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Recent Submissions

  • Symmetry-dependent field-free switching of perpendicular magnetization

    Liu, Liang; Zhou, Chenghang; Shu, Xinyu; Li, Changjian; Zhao, Tieyang; Lin, Weinan; Deng, Jinyu; Xie, Qidong; Chen, Shaohai; Zhou, Jing; Guo, Rui; Wang, Han; Yu, Jihang; Shi, Shu; Yang, Ping; Pennycook, S. J.; Manchon, Aurelien; Chen, Jingsheng (Nature Nanotechnology, Springer Science and Business Media LLC, 2021-01-18) [Article]
    Modern magnetic-memory technology requires all-electric control of perpendicular magnetization with low energy consumption. While spin–orbit torque (SOT) in heavy metal/ferromagnet (HM/FM) heterostructures1,2,3,4,5 holds promise for applications in magnetic random access memory, until today, it has been limited to the in-plane direction. Such in-plane torque can switch perpendicular magnetization only deterministically with the help of additional symmetry breaking, for example, through the application of an external magnetic field2,4, an interlayer/exchange coupling6,7,8,9 or an asymmetric design10,11,12,13,14. Instead, an out-of-plane SOT15 could directly switch perpendicular magnetization. Here we observe an out-of-plane SOT in an HM/FM bilayer of L11-ordered CuPt/CoPt and demonstrate field-free switching of the perpendicular magnetization of the CoPt layer. The low-symmetry point group (3m1) at the CuPt/CoPt interface gives rise to this spin torque, hereinafter referred to as 3m torque, which strongly depends on the relative orientation of the current flow and the crystal symmetry. We observe a three-fold angular dependence in both the field-free switching and the current-induced out-of-plane effective field. Because of the intrinsic nature of the 3m torque, the field-free switching in CuPt/CoPt shows good endurance in cycling experiments. Experiments involving a wide variety of SOT bilayers with low-symmetry point groups16,17 at the interface may reveal further unconventional spin torques in the future.
  • Efficient bifacial monolithic perovskite/silicon tandem solar cells via bandgap engineering

    de Bastiani, Michele; Mirabelli, Alessandro J.; Hou, Yi; Gota, Fabrizio; Aydin, Erkan; Allen, Thomas; Troughton, Joel; Subbiah, Anand Selvin; Isikgor, Furkan Halis; Liu, Jiang; Xu, Lujia; Chen, Bin; Van Kerschaver, Emmanuel; Baran, Derya; Fraboni, Beatrice; Salvador, Michael F.; Paetzold, Ulrich W.; Sargent, E.; De Wolf, Stefaan (Nature Energy, Springer Science and Business Media LLC, 2021-01-11) [Article]
    Bifacial monolithic perovskite/silicon tandem solar cells exploit albedo—the diffuse reflected light from the environment—to increase their performance above that of monofacial perovskite/silicon tandems. Here we report bifacial tandems with certified power conversion efficiencies >25% under monofacial AM1.5G 1 sun illumination that reach power-generation densities as high as ~26 mW cm–2 under outdoor testing. We investigated the perovskite bandgap required to attain optimized current matching under a variety of realistic illumination and albedo conditions. We then compared the properties of these bifacial tandems exposed to different albedos and provide energy yield calculations for two locations with different environmental conditions. Finally, we present a comparison of outdoor test fields of monofacial and bifacial perovskite/silicon tandems to demonstrate the added value of tandem bifaciality for locations with albedos of practical relevance.
  • Response to Zöller et al.'s critique on “Potential short-term earthquake forecasting by farm-animal monitoring”

    Wikelski, Martin; Mueller, Uschi; Scocco, Paola; Catorci, Andrea; Desinov, Lev V.; Belyaev, Mikhail Y.; Keim, Daniel; Pohlmeier, Winfried; Fechteler, Gerhard; Mai, Paul Martin; Goymann, Wolfgang (Ethology, Wiley, 2021-01-11) [Article]
    Zöller et al. (Ethology, 2020) criticize our original publication (Wikelski et al., Ethology, 126(9), 2020, 931) for obvious reasons: we only observed the behavior of one group of farm animals before, during and after one earthquake series in one area of the world. It is clear that no earthquake predictions are possible, and should not be attempted, from this data set. However, what we show is that there is important information within this animal collective pertaining to potential future local forecasting of earthquakes when combined with traditional data sources. We maintain that combining Zöller et al.'s (2020) modeling tools with the adequate use of our data can stimulate novel ways of earthquake forecasting. Future studies should combine both approaches.
  • Coating of Conducting and Insulating Threads with Porous MOF Particles through Langmuir-Blodgett Technique

