bluuebunny/crossref_metadata_2025_split huggingface dataset:
Use of Electronic Clinical Data to Track Incidence and Mortality for SARS-CoV-2–Associated Sepsis
Authors: Shappell Claire N. , Klompas Michael , Chan Christina , Chen Tom , Kanjilal Sanjat , McKenna Caroline , Rhee Chanu ,   CDC Prevention Epicenters Program
Published: September 2023

ImportanceEfforts to quantify the burden of SARS-CoV-2–associated sepsis have been limited by inconsistent definitions and underrecognition of viral sepsis.ObjectiveTo describe the incidence and outcomes of SARS-CoV-2–associated sepsis vs presumed bacterial sepsis using objective electronic clinical criteria.Design, Setting, and ParticipantsThis retrospective cohort study included adults hospitalized at 5 Massachusetts hospitals between March 2020 and November 2022.ExposuresSARS-CoV-2–associated sepsis was defined as a positive SARS-CoV-2 polymerase chain reaction test and concurrent organ dysfunction (ie, oxygen support above simple nasal cannula, vasopressors, elevated lactate level, rise in creatine or bilirubin level, and/or decline in platelets). Presumed bacterial sepsis was defined by modified US Centers for Disease Control and Prevention adult sepsis event criteria (ie, blood culture order, sustained treatment with antibiotics, and organ dysfunction using identical thresholds as for SARS-CoV-2–associated sepsis).Main Outcomes and MeasuresTrends in the quarterly incidence (ie, proportion of hospitalizations) and in-hospital mortality for SARS-CoV-2–associated and presumed bacterial sepsis were assessed using negative binomial and logistic regression models.ResultsThis study included 431 017 hospital encounters from 261 595 individuals (mean [SD] age 57.9 [19.8] years, 241 131 (55.9%) females, 286 397 [66.5%] from academic hospital site). Of these encounters, 23 276 (5.4%) were from SARS-CoV-2, 6558 (1.5%) had SARS-CoV-2–associated sepsis, and 30 604 patients (7.1%) had presumed bacterial sepsis without SARS-CoV-2 infection. Crude in-hospital mortality for SARS-CoV-2–associated sepsis declined from 490 of 1469 (33.4%) in the first quarter to 67 of 450 (14.9%) in the last (adjusted odds ratio [aOR], 0.88 [95% CI, 0.85-0.90] per quarter). Crude mortality for presumed bacterial sepsis was 4451 of 30 604 patients (14.5%) and stable across quarters (aOR, 1.00 [95% CI, 0.99-1.01]). Medical record reviews of 200 SARS-CoV-2–positive hospitalizations confirmed electronic health record (EHR)–based SARS-CoV-2–associated sepsis criteria performed well relative to sepsis-3 criteria (90.6% [95% CI, 80.7%-96.5%] sensitivity; 91.2% [95% CI, 85.1%-95.4%] specificity).Conclusions and RelevanceIn this retrospective cohort study of hospitalized adults, SARS-CoV-2 accounted for approximately 1 in 6 cases of sepsis during the first 33 months of the COVID-19 pandemic. In-hospital mortality rates for SARS-CoV-2–associated sepsis were high but declined over time and ultimately were similar to presumed bacterial sepsis. These findings highlight the high burden of SARS-CoV-2–associated sepsis and demonstrate the utility of EHR-based algorithms to conduct surveillance for viral and bacterial sepsis.
Cryo‐EM structures of CusA Reveal a Mechanism of Metal‐Ion Export
Authors: Moseng Mitchell A. , Klenotic Philip A. , Yu Edward W. 
Published: September 2023

AbstractGram‐negative bacteria utilize the resistance‐nodulation‐cell division (RND) superfamily of efflux pumps to remove toxic compounds from the cell. TheEscherichia coliCusA membrane protein is responsible for recognizing and extruding biocidal Cu(I) and Ag(I) ions. This membrane protein belongs to the heavy‐metal efflux (HME) subfamily of RND efflux transporters. We use single‐particle cryo‐electron microscopy (cryo‐EM) to solve four different structures of the trimeric CusA heavy‐metal efflux pump in the presence of Cu(I). We discovered that different CusA protomers within the trimer are able to bind Cu(I) ions simultaneously. Our structural data allow us to propose a mechanism for ion transport where each CusA protomer functions independently within the trimer.
Transition Metal Catalysts for Depolymerization
Authors: Luk James , Kumar Amit 
Published: September 2023

