bluuebunny/crossref_metadata_2025_split huggingface dataset:
Quantum Dot Passivation of Halide Perovskite Films with Reduced Defects, Suppressed Phase Segregation, and Enhanced Stability
Authors: Hu Long , Duan Leiping , Yao Yuchen , Chen Weijian , Zhou Zizhen , Cazorla Claudio , Lin Chun‐Ho , Guan Xinwei , Geng Xun , Wang Fei , Wan Tao , Wu Shuying , Cheong Soshan , Tilley Richard D. , Liu Shanqin , Yuan Jianyu , Chu Dewei , Wu Tom , Huang Shujuan 
Published: November 2021

AbstractStructural defects are ubiquitous for polycrystalline perovskite films, compromising device performance and stability. Herein, a universal method is developed to overcome this issue by incorporating halide perovskite quantum dots (QDs) into perovskite polycrystalline films. CsPbBr3 QDs are deposited on four types of halide perovskite films (CsPbBr3, CsPbIBr2, CsPbBrI2, and MAPbI3) and the interactions are triggered by annealing. The ions in the CsPbBr3 QDs are released into the thin films to passivate defects, and concurrently the hydrophobic ligands of QDs self‐assemble on the film surfaces and grain boundaries to reduce the defect density and enhance the film stability. For all QD‐treated films, PL emission intensity and carrier lifetime are significantly improved, and surface morphology and composition uniformity are also optimized. Furthermore, after the QD treatment, light‐induced phase segregation and degradation in mixed‐halide perovskite films are suppressed, and the efficiency of mixed‐halide CsPbIBr2 solar cells is remarkably improved to over 11% from 8.7%. Overall, this work provides a general approach to achieving high‐quality halide perovskite films with suppressed phase segregation, reduced defects, and enhanced stability for optoelectronic applications.
Washable and Stretchable Zn–MnO2Rechargeable Cell
Authors: Nguyen Tan N. , Iranpour Bahar , Cheng Evan , Madden John D. W. 
Published: November 2021

AbstractA cell that can operate even when doubled in length, and that withstands washing is demonstrated. The cell employs rechargeable and safe zinc/manganese dioxide chemistry. It incorporates a biocompatible poly(styrene – isobutylene – styrene) (SIBS) polymer as encapsulation, and in all layers. The SIBS‐based separator, made using solvent evaporation‐induced phase separation, has an ionic conductivity of 0.05 S m−1. Electrodes contain carbon black, combined with active particles and SIBS as the binder. Stretchable current collectors are carbon black/carbon nanofiber/SIBS composites and exhibit a sheet resistance of 27 Ω ⬜−1under 100% strain. These components are encapsulated by SIBS membranes into a full cell, thin‐film configuration, creating a single, polymer‐based intrinsically stretchable battery. The resulting cell has a reversible specific capacity of 160 mAh g−1cathode active mass. Capacity retention is 75% following 500 charge and discharge cycles. Owing to the low permeability of SIBS and the excellent adhesion between its layers, the battery has a good shelf‐life (22% mass loss of electrolyte after 523 days) and can withstand 39 washing cycles. The high capacity relative to other stretchable cells, along with the low materials cost, safe chemistry, durability, and washability, make this SIBS cell attractive for wearables and other applications that benefit from stretchability.
Radioactive Ion Beam Production at the Gamma Factory
Authors: Nichita Dragos , Balabanski Dimiter L. , Constantin Paul , Krasny Mieczyslaw W. , Płaczek Wieslaw 
Published: November 2021

AbstractA very intense γ beam of the Gamma Factory facility proposed at CERN can be used to generate radioactive ion beams (RIBs) with high production yields and study the structure of exotic neutron‐rich nuclei. The radioactive nuclides are generated via photo‐fission in several actinide targets and thermalized in high‐purity cryogenic helium, filling a gas cell which is enclosing the targets. Electric fields are used to extract heavy ions and form RIBs which can be send to various selection and measurement stations. Estimates for the production and extraction yields of exotic neutron‐rich nuclei with such a setup are provided. A study of the impact of space charge, build‐up inside the gas cell, on the extraction properties is presented and it is demonstrated that the beam needs to be chopped for achieving optimal extraction yields.
Substrate Profiling of Mitochondrial Caseinolytic Protease P via a Site‐Specific Photocrosslinking Approach
Authors: Nguyen Tuan‐Anh , Gronauer Thomas F. , Nast‐Kolb Timon , Sieber Stephan A. , Lang Kathrin 
Published: November 2021

