bluuebunny/crossref_metadata_2025 huggingface dataset:
Study of a Torque Limiter Based on NiTi Pseudoelastic Tapes
Authors: Nespoli Adelaide , Bassani Enrico , Villa Elena , Passaretti Francesca
Published: September 2021

Herein, a new torsional device based on shape memory alloy elements and operating as torque limiter is presented. It consists of a set of pseudoelastic NiTi tapes working in series configuration. The tapes are assembled radially with respect to the rotational direction and work sequentially in beam‐like bending mode. The trend of the resulting torque may span from pulsating to continuous by changing the number of tapes. Furthermore, the use of NiTi material enables a temperature‐dependent response. Due to the particular mounting, the flag‐shaped pseudoelastic mechanical behavior typical of NiTi is partially hidden; however, the use of pseudoelastic elements provides a stable cyclic response and enables the possibility to tune the output torque.
3D Ordered Porous Hybrid of ZnSe/N‐doped Carbon with Anomalously High Na+ Mobility and Ultrathin Solid Electrolyte Interphase for Sodium‐Ion Batteries
Authors: Li Xueying , Han Zhiyuan , Yang Wenhua , Li Qiang , Li Hongsen , Xu Jie , Li Hongliang , Liu Bing , Zhao Haiguang , Li Shandong , Wang Xia , Wu Xing‐Long
Published: September 2021

Transition metal selenides have been widely used in alkali metal ion batteries owing to their high specific capacities and low cost. However, their reaction kinetics and structural stability are usually poor during cycling, along with ambiguous differences in Li/Na/K‐storage behaviors. Herein, it is revealed that ZnSe possesses better Na+‐diffusion kinetics (including lower diffusion barrier, smaller activation energy, and higher diffusion coefficients) in comparison with Li+ and K+, as evidenced by theoretical calculations and electrochemical studies. The architectural designs of ZnSe‐based anode, including nitrogen‐doped carbon (N,C) and 3D ordered hierarchical pores (3DOHP) to form a 3DOHP ZnSe@N,C hybrid combined with regulating solid electrolyte interphase (SEI), significantly enhance Na+ reaction kinetics and accommodate volume changes. The resulting 3DOHP ZnSe@N,C electrodes exhibit outstanding rate capability and good cycling stability (241.6 mAh g−1 in sodium‐ion batteries (SIBs) at 10 A g−1 after 800 cycles), originating from improved electrical conductivity and shortened ion diffusion paths, accompanied by ultrathin and stable SEI with less Na2CO3/NaF in organic components and boosted Na2Se adsorption as sodiation. Moreover, the Na‐storage mechanism in 3DOHP ZnSe@N,C hybrid is further revealed by in situ studies. Accordingly, this study provides a new perspective for designing high‐performance electrode materials for SIBs.
A Dynamically Hybrid Crosslinked Elastomer for Room‐Temperature Recyclable Flexible Electronic Devices
Authors: Guo Yifan , Yang Lei , Zhang Luzhi , Chen Shuo , Sun Lijie , Gu Shijia , You Zhengwei
Published: September 2021

The rapid development of flexible electronics has resulted in serious pollution in the form of electronic waste. Accordingly, recyclability is highly desirable for these devices, but this remains a significant challenge. A dynamically hybrid crosslinked polyurethane (FPU) elastomer is designed in this study to address this challenge. Distinctive Diels–Alder adducts with suitable dissociation and reassociation dynamics are designed as crosslinking units to provide an efficient time frame for recycling. FPU is maintained in a state with a low crosslinking density after heating at 120 °C for 5 min. FPU‐based electronics can therefore be dissolved in chloroform under ambient conditions to separate the electronic components and polymers for the refabrication of new electronic devices. This is the first reported thermoset elastomer that can be completely recycled at room temperature without chemical treatment to decompose the polymer chain. The design concept is applied by demonstrating the fabrication by recycling of different FPU‐based flexible electronic devices: position sensor, flexible keyboard, and motion sensor. Furthermore, the FPU has many advantages as a material for flexible electronics in terms of its biomimetic mechanical properties, room‐temperature self‐healing, and facile processability. This study provides promising new design principles to develop materials for promoting sustainable flexible electronics.
Simultaneous Manipulation of Interfacial and Defects Polarization toward Zn/Co Phase and Ion Hybrids for Electromagnetic Wave Absorption
Authors: Gao Zhenguo , Lan Di , Zhang Limin , Wu Hongjing
Published: September 2021

