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Chiral phosphoric acid-catalyzed asymmetric synthesis of helically chiral, planarly chiral and inherently chiral molecules. 手性磷酸催化螺旋手性、平面手性和固有手性分子的不对称合成。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-10 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.145
Wei Liu, Xiaoyu Yang
{"title":"Chiral phosphoric acid-catalyzed asymmetric synthesis of helically chiral, planarly chiral and inherently chiral molecules.","authors":"Wei Liu, Xiaoyu Yang","doi":"10.3762/bjoc.21.145","DOIUrl":"10.3762/bjoc.21.145","url":null,"abstract":"<p><p>Chiral molecules, distinguished by nonsuperimposability with their mirror image, play crucial roles across diverse research fields. Molecular chirality is conventionally categorized into the following types: central chirality, axial chirality, planar chirality and helical chirality, along with the more recently introduced inherent chirality. As one of the most prominent chiral organocatalysts, chiral phosphoric acid (CPA) catalysis has proven highly effective in synthesizing centrally and axially chiral molecules. However, its potential in the asymmetric construction of other types of molecular chirality has been investigated comparatively less. This Review provides a comprehensive overview of the recent emerging advancements in asymmetric synthesis of planarly chiral, helically chiral and inherently chiral molecules using CPA catalysis, while offering insights into future developments within this domain.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1864-1889"},"PeriodicalIF":2.1,"publicationDate":"2025-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12434929/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145074309","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Systematic pore lipophilization to enhance the efficiency of an amine-based MOF catalyst in the solvent-free Knoevenagel reaction. 在无溶剂Knoevenagel反应中提高胺基MOF催化剂效率的系统孔脂化。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-09 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.144
Pricilla Matseketsa, Margret Kumbirayi Ruwimbo Pagare, Tendai Gadzikwa
{"title":"Systematic pore lipophilization to enhance the efficiency of an amine-based MOF catalyst in the solvent-free Knoevenagel reaction.","authors":"Pricilla Matseketsa, Margret Kumbirayi Ruwimbo Pagare, Tendai Gadzikwa","doi":"10.3762/bjoc.21.144","DOIUrl":"10.3762/bjoc.21.144","url":null,"abstract":"<p><p>We systematically lipophilized an amine-based metal-organic framework (MOF) catalyst and applied the functionalized MOFs to the Knoevenagel condensation reaction. A well-defined MOF material composed of both amine- and hydroxy-bearing linkers was reacted with a series of aliphatic isocyanates (isopropyl, <i>tert</i>-butyl, <i>n</i>-hexyl, and tetradecyl) and, incongruously, was found to preferentially react at the hydroxy groups. This selective functionalization yielded MOFs in which the catalytically active amines are confined within highly lipophilic pores, reminiscent of many enzyme active sites. We determined that systematically increasing the lipophilicity of the pores results in a commensurate increase of catalyst efficiency.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1854-1863"},"PeriodicalIF":2.1,"publicationDate":"2025-09-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12434926/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145074342","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Photoswitches beyond azobenzene: a beginner's guide. 除偶氮苯外的光开关：初学者指南。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-08 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.143
Michela Marcon, Christoph Haag, Burkhard König
{"title":"Photoswitches beyond azobenzene: a beginner's guide.","authors":"Michela Marcon, Christoph Haag, Burkhard König","doi":"10.3762/bjoc.21.143","DOIUrl":"10.3762/bjoc.21.143","url":null,"abstract":"<p><p>Approaching the vast, colourful world of photoswitches from a different field of study or as an undergraduate student may be overwhelming: azobenzene is undoubtedly the most famous due to its easy synthesis and the extensively studied properties. However, there are several photoswitch classes beyond azobenzene with interesting properties that can be tailored to meet one's needs. In this tutorial review, we aim to explain the important terminology and discuss the synthesis, switching mechanisms, and properties of seven interesting photoswitch classes, namely azoheteroarenes, diazocines, indigoid photoswitches, arylhydrazones, diarylethenes, fulgides, and spiropyrans.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1808-1853"},"PeriodicalIF":2.1,"publicationDate":"2025-09-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12434931/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145074333","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
