bluuebunny/crossref_metadata_2025_split huggingface dataset:
Coagulation Bath‐Assisted 3D Printing of PEDOT:PSS with High Resolution and Strong Substrate Adhesion for Bioelectronic Devices
Authors: Zheng Yi , Wang Yangdong , Zhang Fan , Zhang Shaomin , Piatkevich Kiryl D. , Zhou Nanjia , Pokorski Jonathan K. 
Published: February 2022

AbstractPoly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS) is a promising material because of its favorable electrical and mechanical properties, stability in ambient environments, and biocompatibility. It finds broad application in energy storage, flexible electronics, and bioelectronics. Additive manufacturing opens a plethora of new avenues to form and shape PEDOT:PSS, allowing for the rapid construction of customized geometries. However, there are difficulties in printing PEDOT:PSS while maintaining its attractive properties. A 3D printing method for PEDOT:PSS using a room‐temperature coagulation bath‐based direct ink writing technique is reported. This technique enables fabrication of PEDOT:PSS into parts that are of high resolution and high conductivity, while maintaining stable electrochemical properties. The coagulation bath can be further modified to improve the mechanical properties of the resultant printed part via a one‐step reaction. Furthermore, it is demonstrated that a simple post‐processing step allows the printed electrodes to strongly adhere to several substrates under aqueous conditions, broadening their use in bioelectronics. Employing 3D printing of PEDOT:PSS, a cortex‐wide neural interface is fabricated, and intracranial electrical stimulation and simultaneous optical monitoring of mice brain activity with wide field calcium imaging are demonstrated. This reported 3D‐printing technique eliminates the need for cumbersome experimental setups while offering desired material properties.
Competitive Site Occupation toward Improved Quantum Efficiency of SrLaScO4:Eu Red Phosphors for Warm White LEDs
Authors: Yang Zhiyu , Liu Gaochao , Zhao Yifei , Zhou Yayun , Qiao Jianwei , Molokeev Maxim S. , Swart Hendrik C. , Xia Zhiguo 
Published: February 2022

AbstractThe discovery of Eu2+‐doped high‐efficiency red phosphors remains a vital challenge for white light‐emitting diode (WLED) applications. It is therefore urgent to find effective strategies managing the oxidation state to help reduce Eu3+ to Eu2+ and accordingly increase the photoluminescence quantum yield (PLQY). Herein, a new red‐emitting SrLaScO4:Eu phosphor is designed, and the PLQY is enhanced from 13% to 67% under 450 nm excitation by employing (NH4)2SO4‐assisted sintering. Combined structural analysis, optical spectroscopy, and theoretical calculation reveal that predominant Eu2+ prefers to occupy the Sr2+ sites in the SrLaScO4 enabling red emission, and a competitive site occupation of Eu3+ in La3+ can be restrained, and the reduction mechanism of Eu3+ to Eu2+ originating from the (NH4)2SO4 addition is analyzed. The fabricated WLED device using red‐emitting SrLaScO4:Eu and yellow‐emitting Y3(Al,Ga)5O12:Ce3+ exhibits a high color‐rendering index of 86.7 at a low correlated color temperature of 4005 K. This work provides a feasible reduction strategy for guiding the development of high‐efficiency Eu2+‐doped red phosphor for WLED applications.
3D Switchable Diffractive Optical Elements Fabricated with Two‐Photon Polymerization
Authors: Sandford O'Neill John , Salter Patrick , Zhao Zimo , Chen Bohan , Daginawalla Hassan , Booth Martin J. , Elston Steve J. , Morris Stephen M. 
Published: February 2022