Abstract
The global production and use of plastics is ever increasing, and consequently, so is plastic waste. Chemical recycling or depolymerization offers a potentially sustainable solution to the crisis of plastic pollution, enabling the production of either valuable organic compounds or monomers for a closed‐loop system. A vast amount of such depolymerization processes involve transition‐metal‐based catalysts. This review article provides a synopsis of various methods used for the transition‐metal‐catalyzed depolymerization of plastics. Processes based on both hetero‐ and homogeneous catalysts have been reviewed along with details of commercialized processes where relevant. The content has been divided on the basis of the type of plastics—polyolefins (polyethenes, polystyrene, and polyvinyl chloride), polyesters, polycarbonates, polyamides, polyurethanes, and polyureas. Processes based on pyrolysis, hydrogenolysis, and solvolysis have been discussed throughout the article as promising tools for the depolymerization of plastics. Considering that there is a plethora of literature on plastic degradation, we have focused only on the processes where a transition metal is used as a catalyst under thermal conditions. Therefore, several other processes such as plastic degradation using enzyme, plasma, supercritical solvents, and ionic liquid or photodegradation have been deemed out of scope of this article.
Photocage Complexes for Zn
2+
and Biologically Relevant Metal Ion Release
Authors: Hickey Erin E. , Burdette Shawn C. 
Published: September 2023

Abstract
Photocaged complexes are important chemical tools for studying dynamic events in biology such as signaling and metal ion homeostasis. Several strategies now exist for photocaging metal ions based on the reactivity of light‐active nitroaromatics and similar chromophores. Designing an effective photocage requires balancing several different factors including photoactivity, metal ion selectivity, and ease of access to the desired molecules. The most widely available photocaged complexes are intended for investigating the biochemistry of calcium; however, more recent work has expanded the toolbox to include photocages designed to probe the importance of zinc and copper. In addition, detailed investigations of the photochemistry have revealed some best practices needed to design the best photocage for a particular application.
Engineering Symmetry Breaking Enables Efficient Bulk Spin‐Orbit Torque‐Driven Perpendicular Magnetization Switching
Authors: Chen Lei , Zhang Kun , Li Bo , Hong Bin , Huang Wentao , He Yu , Feng Xueqiang , Zhang Zhizhong , Lin Kelian , Zhao Weisheng , Zhang Yue 
Published: September 2023

AbstractTo overcome the interfacial nature of spin‐orbit torque (SOT) in bilayers, novel bulk SOT (BSOT) is widely investigated to implement high‐density and low‐power spintronic devices. However, the underlying mechanism of efficient BSOT switching remains unclear, especially the anomalously enhanced effective spin Hall angle (θSH) with increasing ferromagnet thickness (tFM), due to lacking simple and high‐tunable material systems. Here, a series of Pt/Co multilayers with invariable thickness gradient and varying stacking numbers is designed to systematically explore BSOT origin and enable efficient switching via engineering symmetry breaking. As tFM increases, the critical current density decreases while the switching efficiency and θSH build up. Comparative experiments directly demonstrate that gradient‐induced local spin current is more efficient than that in the bilayer. Moreover, x‐ray absorption spectroscopy (XAS) results reveal that the increasing stacking number can effectively engineer the symmetry breaking at Pt/Co interface to induce strong interfacial spin‐orbit coupling. On this basis, it is concluded that the BSOT effect, as well as the anomalously enhanced switching efficiency, and θSH arises from gradient‐induced bulk and interface symmetry breaking. These findings clarify the underlying mechanism of BSOT, and broaden the scope of material engineering to improve switching efficiency and inspire more memory and computing applications.
Unveiling the Potential of Colorless Polyimide‐Derived Laser‐Induced Graphene: A Novel Pathway for Advanced Sensor and Energy Harvester Performance
Authors: Jeong Sung‐Yeob , Ito Yusuke , Kwon Yong‐Wan , Sun Huijie , Chung Jae‐Yeop , Suk Myung‐Eun , Sugita Naohiko 
Published: September 2023