    Rauf, Sakandar; Andrés, Miguel A.; Roubeau, Olivier; Gascón, Ignacio; Serre, Christian; Eddaoudi, Mohamed; Salama, Khaled N. (Nanomaterials, MDPI AG, 2021-01-10) [Article]
    The Langmuir-Blodgett (LB) method is a well-known deposition technique for the fabrication of ordered monolayer and multilayer thin films of nanomaterials onto different substrates that plays a critical role in the development of functional devices for various applications. This paper describes detailed studies about the best coating configuration for nanoparticles of a porous metal-organic framework (MOF) onto both insulating or conductive threads and nylon fiber. We design and fabricate customized polymethylmethacrylate sheets (PMMA) holders to deposit MOF layers onto the threads or fiber using the LB technique. Two different orientations, namely, horizontal and vertical, are used to deposit MIL-96(Al) monolayer films onto five different types of threads and nylon fiber. These studies show that LB film formation strongly depends on deposition orientation and the type of threads or fiber. Among all the samples tested, cotton thread and nylon fiber with vertical deposition show more homogenous monolayer coverage. In the case of conductive threads, the MOF particles tend to aggregate between the conductive thread’s fibers instead of forming a continuous monolayer coating. Our results show a significant contribution in terms of MOF monolayer deposition onto single fiber and threads that will contribute to the fabrication of single fiber or thread-based devices in the future.
  • Chain Conformation Control of Fluorene-Benzothiadiazole Copolymer Light-Emitting Diode Efficiency and Lifetime

    Wang, Bingjun; Ye, Hao; Riede, Moritz; Bradley, Donal (ACS Applied Materials & Interfaces, American Chemical Society (ACS), 2021-01-07) [Article]
    The β-phase, in which the intermonomer torsion angle of a fraction of chain segments approaches ∼180°, is an intriguing conformational microstructure of the widely studied light-emitting polymer poly(9,9-dioctylfluorene) (PFO). Its generation can in turn be used to significantly improve the performance of PFO emission-layer-based light-emitting diodes (LEDs). Here, we report the generation of β-phase chain segments in a copolymer, 90F8:10BT, containing 90% 9,9-dioctylfluorene (F8) and 10% 2,1,3-benzothiadiazole (BT) units and show that significant improvements in performance also ensue for LEDs with β-phase 90F8:10BT emission layers, generalizing the earlier PFO results. The β-phase was induced by both solvent vapor annealing and dipping copolymer thin films into a solvent/nonsolvent mixture. Subsequent absorption spectra show the characteristic fluorene β-phase peak at ∼435 nm, but luminescence spectra (∼530 nm peak) and quantum yields barely change, with the emission arising following efficient energy transfer to the lowest-lying excited states localized in the vicinity of the BT units. For ∼5% β-phase chain segment fraction relative to 0% β-phase, the LED luminance at 10 V increased by ∼25% to 5940 cd m<sup>-2</sup>, the maximum external quantum efficiency by ∼61 to 1.91%, and the operational stability from 64% luminance retention after 20 h of operation to 90%. Detailed studies addressing the underlying device physics identify a reduced hole injection barrier, higher hole mobility, correspondingly more balanced electron and hole charge transport, and decreased carrier trapping as the dominant factors. These results confirm the effectiveness of chain conformation control for fluorene-based homo- and copolymer device optimization.
  • Dark Self-Healing Mediated Negative Photoconductivity of Lead-Free Cs3Bi2Cl9 Perovskite Single Crystal