AbstractDirect laser writing is demonstrated by two‐photon polymerization of multi‐element diffractive optical components that can be switched on and off with an applied voltage. By exploiting the 3D capabilities of the laser microfabrication technique, multiple diffractive optical elements are written into a single liquid crystal (LC) layer. The switching behavior of the diffractive optical elements is controlled by simply changing the write‐voltage of the anisotropic polymer structures during fabrication. Initially, 2D diffraction gratings are written at different depths within the LC layer. Each element is then activated by applying a voltage of sufficient amplitude that causes the second diffractive optical element to become inactive. This is then followed by a demonstration of multi‐element computer generated holograms that are written at different depths within the LC layer. By altering the magnitude of the applied voltage, different images/patterns can be observed in the replay field using a simple electrode configuration. These compact and transmissive LC optical components could excel in applications where a degree of switchability is required but a highly pixelated fully programmable device is excessive.
Recent Development of Hierarchical Metal Oxides Based Gas Sensors: From Gas Sensing Performance to Applications
Authors: Yu HaiXia , Guo ChuanYu , Zhang XianFa , Xu YingMing , Cheng XiaoLi , Gao Shan , Huo LiHua 
Published: February 2022

AbstractGas sensors based on metal oxides have attracted wide attention, due to their inherent advantages such as low cost, small size, fast response, and easy usage. Recently, much effort have been put into the design of metal oxide‐based sensing materials to further improve the performance of gas sensors. Among them, the fabrication of hierarchical metal oxide‐based sensing materials has become the most attractive strategy. In this article, the authors widely review the last decade of development of hierarchical metal oxide‐based gas sensors, in which several representative gases including formaldehyde, acetone, H2S, amines, and water are chosen as the analytes to discuss in depth. The application fields cover indoor air quality monitoring, breath analysis, and food quality and safety. The research advances for each gas is summarized from the perspective of excellent sensing performance in terms of low operating temperature and detection limit, high selectivity, fast responses, and humidity independent responses. Furthermore, the accepted sensing mechanism of metal oxide‐based gas sensors and widely used technology to verify these mechanisms are both included. Finally, the outlook and challenges for future investigations of hierarchical metal oxide‐based gas sensors are also discussed from the perspectives of theory and practice.
Procedures and Guidelines for Inputting and Output Smoothening of Kinetic Monte Carlo Distributions
Authors: De Keer Lies , Edeleva Mariya , Figueira Freddy L. , Reyes Pablo , D'hooge Dagmar R. , Van Steenberge Paul H.M. 
Published: February 2022

AbstractPopulation balance modeling is very popular in several branches of modern science, including (bio)chemical engineering, geography, and demography. A growing trend is the use of stochastic solvers (e.g., kinetic Monte Carlo), but care should be taken upon inputting and outputting distributed data for the populations involved. In the present contribution, several procedures and guidelines are formulated facilitating such data treatment. The solutions are exemplified through polymerization and polymer modification case studies, taking the molar mass or chain length as core stochastic variable. It is shown that rediscretization is often necessary, as experimentally measured distributions are not directly interpretable at the input side of stochastic solvers. This rediscretization should take place both for the abscissa and ordinate values of the distributions. As stochastic solvers often display noisy data as model output, attention is paid to the smoothening of the output distributions as well. It is highlighted that the kernel‐smoothening method is very promising, as it can reliably tackle postprocessing of nonsymmetric distributions. Guidelines are formulated regarding the correct interpretation of the distribution tail both for the input and output modifications.
High‐Efficiency Non‐Toxic 2‐Terminal and 4‐Terminal Perovskite‐Transition Metal Dichalcogenide Tandem Solar Cells
Authors: Jayan K Deepthi 
Published: February 2022

