bluuebunny/crossref_metadata_2025_split huggingface dataset:
Exploiting Confinement to Study the Crystallization Pathway of Calcium Sulfate
Authors: Anduix‐Canto Clara , Levenstein Mark A. , Kim Yi‐Yeoun , Godinho Jose R. A. , Kulak Alexander N. , Niño Carlos González , Withers Philip J. , Wright Jonathan P. , Kapur Nikil , Christenson Hugo K. , Meldrum Fiona C. 
Published: September 2021

AbstractCharacterizing the pathways by which crystals form remains a significant challenge, particularly when multiple pathways operate simultaneously. Here, an imaging‐based strategy is introduced that exploits confinement effects to track the evolution of a population of crystals in 3D and to characterize crystallization pathways. Focusing on calcium sulfate formation in aqueous solution at room temperature, precipitation is carried out within nanoporous media, which ensures that the crystals are fixed in position and develop slowly. The evolution of their size, shape, and polymorph can then be tracked in situ using synchrotron X‐ray computed tomography and diffraction computed tomography without isolating and potentially altering the crystals. The study shows that bassanite (CaSO4 0.5H2O) forms via an amorphous precursor phase and that it exhibits long‐term stability in these nanoscale pores. Further, the thermodynamically stable phase gypsum (CaSO4 2H2O) can precipitate by different pathways according to the local physical environment. Insight into crystallization in nanoconfinement is also gained, and the crystals are seen to grow throughout the nanoporous network without causing structural damage. This work therefore offers a novel strategy for studying crystallization pathways and demonstrates the significant impact of confinement on calcium sulfate precipitation, which is relevant to its formation in many real‐world environments.
Additives for Ambient 3D Printing with Visible Light
Authors: Ahn Dowon , Stevens Lynn M. , Zhou Kevin , Page Zachariah A. 
Published: September 2021

AbstractWith 3D printing, the desire is to be “limited only by imagination,” and although remarkable advancements have been made in recent years, the scope of printable materials remains narrow compared to other forms of manufacturing. Light‐driven polymerization methods for 3D printing are particularly attractive due to unparalleled speed and resolution, yet the reliance on high‐energy UV/violet light in contemporary processes limits the number of compatible materials due to pervasive absorption, scattering, and degradation at these short wavelengths. Such issues can be addressed with visible‐light photopolymerizations. However, these lower‐energy methods often suffer from slow reaction times and sensitivity to oxygen, precluding their utility in 3D printing processes that require rapid hardening (curing) to maximize build speed and resolution. Herein, multifunctional thiols are identified as simple additives to enable rapid high‐resolution visible‐light 3D printing under ambient (atmospheric O2) conditions that rival modern UV/violet‐based technology. The present process is universal, providing access to commercially relevant acrylic resins with a range of disparate mechanical responses from strong and stiff to soft and extensible. Pushing forward, the insight presented within this study will inform the development of next‐generation 3D‐printing materials, such as multicomponent hydrogels and composites.
Laser‐Irradiated Holey Graphene‐Supported Single‐Atom Catalyst towards Hydrogen Evolution and Oxygen Reduction
Authors: Khan Kishwar , Liu Tangchao , Arif Muhammad , Yan Xingxu , Hossain Md Delowar , Rehman Faisal , Zhou Sheng , Yang Jing , Sun Chengjun , Bae Sang‐Hoon , Kim Jeehwan , Amine Khalil , Pan Xiaoqing , Luo Zhengtang 
Published: September 2021