    Tailor, Naveen Kumar; Maity, Partha; Saidaminov, Makhsud; Pradhan, Narayan; Satapathi, Soumitra (arXiv, 2021-01-07) [Preprint]
    Halide perovskites are recently emerged as one of the frontline optoelectronic materials for device applications and have been extensively studied in past few years. Among these while, lead-based materials were most widely explored, investigation of optical properties of lead-free perovskites is limited. Being optically active, these materials were expected to show light-induced enhanced photoconductivity and the same was reported for lead halide perovskite single crystals. However, on contrary, herein, light-induced degradation of bismuth halide perovskite Cs3Bi2Cl9 single crystals is reported which was evidenced by negative photoconductivity with slow recovery. The femtosecond transient reflectance (fs-TR) spectroscopy studies further revealed these electronic transport properties were due to the formation of light-activated metastable trap states within the perovskite crystal. The figure of merits of Cs3Bi2Cl9 single-crystal detectors such as responsivity (17 mA/W), detectivity (6.23 X 10power 11 Jones) and the ratio of current in dark to light (~7160) was calculated and it is found that they are comparable or higher to reported perovskite single crystals based positive photodetectors. This observation for lead-free perovskite single crystals which were optically active but showed retroactive photocurrent on irradiation remained unique for such materials.
  • Ion-exchange doped polymers at the degenerate limit: what limits conductivity at 100% doping efficiency?

    Jacobs, Ian E.; D'Avino, Gabriele; Lin, Yue; Lemaur, Vincent; Huang, Yuxuan; Ren, Xinglong; Simatos, Dimitrios; Wood, William; Chen, Chen; Harrelson, Thomas; Mustafa, Tarig; O'Keefe, Christopher A.; Spalek, Leszek; Tjhe, Dion; Statz, Martin; Lai, Lianglun; Finn, Peter A.; Neal, William G.; Strzalka, Joseph; Nielsen, Christian B.; Lee, Jin-Kyun; Barlow, Stephen; Marder, Seth R.; McCulloch, Iain; Fratini, Simone; Beljonne, David; Sirringhaus, Henning (arXiv, 2021-01-05) [Preprint]
    Doping of semiconducting polymers has seen a surge in research interest driven by emerging applications in sensing, bioelectronics and thermoelectrics. A recent breakthrough was a doping technique based on ion-exchange, which separates the redox and charge compensation steps of the doping process. The improved microstructural control this process allows enables us for the first time to systematically address a longstanding but still poorly understood question: what limits the electrical conductivity at high doping levels? Is it the formation of charge carrier traps in the Coulomb potentials of the counterions, or is it the structural disorder in the polymer lattice? Here, we apply ion-exchange doping to several classes of high mobility conjugated polymers and identify experimental conditions that achieve near 100% doping efficiency under degenerate conditions with nearly 1 charge per monomer. We demonstrate very high conductivities up to 1200 S/cm in semicrystalline polymer systems, and show that in this regime conductivity is poorly correlated with ionic size, but strongly correlated with paracrystalline disorder. This observation, backed by a detailed electronic structure model that incorporates ion-hole and hole-hole interactions and a carefully parameterized model of disorder, indicates that trapping by dopant ions is negligible, and that maximizing crystalline order is critical to improving conductivity.
  • Laminar Burning Velocities of Formic Acid and Formic Acid/Hydrogen Flames: An Experimental and Modeling Study

    Osipova, K.N.; Sarathy, Mani; Korobeinichev, Oleg P.; Shmakov, A.G. (Energy & Fuels, American Chemical Society (ACS), 2021-01-05) [Article]
    Laminar flame speed of formic acid and formic acid/hydrogen (4/1) flames was studied both experimentally and numerically. Experiments with flames of pure formic acid were performed at temperatures of 373 and 423 K, while for formic acid/hydrogen flames the temperature value was 368 K. All of the experiments were performed under atmospheric pressure and at an equivalence ratio ranging from 0.5 to 1.5. To measure the laminar flame speed, the heat flux balance technique was applied. Three detailed chemical-kinetic mechanisms were tested on experimental data. Experiments showed that addition of 20% of hydrogen increases the laminar burning velocity of formic acid, for example, at around 1.5 for stoichiometric flames. The comparison of experimental and numerical data showed that all models tend to overestimate laminar burning velocities of studied flames, especially in the case of rich flames. The obtained results indicate that further improvement of existing chemical-kinetic models of formic acid oxidation is highly required.
  • Hole-Type Spacers for More Stable Shale Gas-Produced Water Treatment by Forward Osmosis

