bluuebunny/crossref_metadata_2025_split huggingface dataset:
Anti‐CO Poisoning FePtRh Nanoflowers with Rh‐Rich Core and Fe‐Rich Shell Boost Methanol Oxidation Electrocatalysis
Authors: Liu Hu , Jia Rongrong , Qin Chuanjian , Yang Qin , Tang Zuobin , Li Menggang , Ma Zhenhui 
Published: December 2022

AbstractIntroducing oxophilic metals into Pt‐based alloy catalysts can effectively alleviate the poisoning by CO intermediates (CO*) during methanol oxidation reactions (MOR). However, excessive oxophilic metals on the surface of catalysts tend to form thermodynamically stable carbonyl compound‐like structures, occupying electrocatalytically active sites, which is not conducive to the enhancement of catalytic activity. Herein, a kind of surface segregated FePtRh nanoflowers for effectively eliminating the CO* poisoning during MOR electrocatalysis is presented. The FePtRh nanoflowers are constituted by the Rh‐rich core and Fe‐rich shell. The optimized Fe21Pt66Rh13/C shows a high mass activity of 3.90 A mgPt−1 and a specific activity of 4.85 mA cm−2. It is confirmed that the electron transfer from Pt to Rh or Fe atoms is beneficial for the higher anti‐CO poisoning ability, which mainly originate from the alloying of Rh atoms and surface‐segregated structures. Density functional theory calculations reveal the decreased electrons adsorbed by CO* on both Pt–Pt bridge sites and top sites weakens the strong adsorption energy between Pt atoms and CO* intermediates. The optimal nanoflowers also show excellent performance toward ethanol oxidation reaction (EOR) with a high mass activity of 2.76 A mgPt−1 and the enhanced anti‐CO poisoning ability, as well as the improved stability.
A Novel Signal‐On Electrochemiluminescence Immunosensor for the Detection of NSCLC Antigen Biomarker Based on New Co‐Reaction Accelerators
Authors: Guo Lei , Mu Zhaode , Qing Min , Zhou Jing , Li Huizhen , Wang Lulu , Zhong Muyue , Bai Lijuan 
Published: December 2022

AbstractNon‐small cell lung cancer (NSCLC) is the most common type of lung cancer with substantial morbidity and mortality. Herein, a new signal‐on electrochemiluminescence (ECL) immunosensor based on multiple amplification strategies is constructed for ultrasensitive detection of cytokeratin 19 fragment antigen 21‐1 (CYFRA21‐1) biomarker related to NSCLC. Polyethyleneimine (PEI) functionalized MXene is decorated with NiMn layer double hydroxide (NiMn LDH) to form MXene‐PEI‐NiMn LDH composite. Specially, the La‐MOF@ZIF‐67 bimetallic organic framework (named as LZBM) and MXene‐PEI‐NiMn LDH both served as coreaction accelerators to improve the ECL emission of the luminol‐H2O2 system. To be specific, Au nanoparticles (AuNPs) coated MXene‐PEI‐NiMn LDH is applied to immobilize primary CYFRA21‐1 antibody (Ab1), while AuNPs decorated LZBM was used for the loading of luminol and secondary CYFRA21‐1 antibody (Ab2) to form tracer label. Therefore, the ECL signal of the sandwich‐type immunosensor is significantly enhanced due to the high loading capability for luminol and the synergistic catalytic ability for the decomposition of H2O2 into reactive oxygen species (ROS). Under the optimal experimental conditions, the ECL immunosensor exhibited good analytical performances for CYFRA21‐1 detection with a wide linear range (100 fg mL−1−100 ng mL−1) and a low limit of detection (85.20 fg mL−1), providing a promising method for early diagnosis of NSCLC.
Reshaping de Novo Protein Switches into Bioresponsive Materials for Biomarker, Toxin, and Viral Detection
Authors: d'Amone Luciana , Matzeu Giusy , Quijano‐Rubio Alfredo , Callahan Gregory P. , Napier Bradley , Baker David , Omenetto Fiorenzo G. 
Published: December 2022

