bluuebunny/crossref_metadata_2025_split huggingface dataset:
A Fully Integrated Miniaturized Optical Biosensor for Fast and Multiplexing Plasmonic Detection of High‐ and Low‐Molecular‐Weight Analytes
Authors: Bolognesi Margherita , Prosa Mario , Toerker Michael , Lopez Sanchez Laura , Wieczorek Martin , Giacomelli Caterina , Benvenuti Emilia , Pellacani Paola , Elferink Alexander , Morschhauser Andreas , Sola Laura , Damin Francesco , Chiari Marcella , Whatton Mark , Haenni Etienne , Kallweit David , Marabelli Franco , Peters Jeroen , Toffanin Stefano 
Published: March 2023

AbstractOptical biosensors based on plasmonic sensing schemes combine high sensitivity and selectivity with label‐free detection. However, the use of bulky optical components is still hampering the possibility of obtaining miniaturized systems required for analysis in real settings. Here, a fully miniaturized optical biosensor prototype based on plasmonic detection is demonstrated, which enables fast and multiplex sensing of analytes with high‐ and low molecular weight (80 000 and 582 Da) as quality and safety parameters for milk: a protein (lactoferrin) and an antibiotic (streptomycin). The optical sensor is based on the smart integration of: i) miniaturized organic optoelectronic devices used as light‐emitting and light‐sensing elements and ii) a functionalized nanostructured plasmonic grating for highly sensitive and specific localized surface plasmon resonance (SPR) detection. The sensor provides quantitative and linear response reaching a limit of detection of 10−4 refractive index units once it is calibrated by standard solutions. Analyte‐specific and rapid (15 min long) immunoassay‐based detection is demonstrated for both targets. By using a custom algorithm based on principal‐component analysis, a linear dose–response curve is constructed which correlates with a limit of detection (LOD) as low as 3.7 µg mL−1 for lactoferrin, thus assessing that the miniaturized optical biosensor is well‐aligned with the chosen reference benchtop SPR method.
Generation of 13.9‐mJ Terahertz Radiation from Lithium Niobate Materials
Authors: Wu Xiaojun , Kong Deyin , Hao Sibo , Zeng Yushan , Yu Xieqiu , Zhang Baolong , Dai Mingcong , Liu Shaojie , Wang Jiaqi , Ren Zejun , Chen Sai , Sang Jianhua , Wang Kang , Zhang Dongdong , Liu Zhongkai , Gui Jiayan , Yang Xiaojun , Xu Yi , Leng Yuxin , Li Yutong , Song Liwei , Tian Ye , Li Ruxin 
Published: March 2023

AbstractExtremely strong‐field terahertz (THz) radiation in free space has compelling applications in nonequilibrium condensed matter state regulation, all‐optical THz electron acceleration and manipulation, THz biological effects, etc. However, these practical applications are constrained by the absence of high‐intensity, high‐efficiency, high‐beam‐quality, and stable solid‐state THz light sources. Here, the generation of single‐cycle 13.9‐mJ extreme THz pulses from cryogenically cooled lithium niobate crystals and a 1.2% energy conversion efficiency from 800 nm to THz are demonstrated experimentally using the tilted pulse‐front technique driven by a home‐built 30‐fs, 1.2‐Joule Ti:sapphire laser amplifier. The focused peak electric field strength is estimated to be 7.5 MV cm−1. A record of 1.1‐mJ THz single‐pulse energy at a 450 mJ pump at room temperature is produced and observed that the self‐phase modulation of the optical pump can induce THz saturation behavior from the crystals in the substantially nonlinear pump regime. This study lays the foundation for the generation of sub‐Joule THz radiation from lithium niobate crystals and will inspire more innovations in extreme THz science and applications.
Asymmetrically Coordinated CoB1N3 Moieties for Selective Generation of High‐Valence Co‐Oxo Species via Coupled Electron–Proton Transfer in Fenton‐like Reactions
Authors: Song Junsheng , Hou Nannan , Liu Xiaocheng , Antonietti Markus , Zhang Pengjun , Ding Rongrong , Song Li , Wang Yang , Mu Yang 
Published: March 2023

