bluuebunny/crossref_metadata_2025 huggingface dataset:
Medical and Surgical Episodes Among Hospital Participants in the Bundled Payments for Care Improvement–Advanced Program
Authors: Robbins Keenan J. , Zheng Jie , Waken R. J. , Orav E. John , Epstein Arnold M. , Joynt Maddox Karen E.
Published: December 2024

Importance

Hospital participation in the Bundled Payments for Care Improvement–Advanced (BPCI-A) initiative has been associated with modest savings and stable clinical outcomes overall, but it is unknown whether the program performs differently for medical and surgical or procedural (henceforth, surgical) episodes.

Objective

To assess the association of BPCI-A participation with Medicare spending and clinical outcomes for medical and surgical episodes.

Design, Setting, and Participants

This retrospective difference-in-differences cohort study utilized 100% Medicare fee-for-service inpatient claims for episodes initiated between January 1, 2017, and September 30, 2019, and included 90 days of follow-up. The setting was hospitals participating in BPCI-A and matched nonparticipant hospitals. Participants included Medicare beneficiaries admitted for medical or surgical episodes.

Exposure

BPCI-A participation, beginning in 2018.

Main Outcomes and Measures

Changes in 90-day Medicare payments and clinical outcomes (readmissions, mortality, healthy days at home).

Results

The final sample included 2 895 878 episodes; 1 618 172 (55.9%) were female, 324 186 (11.2%) people under age 65 years, 1 354 246 (46.8%) between 65 and 80 years of age, and 1 217 446 (42.0%) over 80 years of age. Patient characteristics at BPCI-A and comparison hospitals were similar. BPCI-A participation was associated with a decrease in payments for medical episodes (−$882 per episode; 95% CI −$1004 to −$760) and surgical episodes (−$587; 95% CI −$850 to −$324) compared with nonparticipant hospitals (absolute difference between change in medical and surgical episodes, −$295; 95% CI −$584 to −$5). BPCI-A participation was associated with a greater increase in healthy days at home and a greater decrease in both skilled nursing facility (SNF) admissions and SNF length of stay overall, but there were no significant differences between medical and surgical episodes in terms of the association of BPCI-A with changes in these outcomes.

Conclusions and Relevance

In this cohort study analyzing the outcomes of the BPCI-A program for medical and surgical episodes, BPCI-A participation was associated with modestly decreased payments for both medical and surgical episodes compared with nonparticipants. Improvements in clinical outcomes associated with BPCI-A participation were also modest for both types of episodes; this study does not support a hypothesis that either medical or surgical episodes are better-suited for episode-based payments.
Within-Hospital Price Gaps Across National Insurers
Authors: Wang Yang , Xu Jianhui , Anderson Gerard
Published: December 2024

Importance

Commercial prices for hospital care are high and vary widely in the US. Employers and state policymakers are exploring reference-based pricing (RBP) to set their payment rates as multiples of Medicare prices; understanding the range of commercial price variation within a hospital is important for calculating the appropriate price targets that are effectively low to generate savings but also feasible and viable to local hospital markets.

Objective

To examine within-hospital maximum-to-minimum commercial hospital price gaps negotiated by 5 national insurers and estimate plan savings if the minimum prices within each hospital are used as new payment level.

Design, Setting, and Participants

This cross-sectional study used the insurer-disclosed Transparency in Coverage data as of March 2024. There were 40 382 commercial hospital facility prices extracted for 10 common services negotiated by CVS Health, Elevance Health, Blue Cross Blue Shield, Cigna, and United Healthcare, measured at the hospital-service-insurer level relative to the 2024 Medicare prices. For each hospital-service pair, the minimum, enrollment-weighted mean, and maximum prices were calculated, as well as the maximum-to-minimum price gaps. Plan savings were then estimated using the minimum within-hospital prices as the new payment levels.

Exposure

Insurer price disclosure under federal Transparency in Coverage rule.

Main Outcomes and Measures

Maximum-to-minimum commercial price gaps and estimated savings if using the minimum prices at hospital-service level.

Results

Among 40 382 commercial hospital prices negotiated by 5 national insurers, the national means of minimum prices were 168% (95% CI, 167%-169%) of Medicare rates for inpatient services and 220% (95% CI, 215%-226%) of Medicare rates for outpatient services. National mean minimum-to-maximum price gaps were 86% (95% CI, 85%-87%) and 222% (95% CI, 215%-229%) of Medicare rates for inpatient and outpatient services, respectively. If using the minimum within-hospital prices, compared with current prices, payers could save 21% (95% CI, 20%-21%) for inpatient services and 29% (95% CI, 28%-30%) for outpatient services.

Conclusions and Relevance

In this cross-sectional study, commercial prices across different national insurers varied substantially for the same hospital and service. These results suggest that employers and policymakers interested in RBP benchmarking may use the lowest prices among major insurers in their local hospital market as references to negotiate lower prices.
Firearm and Motor Vehicle Pediatric Deaths—Intersections of Age, Sex, Race, and Ethnicity
Authors: Lee Lois K. , Tang Suk-Fong S. , Cull William L. , Fleegler Eric W. , Olson Lynn M.
Published: December 2024

Importance

Injuries from firearms and motor vehicle crashes (MVCs) are the leading causes of death among US children and youths aged 0 to 19 years. Examining the intersections of age group, sex, race, and ethnicity is essential to focus prevention efforts.

Objective

To examine firearm and motor vehicle fatality rates by population subgroups and analyze changes over time.

