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- ItemZwitterionic Dendrimersomes: A Closer Xenobiotic Mimic of Cell Membranes(Weinheim : Wiley-VCH, 2022-10-31) Joseph, Anton; Wagner, Anna M.; Garay-Sarmiento, Manuela; Aleksanyan, Mina; Haraszti, Tamás; Söder, Dominik; Georgiev, Vasil N.; Dimova, Rumiana; Percec, Virgil; Rodriguez-Emmenegger, CesarBuilding functional mimics of cell membranes is an important task toward the development of synthetic cells. So far, lipid and amphiphilic block copolymers are the most widely used amphiphiles with the bilayers by the former lacking stability while membranes by the latter are typically characterized by very slow dynamics. Herein, a new type of Janus dendrimer containing a zwitterionic phosphocholine hydrophilic headgroup (JDPC) and a 3,5-substituted dihydrobenzoate-based hydrophobic dendron is introduced. JDPC self-assembles in water into zwitterionic dendrimersomes (z-DSs) that faithfully recapitulate the cell membrane in thickness, flexibility, and fluidity, while being resilient to harsh conditions and displaying faster pore closing dynamics in the event of membrane rupture. This enables the fabrication of hybrid DSs with components of natural membranes, including pore-forming peptides, structure-directing lipids, and glycans to create raft-like domains or onion vesicles. Moreover, z-DSs can be used to create active synthetic cells with life-like features that mimic vesicle fusion and motility as well as environmental sensing. Despite their fully synthetic nature, z-DSs are minimal cell mimics that can integrate and interact with living matter with the programmability to imitate life-like features and beyond.
- ItemOptical Anisotropy and Momentum-Dependent Excitons in Dibenzopentacene Single Crystals(Washington, DC : ACS Publications, 2022) Graf, Lukas; Liu, Fupin; Naumann, Marco; Roth, Friedrich; Debnath, Bipasha; Büchner, Bernd; Krupskaya, Yulia; Popov, Alexey A.; Knupfer, MartinHigh-quality single crystals of the organic semiconductor (1,2;8,9)-dibenzopentacene were grown via physical vapor transport. The crystal structure─unknown before─was determined by single-crystal X-ray diffraction; polarization-dependent optical absorption measurements display a large anisotropy in the ac plane of the crystals. The overall Davydov splitting is ∼110 meV, which is slightly lower than that in the close relative pentacene (120 meV). Momentum-dependent electron energy-loss spectroscopy measurements show a clear exciton dispersion of the Davydov components. An analysis of the dispersion using a simple 1D model indicates smaller electron- and hole-transfer integrals in dibenzopentacene as compared to pentacene. The spectral weight distribution of the excitation spectra is strongly momentum-dependent and demonstrates a strong momentum-dependent admixture of Frenkel excitons, charge-transfer excitons, and vibrational modes.
- ItemMixed Cu-Fe Sulfides Derived from Polydopamine-Coated Prussian Blue Analogue as a Lithium-Ion Battery Electrode(Washington, DC : ACS Publications, 2022) Bornamehr, Behnoosh; Presser, Volker; Husmann, SamanthaBatteries employing transition-metal sulfides enable high-charge storage capacities, but polysulfide shuttling and volume expansion cause structural disintegration and early capacity fading. The design of heterostructures combining metal sulfides and carbon with an optimized morphology can effectively address these issues. Our work introduces dopamine-coated copper Prussian blue (CuPB) analogue as a template to prepare nanostructured mixed copper-iron sulfide electrodes. The material was prepared by coprecipitation of CuPB with in situ dopamine polymerization, followed by thermal sulfidation. Dopamine controls the particle size and favors K-rich CuPB due to its polymerization mechanism. While the presence of the coating prevents particle agglomeration during thermal sulfidation, its thickness demonstrates a key effect on the electrochemical performance of the derived sulfides. After a two-step activation process during cycling, the C-coated KCuFeS2electrodes showed capacities up to 800 mAh/g at 10 mA/g with nearly 100% capacity recovery after rate handling and a capacity of 380 mAh/g at 250 mA/g after 500 cycles.
- ItemApplication of scanning electrochemical microscopy for topography imaging of supported lipid bilayers(Cambridge : RSC Publ., 2022) Nasri, Zahra; Memari, Seyedali; Striesow, Johanna; Weltmann, Klaus-Dieter; von Woedtke, Thomas; Wende, KristianOxidative stress in cellular environments may cause lipid oxidation and membrane degradation. Therefore, studying the degree of lipid membrane morphological changes by reactive oxygen and nitrogen species will be informative in oxidative stress-based therapies. This study introduces the possibility of using scanning electrochemical microscopy as a powerful imaging technique to follow the topographical changes of a solid-supported lipid bilayer model induced by reactive species produced from gas plasma. The introduced strategy is not limited to investigating the effect of reactive species on the lipid bilayer but could be extended to understand the morphological changes of the lipid bilayer due to the action of membrane proteins or antimicrobial peptides.