AbstractThe potential of laser‐induced graphene (LIG), recognized for its distinct attributes in diverse fields, has significantly grown. However, the creation of LIG using colorless polyimide (CPI) films remains unexplored. This research sheds light on the graphitization technique for generating LIG from CPI films via laser techniques, a process validated through ReaxFF simulations. It is also illustrated that CPI integrated with fluorine atoms possesses an elevated porous configuration, rendering it apt for high‐sensitivity, low‐detection limit pressure sensors. The pressure sensor, constructed with LIG derived from CPI, showcases superior performance metrics such as an exceptional sensitivity rate of 60.340 kPa−1in low‐pressure ranges (1.0–1.5 kPa), prompt response and recovery intervals (27/36 ms), and commendable durability. The sensor's ability is further validated to precisely track human movements. Moreover, the study employs the LIG sourced from CPI as a dielectric‐to‐dielectric triboelectric nanogenerator (TENG), yielding a peak power output of 411.4 mW m−2under a 40 MΩ load resistance. The CPI‐based LIG offers increased porosity in comparison to traditional LIG, which aids in superior functioning in pressure sensors and TENG devices. This research offers a fresh perspective on the application possibilities of CPI‐sourced LIG, notably in pressure sensors and energy harvesting devices.
Multichromism in Halide Perovskites
Authors: Kanwat Anil , Yantara Natalia , Kajal Priyanka , Mathews Nripan 
Published: September 2023

AbstractThe flexibility and adaptability of halide perovskites position them as a promising material for a variety of cutting‐edge technologies. In addition to their primary applications in photovoltaics and light‐emitting diodes, they have recently garnered interest for potential use in switchable technologies, such as smart windows, switchable photovoltaics, memory devices, neuromorphic computing, and sensors. This interest stems from these switchable properties, which allow them to alter color or other physical properties in response to external stimuli like heat, electric fields, light, pressure, and moisture. This review investigates their switching properties and examines their practical applications across a range of emerging chromic technologies. An in‐depth analysis of the mechanisms of reversibility, switchable optical and electrical properties, as well as the chemical and structural transformations these materials undergo is also presented. Furthermore, they are categorized based on their unique switching mechanisms. To assist the research community in developing new multichromic halide perovskite designs, several essential criteria are outlined for effective switchable materials. Lastly, the current challenges faced by these emerging materials are discussed, and a perspective on future developments and potential breakthroughs in this promising research area is offered.
Iodotrimethylsilane as a Reactive Ligand for Surface Etching and Passivation of Perovskite Nanocrystals toward Efficient Pure‐red to Deep‐red LEDs
Authors: Zhao Feng , Duan Hong‐Wei , Li Sheng‐Nan , Pan Jia‐Lin , Shen Wan‐Shan , Li Sheng‐Ming , Zhang Qiao , Wang Ya‐Kun , Liao Liang‐Sheng 
Published: September 2023

AbstractResurfacing perovskite nanocrystals (NCs) with tight‐binding and conductive ligands to resolve the dynamic ligands—surface interaction is the fundamental issue for their applications in perovskite light‐emitting diodes (PeLEDs). Although various types of surface ligands have been proposed, these ligands either exhibit weak Lewis acid/base interactions or need high polar solvents for dissolution and passivation, resulting in a compromise in the efficiency and stability of PeLEDs. Herein, we report a chemically reactive agent (Iodotrimethylsilane, TMIS) to address the trade‐off among conductivity, solubility and passivation using all‐inorganic CsPbI3 NCs. The liquid TMIS ensures good solubility in non‐polar solvents and reacts with oleate ligands and produces in situ HI for surface etching and passivation, enabling strong‐binding ligands on the NCs surface. We report, as a result, red PeLEDs with an external quantum efficiency (EQE) of ≈23 %, which is 11.2‐fold higher than the control, and is among the highest CsPbI3 PeLEDs. We further demonstrate the universality of this ligand strategy in the pure bromide system (CsPbBr3), and report EQE of ≈20 % at 640, 652, and 664 nm. This represents the first demonstration of a chemically reactive ligand strategy that applies to different systems and works effectively in red PeLEDs spanning emission from pure‐red to deep‐red.
Unlocking Catalytic Potential: Exploring the Impact of Thermal Treatment on Enhanced Electrocatalysis of Nanomaterials
Authors: Kogularasu Sakthivel , Lee Yen‐Yi , Sriram Balasubramanian , Wang Sea‐Fue , George Mary , Chang‐Chien Guo‐Ping , Sheu Jinn‐Kong 
Published: September 2023

