bluuebunny/crossref_metadata_2025_split huggingface dataset:
The Electrostatic Attraction and Catalytic Effect Enabled by Ionic–Covalent Organic Nanosheets on MXene for Separator Modification of Lithium–Sulfur Batteries
Authors: Li Pengyue , Lv Haowei , Li Zhonglin , Meng Xueping , Lin Zhang , Wang Ruihu , Li Xiaoju 
Published: March 2021

AbstractIt is of great significance to mediate the redox kinetics and shuttle effect of polysulfides in pursuit of high‐energy‐density and long‐life lithium–sulfur (Li–S) batteries. Herein, a new strategy is proposed based on the electrostatic attraction and catalytic effect of polysulfides for the modification of the polypropylene (PP) separator. Guanidinium‐based ionic–covalent organic nanosheets (iCON) on the surface of Ti3C2 is presented as a coating layer for the PP separator. The synergetic effects of Ti3C2 and iCON provide new platforms to suppress the shuttle effect of polysulfides, expedite the redox kinetics of sulfur species, and promote efficient conversion of the intercepted polysulfides. The functional separator endows carbon nanotube/sulfur cathodes with excellent electrochemical performance. The average capacity decay per cycle within 2000 cycles at 2 C is as low as 0.006%. The separator is even effective in the case of sulfur content of 90 wt% and sulfur loading of 7.6 mg cm−2; the reversible capacity, areal capacity, and volumetric capacity at 0.1 C are as high as 1186 mA h g−1, 9.01 mA h cm−2, and 1201 mA h cm−3, respectively. This work provides a promising approach toward separator modification for the development of high‐performance Li–S batteries.
Anomalous Motion of Charged Domain Walls and Associated Negative Capacitance in Copper–Chlorine Boracite
Authors: Guy Joseph G. M. , Cochard Charlotte , Aguado‐Puente Pablo , Soergel Elisabeth , Whatmore Roger W. , Conroy Michele , Moore Kalani , Courtney Eileen , Harvey Alan , Bangert Ursel , Kumar Amit , McQuaid Raymond G. P. , Gregg J. Marty 
Published: March 2021

AbstractDuring switching, the microstructure of a ferroelectric normally adapts to align internal dipoles with external electric fields. Favorably oriented dipolar regions (domains) grow at the expense of those in unfavorable orientations and this is manifested in a predictable field‐induced motion of the walls that separate one domain from the next. Here, the discovery that specific charged 90°domain walls in copper–chlorine boracite move in the opposite direction to that expected, increasing the size of the domain in which polarization is anti‐aligned with the applied field, is reported. Polarization–field (P–E) hysteresis loops, inferred from optical imaging, show negative gradients and non‐transient negative capacitance, throughout the P–E cycle. Switching currents (generated by the relative motion between domain walls and sensing electrodes) confirm this, insofar as their signs are opposite to those expected conventionally. For any given bias, the integrated switching charge due to this anomalous wall motion is directly proportional to time, indicating that the magnitude of the negative capacitance component should be inversely related to frequency. This passes Jonscher's test for the misinterpretation of positive inductance and gives confidence that field‐induced motion of these specific charged domain walls generates a measurable negative capacitance contribution to the overall dielectric response.
MBene as a Theranostic Nanoplatform for Photocontrolled Intratumoral Retention and Drug Release
Authors: Chen Danyang , Jin Zhaokui , Zhao Bin , Wang Yingshuai , He Qianjun 
Published: March 2021