AbstractThe modeling tool, SCAPS 1D, is applied to simulate a monolithic 2‐T and mechanically stacked 4‐T tandem solar device architectures with methyl ammonium germanium iodide (MAGeI3) perovskite as the active layer of the top cell and transition metal dichalcogenide as the active layer of the bottom cell. To establish the requirement of current density matching between the two subcells of the monolithic 2‐T configuration, a recombination layer composed of indium doped tin oxide (ITO) is also introduced. The thickness of the MAGeI3, TMD, and ITO are optimized to 950, 340, and 100 nm to achieve the current matching condition. The 2‐T device configuration is able to establish a high fill factor (FF) and power conversion efficiency (PCE) of 86.19% and 27.09% after optimizing the physical parameters of the layers. The 4‐T mechanically stacked tandem architecture is also simulated using the SCAPS 1D tool and a maximum possible PCE of 35.11% is achieved after optimizing the physical parameters of the light captivating layers, viz. thickness, the number density of defects and dopants, and the operating conditions viz. temperature, parasitic resistances, and work function of the materials employed as rear contacts.
Surface Valence State Effect of MoO2+x on Electrochemical Nitrogen Reduction
Authors: Wang Jiaqi , Jiang Zhou , Peng Guiming , Hoenig Eli , Yan Gangbin , Wang Mingzhan , Liu Yuanyue , Du Xiwen , Liu Chong 
Published: February 2022

AbstractThe valance of Mo is critical for FeMo cofactor in ambient ammonia synthesis. However, the valence effect of Mo has not been well studied in heterogeneous nanoparticle catalysts for electrochemical nitrogen reduction reaction (NRR) due to the dissolution of Mo as MoO42− in alkaline electrolytes. Here, a MoO2+x catalyst enriched with surface Mo6+ is reported. The Mo6+ is stabilized by a native oxide layer to prevent corrosion and its speciation is identified as (MoO3)n clusters. This native layer with Mo6+ suppresses the hydrogen evolution significantly and promotes the activation of nitrogen as supported by both experimental characterization and theoretical calculation. The as‐prepared MoO2+x catalyst shows a high ammonia yield of 3.95 µg mgcat−1h−1 with a high Faradaic efficiency of 22.1% at −0.2 V versus reversible hydrogen electrode, which is much better than the MoO2 catalyst with Mo6+ etched away. The accuracy of experimental results for NRR is confirmed by various control experiments and quantitative isotope labeling.
Lemon‐Derived Extracellular Vesicles Nanodrugs Enable to Efficiently Overcome Cancer Multidrug Resistance by Endocytosis‐Triggered Energy Dissipation and Energy Production Reduction
Authors: Xiao Qian , Zhao Wei , Wu Chentian , Wang Xuejiao , Chen Jianping , Shi Xiubo , Sha Suinan , Li Jinheng , Liang Xiaomei , Yang Yulu , Guo Haoyan , Wang Ying , Fan Jun‐Bing 
Published: February 2022

AbstractMultidrug resistance remains a great challenge for cancer chemotherapy. Herein, a biomimetic drug delivery system based on lemon‐derived extracellular vesicles (EVs) nanodrugs (marked with heparin‐cRGD‐EVs‐doxorubicin (HRED)) is demonstrated, achieving highly efficient overcoming cancer multidrug resistance. The HRED is fabricated by modifying functional heparin‐cRGD (HR) onto the surface of EVs and then by loading with doxorubicin (DOX). The obtained HRED enable to effectively enter DOX‐resistant cancer cells by caveolin‐mediated endocytosis (main), macropinocytosis (secondary), and clathrin‐mediated endocytosis (last), exhibiting excellent cellular uptake capacity. The diversified endocytosis capacity of HRED can efficiently dissipate intracellular energy and meanwhile trigger downstream production reduction of adenosine triphosphate (ATP), leading to a significant reduction of drug efflux. Consequently, they show excellent anti‐proliferation capacities to DOX‐resistant ovarian cancer, ensuring the efficiently overcoming ovarian cancer multidrug resistance in vivo. The authors believe this strategy provides a new strategy by endocytosis triggered‐energy dissipation and ATP production reduction to design drug delivery system for overcoming cancer multidrug resistance.
Oxide Two‐Dimensional Electron Gas with High Mobility at Room‐Temperature
Authors: Eom Kitae , Paik Hanjong , Seo Jinsol , Campbell Neil , Tsymbal Evgeny Y. , Oh Sang Ho , Rzchowski Mark S. , Schlom Darrell G. , Eom Chang‐Beom 
Published: February 2022