    Alqattan, Jawad; Kim, Youngjin; Kerdi, Sarah; Qamar, Adnan; Ghaffour, NorEddine (Membranes, MDPI AG, 2021-01-03) [Article]
    An appropriate spacer design helps in minimizing membrane fouling which remains the major obstacle in forward osmosis (FO) systems. In the present study, the performance of a hole-type spacer (having holes at the filament intersections) was evaluated in a FO system and compared to a standard spacer design (without holes). The hole-type spacer exhibited slightly higher water flux and reverse solute flux (RSF) when Milli-Q water was used as feed solution and varied sodium chloride concentrations as draw solution. During shale gas produced water treatment, a severe flux decline was observed for both spacer designs due to the formation of barium sulfate scaling. SEM imaging revealed that the high shear force induced by the creation of holes led to the formation of scales on the entire membrane surface, causing a slightly higher flux decline than the standard spacer. Simultaneously, the presence of holes aided to mitigate the accumulation of foulants on spacer surface, resulting in no increase in pressure drop. Furthermore, a full cleaning efficiency was achieved by hole-type spacer attributed to the micro-jets effect induced by the holes, which aided to destroy the foulants and then sweep them away from the membrane surface.
  • Experimental and numerical study of polycyclic aromatic hydrocarbon formation in ethylene laminar co-flow diffusion flames

    Jin, Hanfeng; Guo, Junjun; Li, Tianyu; Zhou, Zhongyue; Im, Hong G.; Farooq, Aamir (Fuel, Elsevier, 2021) [Article]
    Recent literature kinetic studies revealed the importance of new mechanisms for polycyclic aromatic hydrocarbon (PAH) and soot inception beyond hydrogen–abstraction–acetylene–addition (HACA) and hydrogen–abstraction–vinylacetylene–addition (HAVA) mechanisms in the combustion of ethylene and other hydrocarbons. Co-flow diffusion flame is a canonical flame used to investigate the interaction between fluid dynamics and PAH chemistry. In this study, supersonic molecular beam sampling technique was utilized for the first time with synchrotron vacuum ultraviolet photoionization mass spectrometry (SVUV-PIMS) to measure laminar co-flow diffusion flame at atmospheric pressure. We report quantitative measurement of precursor radicals as well as critical intermediates and odd carbon number PAH species. A custom-designed computational code, based on OpenFOAM and Cantera, was adopted to simulate laminar co-flow diffusion flames with literature kinetic model. Chemical kinetic analyses show that addition reactions of odd carbon number species provide considerable contribution to PAH formation processes beside HACA and HAVA mechanisms. Reasonable mass growth reactions are postulated for aromatic species with odd carbon numbers, such as ethynyl-indene, fluorene, benzo-indene, which need further investigations. Reactions of resonantly stabilized radicals followed by ring expansion are shown to be critical for both odd and even carbon number aromatics, and are suggested to be included in future PAH models.
  • Revisiting Reynolds and Nusselt numbers in turbulent thermal convection

    Bhattacharya, Shashwat; Verma, Mahendra K.; Samtaney, Ravi (Physics of Fluids, AIP Publishing, 2021-01-01) [Article]
    In this paper, we extend Grossmann and Lohse’s (GL) model [S. Grossmann and D. Lohse, “Thermal convection for large Prandtl numbers,” Phys. Rev. Lett. 86, 3316 (2001)] for the predictions of Reynolds number (Re) and Nusselt number (Nu) in turbulent Rayleigh–Bénard convection. Toward this objective, we use functional forms for the prefactors of the dissipation rates in the bulk and boundary layers. The functional forms arise due to inhibition of nonlinear interactions in the presence of walls and buoyancy compared to free turbulence, along with a deviation of the viscous boundary layer profile from Prandtl–Blasius theory. We perform 60 numerical runs on a three-dimensional unit box for a range of Rayleigh numbers (Ra) and Prandtl numbers (Pr) and determine the aforementioned functional forms using machine learning. The revised predictions are in better agreement with the past numerical and experimental results than those of the GL model, especially for extreme Prandtl numbers
  • Propane Dehydrogenation Catalyzed by Single Lewis Acid Site in Sn-Beta Zeolite