AbstractHigh‐valence metal species generated in peroxymonosulfate (PMS)‐based Fenton‐like processes are promising candidates for selective degradation of contaminants in water, the formation of which necessitates the cleavage of OH and OO bonds as well as efficient electron transfer. However, the high dissociation energy of OH bond makes its cleavage quite challenging, largely hampering the selective generation of reactive oxygen species. Herein, an asymmetrical configuration characterized by a single cobalt atom coordinated with boron and nitrogen (CoB1N3) is established to offer a strong local electric field, upon which the cleavage of OH bond is thermodynamically favored via a promoted coupled electron–proton transfer process, which serves an essential step to further allow OO bond cleavage and efficient electron transfer. Accordingly, the selective formation of Co(IV)O in a single‐atom Co/PMS system enables highly efficient removal performance toward various organic pollutants. The proposed strategy also holds true in other heteroatom doping systems to configure asymmetric coordination, thus paving alternative pathways for specific reactive species conversion by rationalized design of catalysts at atomic level toward environmental applications and more.
Heterologous Assembly of Pleomorphic Bacterial Microcompartment Shell Architectures Spanning the Nano‐ to Microscale
Authors: Ferlez Bryan H. , Kirst Henning , Greber Basil J. , Nogales Eva , Sutter Markus , Kerfeld Cheryl A. 
Published: March 2023

AbstractMany bacteria use protein‐based organelles known as bacterial microcompartments (BMCs) to organize and sequester sequential enzymatic reactions. Regardless of their specialized metabolic function, all BMCs are delimited by a shell made of multiple structurally redundant, yet functionally diverse, hexameric (BMC‐H), pseudohexameric/trimeric (BMC‐T), or pentameric (BMC‐P) shell protein paralogs. When expressed without their native cargo, shell proteins have been shown to self‐assemble into 2D sheets, open‐ended nanotubes, and closed shells of ≈40 nm diameter that are being developed as scaffolds and nanocontainers for applications in biotechnology. Here, by leveraging a strategy for affinity‐based purification, it is demonstrated that a wide range of empty synthetic shells, many differing in end‐cap structures, can be derived from a glycyl radical enzyme‐associated microcompartment. The range of pleomorphic shells observed, which span ≈2 orders of magnitude in size from ≈25 nm to ≈1.8 µm, reveal the remarkable plasticity of BMC‐based biomaterials. In addition, new capped nanotube and nanocone morphologies are observed that are consistent with a multicomponent geometric model in which architectural principles are shared among asymmetric carbon, viral protein, and BMC‐based structures.
Ultrahigh Performance, Serially Stackable, Breeze Driven Triboelectric Generator via Ambient Air Ionizing Channel
Authors: Son Jin‐ho , Chung Seh‐Hoon , Cha Kyunghwan , Kim Sunghan , Lin Zong‐Hong , Hong Jinkee , Chung Jihoon , Lee Sangmin 
Published: March 2023

AbstractCurrently, wind energy harvesting is in the limelight. However, with the existing electromagnetic wind generators, it is difficult to harvest multifariously‐wasted breezes. To harvest energy from winds at a wide range of speeds, wind‐driven triboelectric nanogenerators (TENGs) are studied. However, a critical limitation of general wind‐driven TENGs is that their power output is low. Therefore, an innovative strategy is necessary to generate high output power even from breeze. Herein, an approach to test a charge‐polarization‐based flutter‐driven TENG (CPF‐TENG) with ambient air ionizing channel (AAIC) is reported. Owing to AAIC, the device generates peak voltage and current outputs of 2000 V and 4 A, respectively. Moreover, because the proposed CPF‐TENG can generate power from breeze, it can be stacked in series to completely harvest wind energy. The stacked CPF‐TENG is demonstrated to operate 3000 light‐emitting diodes (LEDs) and 12 hygrometers, separately, and produce hydrogen at a rate of 342.3 µL h−1 with the electrolysis cell.
Artificial Lipid Biomembranes for Full‐Length SARS‐CoV‐2 Receptor
Authors: Wang Ting , Lin Xiaomei , Li Yuting , Lu Yuan 
Published: March 2023

AbstractThe angiotensin‐converting enzyme 2 (ACE2), as a functional receptor for severe acute respiratory syndrome coronavirus 2 (SARS‐CoV‐2), is essential for assessing potential hosts and treatments. However, many studies are based on its truncated version but not full‐length structure. Indeed, a single transmembrane (TM) helix presents in the full‐length ACE2, influencing its interaction with SARS‐CoV‐2. Therefore, synthesis of the full‐length ACE2 is an urgent requirement. Here, cell‐free membrane protein synthesis systems (CFMPSs) are constructed for full‐length membrane proteins. MscL is screened as a model among ten membrane proteins based on their expression and solubility. Next, CFMPSs are constructed and optimized based on natural vesicles, vesicles with four membrane proteins removed or two chaperonins added, and 37 types of nanodiscs. They all increase membrane protein solubility to over 50%. Finally, the full‐length ACE2 of 21 species are successfully expressed with yields between 0.4 and 0.9 mg mL−1. The definite functional differences from the truncated version suggest that the TM region affects ACE2's structure and function. CFMPSs can be extended to more membrane proteins, paving the way for further applications.
Porous 3D Printable Hydrogels
Authors: Baur Eva , Hirsch Matteo , Amstad Esther 
Published: March 2023