AbstractApproaches for profiling protease substrates are critical for defining protease functions, but remain challenging tasks. We combine genetic code expansion, photocrosslinking and proteomics to identify substrates of the mitochondrial (mt) human caseinolytic protease P (hClpP). Site‐specific incorporation of the diazirine‐bearing amino acid DiazK into the inner proteolytic chamber of hClpP, followed by UV‐irradiation of cells, allows to covalently trap substrate proteins of hClpP and to substantiate hClpP's major involvement in maintaining overall mt homeostasis. In addition to confirming many of the previously annotated hClpP substrates, our approach adds a diverse set of new proteins to the hClpP interactome. Importantly, our workflow allows identifying substrate dynamics upon application of external cues in an unbiased manner. Identification of unique hClpP‐substrate proteins upon induction of mt oxidative stress, suggests that hClpP counteracts oxidative stress by processing of proteins that are involved in respiratory chain complex synthesis and maturation as well as in catabolic pathways.
Efficient Polyester Hydrogenolytic Deconstruction via Tandem Catalysis
Authors: Kratish Yosi , Marks Tobin J. 
Published: November 2021

AbstractUsing a mechanism‐based solvent‐free tandem catalytic approach, commodity polyester plastics such as polyethylene terephthalate (PET), polybutylene terephthalate (PBT), and polyethylene naphthalate (PEN) are rapidly and selectively deconstructed by combining the two air‐ and moisture‐stable catalysts, Hf(OTf)4 and Pd/C, under 1 atm H2, affording terephthalic acid (or naphthalene dicarboxylic acid for PEN) and ethane (or butane for PBT) in essentially quantitative yield. This process is effective for both laboratory grade and waste plastics, and comingled polypropylene remains unchanged. Combined experimental and DFT mechanistic analyses indicate that Hf(OTf)4 catalyzes a mildly exergonic retro‐hydroalkoxylation reaction in which an alkoxy C−O bond is first cleaved, yielding a carboxylic acid and alkene, and this process is closely coupled to an exergonic olefin hydrogenation step, driving the overall reaction forward.
Global Analysis of the Mechanical Properties of Organic Crystals
Authors: Karothu Durga Prasad , Mahmoud Halabi Jad , Ahmed Ejaz , Ferreira Rodrigo , Spackman Peter R. , Spackman Mark A. , Naumov Panče 
Published: November 2021

AbstractOrganic crystals, although widely studied, have not been considered nascent candidate materials in engineering design. Here we summarize the mechanical properties of organic crystals that have been reported over the past three decades, and we establish a global mechanical property profile that can be used to predict and identify mechanically robust organic crystals. Being composed of light elements, organic crystals populate a narrow region in the mechanical property–density space between soft, disordered organic materials and stiff, ordered materials. Two subsets of extraordinarily stiff and hard organic crystalline materials were identified and rationalized by the normalized number density, strength, and directionality of their intermolecular interactions. We conclude that future lightweight, soft, all‐organic components in devices should capitalize on the greatest asset of organic single crystals—namely, the combination of long‐range structural order and softness.
SnF2‐Catalyzed Formation of Polymerized Dioxolane as Solid Electrolyte and its Thermal Decomposition Behavior
Authors: Li Wei , Gao Jian , Tian Huayang , Li Xiaolei , He Shuang , Li Junpeng , Wang Wenlong , Li Lin , Li Hong , Qiu Jieshan , Zhou Weidong 
Published: November 2021

AbstractPolymerized‐dioxolane(P‐DOL) is of potential as a solid‐polymer‐electrolyte(SPE) due to its high Li+‐conductivity, good compatibility with Li‐metal and desired preparation method of in situ polymerization in cells. In this study, SnF2 was demonstrated not only to be an efficient catalyst for the polymerization of DOL at room temperature, but also an effective additive for improving interfacial wettability and suppressing dendrite through the reaction with Li‐metal and the formation of LiF/LixSn based composite solid electrolyte interlayer(SEI). Using the SnF2 polymerized P‐DOL containing 1 M LiTFSI as SPE(P‐DOL‐SPE), obviously denser Li‐deposition was obtained, and the all‐solid‐state(ASS) Li/LiFePO4 cell delivered stable cycling over 350 cycles at 45 °C. At the same time, the irreversible decomposition of P‐DOL‐SPE into formaldehyde and small molecule epoxides are observed at 110 °C, which is even initiated at lower temperature of 40 °C under vacuum. This thermal decomposition of P‐DOL‐SPE in pouch cell causes huge volume swell, and therefore putting a strict limitation on the operating temperature window for the P‐DOL based electrolytes.
Orienting an Organic Semiconductor into DNA 3D Arrays by Covalent Bonds
Authors: Wang Xiao , Deshmukh Rahul , Sha Ruojie , Birktoft Jens J. , Menon Vinod , Seeman Nadrian C. , Canary James W. 
Published: November 2021