    Yue, Yuanyuan; Fu, Jing; Wang, Chuanming; Yuan, Pei; Bao, Xiaojun; Xie, Zailai; Basset, Jean-Marie; Zhu, Haibo (Journal of Catalysis, Elsevier BV, 2021-01) [Article]
    The gap between supply and demand of propylene has become more and more evident, because of a large consumption of the downstream products derived from propylene. Propane dehydrogenation (PDH) constitutes an important alternative for the production of propylene, and thus considerable attention has been paid to the development of eco-friendly and cost-efficient catalysts for this process. Herein, we discover that the Sn-Beta zeolite with Lewis acid sites can activate the C-H bond, and exhibits high catalytic performance in the PDH. XRD, STEM, and XPS characterizations confirm that Sn species are incorporated into the zeolite framework, and H2-TPR suggests that there is a strong interaction between Sn species and zeolite framework. It is found that the Lewis acid is the active site for dehydrogenation reaction, and the Brønsted acid is responsible for cracking reaction. The dehydrogenation rate/cracking rate is positively proportional to the L/B ratio, and a high L/B ratio is beneficial for the propane dehydrogenation reaction. The Na-Sn-Beta-30 catalyst possessing the highest amount of Lewis acid but the lowest Brønsted/Lewis ratio, exhibits the best performance in the PDH, which delivers propane conversion of 40% and propylene selectivity of 92%. Most importantly, these Sn-Beta zeolites are extremely stable without any detectable deactivation under the harsh reaction condition for 72 hours. Density functional theory calculations reveal that both Sn and adjacent O atom or OH group cooperatively act as the active sites. The PDH occurs through the direct reaction mechanism in which hydrogen molecule is produced by the direct coupling of H atom of primary C3H7 motif with the Brønsted proton in closed sites or the proton of water in open sites. It seems that open sites are more reactive than the closed ones, and the intrinsic enthalpy barriers are calculated to be 242 ∼ 301 kJ/mol depending on the hydroxylation extents. These efficient Sn-Beta zeolites could provide a new possibility for the development of a new generation of PDH catalysts with a high stability for the production of propylene.
  • Engineered Microgels—Their Manufacturing and Biomedical Applications

    Alzanbaki, Hamzah; Moretti, Manola; Hauser, Charlotte (Micromachines, MDPI AG, 2021-01-01) [Article]
    Microgels are hydrogel particles with diameters in the micrometer scale that can be fabricated in different shapes and sizes. Microgels are increasingly used for biomedical applications and for biofabrication due to their interesting features, such as injectability, modularity, porosity and tunability in respect to size, shape and mechanical properties. Fabrication methods of microgels are divided into two categories, following a top-down or bottom-up approach. Each approach has its own advantages and disadvantages and requires certain sets of materials and equipments. In this review, we discuss fabrication methods of both top-down and bottom-up approaches and point to their advantages as well as their limitations, with more focus on the bottom-up approaches. In addition, the use of microgels for a variety of biomedical applications will be discussed, including microgels for the delivery of therapeutic agents and microgels as cell carriers for the fabrication of 3D bioprinted cell-laden constructs. Microgels made from well-defined synthetic materials with a focus on rationally designed ultrashort peptides are also discussed, because they have been demonstrated to serve as an attractive alternative to much less defined naturally derived materials. Here, we will emphasize the potential and properties of ultrashort self-assembling peptides related to microgels.
  • Imaging of organic signals in individual fossil diatom frustules with nanoSIMS and Raman spectroscopy

    Akse, Shaun P.; Das, Gobind; Agusti, Susana; Pichevin, Laetitia; Polerecky, Lubos; Middelburg, Jack J. (Marine Chemistry, Elsevier BV, 2021-01) [Article]
    The organic matter occluded in the silica of fossil diatom frustules is thought to be protected from diagenesis and used for paleoceanographic reconstructions. However, the location of the organic matter within the frustule has hitherto not been identified. Here, we combined high spatial resolution imaging by nanoSIMS and Raman micro-spectroscopy to identify where the organic material is retained in cleaned fossil diatom frustules. NanoSIMS imaging revealed that organic signals were present throughout the frustule but in higher concentrations at the pore walls. Raman measurements confirmed the heterogenous presence of organics but could not, because of lower spatial resolution, resolve the spatial patterns observed by nanoSIMS.
  • Noble metal nanowire arrays as an ethanol oxidation electrocatalyst