AbstractSingle‐atom catalysts (SAC) can boost the intrinsic catalytic activity of hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). However, the challenge remains due to the complex synthesis process and insufficient stability. A sustainable approach is applied to synthesizing SACs through laser irradiation and gaining mesoporous graphene oxide (MGO). The surface dangling bonds of nitrogen‐doped MGO (NMGO) extract metal atoms species from Co or Fe metal foams and convert them to SAC via an appropriate synthesis approach. Notably, the Co‐NMGO electrocatalyst requires low potentials of 146 mV to convey a current density of 10 mA cm−2 towards HER. Similarly, the Fe‐NMGO electrocatalyst offers an onset of 0.79 V towards ORR in acidic solution. The individual metal atoms are confirmed via aberration‐corrected scanning transmission electron microscopy, and X‐ray absorption near‐edge structure and extended X‐ray absorption fine structure. Density functional theory calculations by applying the grand canonical potential kinetics model revealed that Co‐NMGO shows the optimum free reaction energy of −0.17 eV at −0.1 V for HER, and Fe‐NMGO has less limiting potential than that of Co‐NMGO for ORR case. This work opens a new approach towards the synthesis of SAC and its mechanistic understandings.
Precise Proton Redistribution for Two‐Electron Redox in Aqueous Zinc/Manganese Dioxide Batteries
Authors: Shen Zhaoxi , Tang Ziqing , Li Chaowei , Luo Lei , Pu Jun , Wen Zhaorui , Liu Yu , Ji Yu , Xie Junpeng , Wang Litong , Yao Yagang , Hong Guo 
Published: September 2021

AbstractThe liquid electrolyte in conventional zinc/manganese dioxide (Zn/MnO2) batteries conduces to the capacity limitation of one‐electron redox from MnO2 to MnOOH, as well as undesired Mn loss with capacity deterioration. Herein, to conquer these challenges, a new idea is proposed on the precise proton redistribution in the hydrogel electrolyte for the preferred two‐electron redox reaction. Specifically, an acidic layer in the hydrogel adjoins the MnO2 cathode to maintain the two‐electron redox, a neutral layer adjoins the zinc anode to inhibit the dendrite growth, which is separated by a mildly alkaline layer to immobilize the proton distribution. The two‐electron redox of MnO2/Mn2+ and anode protection are demonstrated to play key roles in battery performance. Such a battery presents specific capacities of 516 mA h g−1 at 0.05 A g−1, as well as a capacity retention of 93.18% at 5 A g−1 after 5000 cycles without extra Mn2+ addition in the electrolyte. More importantly, fibrous Zn/MnO2 batteries using the tri‐layer electrolyte can sustain 2000 cycles with high initial capacity of 235 mAh g−1 at 1 A g−1. After 6000 times folding in 180°, it can maintain 99.54% capacity. When integrated into user's clothing or portable accessories, the fibrous battery is demonstrated as a great potential in wearable electronics.
Ultrathin NiCo Bimetallic Molybdate Nanosheets Coated CuOx Nanotubes: Heterostructure and Bimetallic Synergistic Optimization of the Active Site for Highly Efficient Overall Water Splitting
Authors: Gu Mingzheng , Deng Xueya , Lin Man , Wang Hao , Gao An , Huang Xiaoming , Zhang Xiaojun 
Published: September 2021

AbstractRational design and construction of bifunctional electrocatalysts with excellent activity and durability is imperative for water splitting. The regulation of the local electronic structure of the active metal sites in polymetallic composites provides a basic idea. Herein, the ultrathin bimetallic molybdate nanosheets are evenly deposited on the CuOx hollow nanotubes on the copper foam substrate to form a hierarchical heterostructure, which can be used as an efficient bifunctional electrocatalyst for overall water splitting. Experimental results prove that the introduction of Ni to form a double metal salt molybdate and CuOx heterostructure design can be optimized by Co cation as best electronic structure of electric catalytic activity center, and can effectively promote the generation of CoOOH active phase at the same time, so that can skillfully optimize the binding strength between the Co site and the oxygen‐containing intermediate, and enhancing catalytic activity. When it is used in the overall water splitting of a double‐electrode alkaline electrolytic cell, the cell voltage of CoNiMoO4‐21/CuOx/CF is 1.532 V at 50 mA cm−2, far exceeding most of the reported conventional bifunctional electrocatalyst. This work has contributed to understanding the central active sites of polymetallic composites and has provided a useful value for the design of efficient electrocatalysts.
Patients withEhlers–Danlossyndrome on the diagnostic odyssey: Rethinking complexity and difficulty as a hero's journey
Authors: Halverson Colin Michael Egenberger , Clayton Ellen Wright , Garcia Sierra Abigail , Francomano Clair 
Published: September 2021