AbstractDe novo designed protein switches are powerful tools to specifically and sensitively detect diverse targets with simple chemiluminescent readouts. Finding an appropriate material host for de novo designed protein switches without altering their thermodynamics while preserving their intrinsic stability over time would enable the development of a variety of sensing formats to monitor exposure to pathogens, toxins, and for disease diagnosis. Here, a de novo protein‐biopolymer hybrid that maintains the detection capabilities induced by the conformational change of the incorporated proteins in response to analytes of interest is generated in multiple, shelf‐stable material formats without the need of refrigerated storage conditions. A set of functional demonstrator devices including personal protective equipment such as masks and laboratory gloves, free‐standing films, air quality monitors, and wearable devices is presented to illustrate the versatility of the approach. Such formats are designed to be responsive to human epidermal growth factor receptor (HER2), anti‐hepatitis B (HBV) antibodies, Botulinum neurotoxin B (BoNT/B), and severe acute respiratory syndrome coronavirus 2 (SARS‐CoV‐2). This combination of form and function offers wide opportunities for ubiquitous sensing in multiple environments by enabling a large class of bio‐responsive interfaces of broad utility.
A Multifunctional “Halide‐Equivalent” Anion Enabling Efficient CsPb(Br/I)3 Nanocrystals Pure‐Red Light‐Emitting Diodes with External Quantum Efficiency Exceeding 23%
Authors: Zhang Jibin , Zhang Tiankai , Ma Zhuangzhuang , Yuan Fanglong , Zhou Xin , Wang Heyong , Liu Zhe , Qing Jian , Chen Hongting , Li Xinjian , Su Shijian , Xie Jianing , Shi Zhifeng , Hou Lintao , Shan Chongxin 
Published: December 2022

AbstractPure‐red perovskite LEDs (PeLEDs) based on CsPb(Br/I)3 nanocrystals (NCs) usually suffer from a compromise in emission efficiency and spectral stability on account of the surface halide vacancies‐induced nonradiative recombination loss, halide phase segregation, and self‐doping effect. Herein, a “halide‐equivalent” anion of benzenesulfonate (BS–) is introduced into CsPb(Br/I)3 NCs as multifunctional additive to simultaneously address the above challenging issues. Joint experiment‐theory characterizations reveal that the BS– can not only passivate the uncoordinated Pb2+‐related defects at the surface of NCs, but also increase the formation energy of halide vacancies. Moreover, because of the strong electron‐withdrawing property of sulfonate group, electrons are expected to transfer from the CsPb(Br/I)3 NC to BS– for reducing the self‐doping effect and altering the n‐type behavior of CsPb(Br/I)3 NCs to near ambipolarity. Eventually, synergistic boost in device performance is achieved for pure‐red PeLEDs with CIE coordinates of (0.70, 0.30) and a champion external quantum efficiency of 23.5%, which is one of the best value among the ever‐reported red PeLEDs approaching to the Rec. 2020 red primary color. Moreover, the BS–‐modified PeLED exhibits negligible wavelength shift under different operating voltages. This strategy paves an efficient way for improving the efficiency and stability of pure‐red PeLEDs.
Delayed Light‐Driven Actuations after Light Stopping
Authors: Hou Kai , Wu Jiaxin , Li Xingchao , Zhang Xuesen , Sun Yongqi , Long Yue , Song Kai 
Published: December 2022

AbstractThe manipulation of light actuators benefits from the advantages of the immediacy of light response. However, the immediacy of light response leads to indispensability of light irradiation in the actuating processes. The actuation after light irradiation stops, i.e., a delayed actuation can execute actuation functions, which is free of direct light irradiation. Here are proposed several delayed actuation systems after light irradiation based on intrinsic delay properties of shape memory alloy materials and additional regulation of soft silicone layers. Continuous motions after light stopping have been realized such as linear and rotating motions. Moreover, the delayed actuation relatively separates the irradiation and actuation, where an operational window period is allowed for task execution in light‐preventing scenarios. The delay principle of light actuation overcomes the limitation of immediate response of light manipulation, and is also applicable to more materials and systems.
Engineered Vasculogenic Extracellular Vesicles Drive Nonviral Direct Conversions of Human Dermal Fibroblasts into Induced Endothelial Cells and Improve Wound Closure
Authors: Rincon‐Benavides Maria A. , Mendonca Natalia Claire , Cuellar‐Gaviria Tatiana Z. , Salazar‐Puerta Ana I. , Ortega‐Pineda Lilibeth , Blackstone Britani N. , Deng Binbin , McComb David W , Gallego‐Perez Daniel , Powell Heather M. , Higuita‐Castro Natalia 
Published: December 2022