AbstractThe prospect of 2‐dimensional electron gases (2DEGs) possessing high mobility at room temperature in wide‐bandgap perovskite stannates is enticing for oxide electronics, particularly to realize transparent and high‐electron mobility transistors. Nonetheless only a small number of studies to date report 2DEGs in BaSnO3‐based heterostructures. Here, 2DEG formation at the LaScO3/BaSnO3 (LSO/BSO) interface with a room‐temperature mobility of 60 cm2 V−1 s−1 at a carrier concentration of 1.7 × 1013 cm–2 is reported. This is an order of magnitude higher mobility at room temperature than achieved in SrTiO3‐based 2DEGs. This is achieved by combining a thick BSO buffer layer with an ex situ high‐temperature treatment, which not only reduces the dislocation density but also produces a SnO2‐terminated atomically flat surface, followed by the growth of an overlying BSO/LSO interface. Using weak beam dark‐field transmission electron microscopy imaging and in‐line electron holography technique, a reduction of the threading dislocation density is revealed, and direct evidence for the spatial confinement of a 2DEG at the BSO/LSO interface is provided. This work opens a new pathway to explore the exciting physics of stannate‐based 2DEGs at application‐relevant temperatures for oxide nanoelectronics.
Hydrogels as Soft Ionic Conductors in Flexible and Wearable Triboelectric Nanogenerators
Authors: Wu Yinghong , Luo Yang , Cuthbert Tyler J. , Shokurov Alexander V. , Chu Paul K. , Feng Shien‐Ping , Menon Carlo 
Published: February 2022

AbstractFlexible triboelectric nanogenerators (TENGs) have attracted increasing interest since their advent in 2012. In comparison with other flexible electrodes, hydrogels possess transparency, stretchability, biocompatibility, and tunable ionic conductivity, which together provide great potential as current collectors in TENGs for wearable applications. The development of hydrogel‐based TENGs (H‐TENGs) is currently a burgeoning field but research efforts have lagged behind those of other common flexible TENGs. In order to spur research and development of this important area, a comprehensive review that summarizes recent advances and challenges of H‐TENGs will be very useful to researchers and engineers in this emerging field. Herein, the advantages and types of hydrogels as soft ionic conductors in TENGs are presented, followed by detailed descriptions of the advanced functions, enhanced output performance, as well as flexible and wearable applications of H‐TENGs. Finally, the challenges and prospects of H‐TENGs are discussed.
Multipotent Poly(Tertiary Amine‐Oxide) Micelles for Efficient Cancer Drug Delivery
Authors: Xiang Jiajia , Shen Yihuai , Zhang Yifan , Liu Xin , Zhou Quan , Zhou Zhuxian , Tang Jianbin , Shao Shiqun , Shen Youqing 
Published: February 2022

AbstractThe cancer drug delivery process involves a series of biological barriers, which require the nanomedicine to exhibit different, even opposite properties for high therapeutic efficacy. The prevailing design philosophy, i.e., integrating these properties within one nanomedicine via on‐demand property transitions such as PEGylation/dePEGylation, complicates nanomedicines’ composition and thus impedes clinical translation. Here, polyzwitterionic micelles of poly(tertiary amine‐oxide)‐block‐poly(ε‐caprolactone) (PTAO‐PCL) amphiphiles that enable all the required functions are presented. The zwitterionic nature and unique cell membrane affinity confer the PTAO micelles long blood circulation, efficient tumor accumulation and penetration, and fast cellular internalization. The mitochondrial targeting capability allows drug delivery into the mitochondria to induce mitochondrial dysfunction and overcome tumor multidrug resistance. As a result, the PTAO/drug micelles exhibit potent anticancer efficacy. This simple yet multipotent carrier system holds great promise as a generic platform for potential clinical translation.
Electronic State Modulation and Reaction Pathway Regulation on Necklace‐Like MnOx‐CeO2@Polypyrrole Hierarchical Cathode for Advanced and Flexible Li–CO2 Batteries
Authors: Deng Qinghua , Yang Yong , Mao Chunfeng , Wang Tianyu , Fang Zhao , Yan Wuwei , Yin Kai , Zhang Yiwei 
Published: February 2022

