bluuebunny/crossref_metadata_2025_split huggingface dataset:
Injectable Nanoparticle‐Based Hydrogels Enable the Safe and Effective Deployment of Immunostimulatory CD40 Agonist Antibodies
Authors: Correa Santiago , Meany Emily L. , Gale Emily C. , Klich John H. , Saouaf Olivia M. , Mayer Aaron T. , Xiao Zunyu , Liong Celine S. , Brown Ryanne A. , Maikawa Caitlin L. , Grosskopf Abigail K. , Mann Joseph L. , Idoyaga Juliana , Appel Eric A. 
Published: August 2022

AbstractWhen properly deployed, the immune system can eliminate deadly pathogens, eradicate metastatic cancers, and provide long‐lasting protection from diverse diseases. Unfortunately, realizing these remarkable capabilities is inherently risky as disruption to immune homeostasis can elicit dangerous complications or autoimmune disorders. While current research is continuously expanding the arsenal of potent immunotherapeutics, there is a technological gap when it comes to controlling when, where, and how long these drugs act on the body. Here, this study explored the ability of a slow‐releasing injectable hydrogel depot to reduce dose‐limiting toxicities of immunostimulatory CD40 agonist (CD40a) while maintaining its potent anticancer efficacy. A previously described polymer‐nanoparticle (PNP) hydrogel system is leveraged that exhibits shear‐thinning and yield‐stress properties that are hypothesized to improve locoregional delivery of CD40a immunotherapy. Using positron emission tomography, it is demonstrated that prolonged hydrogel‐based delivery redistributes CD40a exposure to the tumor and the tumor draining lymph node (TdLN), thereby reducing weight loss, hepatotoxicity, and cytokine storm associated with standard treatment. Moreover, CD40a‐loaded hydrogels mediate improved local cytokine induction in the TdLN and improve treatment efficacy in the B16F10 melanoma model. PNP hydrogels, therefore, represent a facile, drug‐agnostic method to ameliorate immune‐related adverse effects and explore locoregional delivery of immunostimulatory drugs.
Gut Microbiome Analysis Can Be Used as a Noninvasive Diagnostic Tool and Plays an Essential Role in the Onset of Membranous Nephropathy
Authors: Shang Jin , Zhang Yiding , Guo Ruixue , Liu Wenli , Zhang Jun , Yan Ge , Wu Feng , Cui Wen , Wang Peipei , Zheng Xuejun , Wang Ting , Dong Yijun , Zhao Jing , Wang Li , Xiao Jing , Zhao Zhanzheng 
Published: August 2022

AbstractMembranous nephropathy (MN) is a common cause of nephrotic syndrome. The aim is to establish a non‐invasive diagnostic model of MN using differential gut microbiome analysis, and to explore the relationship between the gut microbiome and MN pathogenesis in vivo. 825 fecal samples from MN patients and healthy participants are collected from multiple medical centers across China. Key operational taxonomic units (OTUs) obtained through 16S rRNA sequencing are used to establish a diagnostic model. A rat model of MN is developed to explore the relationship between the gut microbiome and the pathogenesis of MN. The diversity and richness of the gut microbiome are significantly lower in patients with MN than in healthy individuals. The diagnostic model based on seven OTUs achieves an excellent efficiency of 98.36% in the training group and also achieves high efficiency in cross‐regional cohorts. In MN rat model, gut microbiome elimination prevents model establishment, but fecal microbiome transplantation restores the phenotype of protein urine. Gut microbiome analysis can be used as a non‐invasive tool for MN diagnosis. The onset of MN depends on the presence of naturally colonized microbiome. Early intervention in the gut microbiome may help reduce urinary protein level in MN.
Self‐Charging Persistent Mechanoluminescence with Mechanics Storage and Visualization Activities
Authors: Bai Yongqing , Guo Xiuping , Tian Birong , Liang Yongmin , Peng Dengfeng , Wang Zhaofeng 
Published: August 2022

