bluuebunny/crossref_metadata_2025_split huggingface dataset:
Ion–Dipole Interaction Regulation Enables High‐Performance Single‐Ion Polymer Conductors for Solid‐State Batteries
Authors: Wen Kaihua , Xin Chengzhou , Guan Shundong , Wu Xinbin , He Shan , Xue Chuanjiao , Liu Sijie , Shen Yang , Li Liangliang , Nan Ce‐Wen 
Published: June 2022

AbstractSolid polymer electrolytes with large ionic conductivity, high ionic transference number, and good interfacial compatibility with electrodes are highly desired for solid‐state batteries. However, unwanted polarizations and side reactions occurring in traditional dual‐ion polymer conductors hinder their practical applications. Here, single‐ion polymer conductors (SIPCs) with exceptional selectivity for Li‐ion conduction (Li‐ion transference number up to 0.93), high room‐temperature ionic conductivity of about 10−4 S cm−1, and a wide electrochemical stability window (>4.5 V, vs Li/Li+) are prepared by precisely regulating the ion–dipole interactions between Li+ and carbonyl/cyano groups. The resulting SIPCs show an excellent electrochemical stability with Li metal during long‐term cycling at room temperature and 60 °C. LiFePO4‐based solid‐state cells containing the SIPCs exhibit good rate and cycling performance in a wide temperature range from −20 to 90 °C. By the same way of ion–dipole interaction regulation, sodium‐ and potassium‐based SIPCs with both high ionic conductivity and high cationic transference numbers are also prepared. The findings in this work provide guidance for the development of high‐performance SIPCs and other metal‐ion systems beyond Li+.
Fluorinated Perylene‐Diimides: Cathode Interlayers Facilitating Carrier Collection for High‐Performance Organic Solar Cells
Authors: Yao Jia , Ding Shiyu , Zhang Rui , Bai Yang , Zhou Qiuju , Meng Lei , Solano Eduardo , Steele Julian A. , Roeffaers Maarten B. J. , Gao Feng , Zhang Zhi‐Guo , Li Yongfang 
Published: June 2022

AbstractOrganic solar cells (OSCs) have experienced rapid progress with the innovation of near‐infrared (NIR)‐absorbing small‐molecular acceptors (SMAs), while the unique electronic properties of the SMAs raise new challenges in relation to cathode engineering for effective electron collection. To address this issue, two fluorinated perylene‐diimides (PDIs), PDINN‐F and PDINN‐2F, are synthesized by a simple fluorination method, for application as cathode interlayer (CIL) materials. The two bay‐fluorinated PDI‐based CILs possess a lower lowest unoccupied molecular orbital (LUMO) energy level of ≈−4.0 eV, which improves the energy level alignment at the NIR‐SMAs (such as BTP‐eC9)/CIL for a favorable electron extraction efficiency. The monofluorinated PDINN‐F shows higher electron mobility and better improved interfacial compatibility. The PDINN‐F‐based OSCs with PM6:BTP‐eC9 as active layer exhibit an enhanced fill factor and larger short‐circuit current density, leading to a high power conversion efficiency (PCE) exceeding 18%. The devices with PDINN‐F CIL retain more than 80% of their initial PCE after operating at the maximum power point under continuous illumination for 750 h. This work prescribes a facile, cost‐effective, and scalable method for the preparation of stable, high‐performance fluorinated CILs, and instilling promise for the NIR‐SMAs‐based OSCs moving forward.
Thinking sustainably? Identifying Stakeholders' positions toward corporate sustainability in floriculture with Q methodology
Authors: Derksen Dirtje Marie , Mithöfer Dagmar 
Published: June 2022

AbstractThe aim of this study is to explore the different perspectives of floricultural stakeholders on sustainability. Q methodology is used to identify the diversity of viewpoints. Based on 34 statements derived from stakeholder‐interviews and ranked by 12 stakeholders, three perspectives were identified: Attitude over strategy, business‐centered approach, and pragmatic approach. The viewpoints shared a predominantly weak sustainability‐understanding and differed in their evaluation of nature, global sustainability issues and organizational perspectives. The perspectives were inconsistent and ambiguous; the stages of the sustainability spectrum of Landrum can only be regarded as a conceptual guideline leaving the idea of clearly delineated stages behind.
Online learning‐based predictive control of crystallization processes under batch‐to‐batch parametric drift
Authors: Zheng Yingzhe , Zhao Tianyi , Wang Xiaonan , Wu Zhe 
Published: June 2022

