-ligand charge transfer (MLCT) transitions. The ruthenium(III) intermediates resulting from photoinduced MLCT transitions are essential intermediates in the photoredox-cycle of the DSSC. However, their photophysics is much less studied compared to the ruthenium(II) parent systems. To this end, the structural alterations accompanying one-electron oxidation of the RuIm dye series (including a non-carboxylic RuIm precursor, and, carboxylic RuImCOO in solution and anchored to a nanocrystalline TiO2 film) are investigated via in situ experimental and theoretical UV-Vis absorption and resonance Raman (RR) spectroelectrochemistry. The excellent agreement between the experimental and the TDDFT spectra derived in this work allows for an in-depth assignment of UV-Vis and RR spectral features of the dyes. A concordant pronounced wavelength dependence with respect to the charge transfer character has been observed for the model system RuIm, and both RuImCOO in solution and attached on the TiO2 surface. Excitation at long wavelengths leads to the population of ligand-to-metal charge transfer states, i.e. photoreduction of the central ruthenium(III) ion, while high-energy excitation features an intra-ligand charge transfer state localized on the 4H-imidazole moiety. Therefore, these 4H-imidazole ruthenium complexes investigated here are potential multi-photoelectron donors. One electron is donated from MLCT states, and additionally, the 4H-imidazole ligand reveals electron-donating character with a significant contribution to the excited states of the ruthenium(III) complexes upon blue-light irradiation.
- ItemProduction of highly concentrated and hyperpolarized metabolites within seconds in high and low magnetic fields(Cambridge : RSC Publ., 2019) Korchak, Sergey; Emondts, Meike; Mamone, Salvatore; Blümich, Bernhard; Glöggler, StefanHyperpolarized metabolites are very attractive contrast agents for in vivo magnetic resonance imaging studies enabling early diagnosis of cancer, for example. Real-time production of concentrated solutions of metabolites is a desired goal that will enable new applications such as the continuous investigation of metabolic changes. To this end, we are introducing two NMR experiments that allow us to deliver high levels of polarization at high concentrations (50 mM) of an acetate precursor (55% 13C polarization) and acetate (17% 13C polarization) utilizing 83% para-state enriched hydrogen within seconds at high magnetic field (7 T). Furthermore, we have translated these experiments to a portable low-field spectrometer with a permanent magnet operating at 1 T. The presented developments pave the way for a rapid and affordable production of hyperpolarized metabolites that can be implemented in e.g. metabolomics labs and for medical diagnosis.