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Cover Feature: Anticipating Natural Phenolics Through Visible Light-Induced Photorearrangement of Quinones (ChemistryEurope 2/2025)
ChemistryEurope Pub Date : 2025-03-10 DOI: 10.1002/ceur.202580202
Alexander A. Fadeev, Martin Kotora
{"title":"Cover Feature: Anticipating Natural Phenolics Through Visible Light-Induced Photorearrangement of Quinones (ChemistryEurope 2/2025)","authors":"Alexander A. Fadeev,&nbsp;Martin Kotora","doi":"10.1002/ceur.202580202","DOIUrl":"https://doi.org/10.1002/ceur.202580202","url":null,"abstract":"<p><b>The Cover Feature</b> represents the smooth intramolecular photoisomerization of quinones into diverse phenolic compounds in solution under exposure to blue light, which is represented by a “blue moon”. Given that many quinones co-occur in nature with hydroquinones and other hydroxyarenes, such a transformation allows us to anticipate the presence of these substances in natural sources through a light-induced synthesis. More information can be found in the Research Article by A. A. Fadeev and M. Kotora (DOI: 10.1002/ceur.202400094).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202580202","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581800","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Front Cover: Structural Requirements of Synthetic Anionophores for Inorganic Phosphate and Phosphate Esters (ChemistryEurope 2/2025)
ChemistryEurope Pub Date : 2025-03-10 DOI: 10.1002/ceur.202580201
Dr. Aaron Torres-Huerta, Dr. Karolis Norvaisa, Dr. Alessio Cataldo, Pierre-Olivier Tits, Priyanka Rani Panda, Dr. Christopher M. Dias, Prof. Dr. Anthony P. Davis, Dr. Samantha E. Bodman, Dr. Stephen J. Butler, Dr. Hennie Valkenier
{"title":"Front Cover: Structural Requirements of Synthetic Anionophores for Inorganic Phosphate and Phosphate Esters (ChemistryEurope 2/2025)","authors":"Dr. Aaron Torres-Huerta,&nbsp;Dr. Karolis Norvaisa,&nbsp;Dr. Alessio Cataldo,&nbsp;Pierre-Olivier Tits,&nbsp;Priyanka Rani Panda,&nbsp;Dr. Christopher M. Dias,&nbsp;Prof. Dr. Anthony P. Davis,&nbsp;Dr. Samantha E. Bodman,&nbsp;Dr. Stephen J. Butler,&nbsp;Dr. Hennie Valkenier","doi":"10.1002/ceur.202580201","DOIUrl":"https://doi.org/10.1002/ceur.202580201","url":null,"abstract":"<p><b>The Front Cover</b> shows liposomes with synthetic anion receptors embedded in their membrane and different phosphate species to be transported. In their Research Article (DOI: 10.1002/ceur.202400076), H. Valkenier and co-workers show that phosphate diesters are readily transported across lipid bilayers, followed by phosphate monoesters, whereas inorganic phosphate is the most difficult to transport and requires the effective encapsulation by an anion receptor. Artwork by A. Torres-Huerta.\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-03-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202580201","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581799","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Abiotic Ribonucleoside Formation in Aqueous Microdroplets: Mechanistic Exploration, Acidity, and Electric Field Effects
ChemistryEurope Pub Date : 2025-02-09 DOI: 10.1002/ceur.202400093
Maciej Piejko, Javier E. Alfonso-Ramos, Joseph Moran, Thijs Stuyver
{"title":"Abiotic Ribonucleoside Formation in Aqueous Microdroplets: Mechanistic Exploration, Acidity, and Electric Field Effects","authors":"Maciej Piejko,&nbsp;Javier E. Alfonso-Ramos,&nbsp;Joseph Moran,&nbsp;Thijs Stuyver","doi":"10.1002/ceur.202400093","DOIUrl":"https://doi.org/10.1002/ceur.202400093","url":null,"abstract":"<p>Aqueous microdroplets have been reported to dramatically increase the rate of chemical reactions. Proposed mechanisms for this acceleration include confinement effects upon droplet evaporation, and Brønsted acid or electric field catalysis at the air-water interface. However, computational investigations indicate that the operation of these mechanisms is reaction-dependent, with conclusive evidence for a role for electric field catalysis still lacking. Here, we present a computational