AbstractHydrogels are interconnected, polymeric networks filled with water. Their inherent responsiveness to different stimuli, including the presence of salt, solvents, or, depending on their composition, changes in pH or temperature, renders them attractive for actuation and delivery purposes. Yet, the limited diffusivity within hydrogels hampers an efficient exchange of reagents such as active ingredients or solutes. The diffusivity can be increased if pores are incorporated into hydrogels. However, these pores typically weaken hydrogels, preventing their use for load‐bearing applications. This work reports a method to controllably introduce open pores with diameters of 10 s of nanometers into hydrogels whose mechanical properties are still remarkable, with compression moduli above 100 kPa. Importantly, these hydrogels can be 3D printed, thereby opening up possibilities to tune the pore size within hydrogels from the 10 s of nm up to the cm size range. This work leverages the 3D printability of this material to locally vary the degree of porosity while maintaining mechanical properties that enable facile handling of the integral samples. Thereby, this work introduces new opportunities to size‐selectively infiltrate different substances at well‐defined locations.
Effects of Anions and Protein Structures on Protein‐Based Solid Electrolytes
Authors: Ying Chunhua , Wang Chenxu , Zhong Wei‐Hong , Liu Jin 
Published: March 2023

AbstractLow ionic conductivity is one of the main hurdles for the practical application of advanced all‐solid‐state lithium‐ion batteries. Protein‐based solid electrolytes are recently proposed and can potentially provide both high ionic conductivity and high mechanical properties due to the decoupled ion transport mechanism. In this work, the effects of lithium salts and protein structures on the performance of protein‐based electrolytes through both ab initio density functional theory calculations and experiments are systematically investigated. The results show that the anions can be strongly locked by the charged amino acids, thus providing intermediate hopping sites for lithium‐ion, reducing energy barrier for lithium‐ion transport, and then enhancing the ionic conductivity. These calculations also demonstrate that need to be locked at appropriate positions by properly controlling the protein structures in order to provide bridging effects and facilitate lithium‐ion transport. The findings are consistent with the experimental observations and can provide guidance for design and optimization of protein‐based solid electrolytes.
Improved Optical Properties of Lead‐Free Double Perovskite Cs2AgBiBr6 Nanocrystals via Na Ions Doping
Authors: Wang Song , Jiang Wangsheng , Cui Wenjing , Jiang Wenchao , Zhao Min , Sun Jianhui , Liu Binghang , Lai Xiaofeng , Shi Keying , Pan Kai 
Published: March 2023

AbstractLead‐free double perovskite nanocrystals (NCs) are a promising alternative to lead‐based perovskite NCs for optoelectronic materials due to their nontoxic and good moist‐thermal stability. However, most of the lead‐free double perovskite NCs exhibit unsatisfying photoluminescence quantum yield (PLQY); the metal ions doping is an effective method to improve the optical properties. Here, monodisperse, homogeneous cubic morphology of Na+‐doped Cs2AgBiBr6 NCs is prepared via a colloidal synthesis strategy. When Na+ is doped into Cs2AgBiBr6 NCs, the inversion‐symmetry‐induced parity‐forbidden transition is broken. So, the wave function parity of the self‐trapped excitons at Ag atoms is changed, which allows the radiative transition to occur. This leads to a higher PLQY for Na+‐doped Cs2AgBiBr6 NCs (9.08%) than that for Cs2AgBiBr6 NCs (0.40%), and the exciton lifetime is extended from 1.87 ns for Cs2AgBiBr6 NCs to 17.15 ns for Na+‐doped Cs2AgBiBr6 NCs. The Na+ doping elevates the longitudinal optical phonon energy and exciton binding energy, which results in weaker nonradiative transitions during exciton recombination and improved NC thermal stability. So, the Na+‐doped Cs2AgBiBr6 NCs maybe possess potentially valuable applications in optoelectronic devices.
Rewritable Paper Based on Layered Metal–Organic Frameworks with NIR‐Triggered Reversible Color Switching
Authors: Liu Min , Ma Shu‐Hua , Dong Hui , Zeng Feng‐Lian , Jin Xue‐Ting , Luo Yang‐Hui 
Published: March 2023

