bluuebunny/crossref_metadata_2025 huggingface dataset:
Characteristics and Outcomes for Hospitalized Patients With Cutaneous T-Cell Lymphoma
Authors: Glinos George , Wei Grace , Nosewicz Jacob , Abdulla Farah , Chen Pei-Ling , Chung Catherine , Kaffenberger Benjamin H. , Querfeld Christiane , Shinohara Michi M. , Sokol Lubomir , Zain Jasmine , Kumar Ambuj , Seminario-Vidal Lucia
Published: January 2023

Importance

Cutaneous T-cell lymphoma (CTCL) is a group of rare, complex cutaneous malignant neoplasms associated with significant disease burden on patients and the health care system. Currently, the population of patients with CTCL admitted to the hospital remains largely uncharacterized and poorly understood.

Objective

To characterize the clinical characteristics, course of hospitalization, and mortality outcomes of an inpatient CTCL cohort.

Design, Setting, and Participants

This multicenter retrospective cohort study reviewed medical records for adult patients (age ≥18 years) with a CTCL diagnosis per National Comprehensive Cancer Network guidelines admitted for inpatient hospitalization at 5 US academic medical centers with inpatient dermatology consult services and CTCL clinics between August 2016 and August 2020.

Main Outcomes and Measures

Patient demographics, clinical history and findings, hospitalization courses, and mortality outcomes.

Results

A total of 79 hospitalized patients with CTCL were identified, including 52 (70.3%) men and 22 (29.7%) women, with a median (IQR) age at hospitalization of 62.9 (27-92) years. The majority of admitted patients with CTCL were White (65 patients [82.3%]), had disease classified as mycosis fungoides (48 patients [61.5%]), and had advanced-stage disease (≥IIB, 70 patients [89.7%]). Most hospitalizations were complicated by infection (45 patients [57.0%]) and required intravenous antibiotic therapy (45 patients [57.0%]). In-hospital mortality occurred in 6 patients (7.6%) and was associated with higher body mass index (36.5 vs 25.3), history of thromboembolic disease (50.0% vs 12.3%), and diagnosis of sepsis on admission (66.7% vs 20.5%). At 1-year postdischarge, 36 patients (49.3%) patients had died, and mortality was associated with history of solid organ cancers (27.8% vs 10.8%), wound care as the reason for dermatology consultation (58.3% vs 24.3%), and presence of large cell transformation (58.3% vs 22.9%).

Conclusions and Relevance

The findings of this cohort study improve the understanding of hospitalized patients with CTCL and lend valuable insight into identifying factors associated with both in-hospital and long-term mortality outcomes. This refined understanding of the inpatient CTCL population provides a foundation for larger, more robust studies to identify causal risk factors associated with mortality, development of prognostic scoring systems to estimate the probability of hospital mortality. Overall, the findings may prompt physicians caring for patients with CTCL to implement preventive strategies to diminish hospitalization and improve clinical management across this unique disease spectrum.
Comparison of Opioids Prescribed by Advanced Practice Clinicians vs Surgeons After Surgical Procedures in the US
Authors: Priest Caitlin R. , Waljee Jennifer F. , Bicket Mark C. , Hu Hsou-Mei , Chua Kao-Ping
Published: January 2023

Importance

Advanced practice clinicians (APCs), defined as nurse practitioners and physician assistants, are increasingly being incorporated into surgical teams. Despite this inclusion, there are no recent national data on the role of these clinicians in surgical opioid prescribing or the dosing of such prescriptions.

Objective

To calculate the proportion of surgical opioid prescriptions written by APCs and to compare the total and daily dosages of these prescriptions with those written by surgeons.

Design, Setting, and Participants

This cross-sectional study used the Optum’s De-Identified Clinformatics Data Mart, which contains deidentified claims from patients with private insurance and Medicare Advantage plans across the US. Adults and children who underwent 1 of 31 inpatient and outpatient surgical procedures from January 1, 2017, through November 30, 2019, were identified. The analysis was limited to procedures with 1 or more perioperative opioid prescriptions, defined as an opioid prescription dispensed within 3 days of the index date of surgery. Data were analyzed from April 1, 2021, to July 31, 2022.

Exposures

Prescriber specialty.

Main Outcomes and Measures

The outcome was the proportion of perioperative opioid prescriptions and refill prescriptions written by APCs. Linear regression was used to compare the total dosage of perioperative opioid prescriptions written by APCs vs surgeons measured in morphine milligram equivalents (MMEs). Models were adjusted for demographic characteristics, comorbidities, opioid-naive status, year of index date, hospitalization or observation status, surgical complications, and surgeon specialty. Analyses were conducted at the procedure level, and patients with multiple procedures were included.

Results

Analyses included 628 197 procedures for 581 387 patients (358 541 females [57.1%]; mean [SD] age, 56 [18] years). Overall, APCs wrote 119 266 (19.0%) of the 628 197 perioperative opioid prescriptions and 59 679 (25.1%) of the 237 740 refill prescriptions. Perioperative opioid prescriptions written by APCs had higher total dosages compared with those written by surgeons (adjusted difference, 40.0 MMEs; 95% CI, 31.3-48.7 MMEs). This difference persisted in a subgroup analysis limited to opioid-naïve patients (adjusted difference, 15.7 MMEs; 95% CI, 13.9-17.5 MMEs).