Rational manipulation of multimetal hybrid materials (HMs) with tunable substitution or phases is evolving as an effective strategy to meet the controllable electromagnetic (EM) properties and EM wave (EMW) absorption. Herein, a new thermodynamic and kinetic cocontrol strategy is proposed to construct Zn/Co bimetal HMs with tuning ion and phase hybridization for synergistic effect on EM properties for the first time. Auxiliary chelating agent triethanolamine (TEA) dominates the phase separation by stepwise Zn/Co deposition in metal–organic frameworks, then the pyrolysis process under gradient temperature give rise to controllable ion hybridization products due to thermal motion. Benefiting from the tunable collaboration between defects polarization and interfacial polarization, the 700 °C HMs exhibit ultrahigh EM parameters and EMW absorption, of which products with no TEA deliver the effective absorbing bandwidth of 4.80 GHz (1.6 mm) and minimum reflection loss of −45.85 dB. The results indicated that synergistic effect of ion and phase hybridization can improve the defects induced “polarization centers” and coherent interfaces induced interfacial polarization. Furthermore, the comprehensive research and deep understanding on respective contribution of hybridization forms provide a precise inspiration in developing bimetal and even multimetal ferrite with tunable hybridization structure.
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

Characterizing 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

With 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

Single‐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

The 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

Rational 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.
Centrosymmetric‐ and Axisymmetric‐Patterned Flexible Tactile Sensor for Roughness and Slip Intelligent Recognition
Authors: Liu Yafeng , Cui Shaowei , Wei Junhang , Li Haibo , Hu Jingyi , Chen Siyu , Chen Yin , Ma Yinji , Wang Shuo , Feng Xue
Published: September 2021

Next‐generation robots are being designed to function autonomously in complex and unstructured environments. In particular, based on the real‐time measurement and differentiation of normal pressure and shear force, robots can be equipped with the capabilities of damage‐free grasp within minimum force limits, as well as dexterous operation through surface roughness and slip information. Herein, a flexible tactile sensor with a small cylinder protrusion and four arc‐shaped protrusions is developed. Due to its center symmetry and axisymmetry characteristics, the normal pressure and shear force can be decoupled from the complex stress without any interference from torsion. The flexible tactile sensor exhibits good linearity and superior cycling stability and is capable of determining the magnitude and direction of the applied force accurately. The flexible tactile sensor is comfortable to wear, and it is integrated onto the manipulator to realize various delicate and dexterous tasks, such as pressure detection, interaction with fragile objects, and roughness identification. Moreover, intelligent recognition of the sliding and stationary states can be achieved by decoding signals of sliding friction and static friction from the feedback information, leading to real time and precise adjustment of the grasping state of the manipulator.
Small‐Scale Soft Robot with High Speed and Load Capacity Inspired by Kangaroo Hopping
Authors: Wang Qi , Lu Xiaolong , Yuan Ningyi , Ding Jianning
Published: September 2021

Small insect‐scale robots have demonstrated considerable promise in fields such as equipment fault diagnosis, environmental monitoring, scientific investigation, and disaster relief. However, realizing beneficial traits such as high‐speed motion, high load capacity, an internal driving source, and environmental suitability in one small robot is still challenging. Inspired by kangaroo hopping, a small robot is designed with a two‐mass soft structure and driven by electromagnetic force. With the synergistic effect of the hopping motion, the soft robot displays two unique properties: 1) the loaded speed is larger than the unloaded one (0–10 times its body weight) and 2) by changing the driving frequency, the moving direction of the robot, i.e., forward or backward, can be controlled. In addition, the robot displays multiple leading properties, including a high‐motion speed (≈21.5 body lengths s−1) and large load capacity (≈32.5 times its body weight), compared to other robots on the same scale. Furthermore, the robot displays exceptional adaptive capabilities under different circumstances: it traverses slopes, rough and soft surfaces, and even maneuvers underwater. The design strategy and dynamic model adopted in this research provide a reference for future designs and lay a solid foundation for the practical application of high‐performing small robots.
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

