Chemistry - An Asian Journal最新文献

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Recent Advances in Nitrene Chemistry with Emerging Precursors.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401521
Ming Bao, Shanliang Dong, Kewei Chen, Xinfang Xu
{"title":"Recent Advances in Nitrene Chemistry with Emerging Precursors.","authors":"Ming Bao, Shanliang Dong, Kewei Chen, Xinfang Xu","doi":"10.1002/asia.202401521","DOIUrl":"https://doi.org/10.1002/asia.202401521","url":null,"abstract":"<p><p>Nitrene-transfer reaction is one of the powerful synthetic tools in organic chemistry, facilitating a vast array of otherwise unattainable chemical transformations. Different types of nitrene precursors have been exploited and successfully applied in a variety of nitrene-based transformations for the direct construction of nitrogen-containing compounds with structural complexity. Although a few of review articles that focus on the specific nitrene precursors or different type of nitrene reactions have been reported, significant advancements have emerged over the past two decades driven by the introduction and application of novel nitrene precursors, enabling a variety of catalytic transformations for the synthesis of N-heterocyclic frameworks with structural diversity. Thus, a review paper that underscores the progress in nitrene chemistry by focusing on the advancements in nitrene precursors would be timely and highly desirable. In this review article, the advancements in nitrene chemistry, particularly those achieved with newly developed nitrene precursors over the past two decades, have been summarized. The presentation is organized by the type of precursor and further subdivided based on different nitrene reactions by focusing on the key mechanistic aspects, limitation, and synthetic capacity.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401521"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363376","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Ionic Device: From Neuromorphic Computing to Interfacing with the Brain.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401170
Zijia Huang, Tingting Mei, Xinyi Zhu, Kai Xiao
{"title":"Ionic Device: From Neuromorphic Computing to Interfacing with the Brain.","authors":"Zijia Huang, Tingting Mei, Xinyi Zhu, Kai Xiao","doi":"10.1002/asia.202401170","DOIUrl":"https://doi.org/10.1002/asia.202401170","url":null,"abstract":"<p><p>In living organisms, the modulation of ion conductivity in ion channels of neuron cells enables intelligent behaviors, such as generating, transmitting, and storing neural signals. Drawing inspiration from these natural processes, researchers have fabricated ionic devices that replicate the functions of the nervous system. However, this field remains in its infancy, necessitating extensive foundational research in ionic device preparation, algorithm development, and biological interaction. This review summarizes recently developed neuromorphic ionic devices into three categories based on the materials states: liquid, semi-solid, and solid. The neural network algorithms embedded in these devices for neuromorphic computing are introduced, and future directions for the development of bidirectional human-computer interaction and hybrid human-computer intelligence are discussed.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401170"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254116","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Effect of Carbon Nanomaterials Incorporated Polymeric Membrane Separators for Energy Storage Devices.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401618
Md Emdad Hossain, Bashir Ahmed Johan, Syed Shaheen Shah, Muaz Abdallah, Mohammad Mizanur Rahman, Turki Nabieh Baroud, Md Abdul Aziz
{"title":"Effect of Carbon Nanomaterials Incorporated Polymeric Membrane Separators for Energy Storage Devices.","authors":"Md Emdad Hossain, Bashir Ahmed Johan, Syed Shaheen Shah, Muaz Abdallah, Mohammad Mizanur Rahman, Turki Nabieh Baroud, Md Abdul Aziz","doi":"10.1002/asia.202401618","DOIUrl":"https://doi.org/10.1002/asia.202401618","url":null,"abstract":"<p><p>The rapid expansion of the global population and technological advancements have heightened the need for efficient energy conversion and electrochemical energy storage. Electrochemical energy systems like batteries and supercapacitors have seen notable development to meet this demand. However, conventional polymeric membrane separators in these systems face challenges due to limited porosity and poor mechanical and thermal properties, reducing overall electrochemical performance. Researchers