AbstractTumor‐targeted drug delivery by nanomaterials is important to improve tumor therapy efficacy and reduce toxic side effects, but its efficiency is quite limited. In this work, a new type of MBene, zirconium boride nanosheet (ZBN), as a versatile nanoplatform to realize near‐infrared (NIR)‐controlled intratumoral retention and drug release is developed. ZBN exhibits high NIR‐photothermal conversion efficiency (76.8%), surface modification with hyaluronic acid (HA) by polyol−borate esterfication endows ZBN‐HA with good dispersion, and the photopyrolysis of borate ester causes HA detachment and ZBN aggregation, enabling NIR‐controlled intratumoral retention to achieve high intratumoral accumulation. By virtue of surface borate esterfication, polyol chemotherapeutic drug (doxorubicin, DOX), and NO prodrug (β‐galactosyl‐diazeniumdiolate, Gal‐NO) can be efficiently and stably conjugated on the surface of ZBN‐HA (1.21 g DOX or 0.57 g Gal‐NO per gram ZBN) without visible drug leakage, and the photopyrolysis of borate ester enables NIR‐controlled drug release with high responsiveness and controllability. Combined chemothermal/gasothermal therapies based on ZBN‐HA/DOX and ZBN‐HA/NO nanomedicines eradicate primary tumors and interdict tumor metastasis by changing the tumor microenvironment and killing cancer cells in primary tumors. The developed NIR‐photothermal MBene is confirmed as a versatile nanoplatform capable of high‐efficacy tumor‐targeted drug delivery and controlled drug release.
An Ultrasoft Self‐Fused Supramolecular Polymer Hydrogel for Completely Preventing Postoperative Tissue Adhesion
Authors: Yu Jing , Wang Ke , Fan Chuanchuan , Zhao Xiaoye , Gao Jushan , Jing Wanghui , Zhang Xiaoping , Li Jia , Li Yuan , Yang Jianhai , Liu Wenguang 
Published: March 2021

AbstractThe intermolecular H‐bonding density heavily influences the gelation and rheological behavior of hydrogen‐bonded supramolecular polymer hydrogels, thus offering a delicate pathway to tailor their physicochemical properties for meeting a specific biomedical application. Herein, one methylene spacer between two amides in the side chain of N‐acryloyl glycinamide (NAGA) is introduced to generate a variant monomer, N‐acryloyl alaninamide (NAAA). Polymerization of NAAA in aqueous solution affords an unprecedented ultrasoft and highly swollen supramolecular polymer hydrogel due to weakened H‐bonds caused by an extra methylene spacer, which is verified by variable‐temperature Fourier transform infrared (FTIR) spectroscopy and simulation calculation. Intriguingly, poly(N‐acryloyl alaninamide) (PNAAA) hydrogel can be tuned to form a transient network with a self‐fused and excellent antifouling capability that results from the weakened dual amide H‐bonding interactions and enhanced water‐amide H‐bonding interactions. This self‐fused PNAAA hydrogel can completely inhibit postoperative abdominal adhesion and recurrent adhesion after adhesiolysis in vivo. This transient hydrogel network allows for its disintegration and excretion from the body. The molecular mechanism studies reveal the signal pathway of PNAAA hydrogel in inhibiting inflammatory response and regulating fibrinolytic system balance. This self‐fused, antifouling ultrasoft supramolecular hydrogel is promising as a barrier biomaterial for completely preventing postoperative tissue adhesion.
Tunable Electrocatalytic Behavior of Sodiated MoS2 Active Sites toward Efficient Sulfur Redox Reactions in Room‐Temperature Na–S Batteries
Authors: Wang Yanxia , Lai Yangyang , Chu Jun , Yan Zichao , Wang Yun‐Xiao , Chou Shu‐Lei , Liu Hua‐Kun , Dou Shi Xue , Ai Xinping , Yang Hanxi , Cao Yuliang 
Published: March 2021