AbstractThis work considers a seeded fesoterodine fumarate (FF) cooling crystallization and presents the methodology and implementation of a real‐time machine learning modeling‐based predictive controller to handle batch‐to‐batch (B2B) parametric drift. Specifically, an autoencoder recurrent neural network‐based model predictive controller (AERNN‐MPC) is developed to optimize product yield, crystal size, and energy consumption while accounting for the physical constraints on cooling jacket temperature. Deviations in the kinetic parameters are considered in the closed‐loop simulations to account for the B2B parametric drift, and two error‐triggered online update mechanisms are proposed to address issues pertaining to the availability of real‐time crystal property measurements and are incorporated into the AERNN‐MPC to improve the model prediction accuracy. Closed‐loop simulation results demonstrate that the proposed AERNN‐MPC with online update, irrespective of the accessibility to real‐time crystal property data, achieves a desired closed‐loop performance in terms of maximizing product yield and minimizing energy consumption.
Hearing impairment and tinnitus among older construction workers employed at DOE facilities
Authors: Ringen Knut , Dement John M. , Quinn Patricia , Cloeren Marianne , Chen Anna , Cranford Kim , Haas Scott 
Published: June 2022

AbstractBackgroundFew studies have defined the risk of hearing impairment and tinnitus after retirement. This report measures hearing impairment and tinnitus prevalence among older construction trades workers.MethodsThe study cohort included 21,340 participants in a national medical screening program (www.btmed.org). Audiometric hearing impairment was classified according to the Global Burden of Disease Study. Tinnitus was determined by self‐report. An internal subcohort of nonconstruction trades workers served as a reference group. Stratified analyses and multivariate analyses were used to measure the prevalence of hearing impairment and tinnitus by age, sex, and job category.ResultsPrevalence of any hearing impairment was 55.2% (males, 57.7%; females, 26.8%) and increased rapidly with age. Construction trades workers were 40% more likely to have hearing impairment than the reference group. The overall prevalence of tinnitus was 46.52% and followed patterns similar to hearing impairment. Workers with hearing impairment were more likely to also have tinnitus, but tinnitus was frequently reported in the absence of measured hearing impairment.ConclusionsHearing impairment and tinnitus prevalence were much higher in this study than in previous research. A significant reason for the difference is that BTMed follows participants after they have retired. To draw conclusions about the risk for work‐related chronic diseases and disorders it is important to monitor workers through their lifetimes. Also, tinnitus by itself should be given greater significance. These findings reinforce the need to promote noise reduction and hearing conservation in construction.
Intrinsic Ability of the β‐Oxidation Pathway To Produce Bioactive Styrylpyrones
Authors: Huang Ying , Hoefgen Sandra , Gherlone Fabio , Valiante Vito 
Published: June 2022

AbstractNaturally occurring α‐pyrones with biological activities are mostly synthesised by polyketide synthases (PKSs) via iterative decarboxylative Claisen condensation steps. Remarkably, we found that some enzymes related to the fatty acid β‐oxidation pathway in Escherichia coli, namely the CoA ligase FadD and the thiolases FadA and FadI, can synthesise styrylpyrones with phenylpropionic acids in vivo. The two thiolases directly utilise acetyl‐CoA as an extender unit for carbon‐chain elongation through a non‐decarboxylative Claisen condensation, thus making the overall reaction more efficient in terms of carbon and energy consumption. Moreover, using a cell‐free approach, different styrylpyrones were synthesised in vitro. Finally, targeted feeding experiments led to the detection of styrylpyrones in other species, demonstrating that the intrinsic ability of the β‐oxidation pathway allows for the synthesis of such molecules in bacteria, revealing an important biological feature hitherto neglected.
Metal‐Free PAZE‐NH4X3⋅H2O Perovskite for Flexible Transparent X‐ray Detection and Imaging
Authors: Li Zhizai , Peng Guoqiang , Chen Huanyu , Shi Chang , Li ZhenHua , Jin Zhiwen 
Published: June 2022