AbstractPhotoreversible color‐switching materials, which can reversibly change color in response to external light stimuli, have attracted increasing attention for their applications in time‐sensitive information storage and optical data storage fields. But most of the related materials are dyes or redox compounds with ultraviolet as the light source, dramatically limiting the cycling stability during discoloration processes. To address this problem, a near‐infrared (NIR)‐responsive rewritable paper via doping layered Co‐metal–organic frameworks (MOFs) into the stable polyvinylidene fluoride matrix is reported for the first time. Layered Co‐MOF shows a rapid color‐switching characteristic between orange and black blue upon NIR illumination on/off because of the interlayer spacing changes. Benefiting from the soft network structures of the matrix, Co‐MOF can be homogeneously distributed to deliver an outstanding reversibility performance, including rapid response, coloration in a short period, and decoloration within about 3 min in ambient air. The fabrication of new photoreversible color switching system holds great potential in communication security, which offers a viable pathway to achieve ink‐free photoreversible printing.
Base‐Controlled Chemoselective Reaction of High‐Valent Cu(III)−CF3Compounds with Anilines: Access to Formamides or Hydrazines
Authors: Zheng Zhen‐Mei , Chen Ning , Dai Ming‐Suo , Zhang Song‐Lin 
Published: March 2023

AbstractThis study reports reactivity properties of Cu(III)−CF3compounds with anilines, wherein basicity‐dictated distinct reactivities are achieved, giving rise to formamides or hydrazines. Competing generation of difluorocarbene andN‐centered radical is proposed that is controlled by the basicity of the reaction solution. Specifically, under acidic or neutral conditions, reaction of anilines with Cu(III)−CF3compounds produces formamides, where difluorocarbene is involved, undergoing aniline formylation. In contrast, in the presence of a base, this same reaction selectively gives hydrazines instead, where Cu(III)−CF3compounds act as an oxidizing reagent to allow dehydrogenative N−H/N−H coupling of two anilines through anN‐centered radical. The scope of both reactions is studied, and application to medicinally relevant compounds is shown. This study shows the unusual use of high‐valent Cu(III) trifluoromethyl compounds as hydrogen‐abstracting reagents to allow dehydrogenative reactions.magnified image
Artificial Intelligence‐Based Medical Sensors for Healthcare System
Authors: Chen Mingrui , Cui Daxiang , Haick Hossam , Tang Ning 
Published: March 2023

AbstractThe aging population and the prevalence of infectious diseases have impacted the traditional medical order, significantly increasing the burden on healthcare and adversely affecting the socio‐economic system. Medical sensors based on artificial intelligence (AI) provide new ideas for modern medical data collection to monitor the health status of individuals and environmental changes. Meanwhile, with the aid of AI algorithms, the big data processing capabilities of sensor systems have been greatly improved, further realizing early predictions and timely diagnoses. In this paper, a brief overview is offered on the development status of AI‐enabled medical sensors for off‐body detection, near‐body monitoring, disease prediction, and clinical decision support system, and the ongoing challenges and future prospects to move from concept to implementation are discussed. In the foreseeable future, breakthroughs in the combination of medical sensors and AI algorithms are expected to pave the way for early detection and clinical decision support and improve the accuracy and efficiency for disease diagnosis.
Engineering Bifunctional Calcium Alendronate Gene‐Delivery Nanoneedle for Synergistic Chemo/Immuno‐Therapy Against HER2 Positive Ovarian Cancer
Authors: Chen Guochuang , Zeng Leli , Bi Bo , Huang Xiuyu , Qiu Miaojuan , Chen Ping , Chen Zhi‐Ying , He Yulong , Pan Yihang , Chen Yu , Zhao Jing 
Published: March 2023