Conclusions and Relevance

In this cross-sectional analysis, one-fifth of perioperative opioid prescriptions and one-quarter of refill prescriptions were written by APCs. While surgeons wrote most perioperative opioid prescriptions that were intended for perioperative analgesia, higher total dosages from APCs suggest that opioid stewardship initiatives that support the role of APCs may be warranted.
2022 American College of Rheumatology Guideline for Vaccinations in Patients With Rheumatic and Musculoskeletal Diseases
Authors: Bass Anne R. , Chakravarty Eliza , Akl Elie A. , Bingham Clifton O. , Calabrese Leonard , Cappelli Laura C. , Johnson Sindhu R. , Imundo Lisa F. , Winthrop Kevin L. , Arasaratnam Reuben J. , Baden Lindsey R. , Berard Roberta , Bridges S. Louis , Cheah Jonathan T. L. , Curtis Jeffrey R. , Ferguson Polly J. , Hakkarinen Ida , Onel Karen B. , Schultz Grayson , Sivaraman Vidya , Smith Benjamin J. , Sparks Jeffrey A. , Vogel Tiphanie P. , Williams Eleanor Anderson , Calabrese Cassandra , Cunha Joanne S. , Fontanarosa Joann , Gillispie‐Taylor Miriah C. , Gkrouzman Elena , Iyer Priyanka , Lakin Kimberly S. , Legge Alexandra , Lo Mindy S. , Lockwood Megan M. , Sadun Rebecca E. , Singh Namrata , Sullivan Nancy , Tam Herman , Turgunbaev Marat , Turner Amy S. , Reston James
Published: January 2023

Objective

To provide evidence‐based recommendations on the use of vaccinations in children and adults with rheumatic and musculoskeletal diseases (RMDs).

Methods

This guideline follows American College of Rheumatology (ACR) policy guiding management of conflicts of interest and disclosures and the ACR guideline development process, which includes the Grading of Recommendations Assessment, Development and Evaluation (GRADE) methodology. It also adheres to the Appraisal of Guidelines for Research and Evaluation (AGREE) criteria. A core leadership team consisting of adult and pediatric rheumatologists and a guideline methodologist drafted clinical population, intervention, comparator, outcomes (PICO) questions. A review team performed a systematic literature review for the PICO questions, graded the quality of evidence, and produced an evidence report. An expert Voting Panel reviewed the evidence and formulated recommendations. The panel included adult and pediatric rheumatology providers, infectious diseases specialists, and patient representatives. Consensus required ≥70% agreement on both the direction and strength of each recommendation.

Results

This guideline includes expanded indications for some vaccines in patients with RMDs, as well as guidance on whether to hold immunosuppressive medications or delay vaccination to maximize vaccine immunogenicity and efficacy. Safe approaches to the use of live attenuated vaccines in patients taking immunosuppressive medications are also addressed. Most recommendations are conditional and had low quality of supporting evidence.

Conclusion

Application of these recommendations should consider patients’ individual risk for vaccine‐preventable illness and for disease flares, particularly if immunosuppressive medications are held for vaccination. Shared decision‐making with patients is encouraged in clinical settings.
High‐Efficiency Solid‐State Luminescence from Hydrophilic Carbon Dots with Aggregation‐Induced Emission Characteristics
Authors: Wan Zhijun , Li Yuemiao , Zhou Yizi , Peng Dongping , Zhang Xuejie , Zhuang Jianle , Lei Bingfu , Liu Yingliang , Hu Chaofan
Published: January 2023

Carbon dots (CDs) have excellent properties and have made great progress in synthesis and applications. However, it is still a challenge to realize convenient preparation and highly emissive solid‐state luminescence without the assistance of matrix. In this study, high‐efficiency hydrophilic yellow emissive CDs (Y‐CDs) with aggregation‐induced emission (AIE) characteristics are synthesized by a one‐pot microwave method. Y‐CDs show weak yellow emission with a photoluminescence quantum yield (PLQY) of 6.14% in aqueous solutions, but exhibit a significantly enhanced PLQY of 58.35% in the solid state. The AIE characteristic is confirmed by the phenomenon that the fluorescence emission intensity of Y‐CDs continues to increase with the gradual increase of the poor solvent fraction. The AIE phenomenon of Y‐CDs is derived from the suppression of surface piperazine groups motions and decrease of the non‐radiative rate, as is verified by a series of experiments. Finally, based on the high PLQY and AIE property, Y‐CDs are applied as a color‐converting layer on blue‐light‐emitting chips to fabricate white‐light‐emitting diodes with color coordinates of (0.31, 0.35), while Y‐CDs are also explored for their potential applications in anti‐counterfeiting, encryption and bioimaging.
Pre‐Protonated Vanadium Hexacyanoferrate for High Energy‐Power and Anti‐Freezing Proton Batteries
Authors: Dong Xiaoyu , Li Zhiwei , Luo Derong , Huang Kangsheng , Dou Hui , Zhang Xiaogang
Published: January 2023

Proton batteries have been considered as an innovative energy storage technology owing to their high safety and cost‐effectiveness. However, the development of fast‐charging proton batteries with high energy/power density is greatly limited by feasible material selection. Here, the pre‐protonated vanadium hexacyanoferrate (H‐VHCF) is developed as a proton cathode material to alleviate the capacity loss of proton‐free electrode materials during electrochemical tests. The pre‐protonation process realizes fast and long‐distance transport of protons by shortening diffusion path and reducing migration barriers. Benefitting from the enhanced hydrogen bonding network combined with dual redox reactions of V and Fe in protonated H‐VHCF cathode, a high energy density of 74 Wh kg−1 at 1.1 kW kg−1, and a maximum power density of 54 kW kg−1 at 65 Wh kg−1 is achieved for the asymmetric proton batteries coupling with MoO3/MXene anode. Proton transport and double oxidation‐reduction center are verified by theoretical calculations and ex situ experimental measurements. Considering the anti‐freezing availability of proton batteries, 82.5% of its initial capacity is maintained after 10000 cycles under −40 °C at 0.5 A g−1. As a proof‐of‐concept, flexible device fabricated by optimized electrodes and hydrogel electrolytes can power up a light‐emitting diode even under a bent state.
Intrinsically Low Lattice Thermal Conductivity and Anisotropic Thermoelectric Performance in In‐doped GeSb2Te4 Single Crystals
Authors: Chen Peng , Wu Hong , Zhang Bin , Zhou Zizhen , Zheng Sikang , Dai Lu , Huo Yufeng , Zhang De , Yan Yanci , Peng Kunling , Han Guang , Lu Xu , Zhou Xiaoyuan , Wang Guoyu
Published: January 2023