AbstractMetal‐free perovskites are of interest for their chemical diversity and eco‐friendly properties, and recently have been used for X‐ray detection with superior carrier behavior. However, the size and shape complexity of the organic components results in difficulties in evaluating their stability in high‐energy radiation. Herein, we introduce multiple hydrogen‐bond metal‐free PAZE‐NH4X3⋅H2O perovskite, where H2O leads to more hydrogen bonds appearing between organic molecules and the perovskite host. As suggested by the theoretical calculations, multiple hydrogen bonds promote stiffness of the lattice, and increase the diffusion barrier to inhibit ionic migration. Then, low trap density, high μτ products and structural flexibility of PAZE‐NH4Br3⋅H2O give a flexible X‐ray detector with the highest sensitivity of 3708 μC Gyair−1 cm−2, ultra‐low detection limit of 0.19 μGyair−1 s−1 and superior spatial resolution of 5.0 lp mm−1.
Site‐Selective Coordination Assembly of Dynamic Metal‐Phenolic Networks
Authors: Xu Wanjun , Pan Shuaijun , Noble Benjamin B. , Chen Jingqu , Lin Zhixing , Han Yiyuan , Zhou Jiajing , Richardson Joseph J. , Yarovsky Irene , Caruso Frank 
Published: June 2022

AbstractCoordination states of metal‐organic materials are known to dictate their physicochemical properties and applications in various fields. However, understanding and controlling coordination sites in metal‐organic systems is challenging. Herein, we report the synthesis of site‐selective coordinated metal‐phenolic networks (MPNs) using flavonoids as coordination modulators. The site‐selective coordination was systematically investigated experimentally and computationally using ligands with one, two, and multiple different coordination sites. Tuning the multimodal Fe coordination with catechol, carbonyl, and hydroxyl groups within the MPNs enabled the facile engineering of diverse physicochemical properties including size, selective permeability (20–2000 kDa), and pH‐dependent degradability. This study expands our understanding of metal‐phenolic chemistry and provides new routes for the rational design of structurally tailorable coordination‐based materials.
Correlating Electrochemical Kinetic Parameters of Single LiNi1/3Mn1/3Co1/3O2 Particles with the Performance of Corresponding Porous Electrodes
Authors: Li Xu , Li Na , Zhang Kai‐Lun , Huang Jun , Jiao Shuqiang , Chen Hao‐Sen , Song Wei‐Li 
Published: June 2022

AbstractCharacterizing microscale single particles directly is requested for dissecting the performance‐limiting factors at the electrode scale. In this work, we build a single‐particle electrochemical setup and develop a physics‐based model for extracting the solid‐phase diffusion coefficient (Ds) and exchange current density (i0) from electrochemical impedance measurements. We find that the carbon coating on the LiNi1/3Mn1/3Co1/3O2 surface enhances i0. In addition, Ds and i0 decay irreversibly by ≈25 % and ≈10 %, respectively, when the cutoff charge voltage increases from 4.3 V to 4.4 V. Moreover, we correlate intrinsic parameters of single particles with the performance of porous electrodes. Porous electrodes assembled with active particles with higher i0 values deliver a greater capacity and faster capacity fade. The methods developed in this combined experimental and theoretical work can be useful in correlating the single‐particle scale and porous‐electrode scale for other similar systems.
In Operando Visualization and Dynamic Manipulation of Electrochemical Processes at the Electrode–Solution Interface
Authors: Xin Huaijia , Wang Hang , Zhang Wei , Chen Yu , Ji Qinghua , Zhang Gong , Liu Huijuan , Taylor André D. , Qu Jiuhui 
Published: June 2022

AbstractRevealing the dynamic processes at the electrode–solution interface is imperative for understanding electrochemical phenomena. Most techniques have been developed to sense the electrode surface changes at the nanoscale, but provide limited information on potential‐induced interfacial ion redistribution at the mesoscale. Herein, we present an in operando visualization method utilizing a microfabricated electrochemical cell combined with a laser scanning confocal microscope to observe high‐resolution and fast‐response interfacial processes. We report potential‐induced formation and transformation of the Nernst diffusion layer, demonstrating that pulsed voltage dynamically perturbs the interface and promotes ion diffusion. This provides an additional insight into developing a dynamic manipulation method to control the electrochemical process. Our novel visualization method can easily be applied to monitor different ionic behaviors in electrochemical reactions at the mesoscale.
A PEGylated Tin Porphyrin Complex for Electrocatalytic Proton Reduction: Mechanistic Insights into Main‐Group‐Element Catalysis
Authors: Chaturvedi Ashwin , McCarver Gavin A. , Sinha Soumalya , Hix Elijah G. , Vogiatzis Konstantinos D. , Jiang Jianbing 
Published: June 2022