AbstractRoom‐temperature (RT) sodium–sulfur (Na–S) batteries hold great promise for large‐scale energy storage due to the advantages of high energy density, low cost, and resource abundance. The research progress on RT Na–S batteries, however, has been greatly hindered by the sluggish kinetics of the sulfur redox reactions. Herein, an elaborate multifunctional architecture, consisting of N‐doped carbon skeletons and tunable MoS2 sulfiphilic sites, is fabricated via a simple one‐pot reaction followed by in situ sulfurization. Beyond the physical confinement and chemical binding of polarized N‐doped carbonaceous microflowers, the MoS2 active sites play a key role in catalyzing polysulfide redox reactions, especially the conversion from long‐chain Na2Sn (4 ≤ n ≤ 8) to short‐chain Na2S2 and Na2S. Significantly, the electrocatalytic activity of MoS2 can be tunable via adjusting the discharge depth. It is remarkable that the sodiated MoS2 exhibits much stronger binding energy and electrocatalytic behavior compared to MoS2 sites, effectively enhancing the formation of the final Na2S product. Consequently, the S cathode achieves superior electrochemical performance in RT Na–S batteries, delivering a high capacity of 774.2 mAh g−1 after 800 cycles at 0.2 A g−1, and an ultrahigh capacity retention with a capacity decay rate of only 0.0055% per cycle over 2800 cycles.
Chemiresistive Gas Sensors Based on Hollow Heterojunction: A Review
Authors: Liu Yanna , Xiao Song , Du Ke 
Published: March 2021

AbstractChemiresistive gas sensors are widely used in tens of thousands of applications, from health and safety to energy efficiency and emission control. Fabrication of highly effective sensing materials is of great significance for the practical applications in efficient gas detection. Among numerous sensing materials, semiconductor‐based sensing materials with hollow and heterojunction structures demonstrate distinct advantages such as high sensitivity, low operating temperature, and fast response/recovery. In this paper, the mechanism of gas sensing by chemiresistive sensors, as well as the mechanisms responsible for enhanced sensing performance in hollow structure and heterojunction are reviewed. Both single‐shelled and multi‐shelled hollow heterojunction materials applied in gas detection are presented. Then, the design and application of open hollow heterojunction in gas sensing are discussed. This review provides a deeper understanding of innovative works on the material design of high‐performance sensing materials for gas detection. It also summarizes the key technical challenges in material development and points out the perspectives for future studies on the next generating of chemiresistive gas sensing materials.
Enhanced Dye Degradation through Multi‐Particle Confinement in a Porous Silicon Substrate: A Highly Efficient, Low Band Gap Photocatalyst
Authors: Mir Sajjad Husain , Jennings Brian D. , Akinoglu Goekalp Engin , Selkirk Andrew , Gatensby Riley , Mokarian‐Tabari Parvaneh 
Published: March 2021

AbstractA platform is introduced for fabrication of a reusable and highly efficient low band gap photocatalyst by confining gold nanoparticles (AuNPs) in the pores of a nanopatterned Si monolith (AuNSM). Due to their size, a maximum of two AuNPs can assemble in a single pore, thus preventing agglomerations. Their access to the analyte provides more active sites for redox reaction, leading to enhanced efficiency. While proximity of nanoparticles enhances coupling efficiency, confinement prevents rapid recombination of photogenerated charge carriers, a major factor contributing to low efficiency of photocatalytic materials. Degradation of methyl orange (MO) is used to determine the photocatalytic efficacy of AuNSM compared to 1) bare silicon and 2) AuNPs randomly dispersed on silicon. After 90 min of exposure to UV light (λ = 353 nm) in the AuNSM, the MO absorption is <1%, indicating near complete degradation, while it is still 85% and 70% for systems (1) and (2), respectively. Finite element method simulations of the confined structure suggest that the AuNPs act as a mediator/receptacle for photogenerated charges rather than a source of them at this wavelength and thus enhance the performance of the photocatalyst by creating more effective Schottky junctions—preventing recombination of electrons and holes—rather than by a localized surface plasmonic resonance effect.
Synthetic Platelet Microgels Containing Fibrin Knob B Mimetic Motifs Enhance Clotting Responses
Authors: Nandi Seema , Mihalko Emily , Nellenbach Kimberly , Castaneda Mario , Schneible John , Harp Mary , Deal Halston , Daniele Michael , Menegatti Stefano , Barker Thomas H. , Brown Ashley C. 
Published: March 2021