Design, Setting, Participants

This cross-sectional study of firearm and MVC fatalities among US children and youths aged 0 to 19 years from the Centers for Disease Control and Prevention Web-Based Injury Statistics and Query Reporting System from 2011 to 2021. Participants included American Indian and Alaska Native; Asian, Hawaiian Native, and Pacific Islander; Black; Hispanic; and White youths. Data analysis was conducted from July 2023 to May 2024.

Exposure

Firearm or MVC fatality.

Main Outcome Measures

Firearm and MVC fatality rates by year and over time, as measured by the Joinpoint regression annual percent change (APC).

Results

From 2011 to 2021 there were 35 684 firearm and 40 735 MVC fatalities among US youths aged 0 to 19 years. For firearm fatalities, there were 21 332 homicides (59.8%), 12 113 suicides (33.9%), 1359 unintentional shootings (3.8%), 277 by legal enforcement (0.8%), and 603 from unknown intents (1.6%). When considering the intersections of age group, sex, race, and ethnicity, for firearm homicides among youths aged 15 to 19 years, the APCs were similar for Black (21.8%) and Hispanic (22.2%) males from 2018 to 2021, although with different peak rates (104.22 per 100 000 individuals and 17.80 per 100 000 individuals, respectively, in 2021). Black females aged 15 to 19 years demonstrated a dramatic APC increase of 40.7% from 2019 to 2021 (peak rate, 14.07 per 100 000 individuals). For firearm suicide in youths aged 10 to 19 years by sex, Black females had the greatest APC increase of 22.0% from 2016 to 2021. For MVC fatalities, the highest APC increase of 24.9% occurred among American Indian and Alaska Native females aged 15 to 19 years from 2018 to 2021. The highest MVC fatality rates occurred in 2021 among American Indian and Alaska Native males (38.16 per 100 000 individuals) and females (29.31 per 100 000 individuals) aged 15 to 19 years.

Conclusions and Relevance

In this cross-sectional study, US youths aged 0 to 19 years experienced important disparities in firearm and MVC fatality rates and increases over time when considering the intersectionality by age group, sex, race, and ethnicity. These findings suggest that a multipronged strategy focused on individual, community, and policy level approaches for specific high-risk groups for each injury mechanism is necessary to address these leading causes of death in US youths.
C–F Activation with Metal and Organocatalysts
Authors: Hamel Jean‐Denys , Ferlet Rémy , Chabaud Laurent , Paquin Jean‐François
Published: December 2024

Organofluorine compounds feature the strongest single bond to carbon: the CF bond. While generally considered inert, properly devised reaction conditions can lead to the selective cleavage of CF bonds, despite the presence of weaker bonds in the molecule. This chapter outlines the different catalytic reaction pathways that result in partial or exhaustive defluorination of fluorinated units. Throughout the chapter, the emphasis is put on the singular events that lead to CF bond cleavage, not on the methods themselves.
Physical Properties of Fluorinated Compounds
Authors: Linclau Bruno
Published: December 2024

Fluorinated compounds often have distinctive properties. In this chapter, the physical properties of fluorinated compounds are discussed. First, the characteristics of the fluorine atom itself are explained, followed by the characteristics of the CF bond and its associated stereoelectronic effects. This allows understanding of the electronic and steric effects of fluorine and fluorinated groups, which is discussed in the following sections, as well as the influence of fluorination on macroscopic properties, discussed in the final section.
Patient‐specific adaptive planning margin for whole bladder radiation therapy
Authors: Zhang Zhexuan , Liu Chieh‐Wen , Donaghue Jeremy D. , Murray Eric J. , Mian Omar , Xia Ping
Published: December 2024

Background

Whole bladder irradiation is an organ preservation treatment approach for muscle‐invasive bladder cancer (MIBC). Conventional planning margins, typically 15–20 mm, increase normal tissue toxicity and limit possible dose escalation.

Purpose

The study aimed to develop a patient‐specific adaptive margin recipe for whole bladder irradiation to minimize the planning target volume (PTV) while preserving adequate dose coverage.

Methods

Sixteen patients who received whole‐bladder irradiation were retrospectively selected for this study. We proposed a patient‐specific anisotropic adaptive margin recipe, derived from the first five fractions of kV‐CBCTs, to account for inter‐fractional bladder changes. This recipe was validated using kV‐CBCTs from fractions six to ten and the final five fractions. The goal was to achieve a residual volume, defined as the percentage of daily bladder volume (Vdaily) outside the PTV, of less than 5%. Adaptive and conventional plans were created using proposed and conventional margins, respectively. A dosimetric comparison of targets and organs‐at‐risk (OARs) was performed between the two approaches.

Results

(Vdaily) decreased throughout the treatment course. The most notable inter‐fractional bladder variations were in the superior and anterior directions. The patient‐specific anisotropic adaptive margins, averaging 6 mm (± 2.9 mm), achieved a residual volume of less than 5%. Compared to conventional planning, the adaptive approach reduced PTV volume by an average of 135.3 cc (± 46.6 cc). A significant correlation (p < 0.05) was identified between residual volume and adaptive margins in the anterior, superior, left, and right directions. Using the proposed adaptive margins, the median residual volume was 0.71% (interquartile range 0.09%−3.55%), and the median (Vdaily) receiving the prescribed dose was 99.1% (interquartile range 95.3%−99.9%). Adaptive plans demonstrated superior OAR sparing compared to conventional plans.