AbstractElectrocatalytic proton reduction to form dihydrogen (H2) is an effective way to store energy in the form of chemical bonds. In this study, we validate the applicability of a main‐group‐element‐based tin porphyrin complex as an effective molecular electrocatalyst for proton reduction. A PEGylated Sn porphyrin complex (SnPEGP) displayed high activity (−4.6 mA cm−2at −1.7 V vs. Fc/Fc+) and high selectivity (H2Faradaic efficiency of 94 % at −1.7 V vs. Fc/Fc+) in acetonitrile (MeCN) with trifluoroacetic acid (TFA) as the proton source. The maximum turnover frequency (TOFmax) for H2production was obtained as 1099 s−1. Spectroelectrochemical analysis, in conjunction with quantum chemical calculations, suggest that proton reduction occurs via an electron‐chemical‐electron‐chemical (ECEC) pathway. This study reveals that the tin porphyrin catalyst serves as a novel platform for investigating molecular electrocatalytic reactions and provides new mechanistic insights into proton reduction.
Anionic N18 Macrocycles and a Polynitrogen Double Helix in Novel Yttrium Polynitrides YN6 and Y2N11 at 100 GPa
Authors: Aslandukov Andrey , Trybel Florian , Aslandukova Alena , Laniel Dominique , Fedotenko Timofey , Khandarkhaeva Saiana , Aprilis Georgios , Giacobbe Carlotta , Lawrence Bright Eleanor , Abrikosov Igor A. , Dubrovinsky Leonid , Dubrovinskaia Natalia 
Published: June 2022

AbstractTwo novel yttrium nitrides, YN6 and Y2N11, were synthesized by direct reaction between yttrium and nitrogen at 100 GPa and 3000 K in a laser‐heated diamond anvil cell. High‐pressure synchrotron single‐crystal X‐ray diffraction revealed that the crystal structures of YN6 and Y2N11 feature a unique organization of nitrogen atoms—a previously unknown anionic N18 macrocycle and a polynitrogen double helix, respectively. Density functional theory calculations, confirming the dynamical stability of the YN6 and Y2N11 compounds, show an anion‐driven metallicity, explaining the unusual bond orders in the polynitrogen units. As the charge state of the polynitrogen double helix in Y2N11 is different from that previously found in Hf2N11 and because N18 macrocycles have never been predicted or observed, their discovery significantly extends the chemistry of polynitrides.
Preparation of highly branched polyolefins by controlled chain‐walking olefin polymerization
Authors: Lei Tong , Ma Zhanshan , Liu Hongju , Wang Xiaoyue , Li Pei , Wang Feifei , Wu Weitai , Zhang Shaojie , Xu Guoyong , Wang Fuzhou 
Published: June 2022

AbstractA series of α‐diimine nickel(II) catalysts bearing different para‐substituted groups, {[(4‐R‐2,6‐Me2‐C6H2NC)2Nap]NiBr2, Nap: 1,8‐naphthdiyl; R = CHMePh (C1); R = CHPh2 (C2); R = tBu (C3); R = Br (C4); R = Me (C5)}, were synthesized and characterized. The molecular structures of C1 and C3 were determined by single crystal X‐ray analysis and show distorted tetrahedron geometry with C2v symmetry. The catalytic behaviors of these catalysts toward ethylene polymerization were investigated in the presence of diethylaluminum chloride (Et2AlCl) as a cocatalyst. The fast chain‐walking process in N,N‐chelated nickel system can be efficiently modulated via the introduction of para‐sec‐phenethyl substituents with improved thermal stability and catalytic performance. C1‐Et2AlCl exhibited high thermal stabilities and high activities reaching 4.61 × 106 g PE (mol Ni h)−1, producing highly branched amorphous polyethylenes (up to 143 branches/1000C) with high molecular weight and narrow polydispersity. This catalyst system conducted successfully conducted 2‐octene polymerization in comparison with the corresponding 1‐octene polymerization. The result demonstrated 2‐octene polymerized slower than 1‐octene and produced the highly‐branched poly(2‐octene)s with approximately 120 branches/1000C, including methyl, ethyl, amyl, and hexyl branches and a small amount of the long methylene sequence due to monomer isomerization.
No cuts, no buts: Satisfaction of first‐year medical students with a hybrid prosection‐based model for learning gross anatomy during the Covid‐19 pandemic
Authors: Schurr Alissa F. , Burg Brandon J. , Dickinson Edwin , Granatosky Michael C. 
Published: June 2022