have incorporated nanoparticles into the polymer matrix to address these limitations and enhance separator properties. Carbon-based nanomaterials, in particular, have gained prominence due to their unique features, such as surface-dependent characteristics, size, porosity, morphology, and electrical conductivity. These properties make carbon-based nanomaterials advantageous in improving energy storage compared to conventional materials. Advanced carbon-doped polymeric membrane separators have emerged as a potential solution to the issues faced by conventional separators. Adding carbon nanoparticles, such as graphene-based materials and carbon nanotubes to the polymeric separators of batteries and supercapacitors has helped researchers solve problems and improve the electrochemical performance. This review article provides a state-of-the-art overview of carbon-doped polymeric membrane separators, their properties, fabrication processes, and performance in lithium batteries, as well as supercapacitors. It emphasizes advantages of these novel separator materials and suggests future research directions in this field.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401618"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254115","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Impact of Membership Functions on the Performance of AI-Assisted Neuro-Fuzzy System for Analysis of Anion-Responsive Behaviours of Polypyridyl-Imidazole Based Ru(II) Receptors.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401346
Anik Sahoo, Manoranjan Bar, Sohini Bhattacharya, Sujoy Baitalik
{"title":"Impact of Membership Functions on the Performance of AI-Assisted Neuro-Fuzzy System for Analysis of Anion-Responsive Behaviours of Polypyridyl-Imidazole Based Ru(II) Receptors.","authors":"Anik Sahoo, Manoranjan Bar, Sohini Bhattacharya, Sujoy Baitalik","doi":"10.1002/asia.202401346","DOIUrl":"https://doi.org/10.1002/asia.202401346","url":null,"abstract":"<p><p>This study explores the anion sensing properties of mono-, bi-, and trinuclear Ru(II) complexes based on polypyridyl-imidazole ligands with varying numbers of dissociable protons in their secondary coordination sphere. The imidazole protons, influenced by the Ru<sup>2+</sup> centers, facilitate interactions with anions like F<sup>-</sup> and CN<sup>-</sup> in acetonitrile, and CN<sup>-</sup> in water, through hydrogen bonding or via proton abstraction. The spectral properties of the metalloreceptors change in the presence of these anions, and the initial state can be restored with acid, allowing recycling. The complexes exhibit Boolean logic functions (Implication logic gates) using spectral outputs in the presence of specific anions and acids. To address the time and cost constraints of executing comprehensive sensing experiments, an adaptive neuro-fuzzy inference system (ANFIS) with five membership functions (triangular, trapezoidal, generalized bell-shaped, Gaussian, and pi-shaped) was used to predict experimental data and appropriate modeling of the sensing characteristics. Comparison of ANFIS model outputs with experimental data showed a good correlation, with the Gaussian and generalized bell-shaped functions providing high accuracy and close resemblance to experimental data. This neuro-fuzzification approach promises accurate prediction and modeling of sensing data for Ru(II)-based metalloreceptors.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401346"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363374","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Regioselective C-H Thio- and Selenocyanation of Pyrazolo[1,5-a]pyrimidines.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401610
Tanmay Chatterjee, Paramita Pattanayak, Harshil Khandelwal, Shreeja Basappa
{"title":"Regioselective C-H Thio- and Selenocyanation of Pyrazolo[1,5-a]pyrimidines.","authors":"Tanmay Chatterjee, Paramita Pattanayak, Harshil Khandelwal, Shreeja Basappa","doi":"10.1002/asia.202401610","DOIUrl":"https://doi.org/10.1002/asia.202401610","url":null,"abstract":"<p><p>Herein, we report a metal-free, N-chlorosuccinamide (NCS)-mediated, highly efficient, and regioselective C-H thio- and selenocyanation of pyrazolo[1,5-a]pyrimidines using KSCN and KSeCN respectively. The transformation required only NCS (1 equiv) and operated under mild conditions such as ambient temperature and aerobic atmosphere. This method was found to be highly efficient for the C-H thiocyanation of pyrazolo[1,5-a]pyrimidines as compared to our previously developed photocatalytic strategy and also enabled the C-H selenocyanation of the substrates to access 3-selenocyanatopyrazolo[1,5-a]pyrimidines, for the first time, which was unexplored or unsuccessful so far. A wide variety of new pyrazolo[1,5-a]pyrimidines bearing -SCN or -SeCN functional groups were synthesized in good to excellent yield. The developed protocol features a broad substrate scope, high functional group tolerance, mild conditions, high to excellent yield of products, efficient scalability, and synthetic diversifications of products. Mechanistic studies revealed an ionic pathway for this reaction.