AbstractPatients with hypermobile Ehlers–Danlos syndrome, an hereditary disorder of the connective tissue, often face a long and difficult diagnostic odyssey in pursuit of a name for their condition. Clinicians may dismiss subjective symptoms of chronic pain, thus prolonging patients' odysseys and worsening their care and satisfaction and creating antagonisms in the patient–provider relationship. A greater understanding of patient experiences is necessary in order to decrease burdens of this relationship and to improve care. To that end, we conducted 22 in‐depth, semistructured interviews with individuals who had undergone this diagnostic odyssey. We focused on the impact that the odyssey had on their lives, both inside and outside the clinic. Through narrative analysis, we found a sort of “hero's journey” in the description of their cases, highlighting issues of uncertainty and integration as well as honoring their struggles. Interviewees had encountered difficulties in working with clinicians, in multiplying symptoms, and in negative psychosocial consequences. Attention to patients' lived experience may help to build empathy and understanding for the difficult and complex clinical situation presented by Ehlers–Danlos syndrome. Using the hero's journey as a lens onto this experience allows for a more patient‐centered approach to this understanding and has potential value for comprehension of other complex diseases and invisible illnesses.
Anionen‐Anionen‐Chemie mit massenselektierten Fragmentionen auf Oberflächen
Authors: Yang Fangshun , Behrend K. Antonio , Knorke Harald , Rohdenburg Markus , Charvat Ales , Jenne Carsten , Abel Bernd , Warneke Jonas 
Published: September 2021

AbstractWährend Reaktionen zwischen Ionen und neutralen Molekülen in der Gasphase umfangreich untersucht wurden, sind Reaktionen zwischen molekularen Ionen gleicher Polarität weitestgehend unerforscht. Wir zeigen, dass Reaktionen zwischen in der Gasphase erzeugten Fragmentionen und molekularen Ionen derselben Polarität durch Abscheiden beider Reagenzien auf einer Oberfläche mittels Ion Soft‐Landing möglich sind. Reaktive [B12I11]1−‐Anionen wurden auf einer Oberfläche gelandet, auf welcher zuvor, normalerweise unreaktive, [B12I12]2−‐Anionen deponiert wurden. Die Ex‐situ‐Analyse des gebildeten Materials zeigt, dass [B24I23]3−‐Ionen gebildet wurden. DFT‐Rechnungen zeigen, dass das Produkt in der Gasphase metastabil ist. Die ladungsbalancierte Umgebung einer geerdeten Oberfläche kann jedoch das dreifach geladene Produkt stabilisieren, wie Modellrechnungen bestätigen. Dies eröffnet neue Möglichkeiten für die Erzeugung von hochgeladenen Clustern unter Verwendung unkonventioneller Molekülbausteine aus der Gasphase.
A Coral‐Like FeP@NC Anode with Increasing Cycle Capacity for Sodium‐Ion and Lithium‐Ion Batteries Induced by Particle Refinement
Authors: Wang Canpei , Yan Jitong , Li Tianyu , Lv Zhiqiang , Hou Xin , Tang Yongfu , Zhang Huamin , Zheng Qiong , Li Xianfeng 
Published: September 2021