Conclusions

The proposed patient‐specific adaptive margin recipe for whole bladder irradiation resulted in margins smaller than conventional ones, optimized normal tissue sparing, and maintained adequate PTV coverage.
Dynamic Convolutional Neural Networks Based on Adaptive 2D Memristors
Authors: Hong Heemyoung , Chen Xi , Cho Woohyun , Yoo Ho Yeon , Oh Jaewhan , Kim Minseok , Hwang Geunwoo , Yang Yongsoo , Sun Linfeng , Wang Zhongrui , Yang Heejun
Published: December 2024

Convolutional Neural Networks (CNNs) are pivotal in modern digital computing, particularly for tasks like image classification, inspired by the receptive fields of the human brain. Nevertheless, CNNs implemented on conventional digital computers face significant limitations due to inflexible kernels that cannot adjust to dynamic inputs, and the von Neumann architecture, which leads to inefficient data transfer between memory and processing units. This research presents a hardware‐software co‐designed solution, a Dynamic Convolutional Neural Network (dCNN), empowered by three‐terminal adaptive two‐dimensional (2D) memristors. These memristors consist of a vertical heterostructure integrating silver, an atomically thin insulator (CrPS4), and graphene as a semimetal. This configuration allows for the dynamic tuning of conductive filament properties, emulating the heterosynaptic plasticity observed in biological neural systems. The three‐terminal memristor design permits the dCNN to actively adjust kernel weights in its attention layer according to the input stimuli. The empirical tests demonstrate that image classification accuracy using our adaptive 2D memristor‐enhanced dVGG reaches up to 94% on the CIFAR‐10 dataset, which exceeds the performance of static VGG. Furthermore, the energy efficiency of our dVGG significantly outperforms that of GPUs, aligning more closely with the energy dynamics of the human brain in terms of both consumption and classification accuracy.
Biomimetic Pyrolytic MXene‐Based Multifunctional Films with Multi‐Level Structure for Wearable Piezoresistive Devices and Bioelectronics
Authors: Huang Zhaoling , Ge Chengqi , Li Siyuan , Cai Miao , Hui Yun , Liao Xinqin , Zeng Qi
Published: December 2024

MXene films possess excellent controllable electrical conductivity, mechanical and chemical characteristics, showing great potential in the construction of new‐generation flexible wearable devices. However, achieving multifunctional applications of MXene through simple and scalable methods is a major challenge. Inspired by skin tissue, a pyrolysis‐MXene flexible film (P‐MX) with randomly microspine‐like and internal hollow coupled structure is prepared through the combination of interface‐induced self‐assembly, solution thermal deposition, and high‐temperature pyrolysis methods. The multi‐level structure provides more variable conductive paths during compression and ensures structural integrity under high pressure. The synergistic treatment of oxygen plasma and polyvinyl alcohol (PVA) enhances adhesion strength highest up to 46.87 times compared to a single surface treatment strategy between P‐MX sensitive components and flexible substrate. Such P‐MX sensor demonstrates an extremely high sensitivity (76.79 kPa−1 within 0–25.39 kPa), a wide detection range (up to 1275.19 kPa), fast response/ recovery time (22 ms/32 ms), and high cycle reliability (over 18 000 cycles). It can also perceive weak signals (12 mg/4.8 Pa). Additionally, P‐MX exhibits a significant increment in specific capacitance. It exhibits excellent prospects in human‐machine interaction, neural electrodes, and motion detection. These findings open new pathways for the practical application of MXene‐based wearable piezoresistive devices and bioelectronics.
Photoinduced Lattice Compression of Cu for Enhanced Production of Ethylene from CO2
Authors: Li Zhenyao , Wei Wei , Hu Xuli , Zhang Zhen , Hu Yangshun , Wu Yushan , Wang Yao , Xu Junchen , Ding Mingyue
Published: December 2024

While engineering lattice strain has been proven effective in enhancing the electrochemical CO2 reduction performance of a catalyst, the correlation between strain effect and the intrinsic catalytic mechanism has remained elusive. Herein, a photolithography‐inspired method is proposed to regulate Cu(111) lattice strain. By irradiating the photosensitive Cu(Acac) sol–gel, Acac chelate bond undergoes π→π* electronic transition, and the ring‐closed Cu(Acac) decompose into the stabilized Cu(Acac) mesh which presents as nanospots embedded onto the surface of the Cu cluster. The photoinduced nanospots serve to exert compressive strain to the Cu(111) lattice in which the lattice distance is reduced by 5.7–11.4%. Herein, the catalyst with 11.4% lattice compression exhibits enhanced C2H4 production capabilities, reaching a maximal Faradaic efficiency of 57.00%, and a high partial current density of 456.01 mA cm−2. Theoretical calculations reveal that the compressed Cu(111) lattice exhibits reduced surface energies, leading to a significant drop in the C─C coupling reaction free energy from 1.16 eV over the pristine lattice, to 0.57 eV over the 10% compressed lattice. Additionally, the 10% compressed lattice facilitates spontaneous *O splitting immediately after OC─CHO coupling which leads to the generation of C2H4‐favoring *CCH intermediate.
The Epileptiogenic Modified Therapy: Regulating the Dynamic of Microglia via ROS‐Responsive Cascade Nano‐Formulation
Authors: Li Jiaxin , Liu Shuai , Chen Chenghan , Deng Jiahong , Du Zibo , Yang Simin , Deng Hongying , Zhang Zhixia , Huang Yiyu , Fu Jingwen , Zhang Wangming , Poon Wai Sang , Hou Honghao , Wang Jun
Published: December 2024