AbstractNative platelets are crucial players in wound healing. Key to their role is the ability of their surface receptor GPIIb/IIIa to bind fibrin at injury sites, thereby promoting clotting. When platelet activity is impaired as a result of traumatic injury or certain diseases, uncontrolled bleeding can result. To aid clotting and tissue repair in cases of poor platelet activity, synthetic platelet‐like particles capable of promoting clotting and improving wound healing responses have been previously developed in the lab. These are constructed by functionalizing highly deformable hydrogel microparticles (microgels) with fibrin‐binding ligands including a fibrin‐specific whole antibody or a single‐domain variable fragment. To improve the translational potential of these clotting materials, the use of fibrin‐binding peptides as cost‐effective, robust, high‐specificity alternatives to antibodies are explored. Herein, the development and characterization of soft microgels decorated with the peptide AHRPYAAK that mimics fibrin knob “B” and targets fibrin hole “b” are presented. These “fibrin‐affine microgels with clotting yield” (FAMCY) are found to significantly increase clot density in vitro and decrease bleeding in a rodent trauma model in vivo. These results indicate that FAMCYs are capable of recapitulating the platelet‐mimetic properties of previous designs while utilizing a less costly, more translational design.
Functionalized Mouth‐Conformable Interfaces for pH Evaluation of the Oral Cavity
Authors: Matzeu Giusy , Naveh Gili R. S. , Agarwal Siddhart , Roshko Jeffery A. , Ostrovsky‐Snider Nicholas A. , Napier Bradley S. , Omenetto Fiorenzo G. 
Published: March 2021

AbstractOral health monitoring is highly desired, especially for in home use, however, current methods are not sensitive enough and technically convoluted for this purpose. This paper presents incorporation of bioactive materials and colorimetric chemical sensors into routinely used oral appliances transforming them into bioresponsive, conformable interfaces. Specifically, endodontic paper points and dental floss can be functionalized to locally sense and monitor pH variations within the oral cavity via color changes. Moreover, edible colorimetric indicators are developed and used to make sensing, edible devices in the form factor of candies that can dynamically and visually respond to acidity changes in saliva. These interfaces would enable early detection of caries (e.g., using dental floss and paper points) providing low‐cost point of care devices that respond in real‐time by detecting pH variations in biological fluids thus bringing monitoring to home settings .
Abuse‐Tolerant Electrolytes for Lithium‐Ion Batteries
Authors: Chen Zhiqi , Chao Yunfeng , Li Weihua , Wallace Gordon G. , Bussell Tim , Ding Jie , Wang Caiyun 
Published: March 2021

AbstractSafety issues currently limit the development of advanced lithium‐ion batteries (LIBs) and this is exacerbated when they are misused or abused. The addition of small amounts of fillers or additives into common liquid electrolytes can greatly improve resistance to abuse without impairing electrochemical performance. This review discusses the recent progress in such abuse‐tolerant electrolytes. It covers electrolytes with shear thickening properties for tolerating mechanical abuse, electrolytes with redox shuttle additives for suppressing electrochemical abuse, and electrolytes with flame‐retardant additives for resisting thermal abuse. It aims to provide insights into the functioning of such electrolytes and the understanding of electrolyte composition‐property relationship. Future perspectives, challenges, and opportunities towards practical applications are also presented.
Consumer perceptions after long‐term use of alternative irrigation water: A field experiment inIsrael
Authors: Ellis Sean F. , Kecinski Maik , Messer Kent D. , Lipchin Clive 
Published: March 2021