AbstractA quasi‐one‐dimensional organic semiconductor, hepta(p‐phenylene vinylene) (HPV), was incorporated into a DNA tensegrity triangle motif using a covalent strategy. 3D arrays were self‐assembled from an HPV‐DNA pseudo‐rhombohedron edge by rational design and characterized by X‐ray diffraction. Templated by the DNA motif, HPV molecules exist as single‐molecule fluorescence emitters at the concentration of 8 mM within the crystal lattice. The anisotropic fluorescence emission from HPV‐DNA crystals indicates HPV molecules are well aligned in the macroscopic 3D DNA lattices. Sophisticated nanodevices and functional materials constructed from DNA can be developed from this strategy by addressing functional components with molecular accuracy.
Site‐Selective Itaconation of Complex Peptides by Photoredox Catalysis
Authors: Wang Siyao , Zhou QingQing , Zhang Xiaheng , Wang Ping 
Published: November 2021

AbstractSite‐selective peptide functionalization provides a straightforward and cost‐effective access to diversify peptides for biological studies. Among many existing non‐invasive peptide conjugations methodologies, photoredox catalysis has emerged as one of the powerful approaches for site‐specific manipulation on native peptides. Herein, we report a highly N‐termini‐specific method to rapidly access itaconated peptides and their derivatives through a combination of transamination and photoredox conditions. This strategy exploits the facile reactivity of peptidyl‐dihydropyridine in the complex peptide settings, complementing existing approaches for bioconjugations with excellent selectivity under mild conditions. Distinct from conventional methods, this method utilizes the highly reactive carbamoyl radical derived from a peptidyl‐dihydropyridine. In addition, this itaconated peptide can be further functionalized as a Michael acceptor to access the corresponding peptide‐protein conjugate.
Linear Extension of Anthracene via B←N Lewis Pair Formation: Effects on Optoelectronic Properties and Singlet O2Sensitization
Authors: Vanga Mukundam , Sahoo Ashutosh , Lalancette Roger A. , Jäkle Frieder 
Published: November 2021

AbstractThe functionalization of polycyclic aromatic hydrocarbons (PAHs) via B←N Lewis pair formation offers an opportunity to judiciously fine‐tune the structural features and optoelectronic properties, to suit the demands of applications in organic electronic devices, bioimaging, and as sensitizers for singlet oxygen generation. We demonstrate that the N‐directed electrophilic borylation of 2,6‐di(pyrid‐2‐yl)anthracene offers access to linearly extended acene derivativesPy‐BR(R=Et, Ph, C6F5). In comparison to indeno‐fused 9,10‐diphenylanthracene, the formal “BN for CC” replacement inPy‐BRselectively lowers the LUMO, resulting in a much reduced HOMO–LUMO gap. An even more extended conjugated system with seven six‐membered rings in a row (Qu‐BEt) is obtained by borylation of 2,6‐di(quinolin‐8‐yl)anthracene. FluorinatedPy‐BPfshows particularly advantageous properties, including relatively lower‐lying HOMO and LUMO levels, strong yellow‐green fluorescence, and effective singlet oxygen sensitization, while resisting self‐sensitized conversion to its endoperoxide.
A label‐free and signal‐amplifiable assay method for colorimetric detection of carcinoembryonic antigen
Authors: Li Peng , Li Wenqin , Xie Zhuohao , Zhan Haonan , Deng Liehua , Huang Jiahao 
Published: November 2021