AbstractVasculogenic cell therapies have emerged as a powerful tool to increase vascularization and promote tissue repair/regeneration. Current approaches to cell therapies, however, rely mostly on progenitor cells, which pose significant risks (e.g., uncontrolled differentiation, tumorigenesis, and genetic/epigenetic abnormalities). Moreover, reprogramming methodologies used to generate induced endothelial cells (iECs) from induced pluripotent stem cells rely heavily on viral vectors, which pose additional translational limitations. This work describes the development of engineered human extracellular vesicles (EVs) capable of driving reprogramming‐based vasculogenic therapies without the need for progenitor cells and/or viral vectors. EVs are derived from primary human dermal fibroblasts (HDFs), and are engineered to pack transcription factor genes/transcripts of ETV2, FLI1, and FOXC2 (EFF). In addition to EFF, the engineered EVs are also loaded with transcripts of angiogenic factors (e.g., VEGF‐A, VEGF‐KDR, FGF2). In vitro and in vivo studies indicate that such EVs effectively transfected HDFs and drive direct conversions towards iECs within 7‐14 days. Finally, wound healing studies in mice indicate that engineered EVs lead to improved wound closure and vascularity. Altogether, these results show the potential of engineered human vasculogenic EVs to drive direct reprogramming processes of somatic cells towards iECs, and facilitate tissue repair/regeneration.
Boosted Output Voltage of BiSbTe‐Based Thermoelectric Generators via Coupled Effect between Thermoelectric Carriers and Triboelectric Charges
Authors: Kim Sun‐Woo , Kim Jin‐Kyeom , Park Ji Young , Mun Jinhong , Jung Sungwoo , Yang Seong Eun , Lee Geunsik , Lee Pooi See , Song Hyun‐Cheol , Yang Changduk , Park Hye Sung , Son Jae Sung , Baik Jeong Min 
Published: December 2022

AbstractThe present work demonstrates the very first approach to enhancing the output voltage of a thermoelectric generator by introducing highly charged polyimide‐based dielectrics. High charge density over 320 µC m−2 in C60‐containing block polyimide (PI‐b‐C60) having excellent charge retention characteristics is obtained through an ion injection process, attached at the cooling part of a thermoelectric generator consisting of Cu/p‐type BiSbTe/Au/Cr/SiO2/Si. This significantly increases the electric potential difference across the thermoelectric generator (TEG) from 4.2 to 8.2 mV at the temperature difference of 20 K, and this increase can be maintained over 1 day. Density functional theory studies support that the enhancement depends on the dielectric constant and the insulating properties of the dielectric. Finally, a TEG consisting of 81 p‐type BiSbTe legs with PI‐b‐C60 generates an output voltage of 0.632 V, and the charged energy of the 10 mF‐capacitor is boosted by 30 s. These results demonstrate the possibility of large‐area TEG fabrication without the need for modification of the TE materials by introducing a new mechanism which is based on the coupling effect between thermoelectric carriers and triboelectric charges.
Solid‐State Redox Mediators for Decoupled H2 Production: Principle and Challenges
Authors: Ma Yuanyuan , Wu Kangxi , Long Teng , Yang Jianping 
Published: December 2022

AbstractWater splitting driven by renewable energy is considered to be a promising approach for sustainable H2 production. However, the simultaneous generation of H2 and O2 requires the use of a membrane to prevent the gas mixing, which significantly limits the flexibility of H2/O2 separation and H2 transportation, impeding the direct use of renewable sources. In recent years, the concept of decoupled water electrolysis has been proposed along with the utilization of solid‐state redox mediators, by which the H2 and O2 generated at different times and spaces could be separated in absence of membrane. Here, a comprehensive overview of the decoupled water electrolysis using solid‐state redox mediators (SRMs) is presented. After a brief introduction, the SRMs are systematically summarized, including the structural features, the reaction mechanisms, and the properties of decoupled systems. In addition, the coupling of decoupled hydrogen production with other valuable reactions is also involved. Finally, this work discusses the challenges and perspectives for the decoupled water splitting system for commercialization and sustainable H2 production.
The atomic path for constructing single‐helical superstructure of AuCu bimetallic nanoclusters
Authors: Tang Ancheng , Cai Xiao , Liu Yong , Hou Jun , Liu Xu , Chen Mingyang , Zhu Yan 
Published: December 2022

AbstractSingle‐helical or double‐helical structures are common in living organisms. Helical assembly has been found in the artificial nanoparticles, but how they do so remains poorly understood. Here, we exploit atomically precise Au6Cu6 bimetallic nanoparticles (or called nanoclusters) as building blocks to construct a single‐helical Au12Cu12 superstructure in an operative path, thereby providing access to currently elusive mechanistic pathways. We propose that the thermodynamically viable linear‐to‐bent process at a couple of Au6Cu6 nanoclusters imparted by the organic ligands seems to be critical for the helical‐nanostructured arrangement of Au12Cu12. This study could help to offer a new design rule for the exquisitely helical structure assembled from the artificial nanoparticles.
Assessing the benefits of the marine protected area of Punta Coles, southern Peru (south‐east Pacific) on productivity of conspicuous benthic species using pre‐image population analysis
Authors: Tejada Alex , Baldarrago Danny , Pastor Ruslan , Ortiz Marco 
Published: December 2022