AbstractThis study provides the first revealed preference estimates of Israelis' willingness to pay for produce irrigated with alternative water. Results show that Israelis prefer produce irrigated with conventional water over any type of alternative water and that their preferences for alternative water varies by type. These results indicate that there may be long‐run limits to how high consumer demand for alternative water can rise. Policymakers should be cognizant of these findings and gradually expose the public to the unavoidable future of widespread alternative water use. Increased public awareness of water scarcity and alternative water technology will encourage adoption when it is possible and necessary.
The Pivotal Role of Hot Carriers in Plasmonic Catalysis of C−N Bond Forming Reaction of Amines
Authors: Swaminathan Swathi , Rao Vishal Govind , Bera Jitendra K. , Chandra Manabendra 
Published: March 2021

AbstractHere, we demonstrate the simultaneous utilization of both the hot carriers (electrons and holes) in the photocatalytic transformation of benzylamine to N‐benzylidenebenzylamine and the scope of reaction has also been successfully demonstrated with catalytic oxidation of 4‐methoxybenzylamine. The wavelength‐dependent excitation of AuNP allows us to tune the potential energy of charge carriers relative to the redox potential of the reactants which leads to energetically favorable product formation on the nanoparticle surface. We capture the formation of reaction intermediates and products by using in situ Raman spectroscopy, complemented by NMR spectroscopy and GC‐MS. Based on the experimental substantiations, a plausible reaction mechanism has been proposed.
Polymorphism and Fast Potassium‐Ion Conduction in the T5 Supertetrahedral Phosphidosilicate KSi2P3
Authors: Haffner Arthur , Hatz Anna‐Katharina , Zeman Otto E. O. , Hoch Constantin , Lotsch Bettina V. , Johrendt Dirk 
Published: March 2021

AbstractThe all‐solid‐state battery (ASSB) is a promising candidate for electrochemical energy storage. In view of the limited availability of lithium, however, alternative systems based on earth‐abundant and inexpensive elements are urgently sought. Besides well‐studied sodium compounds, potassium‐based systems offer the advantage of low cost and a large electrochemical window, but are hardly explored. Here we report the synthesis and crystal structure of K‐ion conducting T5 KSi2P3 inspired by recent discoveries of fast ion conductors in alkaline phosphidosilicates. KSi2P3 is composed of SiP4 tetrahedra forming interpenetrating networks of large T5 supertetrahedra. The compound passes through a reconstructive phase transition from the known T3 to the new tetragonal T5 polymorph at 1020 °C with enantiotropic displacive phase transitions upon cooling at about 155 °C and 80 °C. The potassium ions are located in large channels between the T5 supertetrahedral networks and show facile movement through the structure. The bulk ionic conductivity is up to 2.6×10−4 S cm−1 at 25 °C with an average activation energy of 0.20 eV. This is remarkably high for a potassium ion conductor at room temperature, and marks KSi2P3 as the first non‐oxide solid potassium ion conductor.
An International Collaborative Study on Trypsin Inhibitor Assay for Legumes, Cereals, and Related Products
Authors: Liu Keshun , Seegers Susan , Cao Wenming , Wanasundara Janitha , Chen Juxing , da Silva Alessandro Esteves , Ross Kristopher , Franco Alexandra Lozano , Vrijenhoek Theo , Bhowmik Pankaj , Li Yonghui , Wu Xin , Bloomer Scott 
Published: March 2021