Layer‐structured GeSb2Te4 is a promising thermoelectric candidate, while its anisotropy of thermal and electrical transport properties is still not clear. In this study, Ge1–xInxSb2Te4 single crystals are grown by Bridgman method, and their anisotropic thermoelectric properties are systematically investigated. Lower electrical conductivity and higher Seebeck coefficient are observed in the c‐axis due to the higher effective mass in this direction. Intrinsically low lattice thermal conductivity is also observed in the c‐axis due to the weak chemical bonding and the strong lattice anharmonicity proved by density functional theory calculation. Indium doping introduces an impurity band in the bandgap of GeSb2Te4 and leads to the locally distorted density of states near the Fermi level, which contributes to enhanced Seebeck coefficient and improved power factor. Ultimately, a peak zT value of 1 at 673 K and an average zT value of 0.68 within 323–773 K are obtained in Ge0.93In0.07Sb2Te4 along the c‐axis direction, which are 54% and 79% higher than that of the pristine GeSb2Te4 single crystal, respectively. This study clarified the origin of intrinsic low lattice thermal conductivity and anisotropy transport properties in GeSb2Te4, and shed light on the performance optimization of other layered thermoelectric materials.
A Thermodynamic Cycle‐Based Electrochemical Windows Database of 308 Electrolyte Solvents for Rechargeable Batteries
Authors: Wang Da , He Tingting , Wang Aiping , Guo Kai , Avdeev Maxim , Ouyang Chuying , Chen Liquan , Shi Siqi
Published: January 2023

Rational design of wide electrochemical window (ECW) electrolytes to pair with high‐voltage cathodes is an emerging trend to push the energy density limits of current rechargeable batteries. Traditional single‐electronic/gas‐phase approximation‐based methods (e.g., highest occupied molecular orbital/lowest unoccupied molecular orbital) are increasingly recognized to have large deviations from experiments when predicting ECWs of electrolytes involving complex solvent interactions. Specifically, by examining available experimental ECWs of 68 electrolyte solvents extracted from ≈140 000 literature sources, which are conventionally divided into five functional‐group categories (covering commonly used carbonate‐based ethylene carbonate (EC)/propylene carbonate (PC) and ether‐based tetrahydrofuran), it is found that mean‐absolute‐errors (MAE) of traditional methods reach up to 3.25 V. Herein, a thermodynamic cycle‐based ECW prediction approach is proposed including two long‐term overlooked reorganization‐energy and solvation‐energy corrections, each of which can be quantified by two geometric descriptors (λ and ΔGsol), reducing MAE below 0.68 V. Following this, a database containing ECWs for 308 electrolyte solvents, obtained by traversing single functional‐group substitutions, is established. Furthermore, two omitted solvents with ECWs over 6.00 V and excellent structural stabilities (bond‐length change < 0.10 Å during redox process) are retrieved by stepwise screening of structural/electronic parallel properties. This study demonstrates the benefits of improving ECW prediction accuracy and accumulating descriptors to accelerate rapid screening of superior battery electrolytes.
Transparent High‐Performance Supramolecular Plastics Operating in All‐Weather Environments
Authors: Chen Jiaoyang , Ma Yuhong , Chen Tao , Du Yingjie , Xu Jianhua , Wang Dong , Yang Jing , Hu Po , Jing Jiajie , Yao Bowen , Fu Jiajun
Published: January 2023

Supramolecular plastics (SMPs) can be made mechanically robust, repairable, and recyclable, rendering themselves promising alternatives to their conventional predecessors to address environmental concerns. However, dense accumulations of noncovalent bonds generally lead to mechanical brittleness as well as intolerance toward heat and moisture. To resolve this issue, a simple strategy of preparing high‐performance SMP by constructing highly dense, but irregular hydrogen‐bond networks with hierarchical structures is proposed. The resultant SMP exhibits an outstanding combination of good comprehensive mechanical properties (high stiffness, strength, and toughness with ductile failure when fracturing), excellent dynamic behaviors (repairability and recyclability), and high tolerances toward moisture and high temperatures (as high as 90 °C). Additionally, the SMP also shows a high dielectric constant, exhibiting great potential for applications such as healable flexible touch screens and energy storage. Last, through structure characterizations and molecular dynamic simulation, this study provides a fundamental insight into the mechanism behind such high‐performances from nano‐ to micro‐scales, which is expected to inspire the design of a wide range of other SMPs that use different chemistries.
Efficient, Color‐Stable, and Long‐Lived White Organic Light‐Emitting Diodes Utilizing Phosphorescent Molecular Aggregates
Authors: Ameri Lydia , Cao Linyu , Tan Xinqiang , Li Jian
Published: January 2023

Highly efficient and stable single‐stack hybrid white organic light‐emitting diode (WOLED) devices are developed using two emissive layers: one with amber‐colored phosphorescent molecular‐aggregate emission from the Pd(II) complex, Pd(II) 7‐(3‐(pyridine‐2‐yl‐κN)phenoxy‐κC)(benzo‐κC)([c]benzo[4,5]imidazo‐κN)[1,2‐a][1,5]naphthyridine, Pd3O8‐Py5, and the other with blue fluorescence emission. An optimized device structure achieves high color stability under various current densities, an external quantum efficiency (EQE) of 45.5%, a power efficiency of 97.4 Lm W−1, and an estimated LT95 (operational time to 95% of the initial luminance) of 50 744 h at an initial luminance of 1000 cd m−2.
Towards Translation of PqsR Inverse Agonists: From In Vitro Efficacy Optimization to In Vivo Proof‐of‐Principle
Authors: Hamed Mostafa M. , Abdelsamie Ahmed S. , Rox Katharina , Schütz Christian , Kany Andreas M. , Röhrig Teresa , Schmelz Stefan , Blankenfeldt Wulf , Arce‐Rodriguez Alejandro , Borrero‐de Acuña José Manuel , Jahn Dieter , Rademacher Jessica , Ringshausen Felix C. , Cramer Nina , Tümmler Burkhard , Hirsch Anna K. H. , Hartmann Rolf W. , Empting Martin
Published: January 2023