Pharmacological treatment of epilepsy presents several challenges, particularly the ineffectiveness of antiseizure medicines (ASMs) in modifying disease. In fact, the removal of reactive oxygen species (ROS) and preconditioning with tolerable dose of nitric oxide (NO) can activate neuroprotective mechanisms during latency and enhance tolerance to oxidative stress during seizures. To address this, a ROS‐responsive cascade Nano‐formulation (RRCN) is developed, which will transform ROS into NO. Remarkably, RRCN significantly reduces seizure severity, prolongs seizure latency, and extends inter‐seizure intervals, though it does not increase the latency of generalized seizures. Microglia, the primary immune cells of the brain, play a crucial role in the initiation and progression of epilepsy. In the kainic acid (KA) epilepsy model, microglial processes elongate, branching increases, and interactions between microglia and neurons are strengthened in the CA1 and CA3 regions of the hippocampus compared to the Vehicle group. RRCN reverses these dynamic changes in microglia and their interactions with neurons, which are mediated by the NO/HIF/ErBb2 pathway. Thus, RRCN can inhibit seizures generalization by preconditioning the dynamic changes of microglia.
Accelerating the Electrochemical Formation of the δ Phase in Manganese‐Rich Rocksalt Cathodes
Authors: Holstun Tucker , Mishra Tara P , Huang Liliang , Hau Han‐Ming , Anand Shashwat , Yang Xiaochen , Ophus Colin , Bustillo Karen , ma Lu , Ehrlich Steven , Ceder Gerbrand
Published: December 2024

Mn‐rich disordered rocksalt materials with Li‐excess (DRX) materials have emerged as a promising class of earth‐abundant and energy‐dense next‐generation cathode materials for lithium‐ion batteries. Recently, an electrochemical transformation to a spinel‐like “δ” phase has been reported in Mn‐rich DRX materials, with improved capacity, rate capability, and cycling stability compared with previous DRX compositions. However, this transformation unfolds slowly over the course of cycling, complicating the development and understanding of these materials. In this work, it is reported that the transformation of Mn‐rich DRX materials to the promising δ phase can be promoted to occur much more rapidly by electrochemical pulsing at elevated temperature, rate, and voltage. To extend this concept, micron‐sized single‐crystal DRX particles are also transformed to the δ phase by the same method, possessing greatly improved cycling stability in the first demonstration of cycling for large, single‐crystal DRX particles. To shed light on the formation and specific structure of the δ phase, X‐ray diffraction, scanning electron nanodiffraction (SEND) and atomic resolution STEM‐HAADF are used to reveal a nanodomain spinel structure with minimal remnant disorder.
Predesign of Covalent‐Organic Frameworks for Efficient Photocatalytic Dehydrogenative Cross‐Coupling Reaction
Authors: Chen Yu , Sun Sheng‐Nan , Chen Xiao‐Hong , Chen Ming‐Lin , Lin Jiao‐Min , Niu Qian , Li Shun‐Li , Liu Jiang , Lan Ya‐Qian
Published: December 2024

The dehydrogenative cross‐coupling reaction is the premier route for synthesizing important 4‐quinazolinone drugs. However, it usually requires high reaction temperature and long reaction time, and the yield of the final product is low. Here two stable and photosensitive covalent‐organic frameworks (COFs), TAPP‐An and TAPP‐Cu‐An are purposefully designed and constructed to serve as unprecedented heterogeneous tandem catalysts to complete dehydrogenative cross‐coupling reactions in a short time and under mild reaction conditions (room temperature and light), leading to the high‐efficient photosynthesis of 4‐quinazolinones. Particularly, TAPP‐Cu‐An is the best heterogeneous catalyst currently available for the synthesis of 4‐quinazolinones, even surpassing all the catalysts reported so far. It also enables one‐step photosynthesis of 4‐quinazolinones with higher conversion (>99%) and selectivity (>99%) in a shorter time, and the product can be easily prepared on a gram scale. Extensive experiments combined with theoretical calculations show that the excellent photogenerated charge separation and transport capability, as well as the synergistic An‐Cu catalysis in TAPP‐Cu‐An are the main driving forces for this efficient reaction.
PEDOTs‐Based Conductive Hydrogels: Design, Fabrications, and Applications
Authors: Li Hai , Cao Jie , Wan Rongtai , Feig Vivian Rachel , Tringides Christina M. , Xu Jingkun , Yuk Hyunwoo , Lu Baoyang
Published: December 2024

Conductive hydrogels combine the benefits of soft hydrogels with electrical conductivity and have gained significant attention over the past decade. These innovative materials, including poly(3,4‐ethylenedioxythiophene) (PEDOTs)‐based conductive hydrogels (P‐CHs), are promising for flexible electronics and biological applications due to their tunable flexibility, biocompatibility, and hydrophilicity. Despite the recent advances, the intrinsic correlation between the design, fabrications, and applications of P‐CHs has been mostly based on trial‐and‐error‐based Edisonian approaches, significantly limiting their further development. This review comprehensively examines the design strategies, fabrication technologies, and diverse applications of P‐CHs. By summarizing design strategies, such as molecular, network, phase, and structural engineering, and exploring both 2D and 3D fabrication techniques, this review offers a comprehensive overview of P‐CHs applications in diverse fields including bioelectronics, soft actuators, energy devices, and solar evaporators. Establishing this critical internal connection between design, fabrication, and application aims to guide future research and stimulate innovation in the field of functional P‐CHs, offering broad benefits to multidisciplinary researchers.
Renal Clearable Chiral Manganese Oxide Supraparticles for In Vivo Detection of Metalloproteinase‐9 in Early Cancer Diagnosis
Authors: Zhang Hongyu , Chen Panpan , Shi Wenxiong , Qu Aihua , Sun Maozhong , Kuang Hua
Published: December 2024