AbstractWe present a coral‐like FeP composite with FeP nanoparticles anchored and dispersed on a nitrogen‐doped 3D carbon framework (FeP@NC). Due to the highly continuous N‐doped carbon framework and a spring‐buffering graphitized carbon layer around the FeP nanoparticle, a sodium‐ion battery with the FeP@NC composite exhibits an ultra‐stable cycling performance at 10 A g−1 with a capacity retention of 82.0 % in 10 000 cycles. Also, particle refinement leads to a capacity increase during cycling. The FeP nanoparticles go through a refining–recombination process during the first cycle and present a global refining trend after dozens of cycles, which results in a gradually increase in graphitization degree and interface magnetization, and further provides more active sites for Na+ storage and contributes to a rising capacity with cycling. The capacity ascending phenomenon can also extend to lithium‐ion batteries.
Insight on the Order of Regioselective Ultrafast Formation of Disulfide Bonds in (Antimicrobial) Peptides and Miniproteins
Authors: Laps Shay , Atamleh Fatima , Kamnesky Guy , Uzi Shaked , Meijler Michael M. , Brik Ashraf 
Published: September 2021

AbstractDisulfide‐rich peptides and proteins are among the most fascinating bioactive molecules. The difficulties associated with the preparation of these targets have prompted the development of various chemical strategies. Nevertheless, the production of these targets remains very challenging or elusive. Recently, we introduced a strategy for one‐pot disulfide bond formation, tackling most of the previous limitations. However, the effect of the order of oxidation remained an underexplored issue. Herein we report on the complete synthetic flexibility of the approach with respect to the order of oxidation of three disulfide bonds in targets that lack the knot motif. In contrast, our study reveals an essential order of disulfide bond formation in the EETI‐II knotted miniprotein. This synthetic strategy was applied for the synthesis of novel analogues of the plectasin antimicrobial peptide with enhanced activities against methicillin‐resistant Staphylococcus aureus (MRSA), a notorious human pathogen.
Preparation of pH‐responsive cellulose nanofibril/sodium alginate based hydrogels for drug release
Authors: Li Yuhang , Wang Cong , Luan Yunhao , Liu Wanyi , Chen Tiantian , Liu Pengtao , Liu Zhong 
Published: September 2021

AbstractIn this work, hydrogels composed of cellulose nanofibril (CNF) and sodium alginate (SA) were prepared as a pH‐responsive release system by controlling the amount of CNF and SA. Scanning electron microscopy, thermogravimetric analysis, and swelling rate methods were used to characterize. The results showed that when the mass ratio of CNF to SA was 2:1, CNF/SA hydrogels with better morphology were obtained. Due to the deprotonation or protonation of calcium alginate, as the pH changing from 1.5 to 11.0, the swelling ratio increased from 7 times to 19 times compared with its dry weight. The drug release behaviors of the CNF/SA hydrogels using ibuprofen (IBU) as a model drug were investigated in vitro. The release of IBU was faster in alkaline conditions and slower in acidic conditions. The drug release mechanism under pH stimulation could be interpreted by the Fickian diffusion and erosion effect based on Korsmeyer‐Peppas model.
Electro‐responsive semi‐IPN hydrogel with enhanced responsive property for forward osmosis desalination
Authors: Xu Zirong , Wu Kelin , Luo Huayong , Wang Qin , Zhang Tian C. , Chen Xiaobing , Rong Hongwei , Fang Qian 
Published: September 2021