Pseudomonas aeruginosa (PA) is an opportunistic human pathogen, which is involved in a wide range of dangerous infections. It develops alarming resistances toward antibiotic treatment. Therefore, alternative strategies, which suppress pathogenicity or synergize with antibiotic treatments are in great need to combat these infections more effectively. One promising approach is to disarm the bacteria by interfering with their quorum sensing (QS) system, which regulates the release of various virulence factors as well as biofilm formation. Herein, this work reports the rational design, optimization, and in‐depth profiling of a new class of Pseudomonas quinolone signaling receptor (PqsR) inverse agonists. The resulting frontrunner compound features a pyrimidine‐based scaffold, high in vitro and in vivo efficacy, favorable pharmacokinetics as well as clean safety pharmacology characteristics, which provide the basis for potential pulmonary as well as systemic routes of administration. An X‐ray crystal structure in complex with PqsR facilitated further structure‐guided lead optimization. The compound demonstrates potent pyocyanin suppression, synergizes with aminoglycoside antibiotic tobramycin against PA biofilms, and is active against a panel of clinical isolates from bronchiectasis patients. Importantly, this in vitro effect translated into in vivo efficacy in a neutropenic thigh infection model in mice providing a proof‐of‐principle for adjunctive treatment scenarios.
A Zinc‐ and Calcium‐Rich Lysosomal Nanoreactor Rescues Monocyte/Macrophage Dysfunction under Sepsis
Authors: Zhao Qin , Gong Zijian , Wang Jiaolong , Fu Liangliang , Zhang Jing , Wang Can , Miron Richard J. , Yuan Quan , Zhang Yufeng
Published: January 2023

Sepsis is a dysregulation of the immune response to pathogens and has high morbidity and mortality worldwide. However, the unclear mapping and course of dysregulated immune cells currently hinders the development of advanced therapeutic strategies to treat sepsis. Here, evidence is provided using single‐cell RNA sequencing from peripheral blood mononuclear cells in sepsis that pathogens attacking monocytes/macrophages disrupt their immune function. The results reveal an enormous decline in monocytes/macrophages in sepsis and chart the evolution of their impaired phagocytosis (Pha) capabilities. Inspired by these findings, nanoparticles, named “Alpha‐MOFs,” are developed that target dysfunctional monocytes/macrophages to actively (A) lift (L) Pha by the release of lysosome‐sensitive ions from a mineralized metal–organic framework (MOF). Alpha‐MOFs have good stability and biosafety in peripheral blood and efficiently targeted monocytes/macrophages. They also release calcium and zinc ions into monocyte/macrophage lysosomes to promote the Pha and degradation of bacteria. Taken together, these results suggest that Alpha‐MOFs rescue monocytes/macrophages dysfunction and effectively improve their survival rate during sepsis.
A Multifunctional Integrated Metal‐Free MRI Agent for Early Diagnosis of Oxidative Stress in a Mouse Model of Diabetic Cardiomyopathy
Authors: Nie Zhuang , Zhang Kun , Chen Xinyu , Wang Jingxin , Gao Huile , Zheng Bingwen , Wu Qihong , Guo Yingkun , Liu Xiangyang , Wang Xu
Published: January 2023

Reactive oxygen species (ROS) are closely associated with the progression of diabetic cardiomyopathy (DCM) and can be regarded as one of its early biomarkers. Magnetic resonance imaging (MRI) is emerging as a powerful tool for the detection of cardiac abnormalities, but the sensitive and direct ROS‐response MRI probe remains to be developed. This restricts the early diagnosis of DCM and prevents timely clinical interventions, resulting in serious and irreversible pathophysiological abnormalities. Herein, a novel ROS‐response contrast‐enhanced MRI nanoprobe (RCMN) is developed by multi‐functionalizing fluorinated carbon nanosheets (FCNs) with multi‐hydroxyl and 2,2,6,6‐tetramethylpiperidin‐1‐oxyl groups. RCMNs capture ROS and then gather in the heart provisionally, which triggers MRI signal changes to realize the in vivo detection of ROS. In contrast to the clinical MRI agents, the cardiac abnormalities of disease mice is detected 8 weeks in advance with the assistance of RCMNs, which greatly advances the diagnostic window of DCM. To the best of the knowledge, this is the first ROS‐response metal‐free T2‐weighted MRI probe for the early diagnosis of DCM mice model. Furthermore, RCMNs can timely scavenge excessively produced ROS to alleviate oxidative stress.
Impact of Charge Carrier Injection/Extraction Performances in Low‐Dimension PEDOT:PSS Organic Electrochemical Transistors
Authors: Sych Galyna , Rannou Patrice , Jullien‐Palletier Maxime , Sadki Saïd , Bonnassieux Yvan , Sanaur Sébastien
Published: January 2023