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401610"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254118","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Dipicolylaminofluorene Derivatives for Fluorescent Sensing of Copper(II) Ion and Glyphosate.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401622
Komthep Silpcharu, Quynh Nguyen Nhu Pham, Mongkol Sukwattanasinitt, Paitoon Rashatasakhon
{"title":"Dipicolylaminofluorene Derivatives for Fluorescent Sensing of Copper(II) Ion and Glyphosate.","authors":"Komthep Silpcharu, Quynh Nguyen Nhu Pham, Mongkol Sukwattanasinitt, Paitoon Rashatasakhon","doi":"10.1002/asia.202401622","DOIUrl":"https://doi.org/10.1002/asia.202401622","url":null,"abstract":"<p><p>The contamination of water by toxic herbicides poses a significant environmental challenge, necessitating the development of reliable detection tools. In this study, novel dipicolylamino derivatives of fluorene and fluorenone were synthesized via Sonogashira cross-coupling reactions with high yields. These compounds demonstrated exceptional selectivity for fluorescence turn-off by Cu(II) ions, with detection limits of 0.99 μM and 1.11 μM in a DMSO-HEPES buffer system. Investigations using Job's plot, fluorescence recovery with EDTA, and mass spectrometry revealed that the sensing mechanism involves complexation between the compounds and Cu(II) ions. Notably, the Cu(II)-fluorene complex exhibited a selective fluorescence turn-on response to glyphosate, achieving a detection limit of 0.93 μM. Quantitative analysis in real water samples demonstrated good recovery rates, underscoring the practical utility of these fluorene and fluorenone derivatives in environmental monitoring.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401622"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Rhodamine-and-Naphthalimide Based Dual-chromophore for Fast and Sensitive Detection of Nerve-agent Mimic and Real Nerve Agents.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-06 DOI: 10.1002/asia.202401491
Rongxin Wang, Shanshan Liu, Xubin Wang, Molin Qin, Zhen Yan, Min Qiao, Liping Ding, Jinglin Kong, Yu Fang
{"title":"A Rhodamine-and-Naphthalimide Based Dual-chromophore for Fast and Sensitive Detection of Nerve-agent Mimic and Real Nerve Agents.","authors":"Rongxin Wang, Shanshan Liu, Xubin Wang, Molin Qin, Zhen Yan, Min Qiao, Liping Ding, Jinglin Kong, Yu Fang","doi":"10.1002/asia.202401491","DOIUrl":"https://doi.org/10.1002/asia.202401491","url":null,"abstract":"<p><p>For the sake of public safety and citizen health, the development of efficient and portable detection devices to nerve agents is critical. In this investigation, a naphthalimide-rhodamine based dual-chromophore, RNI-P, was synthesized and applied to detect nerve-agent mimic diethyl chlorophosphate (DCP) and real nerve agents. The probe exhibits inherently weak fluorescence due to the PET processes from both piperazine and rhodamine units to the naphthalimide unit. It shows rapid fluorescence enhancement to DCP in aqueous solution, demonstrating exceptional sensitivity and selectivity. Furthermore, the probe-inked paper strip can also rapidly respond to DCP vapor when integrated into a lab-made portable sensing platform. The detection limit to DCP vapor can be as low as 130 ppb. Most notably, the probe is capable of quickly and effectively detecting real nerve agents such as sarin and soman in aqueous solution, highlighting its significant potential for practical use. The turn-on responses are attributed to the prohibition of PET processes through protonation of the probe. This study reveals that not only the usual nucleophilic groups but also a second fluorophore can cause effective PET process to the core chromophore and empowers the probe with strong potential for efficient detection of nerve agents.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401491"},"PeriodicalIF":3.5,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143363372","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Twists and Loops: Exploring Lemniscular Vinylogous Benzioctaphyrin(2.0.1.0.2.0.1.0).