AbstractAn electro‐responsive hydrogel with semi‐interpenetrating polymer networks (semi‐IPN) composed of crosslinked poly(2‐acrylamido‐2‐methyl‐l‐propanesulfonic acid‐co‐acrylamide) (P(AMPS‐AM)) and linear polyelectrolyte polyacrylic acid (PAA) was explored. The semi‐IPN hydrogel was characterized with different methods and then used as advanced draw agent toward high water recovery for forward osmosis (FO) desalination. The swelling kinetics of the semi‐IPN hydrogel was investigated, and the electro‐responsive nature of the hydrogel under electric stimulus (in direct contact with electrodes) was determined. Results indicated that in comparison with pure P(AMPS‐AM) hydrogel, the semi‐IPN hydrogel exhibited a loose network structure with more pores. In addition, a higher equilibrium swelling capacity and more pronounced deswelling under electric stimulus can be observed for the semi‐IPN hydrogel. Furthermore, the semi‐IPN hydrogel displayed a similar initial water flux of 2.20 L m−2 h−1 (LMH) from 2 g/L NaCl solution of a lab‐scale FO process. Importantly, the semi‐IPN hydrogel had a 25% increase in water recovery efficiency under the electric stimulus of 15 V, and showed better recyclability during three cycles of regeneration compared with pure P(AMPS‐AM). The mechanism of enhanced dewatering nature for the semi‐IPN hydrogel under electric stimulus was elucidated. These results indicate this new hydrogel's potential as a promising candidate for improving FO performance.
Cu2O‐Catalyzed Conversion of Benzyl Alcohols Into Aromatic Nitriles via the Complete Cleavage of the C≡N Triple Bond in the Cyanide Anion
Authors: Liu Wenbo , Tang Peichen , Zheng Yi , Ren Yun‐Lai , Tian Xinzhe , An Wankai , Zheng Xianfu , Guo Yinggang , Shen Zhenpeng 
Published: September 2021

AbstractNitrogen transfer from cyanide anion to an aldehyde is emerging as a promising method for the synthesis of aromatic nitriles. However, this method still suffers from a disadvantage that a use of stoichiometric Cu(II) or Cu(I) salts is required to enable the reaction. As we report herein, we overcame this drawback and developed a catalytic method for nitrogen transfer from cyanide anion to an alcohol via the complete cleavage of the C≡N triple bond using phen/Cu2O as the catalyst. The present condition allowed a series of benzyl alcohols to be smoothly converted into aromatic nitriles in moderate to high yields. In addition, the present method could be extended to the conversion of cinnamic alcohol to 3‐phenylacrylonitrile.
Development and evaluation of standardized pregnancy identification and trimester distribution algorithms in U.S. IBM MarketScan® Commercial and Medicaid data
Authors: Sumner Kelsey M. , Ehlinger Anna , Georgiou Mary E. , Wurst Keele E. 
Published: September 2021

AbstractObjectivesCreation of new algorithms to identify pregnancies in automated health care claims databases is of public health importance, as it allows us to learn more about medication use and safety in a vulnerable population. Previous algorithms were largely created using international classification of disease codes, but despite the U.S. code transition in 2015, few algorithms are available with the latest ICD‐10‐CM codes.MethodsUsing U.S. IBM MarketScan® Commercial Claims and Encounters and Multi‐State Medicaid databases for women aged 10–64 years during 2014 and 2016, two pregnancy algorithms (ICD‐9‐CM and ICD‐10‐CM) were created using expert clinical review. The algorithms were evaluated by assessing the distribution of pregnancy outcomes (live birth and pregnancy losses) within each time‐based cohort and the ability of the algorithms to identify select medication use during pregnancy. Medication exposure, demographics, comorbidities, and pregnancy outcomes were compared to published literature estimates for the two time periods.ResultsFor the IBM MarketScan® Commercial database, the algorithms identified 687,228 pregnancies in 2014 and 444,293 in 2016. In the IBM MarketScan® Medicaid database, 389,132 pregnancies in 2014 and 406,418 in 2016 were identified. Percentages of most pregnancy outcomes identified using the algorithms were similar to national data sources; however, percentages of preterm births and pregnancy losses were not comparable. Most medication use estimates from the algorithms were similar to or higher than published estimates.ConclusionsBy incorporating the latest ICD‐10‐CM codes, the new algorithms provide more complete estimates of medication use during pregnancy than algorithms using the outdated codes.
Cu2O‐CuO/Chitosan Composites as Heterogeneous Catalysts for Benzylic C−H Oxidation at Room Temperature
Authors: Kanarat Jurin , Bunchuay Thanthapatra , Klysubun Wantana , Tantirungrotechai Jonggol 
Published: September 2021