AbstractIn the evolving field of electrocatalysis, thermal treatment of nano‐electrocatalysts has become an essential strategy for performance enhancement. This review systematically investigates the impact of various thermal treatments on the catalytic potential of nano‐electrocatalysts. The focus encompasses an in‐depth analysis of the changes induced in structural, morphological, and compositional properties, as well as alterations in electro‐active surface area, surface chemistry, and crystal defects. By providing a comprehensive comparison of commonly used thermal techniques, such as annealing, calcination, sintering, pyrolysis, hydrothermal, and solvothermal methods, this review serves as a scientific guide for selecting the right thermal technique and favorable temperature to tailor the nano‐electrocatalysts for optimal electrocatalysis. The resultant modifications in catalytic activity are explored across key electrochemical reactions such as electrochemical (bio)sensing, catalytic degradation, oxygen reduction reaction, hydrogen evolution reaction, overall water splitting, fuel cells, and carbon dioxide reduction reaction. Through a detailed examination of the underlying mechanisms and synergistic effects, this review contributes to a fundamental understanding of the role of thermal treatments in enhancing electrocatalytic properties. The insights provided offer a roadmap for future research aimed at optimizing the electrocatalytic performance of nanomaterials, fostering the development of next‐generation sensors and energy conversion technologies.
Azoxy Compounds—From Synthesis to Reagents for Azoxy Group Transfer Reactions
Authors: Cai Bao‐Gui , Empel Claire , Yao Wei‐Zhong , Koenigs Rene M. , Xuan Jun 
Published: September 2023

AbstractThe azoxy functional group is an important structural motif and represents the formally oxidized counterpart of the azo group. Azoxy compounds find numerous applications ranging from pharmaceuticals to functional materials, yet their synthesis remains underdeveloped with a main focus on the formation symmetric azoxy compounds. To overcome challenges in the synthesis of such unsymmetric azoxy compounds, we designed a process employing readily accessible nitroso compounds and iminoiodinanes. This method builds on the use of visible light irradiation to generate a triplet nitrene from iminoiodinanes, which is trapped by nitroso arenes to give access to sulfonyl‐protected azoxy compounds with a good substrate scope and functional group tolerance. We further describe two applications of these sulfonyl‐protected azoxy compounds as radical precursors in synthesis, where the whole azoxy group can be transferred and employed in C(sp3)−H functionalization of ethers or 1,2‐difunctionalization of vinyl ethers. All of the reactions occurred at room temperature under visible light irradiation without the addition of any photoredox catalysts and additives. Control experiments, mechanism investigations, and DFT studies well explained the observed reactivity.
Exploiting the Catenane Mechanical Bond Effect for Selective Halide Anion Transmembrane Transport
Authors: Min Tay Hui , Johnson Toby G. , Docker Andrew , Langton Matthew J. , Beer Paul D. 
Published: September 2023

AbstractThe first examples of [2]catenanes capable of selective anion transport across a lipid bilayer are reported. The neutral halogen bonding (XB) [2]catenanes were prepared via a chloride template‐directed strategy in an unprecedented demonstration of using XB⋅⋅⋅anion interactions to direct catenane assembly from all‐neutral components. Anion binding experiments in aqueous‐organic solvent media revealed strong halide over oxoanion selectivity, and a marked enhancement in the chloride and bromide affinities of the catenanes relative to their constituent macrocycles. The catenanes additionally displayed an anti‐Hofmeister binding preference for bromide over the larger iodide anion, illustrating the efficacy of employing sigma‐hole interactions in conjunction with the mechanical bond effect to tune receptor selectivity. Transmembrane anion transport studies conducted in POPC LUVs revealed that the catenanes were more effective anion transporters than the constituent macrocycles, with high chloride over hydroxide selectivity, which is critical to potential therapeutic applications of anionophores. Remarkably these outperform existing acyclic halogen bonding anionophores with regards to this selectivity. Record chloride over nitrate anion transport selectivity was also observed. This represents a rare example of the direct translation of intrinsic anion binding affinities to anion transport behaviour, and demonstrates the key role of the catenane mechanical bond effect for enhanced anion transport selectivity.
Nickel‐Catalyzed Asymmetric Synthesis of P‐Stereogenic Phosphanyl Hydrazine Building Blocks
Authors: Wang Chuanyong , Yang Qingliang , Dai Yuan‐Hao , Xiong Jianqi , Zheng Yu , Duan Wei‐Liang 
Published: September 2023