AbstractLi–CO2 batteries provide the possibility for synchronous implementation of carbon neutrality and development of advanced energy storage devices. Catalytic cathodes composed of well‐designed conductive substrates and active materials are critical to the improvement of Li–CO2 batteries. Herein, MnOx‐CeO2 hollow nanospheres are strung together by conductive polypyrrole (PPy) via post‐in‐situ polymerization, and a necklace‐like MnOx‐CeO2@PPy hierarchical cathode with excellent flexibility and self‐supporting feature is constructed. Benefitting from the excellent conductivity of PPy, the binder‐free structure, and the greatly exposed catalytic active sites, the MnOx‐CeO2@PPy based Li–CO2 batteries exhibit superior discharge capacity (13631 mA h g–1 at 100 mA g–1) and cycle performance (253 cycles) as well as a low overpotential of 1.49 V. Of particular note, the flexible freestanding film is confirmed as a potential catalytic cathode for flexible Li–CO2 batteries. The density functional theory calculations, combined with experimental tests, are performed to gain insights into the enhanced substrate adsorption capacity, the optimized electronic structure of the active surface MnOx‐CeO2 (111), the concentrated electrons on the reaction sites Ce, and the electrochemical mechanism. This work initiates the use of conductive polymers for catalytic cathodes in Li–CO2 batteries, which provide new opportunities for promoting the performance of various energy storage devices.
Microbial Disinfection with Supercoiling Capacitive Triboelectric Nanogenerator
Authors: Huo Zheng‐Yang , Lee Dong‐Min , Jeong Jang‐Mook , Kim Young‐Jun , Kim Jihye , Suh In‐Yong , Xiong Peixun , Kim Sang‐Woo 
Published: February 2022

AbstractWater‐borne diseases resulting from pathogen infection are especially challenges in areas with inadequate sanitation and power supply. Here a novel disinfection system is developed for bacterial and viral inactivation in water using a self‐powered supercoiling‐mediated rotational triboelectric nanogenerator (S‐TENG) as a power source to drive a new oxidation‐assisted electroporation mechanism. Owing to its rational design, the S‐TENG achieves an ultrafast rotation (≈7500 rpm), therefore it enables a simultaneous nanowire‐enhanced localized electric field and generation of oxidative species resulting in high disinfection performance: >99.9999% microbial inactivation at a high flux of 15 000 L h‐1 m‐2. An integrated S‐TENG‐powered disinfection prototype using an enlarged electrode (area of 50 cm2) achieves complete disinfection when the gravity‐driven natural water flows through the whole system at a high rate (1 L min‐1). This rapid, self‐powered water disinfection method is a potential solution for urgent water disinfection needs during disasters and pandemics, and water disinfection in areas with inadequate power supply.
Phase Separation of Oppositely Charged Polymers Regulates Bioinspired Silicification
Authors: Zhai Hang , Bendikov Tatyana , Gal Assaf 
Published: February 2022