Patients 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

Während 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

We 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

Disulfide‐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

In 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

An 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.
Myocardial Dysfunction and Heart Failure in Rheumatoid Arthritis
Authors: Park Elizabeth , Griffin Jan , Bathon Joan M.
Published: September 2021

Rheumatoid arthritis (RA) patients have almost twice the risk of heart failure (HF) as individuals without RA, even with adjustment for the presence of ischemic heart disease. Moreover, RA patients remain at a 2‐fold higher risk of mortality from HF compared to non–RA patients. These observations suggest that RA‐specific inflammatory pathways are significant contributors to this increased risk of HF. Herein we summarize the epidemiology of HF in RA patients, the differences in myocardial structure or function between RA patients and non–RA patients without clinical signs of HF, and data on the role of systemic and local inflammation in RA HF pathophysiology. We also discuss the impact of subduing inflammation through the use of RA disease‐modifying therapies on HF and myocardial structure and function, emphasizing gaps in the literature and areas needing further research.
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

Nitrogen 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

Objectives

Creation 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.

Methods

Using 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.

Results

For 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.

Conclusions

By 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

Recently, 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

Renewable 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

Solid 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.
Carbon materials for stable Li metal anodes: Challenges, solutions, and outlook
Authors: Lu Qiongqiong , Jie Yulin , Meng Xiangqi , Omar Ahmad , Mikhailova Daria , Cao Ruiguo , Jiao Shuhong , Lu Yan , Xu Yaolin
Published: September 2021

Lithium (Li) metal is regarded as the ultimate anode for next‐generation Li‐ion batteries due to its highest specific capacity and lowest electrochemical potential. However, the Li metal anode has limitations, including virtually infinite volume change, nonuniform Li deposition, and an unstable electrode–electrolyte interface, which lead to rapid capacity degradation and poor cycling stability, significantly hindering its practical application. To address these issues, intensive efforts have been devoted toward accommodating and guiding Li deposition as well as stabilizing the interface using various carbon materials, which have demonstrated excellent effectiveness, benefiting from their vast variety and excellent tunability of the structure–property relationship. This review is intended as a guide through the fundamental challenges of Li metal anodes to the corresponding solutions utilizing carbon materials. The specific functionalities and mechanisms of carbon materials for stabilizing Li metal anodes in these solutions are discussed in detail. Apart from the stabilization of the Li metal anode in liquid electrolytes, attention has also been paid to the review of anode‐free Li metal batteries and solid‐state batteries enabled by strategies based on carbon materials. Furthermore, we have reviewed the unresolved challenges and presented our outlook on the implementation of carbon materials for stabilizing Li metal anodes in practical applications.
Predictive Catalysis in Olefin Metathesis with Ru‐based Catalysts with Annulated C60 Fullerenes in the N‐heterocyclic Carbenes
Authors: Pablo Martínez Juan , Solà Miquel , Poater Albert
Published: September 2021

Predictive catalysis must be the tool that does not replace experiments, but acts as a selective agent, so that synthetic strategies of maximum profitability are used in the laboratory in a surgical way. Here, nanotechnology has been used in olefin metathesis from homogeneous Ru‐NHC catalysts, specifically annulating a C60 fullerene to the NHC ligand. Based on results with the C60 in the backbone, a sterile change with respect to the catalysis of the metal center, an attempt has been made to bring C60 closer to the metal, by attaching it to one of the two C−N bonds of the imidazole group of the SIMes (1,3‐bis(2,4,6‐trimethylphenyl)imidazolin‐2‐ylidene) ligand (reference NHC ligand of the 2nd generation Grubbs catalysts) to increase the steric pressure of C60 in the first sphere of reactivity of the metal. The DFT calculated thermodynamics and the kinetics of SIMes‐derived systems show that they are efficient catalysts for olefin metathesis.
Diastereoselective Double C−H Functionalization of Chiral Ferrocenes with Heteroaromatics
Authors: Plevová Kristína , Kisszékelyi Péter , Vargová Denisa , Andrejčák Samuel , Tóth Viktor , Fertáľ Lukáš , Rakovský Erik , Filo Juraj , Šebesta Radovan
Published: September 2021