AbstractFew realized the extent of disruption that the Covid‐19 global pandemic would impose upon higher anatomical education. While many institutions were obliged to adopt a fully‐remote online model, the New York Institute of Technology College of Osteopathic Medicine strove to develop a curriculum that would allow medical students to receive an in‐person anatomy education. A hybrid model that emphasized learning from prosected cadavers and self‐study stations was implemented, with the remainder of the students' time directed toward studying at home. Through an anonymous survey aimed at gleaning student satisfaction, this study demonstrates that this hybrid prosection‐based anatomy course aligned with student preferences both assuming no health risk (64.6% agreed) and given the current risk of contracting Covid‐19 (78.5% agreed). Generally, students felt that their education was equal to that of previous years (Likert scale = 3.24 ± 1.05), fostered an appreciation for anatomy (4.56 ± 0.59), promoted teamwork (4.13 ± 0.85), and prepared them for practical examinations (4.18 ± 0.74). Linear mixed‐effect models demonstrated that specific differences in results could be attributed to students' preconceived preferences toward student‐led dissections and to past medical training. Importantly, most students “disagree” (1.97 ± 1.00) that they were concerned about the risk of exposure to Covid‐19 during in‐person anatomy laboratory sessions. Areas requiring improvement were identified by the model, including the provision of access to the cadavers outside of the regularly scheduled laboratory times (3.89 ± 1.08). These findings should be utilized when designing future gross anatomy courses in response to the “new normal”.
Identification ofMycoplasma pneumoniaeby DNA‐modified gold nanomaterials in a colorimetric assay
Authors: Qin Dapeng , Gong Qiuping , Li Xin , Gao Yanping , Gopinath Subash C. B. , Chen Yeng , Yang Zehua 
Published: June 2022

AbstractMycoplasma pneumoniaeis a highly infectious bacterium and the major cause of pneumonia especially in school‐going children.Mycoplasma pneumoniaeaffects the respiratory tract, and 25% of patients experience health‐related problems. It is important to have a suitable method to detectM. pneumoniae, and gold nanoparticle (GNP)‐based colorimetric biosensing was used in this study to identify the specific target DNA forM. pneumoniae. The color of GNPs changes due to negatively charged GNPs in the presence of positively charged monovalent (Na+) ions from NaCl. This condition is reversed in the presence of a single‐stranded oligonucleotide, as it attracts GNPs but not in the presence of double‐stranded DNA. Single standard capture DNA was mixed with optimal target DNA that cannot be adsorbed by GNPs; under this condition, GNPs are not stabilized and aggregate at high ionic strength (from 100 mM). Without capture DNA, the GNPs that were stabilized by capture DNA (from 1 μM) became more stable under high ionic conditions and retaining their red color. The GNPs turned blue in the presence of target DNA at concentrations of 1 pM, and the GNPs retained a red color when there was no target in the solution. This method is useful for the simple, easy, and accurate identification ofM. pneumoniaetarget DNA at higher discrimination and without involving sophisticated equipment, and this method provides a diagnostic forM. pneumoniae.
Controlling Horizontal Growth of Zinc Platelet by OP‐10 Additive for Dendrite‐Free Aqueous Zinc‐Ion Batteries
Authors: Han Dong , Sun Tianjiang , Du Haihui , Wang Qiaoran , Zheng Shibing , Ma Tao , Tao Zhanliang 
Published: June 2022

AbstractRechargeable zinc‐ion batteries based on aqueous electrolytes are advantageous in terms of being environmentally friendly, safe and low cost. However, the problems of zinc dendrites and irreversible by‐products on the Zn metal surface during the charging and discharging processes limit its practical application. Herein, octenyl phenol polyoxyethylene ether‐10 (OP‐10) with an oxygen‐rich chain is used as an electrolyte additive to significantly improve the stability of the Zn anode. With an ultralow addition content of about 0.1 wt %, the OP‐10 can not only promote the uniform deposition of Zn2+ by adjusting the growth orientation of the (002) crystal plane of Zn but also alleviate side‐reaction on the metal surface. Thus, the Zn//Zn cell is stable for more than 800 hours at 1 mA cm−2, and the Zn//Cu cell has a Coulombic efficiency of up to 99.80 %. Further, the Zn//V2O5 ⋅ 1.6H2O battery exhibits outstanding cycle stability over 1000 cycles (maintain 92.12 % at 10 C), which is much superior to pure ZnSO4 electrolyte. OP‐10 not only reduces cost but also increases battery energy density, which is more in line with the modification idea of “small dose and large effect” of additives.