AbstractOvarian cancer is the most lethal gynecological malignancy. Most patients are diagnosed at an advanced stage with widespread peritoneal dissemination and ascites. Bispecific T‐cell engagers (BiTEs) have demonstrated impressive antitumor efficacy in hematological malignancies, but the clinical potency is limited by their short half‐life, inconvenient continuous intravenous infusion, and severe toxicity at relevant therapeutic levels in solid tumors. To address these critical issues, the design and engineering of alendronate calcium (CaALN) based gene‐delivery system is reported to express therapeutic level of BiTE (HER2×CD3) for efficient ovarian cancer immunotherapy. Controllable construction of CaALN nanosphere and nanoneedle is achieved by the simple and green coordination reactions that the distinct nanoneedle‐like alendronate calcium (CaALN‐N) with a high aspect ratio enabled efficient gene delivery to the peritoneum without system in vivo toxicity. Especially, CaALN‐N induced apoptosis of SKOV3‐luc cell via down‐regulation of HER2 signaling pathway and synergized with HER2×CD3 to generate high antitumor response. In vivo administration of CaALN‐N/minicircle DNA encoding HER2×CD3 (MC‐HER2×CD3) produces sustained therapeutic levels of BiTE and suppresses tumor growth in a human ovarian cancer xenograft model. Collectively, the engineered alendronate calcium nanoneedle represents a bifunctional gene delivery platform for the efficient and synergistic treatment of ovarian cancer.
Manipulating Li2S Redox Kinetics and Lithium Dendrites by Core–Shell Catalysts under High Sulfur Loading and Lean‐Electrolyte Conditions
Authors: Zhen Mengmeng , Li Kaifeng , Liu Mingyang 
Published: March 2023

AbstractFor practical lithium–sulfur batteries (LSBs), the high sulfur loading and lean‐electrolyte are necessary conditions to achieve the high energy density. However, such extreme conditions will cause serious battery performance fading, due to the uncontrolled deposition of Li2S and lithium dendrite growth. Herein, the tiny Co nanoparticles embedded N‐doped carbon@Co9S8 core–shell material (CoNC@Co9S8NC) is designed to address these challenges. The Co9S8NC‐shell effectively captures lithium polysulfides (LiPSs) and electrolyte, and suppresses the lithium dendrite growth. The CoNC‐core not only improves electronic conductivity, but also promotes Li+ diffusion as well as accelerates Li2S deposition/decomposition. Consequently, the cell with CoNC@Co9S8NC modified separator delivers a high specific capacity of 700 mAh g−1 with a low‐capacity decay rate of 0.035% per cycle at 1.0 C after 750 cycles under a sulfur loading of 3.2 mg cm−2 and a E/S ratio of 12 µL mg−1, and a high initial areal capacity of 9.6 mAh cm−2 under a high sulfur loading of 8.8 mg cm−2 and a low E/S ratio of 4.5 µL mg−1. Besides, the CoNC@Co9S8NC exhibits an ultralow overpotential fluctuation of 11 mV at a current density of 0.5 mA cm–2 after 1000 h during a continuous Li plating/striping process.
Rapidly Inhibiting the Inflammatory Cytokine Storms and Restoring Cellular Homeostasis to Alleviate Sepsis by Blocking Pyroptosis and Mitochondrial Apoptosis Pathways
Authors: Yan Jiahui , Zhang Jingwen , Wang Yanan , Liu Hong , Sun Xueping , Li Aixin , Cui Pengfei , Yu Liangmin , Yan Xuefeng , He Zhiyu 
Published: March 2023

AbstractPyroptosis, systemic inflammation, and mitochondrial apoptosis are the three primary contributors to sepsis's multiple organ failure, the ultimate cause of high clinical mortality. Currently, the drugs under development only target a single pathogenesis, which is obviously insufficient. In this study, an acid‐responsive hollow mesoporous polydopamine (HMPDA) nanocarrier that is highly capable of carrying both the hydrophilic drug NAD+ and the hydrophobic drug BAPTA‐AM, with its outer layer being sealed by the inflammatory targeting peptide PEG‐LSA, is developed. Once targeted to the region of inflammation, HMPDA begins depolymerization, releasing the drugs NAD+ and BAPTA‐AM. Depletion of polydopamine on excessive reactive oxygen species production, promotion of ATP production and anti‐inflammation by NAD+ replenishment, and chelation of BAPTA (generated by BA‐AM hydrolysis) on overloaded Ca2+ can comprehensively block the three stages of sepsis, i.e., precisely inhibit the activation of pyroptosis pathway (NF‐κB‐NLRP3‐ASC‐Casp‐1), inflammation pathway (IL‐1β, IL‐6, and TNF‐α), and mitochondrial apoptosis pathway (Bcl‐2/Bax‐Cyt‐C‐Casp‐9‐Casp‐3), thereby restoring intracellular homeostasis, saving the cells in a state of “critical survival,” further reducing LPS‐induced systemic inflammation, finally restoring the organ functions. In conclusion, the synthesis of this agent provides a simple and effective synergistic drug delivery nanosystem, which demonstrates significant therapeutic potential in a model of LPS‐induced sepsis.