AbstractRecently, in catalysis, chitosan has been exploited as a macrochelating ligand for metal active species due to the presence of various functional groups in its structure. Moreover, copper‐based catalysts are classified as one of the most environmentally friendly catalytic systems and their use for the oxidation of alkylarene has not been established much. Therefore, in this work, the hydrothermal synthesis of copper oxide‐chitosan composites as heterogeneous catalysts for the benzylic C−H oxidation of alkylarene was investigated. Characterization results reveal mixed phases of CuO and Cu2O, inferring the ability of chitosan to act as a reducing sugar under the hydrothermal condition. The pre‐existing interaction between copper species and chitosan as well as the co‐existence of the Cu2O and CuO structures give rise to the efficient performance of the catalysts. The synthesized composites exhibit high activity for the oxidation of fluorene to 9‐fluorenone at room temperature and small catalyst loading (1 mol % of Cu, >90 % conversion and 100 % selectivity). Superior TOF was observed, and a good scope of substrates can be converted to corresponding ketones in 48–97 % yields with these copper oxide‐chitosan catalysts. In addition, the catalysts can be used for up to nine cycles without significant decrease of the activity.
Hierarchical Bimetallic Electrocatalyst with Amorphous SnO Layer for Highly Efficient Electroreduction of CO2
Authors: Huo Cuizhu , Cao Xinxing , Ye Zixian , Li Yu , Lu Tongbu 
Published: September 2021

AbstractRenewable electricity‐driven reduction of CO2 into value‐added chemicals has been recognized as a promising sustainable energy conversion method to achieve carbon‐neutrality. Although Sn‐based catalysts show excellent selectivity towards CO and HCOOH in CO2 reduction, the reaction activity, i. e. current density, remains quite low (<100 mA cm−2). Herein, a hierarchical bimetallic electrocatalyst consisting of Cu foam‐supported bundle‐like structure and thin amorphous SnO layer was fabricated for efficient electroreduction of CO2 to C1 products (CO and HCOOH). The hierarchical structure ensured higher large electrochemically active surface area, while the thin amorphous SnO layer could efficiently adsorb CO2, and stabilize the *CO2− intermediate formed in the rate‐determining step, thereby boosting the reaction activity of CO2 reduction. As a result, an unprecedented partial current density of 128.6 mA cm−2 was achieved for C1 products at −1.4 V vs. RHE with a Faradaic efficiency of 79.2 % in an H‐type cell. The strategy of integrating optimized structure with active site here may be beneficial to other related energy conversion systems.
Functional additives for solid polymer electrolytes in flexible and high‐energy‐density solid‐state lithium‐ion batteries
Authors: Chen Hao , Zheng Mengting , Qian Shangshu , Ling Han Yeu , Wu Zhenzhen , Liu Xianhu , Yan Cheng , Zhang Shanqing 
Published: September 2021

AbstractSolid polymer electrolytes (SPEs) have become increasingly attractive in solid‐state lithium‐ion batteries (SSLIBs) in recent years because of their inherent properties of flexibility, processability, and interfacial compatibility. However, the commercialization of SPEs remains challenging for flexible and high‐energy‐density LIBs. The incorporation of functional additives into SPEs could significantly improve the electrochemical and mechanical properties of SPEs and has created some historical milestones in boosting the development of SPEs. In this study, we review the roles of additives in SPEs, highlighting the working mechanisms and functionalities of the additives. The additives could afford significant advantages in boosting ionic conductivity, increasing ion transference number, improving high‐voltage stability, enhancing mechanical strength, inhibiting lithium dendrite, and reducing flammability. Moreover, the application of functional additives in high‐voltage cathodes, lithium–sulfur batteries, and flexible lithium‐ion batteries is summarized. Finally, future research perspectives are proposed to overcome the unresolved technical hurdles and critical issues in additives of SPEs, such as facile fabrication process, interfacial compatibility, investigation of the working mechanism, and special functionalities.