    Lam, Zhenhui; Liu, Cuicui; Su, Dongmeng; Tao, Hua Bing; Wang, Hsin Yi; Chen, Jiazang; Xu, Weichang; Zhang, Liping; Zhu, Yihan; Liu, L. M.; Han, Yu; Chen, Hongyu; Liu, Bin (Nanoscale Advances, Royal Society of Chemistry (RSC), 2021) [Article]
    Vertically aligned noble metal nanowire arrays were grown on conductive electrodes based on a solution growth method. They show significant improvement of electrocatalytic activity in ethanol oxidation, from a re-deposited sample of the same detached nanowires. The unusual morphology provides open diffusion channels and direct charge transport pathways, in addition to the high electrochemically active surface from the ultrathin nanowires. Our best nanowire arrays exhibited much enhanced electrocatalytic activity, achieving a 38.0 fold increase in specific activity over that of commercial catalysts for ethanol electrooxidation. The structural design provides a new direction to enhance the electrocatalytic activity and reduce the size of electrodes for miniaturization of portable electrochemical devices.
  • CO2 hydrogenation to methanol and hydrocarbons over bifunctional Zn-doped ZrO2/zeolite catalysts

    Ticali, Pierfrancesco; Salusso, Davide; Ahmad, Rafia; Ahoba-Sam, Christian; Galilea, Adrian; Shterk, Genrikh; Lomachenko, Kirill A.; Borfecchia, Elisa; Morandi, Sara; Cavallo, Luigi; Gascon, Jorge; Bordiga, Silvia; Olsbye, Unni (Catalysis Science & Technology, Royal Society of Chemistry (RSC), 2021) [Article]
    The tandem process of carbon dioxide hydrogenation to methanol and its conversion to hydrocarbons over mixed metal/metal oxide-zeotype catalysts is a promising path to CO$_{2}$ valorization.
  • On the distillation of waste tire pyrolysis oil: A structural characterization of the derived fractions

    Campuzano, Felipe; Abdul Jameel, Abdul Gani; Zhang, Wen; Emwas, Abdul-Hamid M.; Agudelo, Andrés F.; Martínez, Juan Daniel; Sarathy, Mani (Fuel, Elsevier BV, 2020-12-31) [Article]
    Tire pyrolysis oil (TPO) is a complex mixture of hydrocarbons spanning a wide boiling point range. Due to its complexity, direct implementation of TPO to combustion applications has been challenging. Distillation is a simple method for grouping similar compounds, based on their volatility, thereby facilitating further upgrading and use. In this work, TPO was distilled at atmospheric pressure into different fractions (light, low-middle, high-middle, and heavy), and the structural characteristics of each fraction were explored. Therefore, advanced analytical techniques such as GC–MS, APPI FT-ICR MS and 1H and 13C NMR were utilized. For the light fraction, the GC–MS revealed a significant presence of benzene, toluene, and xylene, as well as limonene. From the APPI FT-ICR MS results, the low-middle, high-middle, and heavy fractions were classified into a number of molecular classes. Among these, pure hydrocarbons (HC), hydrocarbons containing one sulfur atom (S1), hydrocarbons containing two oxygen atoms (O2), etc. Here, HC and S1 were found to be the most abundant molecular classes in all fractions. Finally, a structural analysis of the functional groups present in each TPO fraction was conducted by 1H and 13C NMR. Average molecular parameters (AMPs), such as the number of aromatic, naphthenic, and olefinic carbons/hydrogens, were determined. In addition, derived AMPs, such as the aromaticity factor (fa), C/H paraffinic, C/H aromatic, etc., were calculated. Fractionation by distillation resulted in concentration of both the sulfur and aromatic compounds in the heaviest fraction. In this manner, effective application and upgrading strategies could be individually designed for each fraction.
  • Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction.