In this study, polypeptide TGGGPLGVARGKGGC‐induced chiral manganese dioxide supraparticles (MnO2 SPs) are prepared for sensitive quantification of matrix metalloproteinase‐9 (MMP‐9) in vitro and in vivo. The results show that L‐type manganese dioxide supraparticles (L‐MnO2 SPs) exhibited twice the affinity for the cancer cell membrane receptor CD47 (cluster of differentiation, integrin‐associated protein) than D‐type manganese dioxide supraparticles (D‐MnO2 SPs) to accumulate at the tumor site after surface modification of the internalizing arginine‐glycine‐aspartic acid (iRGD) ligand, specifically reacting with the MMP‐9, disassembling into ultrasmall nanoparticles (NPs), and efficiently underwent renal clearance. Furthermore, L‐MnO2 facilitates the quantification of MMP‐9 in mouse tumor xenografts, as demonstrated by circular dichroism (CD) and magnetic resonance imaging (MRI) within 2 h. A strong linear relationship is observed between MMP‐9 concentration and both CD and MRI intensity, ranging from 0.01 to 10 ng mL−1. The corresponding limits of detection (LOD) are 0.0054 ng mL−1 for CD and 0.0062 ng mL−1 for MRI, respectively. hese SPs provide a new approach for exploring chiral advanced biosensors for early diagnosis of cancer.
Coherent‐Precipitation‐Stabilized Phase Formation in Over‐Stoichiometric Rocksalt‐Type Li Superionic Conductors
Authors: Chen Yu , Zhao Xinye , Chen Ke , Koirala Krishna Prasad , Giovine Raynald , Yang Xiaochen , Wang Shilong , Szymanski Nathan J. , Xiong Shuoyan , Lun Zhengyan , Ji Huiwen , Wang Chongmin , Bai Jianming , Wang Feng , Ouyang Bin , Ceder Gerbrand
Published: December 2024

Rationalizing synthetic pathways is crucial for material design and property optimization, especially for polymorphic and metastable phases. Over‐stoichiometric rocksalt (ORX) compounds, characterized by their face‐sharing configurations, are a promising group of materials with unique properties; however, their development is significantly hindered by challenges in synthesizability. Here, taking the recently identified Li superionic conductor, over‐stoichiometric rocksalt Li–In–Sn–O (o‐LISO) material as a prototypical ORX compound, the mechanisms of phase formation are systematically investigated. It is revealed that the spinel‐like phase with unconventional stoichiometry forms as coherent precipitate from the high‐temperature‐stabilized cation‐disordered rocksalt phase upon fast cooling. This process prevents direct phase decomposition and kinetically locks the system in a metastable state with the desired face‐sharing Li configurations. This insight enables us to enhance the ionic conductivity of o‐LISO to be >1 mS cm−1 at room temperature through low‐temperature post‐annealing. This work offers insights into the synthesis of ORX materials and highlights important opportunities in this new class of materials.
Free‐Standing, Transparent Carbon Nanotube Thin Films with High Specific Shielding Effectiveness
Authors: Boyd Samuel J. , Rossi Jamie E. , Broderick Daniel L. , Puchades Ivan , Landi Brian J.
Published: December 2024

Carbon nanotubes (CNTs) are emerging as a candidate shielding material for RF technologies due to their multi‐functional properties such as low density, flexibility, and excellent electrical properties. The present work provides a direct comparison of shielding measurements for single‐wall (SWCNT) and multi‐wall (MWCNT) free‐standing thin films fabricated from chlorosulfonic acid dispersions. CNT thin film properties are varied to create a series of thicknesses ranging from ≈18 to ≈4000 nm, resulting in optical transparencies from 80 to 0%. Shielding effectiveness is measured using a rectangular waveguide setup from 10 to 15 GHz and shows frequency‐independence with values up to 50 dB. Lower shielding effectiveness in MWCNT films relative to SWCNT films of equivalent mass is consistent with theoretical studies that propose a restriction of the electromagnetic interaction to the outer MWCNT walls. The present SWCNT and MWCNT films exhibit density‐ and thickness‐specific shielding effectiveness of 3.3 × 106 dB cm2 g−1, a 10× increase over emerging thin film and transparent conductive materials. Demonstration of shielding effectiveness has been made by measuring signal strength reduction from a Bluetooth device when attenuated by the CNT film. Thus, the present work advances the potential to incorporate transparent, conductive CNT films into RF technologies with arbitrary surface geometry.
Development of a Novel Ultra‐Acidic Self‐Assembling Peptides‐Based Hydrogel System for pH‐Tunable Nanobody Delivery
Authors: Guo Yang , Chu Xiaohui , Deng Yang , Song Liang , Li Fei , Zhang Ming , Xu Fei , Nian Rui , Liu Wenshuai
Published: December 2024

Self‐assembling peptide hydrogels are promising scaffolds for drug delivery, however, the costly chemical synthesis of peptides has limited their widespread application. This study develops an innovative biological recombinant strategy for (RADA)5 peptide production by fusing with a fibronectin fragment in Escherichia coli. Notably, it is reported for the first time, (RADA)5 peptides gelates at an extremely acidic pH of 1.2, indicating potential application in the gastrointestinal tract. Circular dichroism reveals a characteristic β‐sheet structure and transmission electron microscopy exhibits a dense and interwoven nanofiber network. The (RADA)5 peptide hydrogels demonstrate a pH‐responsive release with a substantial nanobody release at pH 6.8 (≈80%) and minimal release at pH 2.0 (<30%). This behavior allows fine‐tuning of nanobody release, potentially enabling retention in the acidic stomach and targeted release in the intestines. Within 24 h, <18% of the encapsulated nanobodies are released at pH 2.0, with sustained release observed upon transition to pH 6.8, achieving a cumulative release of 55% over 14 days. In conclusion, the novel ultra‐acidic (RADA)5 peptide hydrogels are promising for sustained and controlled release of nanobodies in gastrointestinal disease treatment.
Three‐ and Seven‐membered Annulenones as a Lewis Base Catalyst for Enantioselective meso‐Epoxide Opening
Authors: Arae Sachie , Shimoda Yasushi , Kuwajima Mizuki , Kotani Shunsuke , Nakajima Makoto
Published: December 2024