Abstract

The coastal marine protected ecosystem at Punta Coles (as a part of the Reserva Nacional de Islas, Islotes y Puntas Guaneras) is located in a highly exploited area in southern Peru and contains several commercial, bioengineering and other benthic species.
Pre‐image population analysis was used to estimate the transient values of intrinsic growth rate (r) based on biomass and density time series as a proxy of productivity to assess the effectiveness of protection.
The outcomes obtained showed that the gastropods Concholepas concholepas, Fissurella latimartiginata and the tunicate Purya chilensis showed a reduction of productivity during recent years, whilst the sea urchin Loxechinus albus, the barnacle Balanus laevis and the bivalve Semimytilus algosus showed an opposite pattern. Several species exhibited a chaotic dynamic, coinciding with the highest productivity values. In 2016 and 2017, several species exhibited a reduction of their abundance which could be delayed responses explained by changes in oceanographic conditions (reduction of coastal upwelling), La Niña event and illegal harvest.
The above notwithstanding, the results suggest that effective protection of benthic species in the protected ecosystem of Punta Coles have been partially accomplished. Therefore, this work could be considered a baseline study, permitting the subsequent monitoring of productivity of the main species inhabiting the coastal area of Punta Coles.
Pre‐image population analysis could be used as a complimentary analytical tool since it enables the evaluation of transient population parameters (e.g. productivity) thus aiding population management, conservation and monitoring decisions.
An SECM‐Based Spot Analysis for Redoxmer‐Electrode Kinetics: Identifying Redox Asymmetries on Model Graphitic Carbon Interfaces
Authors: Gaddam Raghuram , Sarbapalli Dipobrato , Howard Jason , Curtiss Larry A. , Assary Rajeev S. , Rodríguez‐López Joaquín 
Published: December 2022

AbstractThe fundamental process in non‐aqueous redox flow battery (NRFB) operation revolves around electron transfer (ET) between a current collector electrode and redox‐active organic molecules (redoxmers) in solution. Here, we present an approach utilizing scanning electrochemical microscopy (SECM) to evaluate interfacial ET kinetics between redoxmers and various electrode materials of interest at desired locations. This spot‐analysis method relies on the measurement of heterogeneous electron transfer rate constants (kf or kb) as a function of applied potential (E−E0′). As demonstrated by COMSOL simulations, this method enables the quantification of Butler‐Volmer kinetic parameters, the standard heterogeneous rate constant, k0, and the transfer coefficient, α. Our method enabled the identification of inherent asymmetries in the ET kinetics arising during the reduction of ferrocene‐based redoxmers, compared to their oxidation which displayed faster rate constants. Similar behavior was observed on a wide variety of carbon electrodes such as multi‐layer graphene, highly ordered pyrolytic graphite, glassy carbon, and chemical vapor deposition‐grown graphite films. However, aqueous systems and Pt do not exhibit such kinetic effects. Our analysis suggests that differential adsorption of the redoxmers is insufficient to account for our observations. Displaying a greater versatility than conventional electroanalytical methods, we demonstrate the operation of our spot analysis at concentrations up to 100 mM of redoxmer over graphite films. Looking forward, our method can be used to assess non‐idealities in a variety of redoxmer/electrode/solvent systems with quantitative evaluation of kinetics for applications in redox‐flow battery research.
A comparison of self‐report and discrepancy measures of camouflaging: Exploring sex differences in diagnosed autistic versus high autistic trait young adults
Authors: Milner Victoria , Colvert Emma , Mandy William , Happé Francesca 
Published: December 2022