AbstractFor determining trypsin inhibitor activity (TIA) in soy products, the American Oil Chemists' Society (AOCS) Method Ba 12‐75 has been used. It measures differences in absorbance at 410 nm of bovine trypsin activity toward a synthetic substrate (Nα‐benzoyl‐DL‐arginine‐p‐nitroanilide) in the absence and presence of an inhibitor. Recently, a significantly improved method was developed (JAOCS, 2019, 96:635–645), featuring 5 mL of total assay volume, enzyme‐last sequence, and single inhibitor level in duplicate. It is proposed as the AOCS Method Ba 12a‐2020. As a part of the AOCS method approval process, a collaborative study involving 12 international laboratories was conducted to evaluate the performance of the proposed method. The study involved measuring TIA in 10 selected test samples plus a blind duplicate. They included soybeans, pulses, cereals, and their processed products (flours, concentrates, and isolates). After rigorous statistical treatment of the data, only three outliers were removed from the data of two samples. Repeatability relative standard deviations (RSDr) for the 11 samples ranged from 0.99% to 5.52%. Reproducibility RSD (RSDR) ranged from 7.07% to 22.92%, with seven samples having RSDR around 10% or less. The remaining four samples had very low TIA, and their RSDR values ranged from 13.34% to 22.92%. The study has demonstrated reliable performance of the proposed AOCS method. Several collaborators carried out additional experiments addressing some aspects of the method, leading to further refinements. The proposed method is undergoing evaluation by the AOCS Uniform Methods Committee for adoption as an Official Method for measuring TIA in various legume and grain products.
Preparation of anti‐migration transition layer and its application in cast‐in‐case solid rocket motors
Authors: Zhang Bowen , Li Xiaoyu , Zhang Weihai , Ren Rui , Zhang Zhaobo , Luo Yunjun 
Published: March 2021

AbstractThe polyester‐based transition layers were first synthesized with poly (diethylene glycol adipate), glycerin, and toluene diisocyanate. Then they were coated between the propellant and the liner to improve the bonding performance of the charge and inhibit the migration of the energetic plasticizer in the propellant. The effects of R value (the ratio of the quantity of isocyanate functions NCO with respect to the quantity of hydroxyl functions OH) on migration resistance and bonding performance were also studied. The overall performance was optimized at R = 1.5: after the transition layer was applied, the binding strength was greatly increased from 0.14 to 0.64 MPa, which had good application prospects. Meanwhile, due to the strong interactions between the polar ester groups and N‐butyl‐N‐nitratoethyl nitramine (NENA) in the transition layers, the portion of NENA migrating into liners were reduced from 7.6% to 6.0% (reduced by 21%), indicating that the introduction of polyester transition layers could significantly improve the anti‐migration effect. The activation energies of migration for NENA in the transition layers were about 66.3 ~ 94.3 kJ/mol, which were equivalent to the value of strong hydrogen bonding.
Ionic liquids enhanced performance of PVC gels actuator
Authors: Ali Imdad , Latif Abdul , Hussain Khalid , Shehzad Farooq Khurum , Ali Ahmed , Faisal Rehman , Xudong Li , Dias Otavio Augusto Titton , Weimin Yang , Haoyi Li 
Published: March 2021

AbstractStimulated devices are highly demanded for actuators and artificial muscles in the recent era but susceptible to low deformation at an applied voltage. In the present work, ionic liquids (ILs) based gel films were prepared from the polyvinyl chloride (PVC), dibutyl adipate (DBA), 1‐butyl, 3‐methimidazolium chloride, and 1‐pentyl‐3‐methylimidazolium hexafluorophosphate by a simple solvent evaporation method. The structural, morphological, optical, and mechanical properties of the composite PVC/ILs gel were characterized by Fourier‐transform infrared spectroscopy (FTIR), Large Angle X‐ray scattering (LAXS), UV–visible (UV–vis) absorption spectroscopy, scanning electron micrpscopy (SEM) and elemental mapping. We found that the displacement of plasticized PVC gels‐based actuator was 0.1 mm with the response time of 0.33 s at an induced voltage of 1000 V. The loading of 0.02% of IL (fluorides) with PVC gel showed maximum deformation of 0.16 mm with a relatively rapid response time of 0.2 s. These high deformation and response time values of IL fluoride‐based gels are dramatically higher than reported PVC gels. Likewise, the loading of IL fluorides in the PVC gel showed a high elongation value at the break of about 377%. This work suggests that the flexible gel based on IL fluorides and PVC could be a potential candidate for the fabrication of high‐performance artificial muscles and tunable soft actuators.