Diastereoselective double C−H heteroarylation of chiral ferrocenes provides valuable compounds with multiple functionalities using mild reaction conditions and simple reagents. Pd‐Complexes with chiral mono‐protected amino acids afforded corresponding heteroarylated ferrocenyl amines in good yields and high diastereomeric purities. In this way, a variety of indole, thiophene, pyrrole, or furan substituents were introduced to the ferrocene moiety. Furthermore, a range of relevant functional groups, for example ketone, ester, chloro, nitro, or silyl, are tolerated by this method. An alternative combination of amino acid and ferrocenyl amine configurations was leveraged to provide the complementary diastereomeric products. The products of C−H heteroarylation can be transformed into corresponding phosphines. Absolute configurations of CH‐activation products were confirmed by the combination of X‐ray crystallographic analysis and CD spectroscopy. 19F NMR kinetic study and DFT calculations provided insights into the reaction mechanism and reasons governing stereoinduction.
Stepwise Increase of NdIII‐Based Phosphorescence by AIE‐Active Sensitizer: Broadening the AIPE Family from Transition Metals to Discrete Near‐Infrared Lanthanide Complexes**
Authors: Zhuo Hao , Guan Dao‐Bin , He Jia‐Cun , Xu Hai‐Bing , Zeng Ming‐Hua
Published: September 2021

We designed two near‐infrared (NIR) lanthanide complexes [(L)2‐Nd(NO3)3] (L=TPE2‐BPY for 1, TPE‐BPY for 2) by employing aggregation‐induced emission (AIE)‐active tetraphenylethylene (TPE) derivatives as sensitizers, which possessed matched energy to NdIII, prevented competitive deactivation under aggregation, even shifted the excitation window toward 600 nm by twisted intramolecular charge transfer. Furthermore, benefiting from the 4 f electron shielding effect and antenna effect, the enhanced excitation energies of the AIE‐active sensitizers by structural rigidification transferred into the inert NdIII excited state through 3LMCT, affording the first aggregation‐induced phosphorescence enhancement (AIPE)‐active discrete NIR‐emitting lanthanide complexes. As 1 equipped with more AIE‐active TPE than 2, L→Nd energy transfer efficiency in the former was higher than that in the latter under the same conditions. Consequently, the crystal of 1 exhibited one of the longest lifetimes (9.69 μs) among NdIII‐based complexes containing C−H bonds.
Channel‐reach morphology and landscape properties are linked across a large heterogeneous region
Authors: Lane Belize , Guillon Herve , Byrne Colin , Pasternack Gregory B. , Kasprak Alan , Sandoval‐Solis Samuel
Published: September 2021

Given the complex array of processes influencing river networks, conceptual frameworks of rivers are critical to our understanding of channel processes and response potential, as well as restoration efforts. Yet despite their wide usage, many classifications are based on limited observations over homogenous landscapes, raising questions about their general applicability and quantitative thresholds. Leveraging a large, transect‐based morphological field dataset across California, USA, we use data‐driven methods to evaluate multivariate patterns in channel morphology and linkages with landscape properties considering a diversity of physio‐climatic settings. Emergent patterns highlight the variability in channel form observed across an extensive dataset over heterogeneous but spatially linked watersheds. In general, identified dominant channel attributes and landscape properties align with established channel types defined through expert judgement, but key differences also emerge. Similar to past studies, bed sediment composition and sub‐reach depth variability were discriminating channel attributes. The dominance of landscape properties associated with sediment supply or transport capacity suggests that morphological diversity largely reflects these differences as posited by prior classifications. Results also show some channel forms to be largely independent of valley confinement, with several channel bedforms and dominant grain sizes occurring across valley settings. This data analysis study demonstrates the utility of considering channel reaches and landscapes as multi‐dimensional features to elucidate and test established geomorphic understanding over large field datasets.
Sulfur isotopic and trace‐element compositions of pyrite from the Zankan iron deposit, West Kunlun Orogenic Belt, China: Possible Early Cambrian banded iron formations
Authors: Ding Teng , Wang Jia , Tan Tingting , Zhang Chuanlin , Ye Xiantao , Hao Xiaoshu
Published: September 2021