Organic electrochemical transistors (OECT) are gaining momentum in future applications of biosensors and bioelectronics. Nonetheless, contact (or series) resistances (RS/D) remain underexplored, even though physical processes between the source/drain electrodes and organic mixed ionic‐electron conductors (OMIECs) drive a substantial part of their performances. To address this shortcoming, in this study, low‐dimension OECTs featuring 2 µm‐long poly(3,4‐ethylenedioxythiophene) and polystyrene sulfonate acid (PEDOT:PSS) channel are explored. Normalized contact resistances (RS/D⋅W) values as low as 1.4 W cm are obtained. It is observed that channel PEDOT:PSS thickness is not detrimental to RS/D but is impacting the cut‐off frequency. A figure‐of‐merit (h) expressing the charge‐carrier injection (or extraction, respectively) efficiency shows that planar depletion‐mode OECTs are not contact‐limited up to L = 30 µm channel length. Finally, an unprecedented approach that highlight the importance of optimizing the micro‐fabrication technologies is shown, by decreasing the contact overlap length, according to OMIECs physicochemical contact properties. Indeed, a transfer‐length method coupled to a current‐crowding model allow to fully understand the behavior of low‐dimension PEDOT:PSS OECTs and next, to optimize its circuits design. This is paving the way toward the development of OECTs‐based integrated circuits with faster switching speed, broadening further their scopes and future use as advanced bioelectronics platforms.
The imperative to support Black youths in resisting low and limiting expectations
Authors: Debrosse Régine , Touré Kapo Leslie , Métayer Karen
Published: January 2023

Harmful narratives circulate about Black youths in North America. Deficit narratives portray them, their culture, and their communities as problems, narratives about policing encourage their control and punishment, color‐evasive narratives ignore how race shapes their experiences, and essentialist narratives erase their distinct and often intersectional experiences by presenting them as monolithic. Community psychology and allied fields do not escape these trends, which in turn infuse practice, research, and teaching involving Black youths. The present paper highlights four principles that community psychology and allied fields can adopt to support Black youths in resisting these negative and narrow narratives. They are: (1) emphasizing Black youths' and Black communities' strengths, (2) supporting their agency, (3) adopting culturally relevant practices, and (4) developing critical consciousness through reflections on and deconstruction of these narratives. We hope that the reflections shared in this paper will expand the perspectives infused by researchers and practitioners in community psychology, social work, urban studies, and allied fields who work with Black youths.
Atrophy of the Cholinergic Basal Forebrain can Detect Presynaptic Cholinergic Loss in Parkinson's Disease
Authors: Ray Nicola J. , Kanel Prabesh , Bohnen Nicolaas I.
Published: January 2023

Objectives

Structural imaging of the cholinergic basal forebrain may provide a biomarker for cholinergic system integrity that can be used in motor and non‐motor outcome studies in Parkinson's disease. However, no prior studies have validated these structural metrics with cholinergic nerve terminal in vivo imaging in Parkinson's disease. Here, we correlate cholinergic basal forebrain morphometry with the topography of vesicular acetylcholine transporter in a large Parkinson's sample.

Methods

[18F]‐Fluoroethoxybenzovesamicol vesicular acetylcholine transporter positron emission tomography was carried out in 101 non‐demented people with Parkinson's (76.24% male, mean age 67.6 ± 7.72 years, disease duration 5.7 ± 4.4 years). Subregional cholinergic basal forebrain volumes were measured using magnetic resonance imaging morphometry. Relationships were assessed via volume‐of‐interest based correlation analysis.

Results

Subregional volumes of the cholinergic basal forebrain predicted cholinergic nerve terminal loss, with most robust correlations occurring between the posterior cholinergic basal forebrain and temporofrontal, insula, cingulum, and hippocampal regions, and with modest correlations in parieto‐occipital regions. Hippocampal correlations were not limited to the cholinergic basal forebrain subregion Ch1‐2. Correlations were also observed in the striatum, thalamus, and brainstem.

Interpretation

Cholinergic basal forebrain morphometry is a robust predictor of regional cerebral vesicular acetylcholine transporter bindings, especially in the anterior brain. The relative lack of correlation between parieto‐occipital binding and basal forebrain volumes may reflect the presence of more diffuse synaptopathy in the posterior cortex due to etiologies that extend well beyond the cholinergic system. ANN NEUROL 2023;93:991–998
Stepwise Engineering the Pore Aperture of a Cage‐like MOF for the Efficient Separation of Isomeric C4 Paraffins under Humid Conditions
Authors: Wang Lu , Xue Wenjuan , Zhu Hejin , Guo Xiangyu , Huang Hongliang , Zhong Chongli
Published: January 2023

The separation of isomeric C4 paraffins is an important task in the petrochemical industry, while current adsorbents undergo a trade‐off relationship between selectivity and adsorption capacity. In this work, the pore aperture of a cage‐like Zn‐bzc (bzc=pyrazole‐4‐carboxylic acid) is tuned by the stepwise installation methyl groups on its narrow aperture to achieve both molecular‐sieving separation and high n‐C4H10 uptake. Notably, the resulting Zn‐bzc‐2CH3 (bzc‐2CH3=3,5‐dimethylpyrazole‐4‐carboxylic acid) can sensitively capture n‐C4H10 and exclude iso‐C4H10, affording molecular‐sieving for n‐C4H10/iso‐C4H10 separation and high n‐C4H10 adsorption capacity (54.3 cm3 g−1). Breakthrough tests prove n‐C4H10/iso‐C4H10 can be efficiently separated and high‐purity iso‐C4H10 (99.99 %) can be collected. Importantly, the hydrophobic microenvironment created by the introduced methyl groups greatly improves the stability of Zn‐bzc and significantly eliminates the negative effect of water vapor on gas separation under humid conditions, indicating Zn‐bzc‐2CH3 is a new benchmark adsorbent for n‐C4H10/iso‐C4H10 separation.
Electrochemical Reactivation of Dead Li2S for Li−S Batteries in Non‐Solvating Electrolytes
Authors: Qi Xiaoqun , Yang Fengyi , Sang Pengfei , Zhu Zhenglu , Jin Xiaoyu , Pan Yujun , Ji Jie , Jiang Ruining , Du Haoran , Ji Yongsheng , Fu Yongzhu , Qie Long , Huang Yunhui
Published: January 2023