[3 + 2] Cycloaddition of thioformylium methylide with various arylidene-azolones in the synthesis of 7-thia-3-azaspiro[4.4]nonan-4-ones. [3 + 2]甲基硫代甲酰基与各种芳基唑酮环加成合成7-噻亚-3-氮杂螺[4.4]壬-4-酮。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-05 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.141
Daniil I Rudik, Irina V Tiushina, Anatoly I Sokolov, Alexander Yu Smirnov, Alexander R Romanenko, Alexander A Korlyukov, Andrey A Mikhaylov, Mikhail S Baranov
{"title":"[3 + 2] Cycloaddition of thioformylium methylide with various arylidene-azolones in the synthesis of 7-thia-3-azaspiro[4.4]nonan-4-ones.","authors":"Daniil I Rudik, Irina V Tiushina, Anatoly I Sokolov, Alexander Yu Smirnov, Alexander R Romanenko, Alexander A Korlyukov, Andrey A Mikhaylov, Mikhail S Baranov","doi":"10.3762/bjoc.21.141","DOIUrl":"10.3762/bjoc.21.141","url":null,"abstract":"<p><p>Thioformylium methylide, which is readily generated from chloromethyl(trimethylsilyl)methyl sulfide by the action of fluoride, is used for the synthesis of spirocyclic derivatives from arylidene-azolones. Four types of the corresponding heterocycles have been studied. A series of 7-thia-3-azaspiro[4.4]nonan-4-ones was obtained with yields varying from 17 to 99%. The stereochemical study revealed selective formation of single either <i>cis</i> or <i>trans</i> stereoisomers, dependent on the heterocycle core used.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1791-1798"},"PeriodicalIF":2.1,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415905/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028890","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Fe-catalyzed efficient synthesis of 2,4- and 4-substituted quinolines via C(sp2)-C(sp2) bond scission of styrenes. 苯乙烯的C(sp2)-C（sp2）键裂解在铁催化下高效合成2,4-和4-取代喹啉。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-05 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.142
Prafull A Jagtap, Manish M Petkar, Vaishnavi R Sawant, Bhalchandra M Bhanage
{"title":"Fe-catalyzed efficient synthesis of 2,4- and 4-substituted quinolines via C(sp<sup>2</sup>)-C(sp<sup>2</sup>) bond scission of styrenes.","authors":"Prafull A Jagtap, Manish M Petkar, Vaishnavi R Sawant, Bhalchandra M Bhanage","doi":"10.3762/bjoc.21.142","DOIUrl":"10.3762/bjoc.21.142","url":null,"abstract":"<p><p>Herein, we report a highly efficient, environmentally benign protocol for the domino synthesis of 2,4-disubstituted and 4-substituted quinoline molecules. The developed strategy involves an earth-abundant Fe-catalyzed C(sp<sup>2</sup>)-C(sp<sup>2</sup>) bond cleavage of styrene, followed by the hydroamination of the cleaved synthons with arylamines and subsequent C-H annulation to yield two valuable quinoline derivatives. Key features of this protocol include the use of O<sub>2</sub> as an ideal, green oxidant, operational simplicity and scalability, high atom- and step-economy, and cost-effectiveness, collectively enabling the single-step synthesis of two medicinally relevant N-heterocycles in excellent combined yields.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1799-1807"},"PeriodicalIF":2.1,"publicationDate":"2025-09-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415914/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028823","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Synthesis of chiral cyclohexane-linked bisimidazolines. 手性环己烷连接双咪唑啉的合成。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-04 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.140
Changmeng Xi, Qingshan Sun, Jiaxi Xu