AbstractPersistent mechanoluminescence (ML) with long lifetime is highly required to break the limits of the transient emitting behavior under mechanics stimuli. However, the existing materials with persistent ML are completely trap‐controlled, and a pre‐irradiation is required, which severely hinders the practical applications. In this work, a novel type of ML, self‐charging persistent ML, is created by compositing the Sr3Al2O5Cl2:Dy3+ (SAOCD) powders into flexible polydimethylsiloxane (PDMS) matrix. With no need for any pre‐irradiation, the as‐fabricated SAOCD/PDMS elastomer could exhibit intense and persistent ML under mechanics stimuli directly, which greatly facilitates its applications in mechanics lighting, displaying, imaging, and visualization. By investigating the matrix effects as well as the thermoluminescence, cathodoluminescence, and triboelectricity properties, the interfacial triboelectrification‐induced electron bombardment processes are demonstrated to be responsible for the self‐charged energy in SAOCD under mechanics stimuli. Based on the unique self‐charging processes, the SAOCD/PDMS further exhibits mechanics storage and visualized reading activities, which brings novel ideas and approaches to deal with the mechanics‐related problems in the fields of mechanical engineering, bioengineering, and artificial intelligence.
Wireless Non‐Invasive Monitoring of Cholesterol Using a Smart Contact Lens
Authors: Song Hayoung , Shin Haein , Seo Hunkyu , Park Wonjung , Joo Byung Jun , Kim Jeongho , Kim Jeonghyun , Kim Hong Kyun , Kim Jayoung , Park Jang‐Ung 
Published: August 2022

AbstractHerein, a wireless and soft smart contact lens that enables real‐time quantitative recording of cholesterol in tear fluids for the monitoring of patients with hyperlipidemia using a smartphone is reported. This contact lens incorporates an electrochemical biosensor for the continuous detection of cholesterol concentrations, stretchable antenna, and integrated circuits for wireless communication, which makes a smartphone the only device required to operate this lens remotely without obstructing the wearer's vision. The hyperlipidemia rabbit model is utilized to confirm the correlation between cholesterol levels in tear fluid and blood and to confirm the feasibility of this smart contact lens for diagnostic application of cholesterol‐related diseases. Further in vivo tests with human subjects demonstrated its good biocompatibility, wearability, and reliability as a non‐invasive healthcare device.
Interface Design Considering Intrinsic Properties of Dielectric Materials to Minimize Space‐Charge Layer Effect between Oxide Cathode and Sulfide Solid Electrolyte in All‐Solid‐State Batteries
Authors: Park Bo Keun , Kim Hyeongil , Kim Kyung Su , Kim Hyun‐Seung , Han Seung Ho , Yu Ji‐Sang , Hah Hoe Jin , Moon Janghyuk , Cho Woosuk , Kim Ki Jae 
Published: August 2022

AbstractIntroducing dielectric materials is a promising approach to mitigate space‐charge‐layer (SCL) formation, which negatively affects the electrochemical performance of sulfide‐based all‐solid‐state batteries (ASSBs). Most previous studies have focused on mitigating SCL formation by introducing dielectric materials, overlooking the fact that significant dielectric properties such as the dipole moment direction and the magnitude of the dielectric constant can influence SCL formation. To clarify the unclear mechanism of dielectric materials mitigating SCL formation, paraelectricity, ferroelectricity, and the magnitude of the dielectric constant are investigated to determine their effect on SCL formation. Paraelectric materials possessing no permanent dipole moment can effectively mitigate the SCL formation better than ferroelectric material with strong permanent dipole moment because of the intrinsic characteristics of the paraelectric material, in which the dipole moment can be aligned along the direction of the electric field applied inside of ASSB. Furthermore, paraelectric materials with a larger dielectric constant have a greater effect in mitigating SCL effect than paraelectric materials with a smaller dielectric constant. Thus, these properties should be considered in cathode‐solid‐electrolyte interface design. This study considers relevant dielectric material characteristics that had not been considered previously, suggesting a new paradigm for optimizing the interfacial resistance of sulfide‐based ASSBs originating from SCL formation.
Interfacial Embedding for High‐Efficiency and Stable Methylammonium‐Free Perovskite Solar Cells with Fluoroarene Hydrazine
Authors: Khadka Dhruba B. , Shirai Yasuhiro , Yanagida Masatoshi , Tadano Terumasa , Miyano Kenjiro 
Published: August 2022