AbstractIn nature, simple organisms evolved mechanisms to form intricate biosilica nanostructures, far exceeding current synthetic manufacturing. Based on the properties of extracted biomacromolecules, polycation–polyanion pairs were suggested as moderators of biosilica formation. However, the chemical principles of this polymer‐induced silicification remain unclear. Here, we used a biomimetic polycation–polyanion system to study polymer‐induced silicification. We demonstrate that it is the polymer phase separation process, rather than silica–polymer interactions, which controls silica precipitation. Since ionic strength controls this electrostatic phase separation, it can be used to tune the morphology and structure of the precipitates. In situ cryo electron microscopy highlights the pivotal role of the hydrated polymer condensates in this process. These results pave the road for developing nanoscale morphologies of bioinspired silica based on the chemistry of liquid‐liquid phase separation.
Molecular Catalysts for the Reductive Homocoupling of CO2 towards C2+ Compounds
Authors: Liang Hong‐Qing , Beweries Torsten , Francke Robert , Beller Matthias 
Published: February 2022

AbstractThe conversion of CO2 into multicarbon (C2+) compounds by reductive homocoupling offers the possibility to transform renewable energy into chemical energy carriers and thereby create “carbon‐neutral” fuels or other valuable products. Most available studies have employed heterogeneous metallic catalysts, but the use of molecular catalysts is still underexplored. However, several studies have already demonstrated the great potential of the molecular approach, namely, the possibility to gain a deep mechanistic understanding and a more precise control of the product selectivity. This Minireview summarizes recent progress in both the thermo‐ and electrochemical reductive homocoupling of CO2 toward C2+ products mediated by molecular catalysts. In addition, reductive CO homocoupling is discussed as a model for the further conversion of intermediates obtained from CO2 reduction, which may serve as a source of inspiration for developing novel molecular catalysts in the future.
IgG Anti–Citrullinated Protein Antibody Variable Domain Glycosylation Increases Before the Onset of Rheumatoid Arthritis and Stabilizes Thereafter: A Cross‐Sectional Study Encompassing ~1,500 Samples
Authors: Kissel Theresa , Hafkenscheid Lise , Wesemael Tineke J. , Tamai Mami , Kawashiri Shin‐ya , Kawakami Atsushi , El‐Gabalawy Hani S. , van Schaardenburg Dirkjan , Rantapää‐Dahlqvist Solbritt , Wuhrer Manfred , van der Helm‐van Mil Annette H. M. , Allaart Cornelia F. , van der Woude Diane , Scherer Hans U. , Toes Rene E. M. , Huizinga Tom W. J. 
Published: February 2022

ObjectiveThe autoimmune response in rheumatoid arthritis (RA) is marked by the presence of anti–citrullinated protein antibodies (ACPAs). A notable feature of IgG ACPA is the abundant expression of N‐linked glycans in the variable domain. However, the presence of ACPA variable domain glycosylation (VDG) across disease stages, and its response to therapy, are poorly described. To understand its dynamics, we investigated the abundance of IgG ACPA VDG in 1,498 samples from individuals in different clinical stages.MethodsUsing liquid chromatography, we analyzed IgG ACPA VDG profiles in 7 different cohorts from Japan, Canada, The Netherlands, and Sweden. We assessed 106 healthy individuals, 228 individuals with presymptomatic RA, 277 individuals with arthralgia, 307 patients with new‐onset/early RA, and 117 RA patients after prespecified treatment regimens. Additionally, we measured VDG in 234 samples from patients with RA who did or did not achieve long‐term drug‐free remission (DFR) during up to 16 years follow‐up.ResultsIgG ACPA VDG significantly increased (P < 0.0001) toward disease onset and was associated with ACPA levels and epitope spreading prior to diagnosis. A slight increase in VDG was observed in patients with established RA, with a moderate influence of treatment (P = 0.007). In patients in whom DFR was later achieved, IgG ACPA VDG was already reduced at the time of RA onset.ConclusionThe abundance of IgG ACPA VDG increases toward RA onset and correlates with maturation of the ACPA response. While IgG ACPA VDG levels are fairly stable in established disease, a lower degree of VDG at RA onset correlates with DFR. Although the underlying biologic mechanisms remain elusive, our data support the concept that VDG relates to an expansion of the ACPA response in the pre‐disease phase and contributes to disease development.