The use of non‐solvating, or as‐called sparingly‐solvating, electrolytes (NSEs), is regarded as one of the most promising solutions to the obstacles to the practical applications of Li−S batteries. However, it remains a puzzle that long‐life Li−S batteries have rarely, if not never, been reported with NSEs, despite their good compatibility with Li anode. Here, we find the capacity decay of Li−S batteries in NSEs is mainly due to the accumulation of the dead Li2S at the cathode side, rather than the degradation of the anodes or electrolytes. Based on this understanding, we propose an electrochemical strategy to reactivate the accumulated Li2S and revive the dead Li−S batteries in NSEs. With such a facile approach, Li−S batteries with significantly improved cycling stability and accelerated dynamics are achieved with diglyme‐, acetonitrile‐ and 1,2‐dimethoxyethane‐based NSEs. Our finding may rebuild the confidence in exploiting non‐solvating Li−S batteries with practical competitiveness.
Isolation of an Annulated 1,4‐Distibabenzene Diradicaloid
Authors: Steffenfauseweh Henric , Rottschäfer Dennis , Vishnevskiy Yury V. , Neumann Beate , Stammler Hans‐Georg , Szczepanik Dariusz W. , Ghadwal Rajendra S.
Published: January 2023

The first 1,4‐distibabenzene‐1,4‐diide compound [(ADC)Sb]2 (5) based on an anionic dicarbene (ADC) (ADC=PhC{N(Dipp)C}2, Dipp=2,6‐iPr2C6H3) is reported as a bordeaux‐red solid. Compound 5, featuring a central six‐membered C4Sb2 ring with formally SbI atoms may be regarded as a base‐stabilized cyclic bis‐stibinidene in which each of the Sb atoms bears two lone‐pairs of electrons. 5 undergoes 2 e‐oxidation with Ph3C[B(C6F5)4] to afford [(ADC)Sb]2[B(C6F5)4]2 (6) as a brick‐red solid. Each of the Sb atoms of 6 has an unpaired electron and a lone‐pair. The broken‐symmetry open‐shell singlet diradical solution for (6)2+ is calculated to be 2.13 kcal mol−1 more stable than the closed‐shell singlet. The diradical character of (6)2+ according to SS‐CASSCF (state‐specific complete active space self‐consistent field) and UHF (unrestricted Hartree‐Fock) methods amounts to 36 % and 39 %, respectively. Treatments of 6 with (PhE)2 yield [(ADC)Sb(EPh)]2[B(C6F5)4]2 (7‐E) (E=S or Se). Reaction of 5 with (cod)Mo(CO)4 affords [(ADC)Sb]2Mo(CO)4 (8).
Transient and Dissipative Host–Guest Hydrogels Regulated by Consumption of a Reactive Chemical Fuel
Authors: Su Bo , Chi Teng , Ye Zhou , Xiang Yuanhui , Dong Ping , Liu Dongping , Addonizio Christopher J. , Webber Matthew J.
Published: January 2023

The transient self‐assembly of molecules under the direction of a consumable fuel source is fundamental to biological processes such as cellular organization and motility. Such biomolecular assemblies exist in an out‐of‐equilibrium state, requiring continuous consumption of high energy molecules. At the same time, the creation of bioinspired supramolecular hydrogels has traditionally focused on associations occurring at the thermodynamic equilibrium state. Here, hydrogels are prepared from cucurbit[7]uril host–guest supramolecular interactions through transient physical crosslinking driven by the consumption of a reactive chemical fuel. Upon action from this fuel, the affinity and dynamics of CB[7]–guest recognition are altered. In this way, the lifetime of transient hydrogel formation and the dynamic modulus obtained are governed by fuel consumption, rather than being directed by equilibrium complex formation.
Optimized Sieving Effect for Ethanol/Water Separation by Ultramicroporous MOFs
Authors: Zheng Xiaoqing , Chen Liangji , Zhang Hao , Yao Zizhu , Yang Yisi , Xiang Fahui , Li Yunbin , Xiang  Shengchang , Zhang Zhangjing , Chen Banglin
Published: January 2023

High‐purity ethanol is a promising renewable energy resource, however separating ethanol from trace amount of water is extremely challenging. Herein, two ultramicroporous MOFs (UTSA‐280 and Co‐squarate) were used as adsorbents. A prominent water adsorption and a negligible ethanol adsorption identify perfect sieving effect on both MOFs. Co‐squarate exhibits a surprising water adsorption capacity at low pressure that surpassing the reported MOFs. Single crystal X‐ray diffraction and theoretical calculations reveal that such prominent performance of Co‐squarate derives from the optimized sieving effect through pore structure adjustment. Co‐squarate with larger rhombohedral channel is suitable for zigzag water location, resulting in reinforced guest‐guest and guest‐framework interactions. Ultrapure ethanol (99.9 %) can be obtained directly by ethanol/water mixed vapor breaking through the columns packed with Co‐squarate, contributing to a potential for fuel‐grade ethanol purification.
Synthesis and characterization of new bio‐based nonmigrating poly(vinyl chloride) plasticizers
Authors: Nosal‐Kovalenko Hanna , Krasuska Agata , Warzała Marek , Robaszkiewicz Andrzej , Ledniowska Kerstin , Stańczyk Dorota , Hordyjewicz‐Baran Zofia , Bartoszewicz Maria , Semeniuk Izabela , Zarębska Magdalena
Published: January 2023