AbstractPerovskite solar cells (PSCs) with state‐of‐the‐art efficiencies contain thermally unstable methylammonium (MA). Here, interfacial passivation with pentafluorophenylhydrazine (5F‐PHZ) to fabricate efficient and stable MA/Br‐free PSCs is introduced. The 5F‐PHZ surface treatment quenches the PbI2 and δ‐perovskite phase formed in the pristine film. The surface passivation ameliorates the film chemistries at the surface with modulation of interface band alignment as a consequence of halogen bonding with fluoroarene moieties or NH–NH2 terminals. This results in a much longer carrier lifetime with the passivation at the surface and grain boundaries trap centers. As a result, it boosts the power conversion efficiency (PCE) (area ≈ 1 cm2) from 18.10% to 22.29% (VOC ≈ 1.096–1.178 V) with superior operational thermal stability. A certified PCE of 21.01% with a large area of ≈1.026 cm2 is also achieved. It is found that the surface passivation forms an interfacial embedded layer subsequent to attenuation of defect densities and suppression of ion migration, which is supported by density‐function‐theory calculation. Importantly, this approach is effective in enhancing the PCE of narrow and wide bandgap perovskite systems. Thus, this work opens up a new technique for interface modulation with fluoroarene functional derivatives to achieve superior device performance and stability.
Transport properties of graphene oxide nanofiltration membranes: Electrokinetic modeling and experimental validation
Authors: Wang Zhongzhen , Xu Chunyan , Fu Qiang , Nair Sankar 
Published: August 2022

AbstractThere is a need for developing reliable models for water and solute transport in graphene oxide (GO) membranes for advancing their emerging industrial water processing applications. In this direction, we develop predictive transport models for GO and reduced‐GO (rGO) membranes over a wide solute concentration range (0.01–0.5 M) and compositions, based on the extended Nernst–Planck transport equations, Donnan equilibrium condition, and solute adsorption models. Some model parameters are obtained by fitting experimental permeation data for water and unary (single‐component) aqueous solutions. The model is validated by predicting experimental permeation behavior in binary solutions, which display very different characteristics. Sensitivity analysis of salt rejections as a function of membrane design parameters (pore size and membrane charge density) allows us to infer design targets to achieve high salt rejections. Such models will be useful in accelerating structure‐separation property relationships of GO membranes and for separation process design and optimization.
Kinetic and thermodynamic studies on [Omim]Cl/ZnCl2 catalyzed synthesis of polyoxymethylene dimethyl ethers
Authors: Wang Gang , Zhao Shirun , Yao Haoyu 
Published: August 2022

AbstractPolyoxymethylene dimethyl ethers (OMEs) emerging as green additives for soot emission suppression receive significant attention due to their similar physical properties to diesel. Herein, the transformative pathways of dimethoxymethane (DMM) and trioxane reactions for OMEs production catalyzed by [Omim]Cl/ZnCl2 having different ZnCl2 content were demonstrated in combination with the clarification of active species, kinetic and thermodynamic properties, and chemical nature for trioxane decomposition and subsequential formaldehyde insertion steps. The role of [Omim]Cl, which could transform to [Omim]ZnCl3 or [Omim]Zn2Cl5 under different ZnCl2 content, laid in the formation of active zinc species and promotion of their homogeneity with reactants. The DMM chain growth, which followed the same mechanism and kinetic law, showed kinetic and thermodynamic regimes and had identical equilibrium distribution of OMEs. Only Zn2Cl5− species were active for trioxane decomposition, which was the kinetic‐relevant step, while both ZnCl3− and Zn2Cl5− were effective for DMM chain elongation.
Genetics and epigenetics of self‐injurious thoughts and behaviors: Systematic review of the suicide literature and methodological considerations
Authors: Mirza Salahudeen , Docherty Anna R. , Bakian Amanda , Coon Hilary , Soares Jair C. , Walss‐Bass Consuelo , Fries Gabriel R. 
Published: August 2022

AbstractSuicide is a multifaceted and poorly understood clinical outcome, and there is an urgent need to advance research on its phenomenology and etiology. Epidemiological studies have demonstrated that suicidal behavior is heritable, suggesting that genetic and epigenetic information may serve as biomarkers for suicide risk. Here we systematically review the literature on genetic and epigenetic alterations observed in phenotypes across the full range of self‐injurious thoughts and behaviors (SITB). We included 577 studies focused on genome‐wide and epigenome‐wide associations, candidate genes (SNP and methylation), noncoding RNAs, and histones. Convergence of specific genes is limited across units of analysis, although pathway‐based analyses do indicate nervous system development and function and immunity/inflammation as potential underlying mechanisms of SITB. We provide suggestions for future work on the genetic and epigenetic correlates of SITB with a specific focus on measurement issues.
An Fe6C Core in All Nitrogenase Cofactors
Authors: Decamps Laure , Rice Derek B. , DeBeer Serena 
Published: August 2022