AbstractCatalytic asymmetric methods for the synthesis of synthetically versatile P‐stereogenic building blocks offer an efficient and practical approach for the diversity‐oriented preparation of P‐chiral phosphorus compounds. Herein, we report the first nickel‐catalyzed synthesis of P‐stereogenic secondary aminophosphine‐boranes by the asymmetric addition of primary phosphines to azo compounds. We further demonstrate that the P−H and P−N bonds on these phosphanyl hydrazine building blocks can be reacted sequentially and stereospecifically to access various P‐stereogenic compounds with structural diversity.
A synergistic strategy for fabricating a highly flexible poly(m‐phenylene isophthalamide) nanofiber‐reinforced polyimide aerogel for high‐temperature filtration
Authors: Yue Wanli , Cao Ying , Han Ruikai , Ren Libing , Liu Simeng , Liu Fan , He Jianxin , Shao Weili , Chen Li 
Published: September 2023

AbstractParticulate matter (PM) has a significant impact on air quality, especially the PM produced by automobile exhaust and high temperature environment. Therefore, it is of great significance to develop a technology that can effectively intercept fine PM under high temperature conditions. This study reports the construction of poly(m‐phenylene isophthalamide) (PMIA) nanofiber‐reinforced polyimide aerogel (PPNFAs) filters using freeze‐drying and electrospinning for high temperature filtration. After 100 compression cycles, the maximum compressive stress of PPNFAs is reduced by only 15%. When the content of PMIA is 0.65 wt%, PPNFAs has a high porosity (97.35%), high specific surface area (8.87 m2 g−1) and highest dust holding capacity (124.8 m2 g−1). After 15 days of continuous heating test at 300°C, the filtration efficiency of PPNFAs filter for different diameter particles of impurities remained above 98%. Therefore, the PPNFAs filter prepared in this study provides a new design concept for a new generation of high temperature filters.
Low velocity impact behaviors and highly residual compressive strength of epoxy foam‐filled 3D woven composites
Authors: Yang Xiaori , Zheng Liangang , Xie Zhangting , Xu Fujun 
Published: September 2023

AbstractIn this work, a new type of epoxy foam‐filled 3D woven spacer composites (FF‐3DWSCs) was designed and manufactured by self‐made 3D loom and foaming technology. The low velocity impact behaviors, residual compressive properties and strengthening mechanisms of epoxy foam were systemically investigated. As the results, the FF‐3DWSCs showed higher impact load of 4000–5200 N than that of 3D woven spacer composites (3DWSCs) (2800–4300 N) at the energy from 10 to 40 J. The residual compressive strength of FF‐3DWSCs (23.85 MPa) was maintained at about 80% after 30 J energy impact. Due to the good compatibility of the epoxy foam and the epoxy resin and the synergistic effect between the pile yarn and the epoxy foam, the interface between epoxy foam and fiber/epoxy was strong. Therefore, the novel FF‐3DWSCs proposed here exhibited excellent impact properties and energy absorption capacity and can be used as a candidate material in the field of high‐performance composites.
Synergistic toughening and reinforcement of poly(lactic acid) with epoxy‐terminated hyperbranched polymers
Authors: Zhou Sudan , Guo Maolin , Jin Yujuan , Sun Jianjian , Tian Huafeng , Hu Jing 
Published: September 2023

AbstractPoly(lactic acid) (PLA) is an eco‐friendly and biodegradable material. However, its molecular chain was rigid and showed limited toughness. In this work, PLA was modified with epoxy‐terminated hyperbranched polymer (EHBP) by melt blending to improve the toughness. The results showed that epoxy groups within EHBP reacted with carboxyl and hydroxyl groups of PLA, forming chemical micro‐crosslinking. In addition, intermolecular hydrogen bonds were also formed between EHBP and PLA. The combined action of the above two aspects ultimately improved the toughness and strength of PLA. The mechanical property tests results showed that the mechanical properties of PLA improved best when 2.5 phr of EHBP was added. At this point, compared with neat PLA, the maximum tensile strength, impact strength, elongation at break, and flexural modulus of PLA/EHBP increased by 17.4%, 54.5%, 107.1%, and 25.8%, respectively, compared to those of neat PLA. It achieves the goal of simultaneously enhancing the toughness and strength of PLA and subsequently expands its potential application applications.