AbstractIn this work, an innovative colorimetric assay method for the determination of carcinoembryonic antigen is developed with aptamer probes utilized as recognition element. DNA hybridization chain reaction is used as signal amplification technique, and peroxidase‐mimicking hemin/G‐quadruplex‐assisted catalytic oxidation of 2,2'‐azino‐bis‐3‐ethylbenzothiazoline‐6‐sulfonic acid (ABTS) is deployed as signal reporting mechanism. The detection principle was firstly verified by using gel electrophoresis analysis and absorbance measurements. After condition optimization, a detection limit was theoretically determined as 24.8 ng/ml. Furthermore, the method exhibited good selectivity and satisfactory recovery rates (92.2%–108.6%) in serum samples. Moreover, the sensing scheme is easily extended for the detection of other analytes via similar target‐aptamer recognition principle. To sum up, this is an enzyme‐ and label‐free, cost‐effective yet signal‐amplifiable assay scheme for the determination of tumor markers with promising simplicity and selectivity, practical utility, and potential universality.
Validation of a robust and rapid liquid chromatography tandem mass spectrometric method for the quantitative analysis of navitoclax
Authors: Scott Susan C. , Anders Nicole M. , He Ping , Hemingway Avelina , Gore Steven D. , Hann Christine L. , Rudek Michelle A. 
Published: November 2021

AbstractThe Bcl‐2 family small molecule inhibitor navitoclax is being clinically evaluated to treat multiple cancers including lymphoid malignancies and small cell lung cancer. A sensitive and reliable method was developed to quantitate navitoclax in human plasma using liquid chromatography with tandem mass spectrometry with which to perform detailed pharmacokinetic studies. Sample preparation involved protein precipitation using acetonitrile. Separation of navitoclax and the internal standard, navitoclax‐d8, was achieved with a Waters Acquity UPLC BEH C18 column using isocratic flow over a 3 min total analytical run time. A SCIEX 4500 triple quadrupole mass spectrometer operated in positive electrospray ionization mode was used for the detection of navitoclax. The assay range was 5–5,000 ng/ml and proved to be accurate (89.5–104.9%) and precise (CV ≤ 11%). Long‐term frozen plasma stability for navitoclax at −70°C was at least 43 months. The method was applied for the measurement of total plasma concentration of navitoclax in a patient receiving a 250 mg daily oral dose.
Development of a student engagement score for online undergraduate engineering courses using learning management system interaction data
Authors: Kittur Javeed , Bekki Jennifer , Brunhaver Samantha 
Published: November 2021

AbstractAlthough researchers agree that student engagement in online courses is a function of time dedicated to course‐related activities, there is little consensus about the best way to quantify the construct. This study introduces a measure for undergraduate engineering students' engagement in online courses using their interactions with their online course learning management system (LMS). Data from 81 courses offered by three fully online, undergraduate engineering degree programs generated a total of 3848 unique student–course combinations (approximately 2.7 million rows of LMS interaction data), to which we applied a five‐step process to calculate a single score representing student LMS engagement. First, we converted the students' LMS interaction data into a set of natural features representing the time they spent per 3‐day period on various course elements, such as quizzes, assignments, discussion forums, and so forth, and how these times changed across the duration of the course. We then used the natural features to derive 216 relative features describing deviations from typical interaction patterns among students in the same course. Next, we conducted association rule mining on a training portion of the data set to generate rules separately describing the behavior of students who completed the course (completers) and those who chose to drop early (leavers). The rules generated were applied to students from the testing portion of the data set to compute the percentage of unique rules met by completers and leavers. Finally, the mathematical difference between the percentages of completer and leaver rules met by each student was found to be the best measure of student engagement.
Renal toxicities in immune checkpoint inhibitors with or without chemotherapy: An observational, retrospective, pharmacovigilance study leveraging US FARES database
Authors: Hu Fangyuan , Zhai Yinghong , Yuan Lei , Liang Jizhou , Xu Jinfang , Guo Xiaojing , Zhou Xiang , Lin Zhen , Sun Jinhai , Ye Xiaofei , He Jia 
Published: November 2021