{"title":"Synthesis of chiral cyclohexane-linked bisimidazolines.","authors":"Changmeng Xi, Qingshan Sun, Jiaxi Xu","doi":"10.3762/bjoc.21.140","DOIUrl":"10.3762/bjoc.21.140","url":null,"abstract":"<p><p>Both chiral bisoxazolines and bisimidazolines are efficient chiral ligands in metal-catalyzed asymmetric organic transformations. Chiral cyclohexane-linked bisimidazolines were prepared from optically active cyclohexane-1,2-dicarboxylic acid and 1,2-diphenylethane-1,2-diamines via the monosulfonylation of 1,2-diphenylethane-1,2-diamines, condensation of <i>N</i>-sulfonylated 1,2-diphenylethane-1,2-diamines and cyclohexane-1,2-dicarboxylic acid, and the final cyclization with the in situ generated Hendrickson reagent.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1786-1790"},"PeriodicalIF":2.1,"publicationDate":"2025-09-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415896/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028830","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Research progress on calixarene/pillararene-based controlled drug release systems. 杯芳烃/柱芳烃类药物控释系统的研究进展。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-03 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.139
Liu-Huan Yi, Jian Qin, Si-Ran Lu, Liu-Pan Yang, Li-Li Wang, Huan Yao
{"title":"Research progress on calixarene/pillararene-based controlled drug release systems.","authors":"Liu-Huan Yi, Jian Qin, Si-Ran Lu, Liu-Pan Yang, Li-Li Wang, Huan Yao","doi":"10.3762/bjoc.21.139","DOIUrl":"10.3762/bjoc.21.139","url":null,"abstract":"<p><p>Intelligent controlled-release drug delivery systems that are responsive to various external stimuli have garnered significant interest from researchers and have broad applications in the biomedical field. Aromatic macrocycles, including calixarenes and pillararenes, are considered ideal candidates for the construction of supramolecular drug delivery systems because of their simple synthesis, ease of modification, electron-rich and hydrophobic cavities, and highly selective molecular recognition. In recent years, numerous supramolecular drug delivery systems utilizing aromatic macrocycles have been developed. This review article provides an overview of the advancements of controlled drug release systems based on host-guest selective recognition, self-assembly, and nano-valves by the use of of calixarenes and pillararenes from five perspectives: pH, light, enzyme, hypoxia, and multi-stimuli combination responses. Furthermore, the article projects the future clinical application prospects of controlled-release technologies, with the aim of offering a reference for the utilization of aromatic macrocycles in drug-controlled release applications.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1757-1785"},"PeriodicalIF":2.1,"publicationDate":"2025-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415917/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Unique halogen-π association detected in single crystals of C-N atropisomeric N-(2-halophenyl)quinolin-2-one derivatives and the thione analogue. N-（2-卤代苯基）喹啉-2- 1衍生物和硫酮类似物单晶中独特的卤素-π缔合。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-09-01 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.138
Mai Uchibori, Nanami Murate, Kanako Shima, Tatsunori Sakagami, Ko Kanehisa, Gary James Richards, Akiko Hori, Osamu Kitagawa
{"title":"Unique halogen-π association detected in single crystals of C-N atropisomeric <i>N</i>-(2-halophenyl)quinolin-2-one derivatives and the thione analogue.","authors":"Mai Uchibori, Nanami Murate, Kanako Shima, Tatsunori Sakagami, Ko Kanehisa, Gary James Richards, Akiko Hori, Osamu Kitagawa","doi":"10.3762/bjoc.21.138","DOIUrl":"10.3762/bjoc.21.138","url":null,"abstract":"<p><p>In single crystals of C-N atropisomeric <i>N</i>-(2-halophenyl)quinolin-2-one and the thione analogue, a unique association based on a halogen-π interaction was detected. In racemic and optically pure <i>N</i>-(2-bromo- or 2-chlorophenyl)quinolin-2-ones, homochiral layered polymers, which consist of (<i>P</i>)- or (<i>M</i>)-atropisomers, were formed through intermolecular halogen-π association. The halogen-π association in the racemates is due to a halogen bond (C-X···π) between a σ-hole on the halogen atom and a π-electron on the quinolinone benzene ring, while that in optically pure forms is caused by an n-π* interaction between a lone electron pair on the halogen atom and a π* orbital of the quinolinone. In contrast to the formation of the homochiral layered polymer in quinolinones, in racemic <i>N</i>-(2-bromophenyl)quinoline-2-thione, heterochiral layered polymers, in which (<i>P</i>)- and (<i>M</i>)-atropisomers were alternately connected, were formed through an n-π* interaction between a lone electron pair on the bromine atom and a π* orbital of the quinoline-2-thione.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1748-1756"},"PeriodicalIF":2.1,"publicationDate":"2025-09-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415909/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028852","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Preparation of a furfural-derived enantioenriched vinyloxazoline building block and exploring its reactivity. 糠醛衍生富集对映体的乙烯基氯唑啉基块的制备及其反应性研究。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-08-29 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.136