This study describes the synthesis of new nonmigrating PVC plasticizers based on oleic acid as the main raw material. Their structures and production routes were planned to ensure that the resulting synthesis by‐products could also act as PVC plasticizers. All received Esters 1, 2, and 3 revealed plasticizing effect on PVC. Achieved results of elongation at break (260%) for PVC composites with Ester 2 (C11) and Ester 3 (C14) were comparable to those recorded for diisononyl phthalate (DINP) and dioctyl terephthalate (DOTP) (C2 and C5), and only 15% lower for Ester 1 (C8). As intended, the developed plasticizers showed high resistance to migration. The Ester 3 proved to be an extremely migration‐resistant bio‐based plasticizer, due to its high oxirane ring content and large molecule size. After 28 days of survey, the loss of this plasticizer from the PVC sample with 50 PHR of plasticizer was 4.7%, which is nearly 80% lower compared to DINP. Ester 2 was slightly less resistant to migration—with 14.1% mass loss observed after 28 days, which can be attributed to the smaller size of its molecules. Additionally, PVC composites containing Esters 1, 2, and 3 exhibited higher thermal stability compared to composites with DINP or DOTP. T10% for PVC composites with 60 PHR of Esters 1, 2, and 3 was recorded at 286.2°C, 282.8°C, and 286.4°C, respectively. Thus, the developed esters can act not only as PVC plasticizers, but also as thermal stabilizers.
Unique graphene‐carbon black hybrid nanofiller by a micromechanical cleavage technique as a reinforcing agent in elastomers: Fundamental and experimental studies
Authors: Roy Amrita , Kar Saptarshi , Ghosal Ranjan , Mukhopadhyay Rabindra , Naskar Kinsuk , Bhowmick Anil K.
Published: January 2023

In this work, a synthetic technique was developed which effected delamination of graphite into graphene with simultaneous disaggregation of carbon black clusters and formation of secondary attachment between the two. Styrene butadiene rubber nanocomposite with this hybrid filler exhibited substantial reinforcement in the mechanical properties, wear resistance and rubber‐filler interactions. The hybrid nanofiller was superior to conventional carbon black, imparting 57% increase in tensile strength of the nanocomposite. The composite with the hybrid filler also exhibited improved modulus and traction. A detailed analysis of mechanism of reinforcement by the hybrid filler is proposed by the computation of root mean square end‐to‐end network chain distance and the lateral tube dimension employing the entangled‐bound‐rubber‐tube (EBT) model. This neoteric hybrid nanofiller overcame the so‐called dispersibility issues and could be exploited as a part of replacement of carbon black, a synthetic material from fossil fuel by sustainable natural filler.
The improved low‐field electro‐actuation of dielectric elastomer composites regulated by entirely‐inorganicBaTiO3@TiO2core‐shell construction
Authors: Wei Xiuping , Zhao Hang , Yin Lei , Miao Zhiying , Ding Xiaoyu , Wang Qian , Bai Jinbo
Published: January 2023

Dielectric elastomer (DE) as an important electro‐active polymer (EAP), is capable of providing a large elastic deformation under an external electric field. However, the excellent electro‐actuated performance is usually obtained under high electric fields, which greatly limits the practical application range of DE, especially in the field of in vivo organisms. Thus, it is essential to make a reasonable structural regulation to achieve an effectively improved electro‐actuation of DE materials under low driving electric fields. Herein, a typical BaTiO3@TiO2entirely‐inorganic core‐shell construction was prepared through the micro‐emulsion method. Meanwhile, a series of polydimethylsiloxane (PDMS)‐based DE composites incorporated with different fractions of BaTiO3@TiO2were synthesized by solution blending and compression molding. The BaTiO3@TiO2core‐shell construction endows DE composites with an enlarged heterogeneous interface and enhanced interfacial polarization synchronously, which is also benefit to maintain the flexibility of DE materials. The buffer effect offered by TiO2shell is helpful to alleviate the local electric field concentration at the fillers‐matrix interface in DE when being withstood an exponentially‐growing electric field. Specifically, the maximum electro‐actuated strain of 21% under a low electric field (40 V·μm−1) is obtained from the DE composite filled with 4 wt% BaTiO3@TiO2, which is 290% higher than that of pristine PDMS (5.38% at 40 V·μm−1). It is shown that the well‐designed inorganic core‐shell construction can effectively improve the electromechanical conversion capability of DE composites. This study provides a promising approach to obtain an optimized electro‐actuation under low electric fields.
Synergetic improvement of the thermal conductivity and interlaminar fracture toughness of carbon fiber/epoxy composites by interleaving BN@ZnO particles
Authors: Gu Guohua , Zhang Yuqi , Dong Shuhua , Wei Chuncheng , Lin Zhitao , Shen Hongwang , Meng Fantao
Published: January 2023

Synergetic improvement of the thermal conductivity and interlaminar fracture toughness of carbon fiber/epoxy resin composites (CF/EP) is a challenging research job. In this work, hexagonal boron nitride coated ZnO (BN@ZnO) particles were firstly prepared by sol–gel method and BN@ZnO composite laminates were manufactured by mold pressing process. X‐ray diffraction, x‐ray electron spectroscopy and scanning electron microscopy were used to analyze the structure, chemical components and morphology of the BN@ZnO and composite laminates. The effects of BN@ZnO on the impact strength, model II interlaminar fracture toughness (GIIC) and thermal conductivity of composite laminates are investigated. The results show that the interlaminar fracture toughness and thermal conductivity of composite laminates are synergistically enhanced owing to the introduction of hybrid fillers with different dimensions and morphology. The thermal conductivity of the 10 wt% BN@ZnO coated composite laminates is increased by 78% and 90% at 25 and 100°C, respectively. The mechanical properties of composite laminates are enhanced. The model II interlaminar fracture toughness of 2 wt% BN@ZnO composite laminates is 15.4% higher than pure laminate. This work is of significance to realize the structural and functional integration of composite materials.
Synthesis and characterization of multi‐ionic block copolymers and blended membranes for chemical protective clothing applications
Authors: Tarazona Karen Barrios , Ramos‐Rivera Gilberto , Suleiman David
Published: January 2023