AbstractThe biological process of dinitrogen reduction to ammonium occurs at the cofactors of nitrogenases, the only enzymes that catalyze this challenging chemical reaction. Three types of nitrogenases have been described, named according to the heterometal in their cofactor: molybdenum, vanadium or iron nitrogenases. Spectroscopic and structural characterization allowed the unambiguous identification of the cofactors of molybdenum and vanadium nitrogenases and revealed a central μ6‐carbide in both of them. Although genetic studies suggested that the cofactor of the iron nitrogenase contains a similar Fe6C core, this has not been experimentally demonstrated. Here we report Valence‐to‐Core X‐ray Emission Spectroscopy providing experimental evidence that this cofactor contains a carbide, thereby making the Fe6C core a feature of all nitrogenase cofactors.
Molecular Doping of Flexible Lead‐Free Perovskite‐Polymer Thick Membranes for High‐Performance X‐Ray Detection
Authors: Liu Xinmei , Li Haojin , Cui Qingyue , Wang Shumei , Ma Chuang , Li Nan , Bu Nuo , Yang Tinghuan , Song Xin , Liu Yucheng , Yang Zhou , Zhao Kui , Liu Shengzhong (Frank) 
Published: August 2022

AbstractX‐ray detectors have broad applications in medicine and industry. Although flexible lead‐free perovskite films are competitive because of their lightweight and low toxicity, they are less efficient due to low charge transport. Herein, we report low‐toxicity, flexible X‐ray detectors based on p‐type doped MA3Bi2I9 (MA=methylammonium) perovskite‐filled membranes (PFMs). Strong coordination between dopant 2,3,5,6‐tetrafluoro‐7,7,8,8‐tetracyanoquinodimethane (F4‐TCNQ) and MA3Bi2I9 and the establishment of charge‐transfer complex (CPX) improved the conductivity by four times. The flexible X‐ray detector achieved a high sensitivity of 2065 μC Gyair−1 cm−2 and an ultra‐low detection limit of 2.71 nGyair s−1, which is among the highest values in all environmentally friendly flexible X‐ray detectors. Importantly, the PFMs retained excellent charge transport under mechanical stress. All of those make flexible MA3Bi2I9 membranes more competitive as next‐generation X‐ray detection.
Fluorinated Copolypeptide‐Stabilized Microbubbles with Maleimide‐Decorated Surfaces as Long‐Term Ultrasound Contrast Agents
Authors: Cen Jie , Ye Xianjun , Liu Xiao , Pan Wenhao , Zhang Lei , Zhang Guoying , He Nianan , Shen Aizong , Hu Jinming , Liu Shiyong 
Published: August 2022

AbstractGas‐filled microbubbles (MBs) have been clinically used as ultrasound (US) contrast agents for disease diagnosis and treatment. However, it remains a great challenge to resolve the dilemma of stability and contrast enhancement of MBs. Herein, amphiphilic copolypeptides bearing fluorinated blocks are synthesized to stabilize perfluorocarbon (PFC)‐filled MBs, exhibiting unique stability under both long‐term storage and US imaging conditions. The fluorinated inner layer reduces the internal Laplace pressure and greatly improves the stability of MBs, which can be further reinforced by crosslinking of the dipropargyl‐containing middle blocks. To overcome the suppressed nonlinear oscillation of polymer shells, maleimide groups are introduced onto the surface of MBs, enabling in situ reaction with plasma proteins to enhance second harmonic signals without compromising the stability of MBs, conferring better US imaging performance than that of SonoVueTMMBs.
A Water‐Soluble Antimony‐Rich Polyoxometalate with Broad‐Spectrum Antitumor Activities
Authors: Xiao Hui‐Ping , Hao Ya‐Shuai , Li Xin‐Xiong , Xu Peng , Huang Ming‐Dong , Zheng Shou‐Tian 
Published: August 2022

AbstractHerein, a giant Sb‐rich polyoxometalate (POM) {Sb21Tb7W56} is reported, which contains the largest number of Sb atoms in a POM so far. The Sb‐rich POM has many interesting structural features and is a rare example of a soluble and water‐stable giant POM. Biomedical studies indicate that the Sb‐rich POM exhibits broad‐spectrum antitumor activity against various cancer cell lines by reactivating the P53‐dependent apoptotic processes and disrupting the mitochondrial membrane. In addition, this Sb‐rich POM was capable of suppressing the growth and metastasis of a breast cancer in vivo. This work demonstrates that Sb‐rich POMs are promising candidates for the development of new anticancer drugs.
Site‐Selective Hydrogenation of Electron‐Poor Alkenes and Dienes Enabled by a Rhodium‐Catalyzed Hydride Addition/Protonolysis Mechanism**
Authors: Kong Duanyang , Qiqige Qiqige , McNutt Wesley , Paciello Rocco , Schäfer Ansgar , Schelwies Mathias , Lundgren Rylan J. 
Published: August 2022