AbstractBackgroundImmune checkpoint inhibitors (ICIs) have elicited durable antitumor responses in multiple types of cancers. However, ICIs could also induce potential toxicities that involve all organs, including renal system. In this study, we aimed to conduct a comprehensive description of the ICIs‐induced renal toxicities and the potential effects of chemotherapy.MethodsWe conducted a pharmacovigilance study based on US Food and Drug Administration (FDA) Adverse Event Reporting System (FAERS) database between 01 January 2014 and 30 June 2019. Disproportionality analysis was used to assess the association between ICIs and renal adverse events (AEs), including reporting odds ratio (ROR) and information component (IC). ROR025 and IC025 are, respectively, 95% confidence interval lower end of ROR and IC. If the value of ROR025 exceeding one or IC025 higher than zero, then a signal was considered statistically significant.ResultsA total of 30,602,758 reports were extracted from the database, with 4578 reports for ICIs‐associated renal AEs. Renal AEs were more frequently reported in anti‐PD‐1/PD‐L1 versus anti‐CTLA‐4 monotherapy group (ROR: 1.75, 95% CI: 1.52–2.01). Similarly, renal AEs were more commonly reported in ICIs polytherapy other than monotherapy group (ROR: 1.18, 95% CI: 1.10–1.27). Notably, ICIs plus chemotherapy strategies reported more renal toxicities compared to sole ICIs regimens (ROR: 1.30, 95% CI: 1.17–1.45), whereas exhibited lower fatality outcome rates. Importantly, acute kidney injury (1139, 24.88%) and renal failure (464, 10.14%) were the top two most commonly reported ICIs‐associated renal AEs, and also observed with the top two highest level of fatality outcome rates.ConclusionsA spectrum of renal AEs was detected in ICIs regimens and could be reinforced by ICIs combination. Compared to sole ICIs regimens, ICIs plus chemotherapy strategy reported more renal toxicities but lower fatality outcome rates. With the increasing popularity of ICIs especially combination strategies, it is vital important for clinicians to guarantee balance between durable clinical effects and potential renal toxicities in latest immunotherapy strategies.
The change over time of vital signs with consideration for opioid use in the last 2 weeks of life among cancer patients in a palliative care unit: Continuous measurement of vital signs using a non‐wearable monitor
Authors: Tanaka Haruka , Fukui Sakiko , Maeda Isseki , Hatano Yutaka , Higuchi Akari , Higami Yoko , Yamakawa Miyae , Utsumi Momoe 
Published: November 2021

AbstractObjectivesThe aim of this study was to examine the following by using a non‐wearable monitor: (ⅰ) the trajectory of vital signs (VS) in the last 2 weeks of life among cancer patients, and (ⅱ) the difference in change over time of VS between cancer patients with and without opioid use.MethodsWe conducted a longitudinal study involving cancer patients in a palliative care unit (PCU) from April 2018 to October 2019. VS were collected continuously using a non‐wearable monitor, and we calculated the means of respiratory rate (RR) and heart rate (HR) per hour, and counts of apnea per hour as outcome variables. Explanatory variables were time (subtracting time of death from measurement time of VS, divided by 36) and opioid use. Mean difference (MD) of time represented the slope per hour of VS values. First, we analyzed the associations between VS per hour and time using a linear mixed model (LMM) with random intercepts and slope over time. Second, we analyzed the associations between VS and interaction term between time and opioid use.ResultsWe analyzed 26 cancer patients. RR (MD: 0.27 beats/min [95% CI: 0.27–0.28]), HR (MD: 1.51 beats/min [95% CI: 1.50–1.52]), and apnea (MD: 0.71 count/hour [95% CI: 0.70–0.72]) significantly increased hourly. In addition, RR was significantly associated with interaction term (MD: −1.59 beats/min [95% CI: −3.11 to −0.07]), which indicates that there is a difference in the slope of RR between opioid users and non‐users.ConclusionsWe have successfully described the trajectory of VS in high‐resolution under conditions of a natural end of life in PCU.
A Specialized Dehydrogenase Provides l‐Phenyllactate for FR900359 Biosynthesis
Authors: Klöppel Sophie , Richarz René , Wirtz Daniel A. , Vasenda Natalia , König Gabriele M. , Crüsemann Max 
Published: November 2021

Abstractd‐Phenyllactate (PLA) is a component of the selective Gq protein inhibitor and nonribosomal cyclic depsipeptide FR900359 (FR). Here we report a detailed biochemical investigation of PLA biosynthesis and its incorporation into the natural product FR. The enzyme FrsC, member of the lactate/malate dehydrogenase superfamily, was shown to catalyze the formation of l‐PLA from phenylpyruvate. FrsC was kinetically characterized and its substrate specificity determined. Incorporation of l‐PLA was probed by assaying the adenylation domain FrsE‐A3 and feeding studies with a Chromobacterium vaccinii ΔfrsC mutant, confirming preferred activation of l‐PLA followed by on‐line epimerization to d‐PLA. Finally, detailed bioinformatic analyses of FrsC revealed its close relation to malate dehydrogenases from primary metabolism and suggest extensions in the substrate binding loop to be responsible for its adaptation to accepting larger aromatic substrates with high specificity.