This study discusses the synthesis of sulfonated amine block copolymers and the effect of multiple ionic domains and counter‐ion substitution on polymeric membranes' morphology and transport properties for chemical protective clothing (CPC) applications. The monomers 2‐(tert‐butylamino) ethyl methacrylate, 2‐ethoxy ethyl methacrylate, and styrene were used to prepare the block copolymers by atom transfer radical polymerization (ATRP). The copolymers were then sulfonated by chemical grafting with pendants sulfobutyl groups onto the polymer structure. Properties of the resulting membranes were evaluated as a function of block composition, incorporation of sulfonic groups, and counter‐ion substitution. Blended membranes with sulfonated poly(styrene‐isobutylene‐styrene) (SIBS) were also studied. A series of materials characterization techniques (e.g., Fourier‐transform infrared spectroscopy [FT‐IR], thermogravimetric analysis [TGA], atomic force microscopy [AFM], Small‐angle X‐ray scattering [SAXS]/wide‐angle X‐ray scattering [WAXS]) were performed to describe the changes to the membranes. The results indicate that synthesized copolymers lack phase segregation mainly because of a low sulfonation on the central amine block, leading the material to have a low Water/DMMP selectivity. As the sulfonated copolymers were blended with SIBS 75, the breathability of the membranes were enhanced 1.5 times, and almost all candidates achieved the water vapor transport rate limit of 1500 g m−2 day−1. Finally, the better‐found candidates for DMMP CPC were Mg2+ membranes, achieving selectivity between 20 and 90 range.
Lung abscess due to Streptococcus intermedius associated with SARS CoV‐2 infection in pregnancy: Unusual presentation and complication of a commensal bacteria during pregnancy
Authors: Bueno Cristian Orlando Porras , Trillos Sharon Julieth González , Rosales Diana Jimena Cano , García Edgar Augusto Bernal
Published: January 2023

Streptococcus intermedius is a commensal bacterium reported in a few cases as the causative agent of brain and lung abscesses, pneumonia, and endocarditis. Lung abscesses due to Streptococcus intermedius are rare, especially in pregnancy. We describe the first case of lung abscess due to Streptococcus intermedius in a pregnant woman.
High‐Titer Bio‐Styrene Production Afforded by Whole‐Cell Cascade Biotransformation
Authors: Messiha Hanan L. , Scrutton Nigel S. , Leys David
Published: January 2023

Biosynthetic routes based on cost‐efficient, eco‐friendly, and sustainable platforms for compounds such as styrene are urgently needed. The biosynthesis of styrene from L‐phenylalanine (L‐Phe) via trans‐cinnamate has long been established, but styrene toxicity limits yields. This study demonstrates that whole‐cell cascade biotransformation employing an E. coli consortium expressing respectively phenylalanine ammonia‐lyase and ferulic acid decarboxylase negates both the issue of styrene toxicity and the need for enzyme purification. Using resting or lyophilised cells, efficient conversion of L‐Phe to styrene (up to ∼24 g/L) is readily achieved and combined with robust extraction methods. The use of L‐Phe enriched biomass with the E. coli consortium yields an equally robust and rapid production and isolation of renewable styrene. This study establishes an improved strategy for industrial bio‐production of styrene, and by extension other toxic or reactive chemicals from corresponding bio‐compatible precursors.
Influence of Support Material on the Structural Evolution of Copper during Electrochemical CO2 Reduction
Authors: Koh Ezra S. , Geiger Simon , Gunnarson Alexander , Imhof Timo , Meyer Gregor M. , Paciok Paul , Etzold Bastian J. M. , Rose Marcus , Schüth Ferdi , Ledendecker Marc
Published: January 2023

The copper‐catalyzed electrochemical CO2 reduction reaction represents an elegant pathway to reduce CO2 emissions while producing a wide range of valuable hydrocarbons. The selectivity for these products depends strongly on the structure and morphology of the copper catalyst. However, continued deactivation during catalysis alters the obtained product spectrum. In this work, we report on the stabilizing effect of three different carbon supports with unique pore structures. The influence of pore structure on stability and selectivity was examined by high‐angle annular dark field scanning transmission electron microscopy and gas chromatography measurements in a micro‐flow cell. Supporting particles into confined space was found to increase the barrier for particle agglomeration during 20 h of chronopotentiometry measurements at 100 mA cm−2 resembling long‐term CO2 reduction conditions. We propose a catalyst design preventing coalescence and agglomeration in harsh electrochemical reaction conditions, exemplarily demonstrated for the electrocatalytic CO2 reduction. With this work, we provide important insights into the design of stable CO2 electrocatalysts that can potentially be applied to a wide range of applications.
Metal organic polymers with dual catalytic sites for oxygen reduction and oxygen evolution reactions
Authors: Liu Sijia , Liu Minghao , Li Xuewen , Yang Shuai , Miao Qiyang , Xu Qing , Zeng Gaofeng
Published: January 2023

Metal–organic frameworks and covalent organic frameworks have been widely employed in electrochemical catalysis owing to their designable skeletons, controllable porosities, and well‐defined catalytic centers. However, the poor chemical stability and low electron conductivity limited their activity, and single‐functional sites in these frameworks hindered them to show multifunctional roles in catalytic systems. Herein, we have constructed novel metal organic polymers (Co‐HAT‐CN and Ni‐HAT‐CN) with dual catalytic centers (metal–N4 and metal–N2) to catalyze oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). By using different metal centers, the catalytic activity and selectivity were well‐tuned. Among them, Co‐HAT‐CN catalyzed the ORR in a 4e− pathway, with a half‐wave potential of 0.8 V versus RHE, while the Ni‐HAT‐CN catalyze ORR in a 2e− pathway with H2O2 selectivity over 90%. Moreover, the Co‐HAT‐CN delivered an overpotential of 350 mV at 10 mA cm−2 with a corresponding Tafel slope of 24 mV dec−1 for OER in a 1.0 M KOH aqueous solution. The experimental results revealed that the activities toward ORR were due to the M–N4 sites in the frameworks, and both M–N4 and M–N2 sites contributed to the OER. This work gives us a new platform to construct bifunctional catalysts.