- ItemSynthesis of 3,4-Dihydro-2H-Pyrroles from Ketones, Aldehydes, and Nitro Alkanes via Hydrogenative Cyclization(Weinheim : Wiley-VCH, 2022) Klausfelder, Barbara; Blach, Patricia; de Jonge, Niels; Kempe, RhettSyntheses of N-heterocyclic compounds that permit a flexible introduction of various substitution patterns by using inexpensive and diversely available starting materials are highly desirable. Easy to handle and reusable catalysts based on earth-abundant metals are especially attractive for these syntheses. We report here on the synthesis of 3,4-dihydro-2H-pyrroles via the hydrogenation and cyclization of nitro ketones. The latter are easily accessible from three components: a ketone, an aldehyde and a nitroalkane. Our reaction has a broad scope and 23 of the 33 products synthesized are compounds which have not yet been reported. The key to the general hydrogenation/cyclization reaction is a highly active, selective and reusable nickel catalyst, which was identified from a library of 24 earth-abundant metal catalysts.
- ItemPhotophysics of Anionic Bis(4H-imidazolato)CuI Complexes(Weinheim : Wiley-VCH, 2022) Seidler, Bianca; Tran, Jens H.; Hniopek, Julian; Traber, Philipp; Görls, Helmar; Gräfe, Stefanie; Schmitt, Michael; Popp, Jürgen; Schulz, Martin; Dietzek‐Ivanšić, BenjaminIn this paper, the photophysical behavior of four panchromatically absorbing, homoleptic bis(4H-imidazolato)CuI complexes, with a systematic variation in the electron-withdrawing properties of the imidazolate ligand, were studied by wavelength-dependent time-resolved femtosecond transient absorption spectroscopy. Excitation at 400, 480, and 630 nm populates metal-to-ligand charge transfer, intraligand charge transfer, and mixed-character singlet states. The pump wavelength-dependent transient absorption data were analyzed by a recently established 2D correlation approach. Data analysis revealed that all excitation conditions yield similar excited-state dynamics. Key to the excited-state relaxation is fast, sub-picosecond pseudo-Jahn-Teller distortion, which is accompanied by the relocalization of electron density onto a single ligand from the initially delocalized state at Franck-Condon geometry. Subsequent intersystem crossing to the triplet manifold is followed by a sub-100 ps decay to the ground state. The fast, nonradiative decay is rationalized by the low triplet-state energy as found by DFT calculations, which suggest perspective treatment at the strong coupling limit of the energy gap law.
- ItemApplications of MXenes in human-like sensors and actuators(New York, NY [u.a.] : Springer, 2022) Pang, Jinbo; Peng, Songang; Hou, Chongyang; Wang, Xiao; Wang, Ting; Cao, Yu; Zhou, Weijia; Sun, Ding; Wang, Kai; Rümmeli, Mark H.; Cuniberti, Gianaurelio; Liu, HongHuman beings perceive the world through the senses of sight, hearing, smell, taste, touch, space, and balance. The first five senses are prerequisites for people to live. The sensing organs upload information to the nervous systems, including the brain, for interpreting the surrounding environment. Then, the brain sends commands to muscles reflexively to react to stimuli, including light, gas, chemicals, sound, and pressure. MXene, as an emerging two-dimensional material, has been intensively adopted in the applications of various sensors and actuators. In this review, we update the sensors to mimic five primary senses and actuators for stimulating muscles, which employ MXene-based film, membrane, and composite with other functional materials. First, a brief introduction is delivered for the structure, properties, and synthesis methods of MXenes. Then, we feed the readers the recent reports on the MXene-derived image sensors as artificial retinas, gas sensors, chemical biosensors, acoustic devices, and tactile sensors for electronic skin. Besides, the actuators of MXene-based composite are introduced. Eventually, future opportunities are given to MXene research based on the requirements of artificial intelligence and humanoid robot, which may induce prospects in accompanying healthcare and biomedical engineering applications. [Figure not available: see fulltext.]