This is the report on the Lewis base catalysis of annulenones. Additionally, the synthesis of chiral annulenone catalysts and their application in asymmetric ring‐opening reactions of meso‐epoxides is shown. Annulenones, such as cyclopropenones and tropones, function as Lewis bases owing to their inherent polarity caused by aromaticity, resulting in the activation of silicon tetrachloride, which catalyzes the ring‐opening reaction of meso‐epoxides. Moreover, various chiral annulenone catalysts have been designed and synthesized, and microwave irradiation has been shown to improve the synthetic efficiency of chiral tropones. The chiral annulenones successfully catalyzed the asymmetric ring‐opening reaction of meso‐epoxides, resulting in the formation of 1,2‐chlorohydrins in a high yield and high enantioselectivity (up to 90% ee in 96% yield). These results represent the example of three‐ and seven‐membered annulenones as a chiral Lewis base catalyst.
Regioselective Hydrothiolation of Terminal Alkynes using Half‐Sandwich Ni(ii) Catalysts bearing Bidentate NHC‐Carboxylate Ligands
Authors: Sanz‐Garrido Jorge , Andrés Román , Gonzalez‐Arellano Camino , Flores Juan C.
Published: December 2024

A half‐sandwich nickel complex containing an NHC‐carboxylate chelate ligand (i. e., [Ni(η5‐Cp)(κ2‐C,O‐NHC)]) derived from the (S)‐leucine has been identified for the selective hydrothiolation of terminal acetylenes toward challenging Markovnikov‐type α‐vinyl thioethers, even with aryl alkynes. The activity and selectivity exhibited by the nickel complex are comparable, if not superior, to those of complexes of rhodium reported to be the best catalysts to date for the Markovnikov addition in the thiol‐yne reaction. The experimental data are consistent with the participation of the coordinated carboxylate group in the catalytic reaction as an intermolecular acid‐base co‐catalyst, favoring the formation of nickel‐thiolate intermediates.
Does Encapsulation of π‐Conjugated Polymer Nanoparticles within Biodegradable PEG–PLGA Matrices Mitigate Photoinduced Free Radical Production and Phototoxicity?
Authors: Modicano Paola , Trutschel Marie‐Luise , Phan‐Xuan Thüong , Matarèse Bruno F. E. , Urbano Laura , Green Mark , Mäder Karsten , Dailey Lea Ann
Published: December 2024

Lipophilic π‐conjugated polymers (CPs) encapsulated within self‐assembling diblock copolymer poly(ethylene glycol) methyl ether‐block‐poly(lactide‐co‐glycolide) (PEG–PLGA) nanoparticles, are interesting candidates for photodynamic and photothermal therapies. Upon irradiation, CPs generate reactive oxygen species (ROS), which may either cause local phototoxicity or could be exploited for photodynamic therapy. The propensity of the PEG–PLGA matrix to scavenge ROS has never been investigated. Here the ability of two PEG–PLGA structures (PEG2 kDa–PLGA4.5 kDa vs PEG5 kDa–PLGA55 kDa) to mitigate the release of ROS generated by four different CPs (PFO, F8BT, CN‐PPV, and PCPDTBT) following irradiation (5 J cm−2) at 385, 455, and 656 nm is studied. The molar content of the PEG–PLGA matrix, rather than the molecular weight or composition, appeared to be the most influential factor, i.e., lower molar concentrations of the matrix polymer are associated with significant increases in phototoxicity. Multivariate analysis reveals that the combination of CP photophysical properties and nanoparticle matrix properties are important for understanding CP nanoparticle‐induced phototoxicity.
Transient Chemo‐Mechanical Model of Lithium Plating Impacted by External Pressure
Authors: Meyer Julia M. , Mukherjee Partha P. , Collins Lincoln N. , Roberts Scott A.
Published: December 2024

Lithium anodes show great promise in commercial applications, but are hindered by lithium plating and dendrite growth which cause safety concerns during long‐term cell operation. Stack pressure is experimentally observed to improve cell lifetime; however, the relationship between stress and lithium deposition has remained difficult to elucidate. In this work, a transient, 3D, finite‐element model of the evolution of a lithium anode due to stripping and plating is developed. The evolution of a microscale protrusion on the anode surface is tracked over one charge‐discharge cycle with respect to stack pressure and lithium yield strength. Lithium plastic deformation, nonconformal anode‐separator contact, and separator porosity effects are accounted for. Over the course of several hours of stripping/plating, the anode surface evolves to a similar morphology under pressure regardless of the initial conditions due to lithium plastic deformation and hardening. The rate of this evolution highly depends on the applied pressure and assumed lithium yield strength.
Cl− Boosted Active and Stable Seawater Reduction on Pt/CoP Nanoarray Electrocatalysts
Authors: Liu Wei , Guo Xinlong , Jiang Zheheng , Yu Jiage , Zhou Linlin , Li Tianshui , Guo Yinghao , Li Shihang , Ding Boyu , Wang Kairui , Yang Yongqiang , Xin Huijun , Zhou Daojin , Kuang Yun , Sun Xiaoming
Published: December 2024