    Zhu, Peng; Xia, Chuan; Liu, Chun-Yen; Jiang, Kun; Gao, Guanhui; Zhang, Xiao; Xia, Yang; Lei, Yongjiu; Alshareef, Husam N; Senftle, Thomas P; Wang, Haotian (Proceedings of the National Academy of Sciences of the United States of America, Proceedings of the National Academy of Sciences, 2020-12-31) [Article]
    Electrochemical CO2 or CO reduction to high-value C2+ liquid fuels is desirable, but its practical application is challenged by impurities from cogenerated liquid products and solutes in liquid electrolytes, which necessitates cost- and energy-intensive downstream separation processes. By coupling rational designs in a Cu catalyst and porous solid electrolyte (PSE) reactor, here we demonstrate a direct and continuous generation of pure acetic acid solutions via electrochemical CO reduction. With optimized edge-to-surface ratio, the Cu nanocube catalyst presents an unprecedented acetate performance in neutral pH with other liquid products greatly suppressed, delivering a maximal acetate Faradaic efficiency of 43%,partial current of 200 mA·cm−2, ultrahigh relative purity of up to 98 wt%, and excellent stability of over 150 h continuous operation. Density functional theory simulations reveal the role of stepped sites along the cube edge in promoting the acetate pathway. Additionally, a PSE layer, other than a conventional liquid electrolyte, was designed to separate cathode and anode for efficient ion conductions, while not introducing any impurity ions into generated liquid fuels. Pure acetic acid solutions, with concentrations up to 2 wt% (0.33 M), can be continuously produced by employing the acetate-selective Cu catalyst in our PSE reactor.
  • Arabidopsis Plant Natriuretic Peptide Is a Novel Interactor of Rubisco Activase

    Turek, Ilona; Gehring, Christoph A; Irving, H R (Life, MDPI AG, 2020-12-31) [Article]
    Plant natriuretic peptides (PNPs) are a group of systemically acting peptidic hormones affecting solute and solvent homeostasis and responses to biotrophic pathogens. Although an increasing body of evidence suggests PNPs modulate plant responses to biotic and abiotic stress, which could lead to their potential biotechnological application by conferring increased stress tolerance to plants, the exact mode of PNPs action is still elusive. In order to gain insight into PNP-dependent signalling, we set out to identify interactors of PNP present in the model plant Arabidopsis thaliana, termed AtPNP-A. Here, we report identification of rubisco activase (RCA), a central regulator of photosynthesis converting Rubisco catalytic sites from a closed to an open conformation, as an interactor of AtPNP-A through affinity isolation followed by mass spectrometric identification. Surface plasmon resonance (SPR) analyses reveals that the full-length recombinant AtPNP-A and the biologically active fragment of AtPNP-A bind specifically to RCA, whereas a biologically inactive scrambled peptide fails to bind. These results are considered in the light of known functions of PNPs, PNP-like proteins, and RCA in biotic and abiotic stress responses.
  • Ruddlesden–Popper-Phase Hybrid Halide Perovskite/Small-Molecule Organic Blend Memory Transistors

    Gedda, Murali; Yengel, Emre; Faber, Hendrik; Paulus, Fabian; Kreß, Joshua A.; Tang, Ming-Chun; Zhang, Siyuan; Hacker, Christina A.; Kumar, Prashant; Naphade, Dipti R.; Vaynzof, Yana; Volonakis, George; Giustino, Feliciano; Anthopoulos, Thomas D. (Advanced Materials, Wiley, 2020-12-31) [Article]
    Controlling the morphology of metal halide perovskite layers during processing is critical for the manufacturing of optoelectronics. Here, a strategy to control the microstructure of solution-processed layered Ruddlesden-Popper-phase perovskite films based on phenethylammonium lead bromide ((PEA)<sub>2</sub> PbBr<sub>4</sub> ) is reported. The method relies on the addition of the organic semiconductor 2,7-dioctyl[1]benzothieno[3,2-b]benzothiophene (C<sub>8</sub> -BTBT) into the perovskite formulation, where it facilitates the formation of large, near-single-crystalline-quality platelet-like (PEA)<sub>2</sub> PbBr<sub>4</sub> domains overlaid by a ≈5-nm-thin C<sub>8</sub> -BTBT layer. Transistors with (PEA)<sub>2</sub> PbBr<sub>4</sub> /C<sub>8</sub> -BTBT channels exhibit an unexpectedly large hysteresis window between forward and return bias sweeps. Material and device analysis combined with theoretical calculations suggest that the C<sub>8</sub> -BTBT-rich phase acts as the hole-transporting channel, while the quantum wells in (PEA)<sub>2</sub> PbBr<sub>4</sub> act as the charge storage element where carriers from the channel are injected, stored, or extracted via tunneling. When tested as a non-volatile memory, the devices exhibit a record memory window (>180 V), a high erase/write channel current ratio (10<sup>4</sup> ), good data retention, and high endurance (>10<sup>4</sup> cycles). The results here highlight a new memory device concept for application in large-area electronics, while the growth technique can potentially be exploited for the development of other optoelectronic devices including solar cells, photodetectors, and light-emitting diodes.

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