Madara Darzina, Anna Lielpetere, Aigars Jirgensons
{"title":"Preparation of a furfural-derived enantioenriched vinyloxazoline building block and exploring its reactivity.","authors":"Madara Darzina, Anna Lielpetere, Aigars Jirgensons","doi":"10.3762/bjoc.21.136","DOIUrl":"10.3762/bjoc.21.136","url":null,"abstract":"<p><p><i>N-</i>Alloc-protected furfuryl amino alcohols derived from furfural and ʟ- or ᴅ-valinol were subjected to Torii-type ester electrosynthesis to obtain the corresponding unsaturated esters. These served as key intermediates to prepare (<i>S</i>)- and <i>(R)-</i>enantioenriched unsaturated amides by <i>N</i>-Alloc deprotection which induced concomitant methoxymethyl group cleavage, <i>O-</i>to-<i>N</i> rearrangement, and isomerization of the double bond. An oxazoline ring formation in the resulting unsaturated amides provided the corresponding enantioenriched vinyloxazoline. The reactivity of the electron-deficient double bond in the vinyloxazoline was explored in several reactions. Out of these, the aza-Diels-Alder reaction with TsNCO was successful, leading to a highly diastereoselective formation of an oxazolo[3,2-<i>c</i>]pyrimidine derivative.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1737-1741"},"PeriodicalIF":2.1,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415904/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028881","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Thermodynamics and polarity-driven properties of fluorinated cyclopropanes. 氟化环丙烷的热力学和极性驱动性质。
IF 2.1 4区 化学
Beilstein Journal of Organic Chemistry Pub Date : 2025-08-29 eCollection Date: 2025-01-01 DOI: 10.3762/bjoc.21.137
Matheus P Freitas
{"title":"Thermodynamics and polarity-driven properties of fluorinated cyclopropanes.","authors":"Matheus P Freitas","doi":"10.3762/bjoc.21.137","DOIUrl":"10.3762/bjoc.21.137","url":null,"abstract":"<p><p>Cyclopropane is a significant alicyclic motif, widely utilized in medicinal chemistry, while fluorination serves as a powerful tool to modulate properties that enhance the performance of pharmaceuticals and materials. This quantum-chemical study explores the energetic implications of fluorinating cyclopropane, providing insights into molecular characteristics arising from the polar C-F bond. Isodesmic reactions revealed that the conversion of cyclopropane and methyl fluoride into mono-, di-, tri-, tetra-, penta-, and hexafluorinated cyclopropanes is exothermic, except for the all-<i>cis</i>-1,2,3-trifluorocyclopropane (<b>1.2.3-c.c.</b>). Compounds featuring geminal fluorines are particularly stabilized due to anomeric-like <i>n</i> <sub>F</sub> → σ*<sub>CF</sub> interactions. Generally, <i>cis</i>-C-F bonds are less favored than their <i>trans</i> counterparts, not primarily because of steric repulsion, but due to reduced stabilizing electron-delocalization interactions. Among the series, <b>1.2.3-c.c.</b> stands out as the most polar compound, enabling unique stacking interactions between its electrostatically complementary negative and positive faces. These interactions are mediated through electrostatic hydrogen bonds. This \"Janus-like\" polarity also facilitates interactions with ions, particularly sodium and chloride. These findings contribute valuable insights for the rational design of drugs and advanced materials, particularly those whose properties rely on the polarity and spatial arrangement of C-F bonds within a cyclopropane framework.</p>","PeriodicalId":8756,"journal":{"name":"Beilstein Journal of Organic Chemistry","volume":"21 ","pages":"1742-1747"},"PeriodicalIF":2.1,"publicationDate":"2025-08-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12415895/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"145028899","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
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