Hydrogen evolution in alkaline condition is kinetically unfavorable and requires active and stable electrocatalysts, not to mention the complex composition of seawater in catalytic alkaline seawater electrolysis. Herein, highly dispersed Pt on CoP nanoarray (denoted as Pt/CoP) is decorated as a hydrogen evolution electrocatalyst and further improved its activity by modulating the binding interaction between free Cl− in alkaline seawater and Pt/CoP. Compared to the blank control without Cl−, which requires an overpotential of 76 mV, this cathode exhibits an overpotential as low as 39 mV to reach −100 mA cm−2 after the addition of NaCl to the electrolyte. Characterizations and theoretical simulations demonstrate that Cl−coordinates with Pt species and strengthen the intermediates adsorption by reducing the electropositivity of the Pt sites. Furthermore, by coupling the Pt/CoP cathode with Ir/CoFe‐LDH anode, whose activity can also be boosted by Cl anions, the assembled seawater electrolyzer only required 1.75 V to 1 A cm−2 and stably operate for over 100 h. This work presents a major leap in electrode development for ultra‐high performance seawater electrolysis, highlighting that Cl−, which is generally considered detrimental, can be effectively harnessed.
Tuning the morphology of supramolecular aggregates for nanocarrier‐based drug delivery
Authors: Ji Xiongtao , Wang Na , Wang Jingkang , Huang Yunhai , Wang Ting , Huang Xin , Hao Hongxun
Published: December 2024

Due to the unique drug delivery mode and specific therapy, nano‐formulations are of interest for biomedical applications and treating many diseases. However, traditional method of nano‐formulation construction via additional carriers or structural modifications of therapeutic drugs might be cumbersome or low loading‐efficient. Herein, the kinetics, accessible pathways, and final outcomes of supramolecular assembly processes of therapeutic drugs are investigated in detail. It was found that the supramolecular aggregates of cephradine (CEP) undergoes a morphological transformation from anisotropic nanofiber (EtOH) to isotropic spherical nanoparticle (H2O), similar to “plants took root, sprouted, blossomed and bore fruit.” Moreover, the assembly kinetics results reveal the assembly pathways of nucleation elongation in H2O and surface‐catalyzed secondary nucleation in EtOH. The method presented in this work has the potential to be used for efficiently designing specific nano‐formulations.
Nonrecurrent Triplication of 5q21.3q23.3: A Case Report and Review of the Literature
Authors: Ginter Jacob A. , Beaudry Sarah , Guseva Natalya , Nagy Jaime , Stence Aaron A. , Sidhu Alpa
Published: December 2024

Triplications involving 5q21.3q23.3 are rare, and a phenotype has not been established. Here, we present a 4‐month‐old male with dysmorphic facial features and congenital cardiac malformation. Chromosomal microarray identified a pathogenic triplication of 5q21.3q23.3 with chromosome analysis showing the extra 5q material inserted into 16q. Optical genome mapping (OGM) was performed to further characterize the triplication. We compared the clinical features of our proband with previous case reports of individuals with duplications or triplications in the region to identify a phenotype. Common features appear to include short stature, developmental delays, learning difficulties, and cardiac malformations. We discuss genes in the region with a reported role in cardiac development, hypothesize that the triplication may have resulted from microhomology‐mediated break‐induced replication, and discuss the utility and limitations of OGM in this case. To our knowledge, this is the first reported case of a de novo triplication of 5q21.3q23.3.
Identification of a Founder GLDN Variant Associated With “Lethal” Arthrogryposis in Nunavik Inuit: Implications for Obstetrical and Long‐Term Survivors' Management
Authors: McAdam Alexa , Ito Yoko A. , Richard Marilyn , Spiegelman Dan , Rochefort Daniel , Xiong Lan , Oskoui Maryam , Zielinski David , Rouleau Guy A. , Zhou Sirui ,   Care4Rare Canada Consortium, Boykott Kym M. , De Bie Isabelle
Published: December 2024

Biallelic variants in GLDN have recently been associated with lethal congenital contracture syndrome 11 (LCCS11), a form of fetal akinesia deformation sequence (FADS) with high neonatal mortality. In this report, we describe five individuals from two Canadian Inuit families originating from different communities in Nunavik all affected with FADS and harboring a rare homozygous missense variant, [NM_181789.4:c.82G >C p.(Ala28Pro)] in GLDN. Two pregnancies presented with significant obstetrical complications including placental abruption and hemorrhage. Four infants died shortly after birth, while one survived past the neonatal period. This individual, while apparently asymptomatic during infancy, then presented with progressive neuromuscular and respiratory compromise that became more evident in adolescence. Data from a Nunavik Inuit cohort demonstrated a minor allele frequency (MAF) of 0.03571 for this variant compared to 0.00001341 in the general population, suggesting a founder effect in the Nunavik Inuit population. Our findings support the presence of a founder variant associated with LCCS11 in Nunavik Inuit populations. Our data corroborate those of other reports, demonstrating that LCCS11 is not universally lethal, but long‐term survivors are at risk of progressive neuromuscular compromise. We also highlight in this report the significant obstetrical complications associated with this fetal‐onset condition.
Rhodium(III)‐Catalyzed Arylation of Dimethyl Itaconate: Facile Access to Substituted Benzylidenesuccinates
Authors: Takatsuji Yuito , Usuki Yoshinosuke , Satoh Tetsuya
Published: December 2024

The rhodium(III)‐catalyzed arylation of dimethyl itaconate with arylboronic acids proceeds smoothly under mild conditions to produce benzylidenesuccinates. The present reaction provides a simple synthesis route to benzylidenesuccinates, which are of interest due to their biological activities, from readily available substrates.
Glutathione Peroxidase‐Mimics Organoselenium Amines: Anti‐Ferroptotic Properties and an In Silico Study of 15‐Lipoxygenase‐2
Authors: Sodhi Nikhil , Kumar Manish , Yadav Manisha , Kadian Rajni , Atici Sena , Friedmann Angeli Jose Pedro , Singh Vijay P.
Published: December 2024