investigation of the reported abiotic phosphorylation of ribose and the subsequent formation of ribonucleosides, focusing on acidity and oriented external electric field (OEEF) effects. The most plausible reaction mechanism identified involves the protonation of ribose, followed by carbocation formation and an S<sub><i>N</i></sub>2 substitution step. Without an OEEF, all considered pathways are thermally inaccessible. However, in the presence of a significant OEEF, the S<sub><i>N</i></sub>2-based pathway, leading to the <i>β</i>-ribonucleoside isomer, becomes highly stabilized, reducing the energetic span to a thermally accessible 12–13 kcal/mol. Surprisingly, the OEEF-mediated reaction closely mirrors the enzymatic mechanism of phosphorolysis via S<sub><i>N</i></sub>2 substitution, including a pronounced anomeric selectivity. Our results support the hypothesis that some reactions in aqueous microdroplets are accelerated by electric fields and provide further evidence for the importance of electrostatic catalysis in biological systems, particularly for phosphorylase enzymes.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400093","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581357","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Palladium-Catalyzed Selectivity Controlled Highly Efficient Carbonylative Synthesis of Isoquinoline-1,3(2H,4H)-diones and Indanones
ChemistryEurope Pub Date : 2025-02-07 DOI: 10.1002/ceur.202400105
Ren-Rui Xu, Chang-Sheng Kuai, Prof. Dr. Xiao-Feng Wu
{"title":"Palladium-Catalyzed Selectivity Controlled Highly Efficient Carbonylative Synthesis of Isoquinoline-1,3(2H,4H)-diones and Indanones","authors":"Ren-Rui Xu,&nbsp;Chang-Sheng Kuai,&nbsp;Prof. Dr. Xiao-Feng Wu","doi":"10.1002/ceur.202400105","DOIUrl":"https://doi.org/10.1002/ceur.202400105","url":null,"abstract":"<p>Compared to the methods that rely on complex and structurally unique substrates for the synthesis of heterocyclic compounds through intra- and intermolecular cyclization, strategies starting from simple and readily available substrates, combined with finely tuned catalytic system to achieve different chemoselectivity, offer significant advantages in terms of efficiency, cost-effectiveness, and versatility. Herein, we present a palladium-catalyzed carbonylation strategy that enables the selective and efficient synthesis of isoquinoline-1,3(2<i>H</i>,4<i>H</i>)-dione and indanone derivatives via distinct reaction pathways. Notably, the chemoselectivity was not determined by the differences in reactivity at the reaction sites but instead arises from the generation of distinct active palladium species under nearly identical reaction conditions, which subsequently react on the same reaction site but lead to different products.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400105","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581742","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Anticipating Natural Phenolics Through Visible Light-Induced Photorearrangement of Quinones
ChemistryEurope Pub Date : 2025-02-03 DOI: 10.1002/ceur.202400094
Alexander A. Fadeev, Martin Kotora
{"title":"Anticipating Natural Phenolics Through Visible Light-Induced Photorearrangement of Quinones","authors":"Alexander A. Fadeev,&nbsp;Martin Kotora","doi":"10.1002/ceur.202400094","DOIUrl":"https://doi.org/10.1002/ceur.202400094","url":null,"abstract":"<p>A general protocol for the photorearrangement of substituted benzo- and naphthoquinones using monochromatic blue light irradiation in solution was developed. During this process, the quinone ring is transformed into the hydroquinone, while the substituent undergoes desaturation or annulation onto the proximal oxygen of the formed hydroquinone. We found that desaturation was preferred for acyclic saturated substituents, such as alkyl groups, and the tendency for annulation was observed for both cyclic and acyclic unsaturated substituents (allyl, alkenyl, aryl). The diversity of the participating substituents and the functional group tolerance of this transformation allowed us to prepare 10 natural phenolic compounds, suggesting that visible light may likewise induce their formation from the respective quinones in natural sources.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400094","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581477","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Structural Requirements of Synthetic Anionophores for Inorganic Phosphate and Phosphate Esters