Abundant iron deposits characterized by stratified orebodies have recently been discovered in the Taxkorgan Terrane, West Kunlun Orogenic Belt, China. Of these deposits, the Zankan iron deposit was the first to be discovered and has the largest estimated tonnage. However, the iron mineralization types for this deposit and others in this area are uncertain, mainly because of the apparent conflict between their typical banded architecture and Cambrian ages. In this study, in situ sulfur isotopic and trace‐element compositions of pyrite, including that in orebodies coexisting with magnetite (Py(o)), pyrite veinlets in strata (Py(v)), and rhyolite and magnetite veins cross‐cutting rhyolite (Py(r)), were conducted to ascertain the genesis of the Zankan deposit. Our results reveal that the pyrite in Zankan deposit has marked positive δ34S values (17.20‰–29.86‰). In addition, Py(o) has low Co/Ni ratios, which are distinct to Py(r) and Py(v), meaning that they belong to typical marine chemical precipitates and magmatic–hydrothermal pyrite, respectively. The coexistence of pyrite and magnetite suggests that the Zankan iron deposit was precipitated in a euxinic basin. Together, our results suggest that seawater sulfate concentrations were low, and the scale and sulfur isotopic compositions of this euxinic basin were most likely dominated by changes in sea level eustacy, which controlled the proportions of seawater and riverine inputs. Comparison with typical Precambrian banded iron formations (BIFs) suggests that the Zankan iron deposit belongs to a unique class of Cambrian BIFs that were controlled predominantly by basins in a shelf environment with locally anoxic conditions.
Predicting vaccine hesitancy from area‐level indicators: A machine learning approach
Authors: Carrieri Vincenzo , Lagravinese Raffele , Resce Giuliano
Published: September 2021

Vaccine hesitancy (VH) might represent a serious threat to the next COVID‐19 mass immunization campaign. We use machine learning algorithms to predict communities at a high risk of VH relying on area‐level indicators easily available to policymakers. We illustrate our approach on data from child immunization campaigns for seven nonmandatory vaccines carried out in 6062 Italian municipalities in 2016. A battery of machine learning models is compared in terms of area under the receiver operating characteristics curve. We find that the Random Forest algorithm best predicts areas with a high risk of VH improving the unpredictable baseline level by 24% in terms of accuracy. Among the area‐level indicators, the proportion of waste recycling and the employment rate are found to be the most powerful predictors of high VH. This can support policymakers to target area‐level provaccine awareness campaigns.
Urban to rural COVID‐19 progression in India: The role of massive migration and the challenge to India's traditional labour force policies
Authors: Sahoo Prafulla Kumar , Biswal Suchismita , Kumar Hemant , Powell Mike
Published: September 2021

The coronavirus disease‑2019 (COVID‐19) has emerged as a deadliest disease in the 21st century. Initially in India, this disease was concentrated in major urban cities like Mumbai, Delhi, Gujarat, and Chennai, which were the national hotspots for the COVID‐19 pandemic. However, in subsequent months, returning migrants (mainly day labour) brought the disease back to their home; this vector triggered significant spread to semi‐urban and rural areas. This highlighted serious concerns in rural India, where access to sophisticated healthcare and mitigation strategies were lacking. There is little data on this new pattern of disease spread. This article provides a short review for tracking the spread of COVID‐19 into major rural states in India based on understanding urban‐rural workforce migration relative to the growing proportion of the nation's COVID‐19 caseload between May‐September 2020.
Three‐dimensional flow past a porous vertical plate in a porous medium with sinusoidal suction and permeability in the presence of thermal diffusion
Authors: Ahmed Nazibuddin , Bordoloi Rajdeep
Published: September 2021

An analytical solution, based on the asymptotic series expansion method, for the problem of a fully developed chemically reactive laminar three‐dimensional flow through a porous vertical infinite plate in a porous medium with sinusoidal permeability as suction in the existence of appreciable radiation is presented. The effects of the physical parameters entering into the problem on the flow and transport characteristics are studied and demonstrated through graphs. The flow is three‐dimensional due to sinusoidal suction as well as porosity. It is found that concentration of the fluid rises due to thermal diffusion (Soret) effect. Furthermore, it is seen that fluid velocity is increased for increasing thermal diffusion effect. Also, viscous drag at the plate is increased under the Soret effect.