- ItemEffects of increasing air temperature on skin and respiration heat loss from dairy cows at different relative humidity and air velocity levels(Savoy, Ill. : ADSA, 2022) Zhou, M.; Huynh, T.T.T.; Groot Koerkamp, P.W.G.; van Dixhoorn, I.D.E.; Amon, T.; Aarnink, A.J.A.The focus of this study was to identify the effects of increasing ambient temperature (T) at different relative humidity (RH) and air velocity (AV) levels on heat loss from the skin surface and through respiration of dairy cows. Twenty Holstein dairy cows with an average parity of 2.0 ± 0.7 and body weight of 687 ± 46 kg participated in the study. Two climate-controlled respiration chambers were used. The experimental indoor climate was programmed to follow a diurnal pattern with ambient T at night being 9°C lower than during the day. Night ambient T was gradually increased from 7 to 21°C and day ambient T was increased from 16 to 30°C within an 8-d period, both with an incremental change of 2°C per day. A diurnal pattern for RH was created as well, with low values during the day and high values during the night (low: RH_l = 30-50%; medium: RH_m = 45-70%; and high: RH_h = 60-90%). The effects of AV were studied during daytime at 3 levels (no fan: AV_l = 0.1 m/s; fan at medium speed: AV_m = 1.0 m/s; and fan at high speed: AV_h = 1.5 m/s). The AV_m and AV_h were combined only with RH_m. In total, there were 5 treatments with 4 replicates (cows) for each. Effects of short and long exposure time to warm condition were evaluated by collecting data 2 times a day, in the morning (short: 1-h exposure time) and afternoon (long: 8-h exposure time). The cows were allowed to adapt to the experimental conditions during 3 d before the main 8-d experimental period. The cows had free access to feed and water. Sensible heat loss (SHL) and latent heat loss (LHL) from the skin surface were measured using a ventilated skin box placed on the belly of the cow. These heat losses from respiration were measured with a face mask covering the cow's nose and mouth. The results showed that skin SHL decreased with increasing ambient T and the decreasing rate was not affected by RH or AV. The average skin SHL, however, was higher under medium and high AV levels, whereas it was similar under different RH levels. The skin LHL increased with increasing ambient T. There was no effect of RH on the increasing rate of LHL with ambient T. A larger increasing rate of skin LHL with ambient T was observed at high AV level compared with the other levels. Both RH and AV had no significant effects on respiration SHL or LHL. The cows lost more skin sensible heat and total respiration heat under long exposure than short exposure. When ambient T was below 20°C the total LHL (skin + respiration) represented approx. 50% of total heat loss, whereas above 28°C the LHL accounted for more than 70% of the total heat loss. Respiration heat loss increased by 34 and 24% under short and long exposures when ambient T rose from 16 to 32°C.
- ItemNanocellulose and PEDOT:PSS composites and their applications(London [u.a.] : Taylor & Francis, 2022) Brooke, Robert; Lay, Makara; Jain, Karishma; Francon, Hugo; Say, Mehmet Girayhan; Belaineh, Dagmawi; Wang, Xin; Håkansson, Karl M. O.; Wågberg, Lars; Engquist, Isak; Edberg, Jesper; Berggren, MagnusThe need for achieving sustainable technologies has encouraged research on renewable and biodegradable materials for novel products that are clean, green, and environmentally friendly. Nanocellulose (NC) has many attractive properties such as high mechanical strength and flexibility, large specific surface area, in addition to possessing good wet stability and resistance to tough chemical environments. NC has also been shown to easily integrate with other materials to form composites. By combining it with conductive and electroactive materials, many of the advantageous properties of NC can be transferred to the resulting composites. Conductive polymers, in particular poly(3,4-ethylenedioxythiophene:poly(styrene sulfonate) (PEDOT:PSS), have been successfully combined with cellulose derivatives where suspensions of NC particles and colloids of PEDOT:PSS are made to interact at a molecular level. Alternatively, different polymerization techniques have been used to coat the cellulose fibrils. When processed in liquid form, the resulting mixture can be used as a conductive ink. This review outlines the preparation of NC/PEDOT:PSS composites and their fabrication in the form of electronic nanopapers, filaments, and conductive aerogels. We also discuss the molecular interaction between NC and PEDOT:PSS and the factors that affect the bonding properties. Finally, we address their potential applications in energy storage and harvesting, sensors, actuators, and bioelectronics.
- ItemOptical, electrical and chemical properties of PEO:I2 complex composite films(Heidelberg [u.a.] : Springer, 2022) Telfah, Ahmad; Al-Bataineh, Qais M.; Tolstik, Elen; Ahmad, Ahmad A.; Alsaad, Ahmad M.; Ababneh, Riad; Tavares, Carlos J.; Hergenröder, RolandSynthesized PEO:I2 complex composite films with different I2 concentrations were deposited onto fused silica substrates using a dip-coating method. Incorporation of PEO films with I2 increases the electrical conductivity of the composite, reaching a maximum of 46 mS/cm for 7 wt% I2. The optical and optoelectronic properties of the complex composite films were studied using the transmittance and reflectance spectra in the UV-Vis region. The transmittance of PEO decreases with increasing I2 content. From this study, the optical bandgap energy decreases from 4.42 to 3.28 eV as I2 content increases from 0 to 7 wt%. In addition, the refractive index for PEO films are in the range of 1.66 and 2.00.1H NMR spectra of pure PEO film shows two major peaks at 3.224 ppm and 1.038 ppm, with different widths assigned to the mobile polymer chains in the amorphous phase, whereas the broad component is assigned to the more rigid molecules in the crystalline phase, respectively. By adding I2 to the PEO, both peaks (amorphous and crystal) are shifted to lower NMR frequencies indicating that I2 is acting as a Lewis acid, and PEO is acting as Lewis base. Hence, molecular iodine reacts favorably with PEO molecules through a charge transfer mechanism, and the formation of triiodide (I3-), the iodite (IO2-) anion, I 2· · · PEO and I2+···PEO complexes. PEO:I2 complex composite films are expected to be suitable for optical, electrical, and optoelectronic applications.
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