AbstractThe transition metal catalyzed hydrogenation of alkenes is a well‐developed technology used on lab scale as well as on large scales in the chemical industry. Site‐ and chemoselective mono‐hydrogenations of polarized conjugated dienes remain challenging. Instead, stoichiometric main‐group hydrides are used rather than H2. As part of an effort to develop a scalable route to prepare geranylacetone, we discovered that Rh(CO)2acac/xantphos based catalysts enable the selective mono‐hydrogenation of electron‐poor 1,3‐dienes, enones, and other polyunsaturated substrates. D‐labeling and DFT studies support a mechanism where a nucleophilic RhI‐hydride selectively adds to electron‐poor alkenes and the resulting Rh‐enolate undergoes subsequent inner‐sphere protonation by alcohol solvent. The finding that (Ln)Rh(H)(CO) type catalysts can enable selective mono‐hydrogenation of electron‐poor 1,3‐dienes provides a valuable tool in the design of related chemoselective hydrogenation processes.
Management of Donor and Acceptor Building Blocks in Dopant‐Free Polymer Hole Transport Materials for High‐Performance Perovskite Solar Cells
Authors: Fu Qiang , Liu Hang , Li Shitong , Zhou Tong , Chen Mingqian , Yang Yang , Wang Jian , Wang Rui , Chen Yongsheng , Liu Yongsheng 
Published: August 2022

AbstractThe dominant hole transport material (HTM) in state‐of‐the‐art perovskite solar cells (PSCs) is Spiro‐OMeTAD, which needs to be doped using hydrophilic dopants to improve its hole mobility and conductivity, resulting in inferior device stability. Here, we propose an effective molecular design strategy to construct dopant‐free polymer HTMs by selecting four structurally related polymers and investigating their structure–property relationship. It is found that the donor and acceptor units with longitudinal conjugate extension, such as BDT‐T and BDD, could not only enhance the planarity of the conjugated polymer backbone and tune the energy levels but also promote the face‐on orientation, resulting in superior charge extraction and transport. The optimized device utilizing dopant‐free polymer HTM shows a high open‐circuit voltage of 1.19 V and a champion efficiency of 24.04 % with greatly improved operational stability, making it among the best performance PSCs based on dopant‐free HTMs.
Silica supported spinel structured cobalt ferrite multifunctional nanocatalyst for hydration of nitriles and oxidative decarboxylation of phenylacetic acids
Authors: Hazarika Shikharani , Borah Geetika 
Published: August 2022

The silica‐supported cobalt ferrite spinel nanocatalyst has been successfully synthesized by the coprecipitation method and extensively characterized by FTIR, XRD, SEM‐EDX, TEM, BET, VSM, XPS, TGA, and ICP‐AES analysis. The bands observed at 3435 cm−1(νOHof Si‐OH) and 1637 cm−1(γOHof Si‐OH) in the FTIR spectrum of the as‐synthesized nanocatalyst unambiguously tell the presence of silica support. Moreover, a very weak intensity and a medium intensity peak at 683 cm−1and 463 cm−1suggested intrinsic stretching vibrations of Fe‐O and Co‐O of cobalt ferrite, respectively. The XRD pattern confirms the formation of CoFe2O4spinel. The average crystallite size was found to be 5.4 nm as calculated by using the Debye–Scherrer equation based on the (220) plane while the average particle size was found to be 5.08 nm from TEM analysis. The crystalline nature of the nanocomposite was confirmed by the SAED pattern. The successful incorporation of CoFe2O4on the surface of silica was established by the BET surface area measurements. The silica‐supported cobalt ferrite nanocatalyst has been explored as a heterogeneous multifunctional catalyst for hydration of nitriles and oxidative decarboxylation of phenylacetic acids as well under mild reaction conditions with moderate to excellent isolated yield of the desired products (60–99%). The catalyst was magnetically recoverable within a time frame of ~90 s and reusable up to the fifth catalytic cycle without profound loss of activity. A magnetic hysteresis study was performed to elucidate the magnetic behavior of the catalyst. The saturation magnetization value of 39.785 emu/g with a coercivity value of 110.87 Oe and saturation remanence value of 5.185 emu/g clearly indicated the presence of a ferromagnetic component in the material.