ChemistryEurope Pub Date : 2025-02-03 DOI: 10.1002/ceur.202400076
Dr. Aaron Torres-Huerta, Dr. Karolis Norvaisa, Dr. Alessio Cataldo, Pierre-Olivier Tits, Priyanka Rani Panda, Dr. Christopher M. Dias, Prof. Dr. Anthony P. Davis, Dr. Samantha E. Bodman, Dr. Stephen J. Butler, Dr. Hennie Valkenier
{"title":"Structural Requirements of Synthetic Anionophores for Inorganic Phosphate and Phosphate Esters","authors":"Dr. Aaron Torres-Huerta,&nbsp;Dr. Karolis Norvaisa,&nbsp;Dr. Alessio Cataldo,&nbsp;Pierre-Olivier Tits,&nbsp;Priyanka Rani Panda,&nbsp;Dr. Christopher M. Dias,&nbsp;Prof. Dr. Anthony P. Davis,&nbsp;Dr. Samantha E. Bodman,&nbsp;Dr. Stephen J. Butler,&nbsp;Dr. Hennie Valkenier","doi":"10.1002/ceur.202400076","DOIUrl":"https://doi.org/10.1002/ceur.202400076","url":null,"abstract":"<p>The transmembrane transport of anions is a promising application of synthetic anion receptors. Numerous anionophores have been developed for chloride over the past decades. Despite the biological relevance of phosphate and phosphate esters, very few reports on their transport by synthetic systems exist. Here we report a systematic study on the transport of diphenyl phosphate, phenyl phosphate, and inorganic phosphate by five different anionophores. The transport of these phosphates into liposomes was monitored by fluorescence spectroscopy, <sup>31</sup>P NMR spectroscopy, and an ion selective electrode. The results of these experiments showed that diphenyl phosphate is readily transported by most chloride ionophores. The transport of phenyl phosphate is more challenging but can be enhanced by better shielding of the phosphate group. Inorganic phosphate is the most challenging to transport and this was achieved using a macrocyclic anionophore with eight preorganised H-bond donors. These results pave the way for the development of anionophores for inorganic phosphate as well as phosphate esters.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400076","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
An Umpolung Approach for C2-Selective C−H Amination of Azines by Palladium Catalysis
ChemistryEurope Pub Date : 2025-02-03 DOI: 10.1002/ceur.202400092
Qikun Wu, Prof. Dr. Kei Muto, Prof. Dr. Junichiro Yamaguchi
{"title":"An Umpolung Approach for C2-Selective C−H Amination of Azines by Palladium Catalysis","authors":"Qikun Wu,&nbsp;Prof. Dr. Kei Muto,&nbsp;Prof. Dr. Junichiro Yamaguchi","doi":"10.1002/ceur.202400092","DOIUrl":"https://doi.org/10.1002/ceur.202400092","url":null,"abstract":"<p>The site-selective C−H amination of azines is a critical challenge due to the broad applications of amino azines in biologically important compounds. In this work, we report a conceptually novel approach to the electrophilic C2-selective C−H amination of azines using <i>O</i>-benzoylhydroxylamines, catalyzed by a benzyl–palladium complex. A key feature of this transformation is the formation of the distal C−N bond via a benzyl–Pd intermediate, facilitated by a malonate substituent on the azine as a remote directing group. This strategy effectively overrides the inherent polarity mismatch typically observed in electrophilic C2-C−H aminations. The reaction exhibits high site-selectivity and demonstrates towards amine-sensitive functional group, highlighting its synthetic utility.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400092","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581480","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The Reductive Addition–Oxidative Elimination Mechanism
ChemistryEurope Pub Date : 2025-02-03 DOI: 10.1002/ceur.202400086
Dr. Belén Lerma–Berlanga, Dr. Antonio Leyva–Pérez.