In search for better synthetic antioxidants, aminic organoselenides carrying amine and benzamide groups at ortho‐positions to the selenium atom were synthesized from alkyl halides and in situ generated sodiumselenolates as nucleophile by the sodium borohydride reduction of corresponding diselenides. The single crystal X‐ray structure of one compound showed the weak intramolecular Se⋅⋅⋅H interactions with free amine group. The presence of Se⋅⋅⋅H interactions was further confirmed using natural bond orbital (NBO) and atoms in molecules (AIM) calculations, respectively. The glutathione peroxidase enzyme (GPx)‐like antioxidant activity of all compounds was evaluated using thiophenol assay. The best antioxidant exhibited nearly 5 and 10 times greater activities than Oct2Se2 and Ph2Se2 used as references, respectively. The most active catalysts carrying a strong electron‐donating group were further investigated at different concentrations of thiol for determining the catalytic parameters. These GPx mimics have shown anti‐ferroptotic activity in a 4‐OH‐tamoxifen (TAM) inducible GPx4 knockout cell line and protected cells from cell death induced by loss of GPx4 enzyme. In silico molecular docking studies showed that all antioxidants demonstrated promising Moldock scores with human 15‐lipoxygenase‐2 enzyme.
Synthesis of Bridged and Fused Tetracycles via Rhodium‐Catalyzed C−H Allylation/Cycloaddition of Azomethine Imines with MBH Adducts and Allyl Acetates
Authors: Sun Yang , Wang Yiyan , Zhang Lijun , Zhong Rui , Wang Hui
Published: December 2024

A rhodium‐catalyzed cascade C−H allylation combined with exo‐ and endo‐type [3+2] dipolar cycloaddition of aryl azomethine imines with Morita‐Baylis‐Hillman (MBH) adducts and allyl acetates is described. This process, which is operationally simple and proceeds efficiently in air and moisture under neat conditions, facilitates diverse bridged and fused tetracycles as single diastereomers. The reaction showcases a broad substrate scope and good functional group compatibility. Furthermore, its practicality is further demonstrated through successful scale‐up and synthetic applications.
Overview of Alzheimer's Disease Neuroimaging Initiative and future clinical trials
Authors: Weiner Michael W. , Kanoria Shaveta , Miller Melanie J. , Aisen Paul S. , Beckett Laurel A. , Conti Catherine , Diaz Adam , Flenniken Derek , Green Robert C. , Harvey Danielle J. , Jack Clifford R. , Jagust William , Lee Edward B. , Morris John C. , Nho Kwangsik , Nosheny Rachel , Okonkwo Ozioma C. , Perrin Richard J. , Petersen Ronald C. , Rivera‐Mindt Monica , Saykin Andrew J. , Shaw Leslie M. , Toga Arthur W. , Tosun Duygu , Veitch Dallas P. ,   for the Alzheimer's Disease Neuroimaging Initiative
Published: December 2024

The overall goal of the Alzheimer's Disease Neuroimaging Initiative (ADNI) is to optimize and validate biomarkers for clinical trials while sharing all data and biofluid samples with the global scientific community. ADNI has been instrumental in standardizing and validating amyloid beta (Aβ) and tau positron emission tomography (PET) imaging. ADNI data were used for the US Food and Drug Administration (FDA) approval of the Fujirebio and Roche Elecsys cerebrospinal fluid diagnostic tests. Additionally, ADNI provided data for the trials of the FDA‐approved treatments aducanumab, lecanemab, and donanemab.

More than 6000 scientific papers have been published using ADNI data, reflecting ADNI's promotion of open science and data sharing. Despite its enormous success, ADNI has some limitations, particularly in generalizing its data and findings to the entire US/Canadian population. This introduction provides a historical overview of ADNI and highlights its significant accomplishments and future vision to pioneer “the clinical trial of the future” focusing on demographic inclusivity.

Highlights

The Alzheimer's Disease Neuroimaging Initiative (ADNI) introduced a novel model for public‐private partnerships and data sharing.

It successfully validated amyloid and Tau PET imaging, as well as CSF and plasma biomarkers, for diagnosing Alzheimer's disease.

ADNI generated and disseminated vital data for designing AD clinical trials.
The Alzheimer's Association clinical practice guideline for the diagnostic evaluation, testing, counseling, and disclosure of suspected Alzheimer's disease and related disorders (DETeCD‐ADRD): Validated clinical assessment instruments
Authors: Atri Alireza , Dickerson Bradford C. , Clevenger Carolyn , Karlawish Jason , Knopman David , Lin Pei‐Jung , Norman Mary , Onyike Chiadi , Sano Mary , Scanland Susan , Carrillo Maria
Published: December 2024

US clinical practice guidelines for the diagnostic evaluation of cognitive impairment due to Alzheimer's Disease (AD) or AD and related dementias (ADRD) are decades old and aimed at specialists. This evidence‐based guideline was developed to empower all—including primary care—clinicians to implement a structured approach for evaluating a patient with symptoms that may represent clinical AD/ADRD. As part of the modified Delphi approach and guideline development process (7374 publications were reviewed; 133 met inclusion criteria) an expert workgroup developed recommendations as steps in a patient‐centered evaluation process. The workgroup provided a summary of validated instruments to measure symptoms in daily life (including cognition, mood and behavior, and daily function) and to test for signs of cognitive impairment in the office. This article distills this information to provide a resource to support clinicians in the implementation of this approach in clinical practice. The companion articles provide context for primary care and specialty clinicians with regard to how to fit these instruments into the workflow and actions to take when integration of performance on these instruments with clinical profile and clinician judgment support potential cognitive impairment.