AbstractCamouflaging describes masking or compensating for autistic traits and/or related difficulties. Some evidence suggests autistic females camouflage more than autistic males, potentially contributing to delayed or missed diagnosis. Studies predominantly adopt self‐report measures of camouflaging, potentially reflecting a person's intent to camouflage without accurately measuring effectiveness (i.e., success in fulfilling the intended effect of minimizing the appearance of autistic traits) of camouflaging. Discrepancy scores between underlying cognitive difficulties (e.g., theory of mind) and observed autistic traits (henceforth camoToM), or between self‐reported autistic traits and observed autistic traits (henceforth camoSRS), may provide a more accurate measure of camouflaging effectiveness. Three measures of camouflaging administered to autistic males (n = 46) and females (n = 40), and adults with equally high levels of autistic traits but no diagnosis (n = 45 males, n = 43 females) recruited from a large population‐based sample were compared. Self‐report measures of camouflaging were significantly correlated with camoSRS scores only. Both discrepancy scores were correlated with each other. Adults with high autistic traits, but no diagnosis, had higher discrepancy camouflaging scores than diagnosed adults, but self‐reported scores were similar. Diagnosed females scored higher than diagnosed males across all camouflaging measures, but no sex difference occurred in the high trait group. This might indicate that autistic females have higher intentions and greater effectiveness when camouflaging, compared with autistic males. For camoSRS only, high trait males scored significantly higher than diagnosed males; no group difference occurred for females. These results suggest that, despite all participants intending to camouflage to some extent, effective camouflaging as measured by discrepancy scores is higher in undiagnosed high autistic trait individuals. One interpretation is that effective camouflaging reduces the likelihood of autism diagnosis in males and females with high autistic traits.
Aufstockungen auf Siedlungsbauten der 1950er‐ und 1960er‐Jahre – Eine Potenzialanalyse am Fallbeispiel Hamburger Wohnungsgenossenschaftsbauten
Authors: Meyer Kathrin , Klotz Peter‐Matthias 
Published: December 2022

AbstractAngesichts der wachsendenden Haushaltszahl in deutschen Großstädten mit einhergehender Wohnungsnachfrage sowie des hohen Flächen‐ und Ressourcenverbrauchs im Neubau wird am Fallbeispiel der Stadt Hamburg das Potenzial der Nachverdichtung durch Aufstockung untersucht. Ausgangslage bildet die These, dass drei‐ bis viergeschossige Siedlungsbauten der 1950er‐ und 1960er‐Jahre aufgrund ausreichender Lastreserven und der Abstände zu angrenzender Bebauung gute Voraussetzungen für ein‐ bis zweigeschossige Aufstockungen bieten. Untersuchungsgegenstand sind Mehrfamilienwohngebäude Hamburger Wohnungsbaugenossenschaften. Der Aufsatz soll Entscheidungsgrundlagen für zukünftige Aufstockungsvorhaben auf drei‐ bis viergeschossigen Siedlungsbauten zur Verfügung stellen. Die Aufstockungspotenzialanalyse erfolgt in drei Betrachtungsebenen: Stadt, Gebäude und Konstruktion. Auf der Ebene Stadt wurde das quantitative Potenzial für Wohnungsneubauten durch Aufstockung auf den o. g. Gebäuden anhand von digitalem Karten‐ und Bildmaterial untersucht und somit die Relevanz bestätigt. Für die Gebäudeebene wurden Wohngebäudetypologien anhand von Bestandsplänen definiert. Auf der Ebene Konstruktion wurden anhand von Bestandsstatiken vorhandene Lastreserven analysiert. Ausgehend von der Wohngebäudetypologie sowie den rechtlichen und bautechnischen Vorgaben können mithilfe der formulierten Entscheidungsgrundlagen Annahmen zu Aufstockungsmöglichkeiten getroffen und Handlungsoptionen hergeleitet werden.
Advances in MoS2based Hollow Structural Materials for High‐Performance Metal‐Ion Batteries
Authors: Zhang Hui , Wang Yashi , Guo Shilong , Hui Yiqing , Wei Hanyue , Song Jianjun , Zhao Xiaoxian 
Published: December 2022

AbstractThe construction of a hollow structure could promote the diffusion of electrons and ions to improve the electrochemical performance of MoS2based materials for metal‐ion batteries. Herein, we summarize the preparation technique of MoS2hollow structural materials with different dimensions. The approaches to construct 0D hollow MoS2materials for electrodes of metal‐ion batteries can be divided into the hard template approach, soft template approach, self‐template approach, and template‐free approach. Among them, the hard template approach and self‐sacrifice template approach are controllable but complicated, the soft template approach and template‐free approach are simple and scalable but not controllable. Furthermore, as the electrode material of metal‐ion batteries including lithium‐ion battery, sodium‐ion battery, potassium‐ion battery or magnesium‐ion battery, the 0D hollow structural MoS2based materials could improve the diffusion kinetics of ion and electron and restrict the stack of MoS2. Furthermore, the 1D hollow MoS2can provide oriented electron diffusion along with the axial direction, and the 3D hollow MoS2can offer perforative pores for permeation of electrolytes and more active sites, which results in excellent rate capability and cycling stability. This paper could give inspiration for constructing MoS2hollow structural materials with different dimensions and provide a constructive suggestion for synthesizing hollow materials with excellent electrochemical performance.