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-05 DOI: 10.1002/asia.202401548
Rampal Vishwakarma, Narayan Ch Jana, Mainak Das, Alagar Srinivasan
{"title":"Twists and Loops: Exploring Lemniscular Vinylogous Benzioctaphyrin(2.0.1.0.2.0.1.0).","authors":"Rampal Vishwakarma, Narayan Ch Jana, Mainak Das, Alagar Srinivasan","doi":"10.1002/asia.202401548","DOIUrl":"https://doi.org/10.1002/asia.202401548","url":null,"abstract":"<p><p>Octaphyrins, offer unparalleled opportunities for designing complex molecular architectures with distinct physical and chemical properties. However, lemniscate-shaped benzioctaphyrins remain scantily explored, leaving a gap in understanding how this unconventional geometry/shape influences macrocyclic behaviour. In this study, we explore the design, synthesis, and structural properties of benzioctaphyrin by incorporating the bis-E-stilbene unit, where a vinylene π-bridge connects phenylene rings. The benzioctaphyrin(2.0.1.0.2.0.1.0) adopts a lemniscate topology to alleviate steric strain, with protonation inducing conformational desymmetrization. The presence of a meta-phenylene unit thwarts the global π-conjugation, rendering the macrocycle nonaromatic. Notably, this work represents the first exploration of the oligomeric vinylene group in benzioctaphyrin framework. It offers new insights into how structural modifications influence topology, π-electron delocalization, and macrocyclic flexibility, setting the stage for future advancements in topologically unique porphyrinoid systems.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401548"},"PeriodicalIF":3.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187721","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
MXenes: Are They Ready for Direct Air Capture of CO2?
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-05 DOI: 10.1002/asia.202401822
Konok Chandra Bhowmik, Md Arafat Rahman, Yunus Ahmed, Tasmia Binte Hai
{"title":"MXenes: Are They Ready for Direct Air Capture of CO2?","authors":"Konok Chandra Bhowmik, Md Arafat Rahman, Yunus Ahmed, Tasmia Binte Hai","doi":"10.1002/asia.202401822","DOIUrl":"https://doi.org/10.1002/asia.202401822","url":null,"abstract":"<p><p>Although Direct Air Capture (DAC) of CO2 is a potential technology for climate change mitigation, the cost, scalability, and efficiency of existing materials and techniques are severely limited. MXenes, a type of two-dimensional materials, have drawn interest due to their remarkable conductivity, enormous surface area, and adjustable chemistry, however, their potential for DAC has not yet been thoroughly investigated. Recent developments in MXene synthesis and functionalization are comprehensively reviewed, with an emphasis on how these characteristics might be used to enhance improve CO2 adsorption and capture efficiency. In addition, the difficulties of stability, scalability, and economic feasibility for real-world applications are evaluated. Our findings demonstrate the great potential of MXenes for DAC and offer fresh perspectives on how their special qualities might overcome current constraints. This study presents a new viewpoint on MXenes as a feasible CO2 capture option, indicating new avenues for future research and development, even though further optimization is required.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401822"},"PeriodicalIF":3.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143254117","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Intricacies of Carbon Dot Photoluminescence for Emerging Applications: A Review.
IF 3.5 3区 化学
Chemistry - An Asian Journal Pub Date : 2025-02-05 DOI: 10.1002/asia.202401470
Nilanjana Nandi, Priyanka Sarkar, Neha Barnwal, Kalyanasis Sahu
{"title":"Intricacies of Carbon Dot Photoluminescence for Emerging Applications: A Review.","authors":"Nilanjana Nandi, Priyanka Sarkar, Neha Barnwal, Kalyanasis Sahu","doi":"10.1002/asia.202401470","DOIUrl":"https://doi.org/10.1002/asia.202401470","url":null,"abstract":"<p><p>Discovered in 2004, carbon dots (CDs) have already traversed a long journey, generating many promising research directions. Its cheapness, ease of synthesis, high water-solubility, tunable emission, and excellent biocompatibility make it a single-point solution to many problems, and tremendous efforts were invested into understanding the structure-property-function relationship, which eases the engineering of the CD properties suitable for a desired application. From the usual random choice of precursors or carbon materials as a starting point in the early days, more systematic approaches are now available for choosing proper starting materials and appropriate experimental conditions (solvent medium, reaction temperature, reaction duration, pH, etc) to customize its photoluminescence. The presence of impurities has a crucial role in the outcome and applicability of photoluminescence. Recently, a significant focus has been on the long-wavelength emissive CDs, particularly in the red to near-infrared (NIR) regions, for better penetration into live cells and to circumvent autofluorescence problems. Proper design can harvest phosphorescence from CDs. Many excellent reviews are available, focusing on different facets of CD prospects. Hence, we will only highlight the importance of the optical properties of CDs. We will mention some of the new works that have appeared in the last five years.</p>","PeriodicalId":145,"journal":{"name":"Chemistry - An Asian Journal","volume":" ","pages":"e202401470"},"PeriodicalIF":3.5,"publicationDate":"2025-02-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143187622","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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