{"title":"The Reductive Addition–Oxidative Elimination Mechanism","authors":"Dr. Belén Lerma–Berlanga,&nbsp;Dr. Antonio Leyva–Pérez.","doi":"10.1002/ceur.202400086","DOIUrl":"https://doi.org/10.1002/ceur.202400086","url":null,"abstract":"<p>The oxidative addition–reductive elimination (OARE) mechanism of reactive molecules on metal atoms is a cornerstone of modern chemistry. However, the complementary reductive addition–oxidative elimination (RAOE) mechanism is barely considered, despite a first reduction reaction between metal atoms and the incoming organic reactant makes chemical sense in a plethora of processes. Here we show, in a chronological order, early precedents in the literature which indicated the possibility of a general RAOE mechanism, the few systems explicitly reported so far (including a catalytic system) and some other reactions where a RAOE mechanism would satisfactorily explain the mechanistic evidences found. These examples, together, strongly suggest that researchers should consider the RAOE mechanism during their investigations, and not simply adjust their conclusions to the omnipresent OARE mechanism. This new line of thinking might open new avenues in the design of chemical reactions, particularly catalytic ones.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-02-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400086","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143581475","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Selective Borylation of C(sp3)−H Bond of Methyl Ethers Catalyzed by Iron Complexes Bearing Anionic Benzene-Based PCP-Pincer Ligands 含有阴离子苯基五氯苯酚-钳配体的铁络合物催化的甲基醚 C（sp3）-H 键选择性硼酰化反应
ChemistryEurope Pub Date : 2025-01-28 DOI: 10.1002/ceur.202400100
Shogo Kuriyama, Yuto Suga, Ken Sakata, Yoshiaki Nishibayashi
{"title":"Selective Borylation of C(sp3)−H Bond of Methyl Ethers Catalyzed by Iron Complexes Bearing Anionic Benzene-Based PCP-Pincer Ligands","authors":"Shogo Kuriyama,&nbsp;Yuto Suga,&nbsp;Ken Sakata,&nbsp;Yoshiaki Nishibayashi","doi":"10.1002/ceur.202400100","DOIUrl":"https://doi.org/10.1002/ceur.202400100","url":null,"abstract":"<p>Highly selective catalytic C(sp<sup>3</sup>)−H borylation of methoxy groups has been achieved using newly synthesized iron complexes bearing benzene-based PCP-type pincer ligands as catalysts. Reactions of various aryl and alkyl methyl ethers as substrates with bis(pinacolato)diboron under mild reaction conditions proceeded to afford the corresponding methoxy borylated products in good to high yields. A successful example of the iron-catalyzed C(sp<sup>3</sup>)−H borylation of a methylene group of tetrahydrofuran (THF) was also presented. A plausible reaction pathway is proposed based on the experimental result of some stoichiometric reactions and DFT calculations on a model reaction, where iron-boryl and -alkyl complexes may work as key intermediates.</p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 2","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202400100","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143582085","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cover Feature: Applying Metallo-Organic Ligand Design Principles to the Stereoselective Synthesis of a Peptide-Based Pd2L4X4 Cage (ChemistryEurope 1/2025)
ChemistryEurope Pub Date : 2025-01-12 DOI: 10.1002/ceur.202580102
Dr. Dominic F. Brightwell, Dr. Kushal Samanta, Dr. Jimmy Muldoon, Dr. Patricia C. Fleming, Dr. Yannick Ortin, Dr. Lina Mardiana, Dr. Paul G. Waddell, Dr. Michael J. Hall, Dr. Ewan R. Clark, Dr. Felipe Fantuzzi, Dr. Aniello Palma
{"title":"Cover Feature: Applying Metallo-Organic Ligand Design Principles to the Stereoselective Synthesis of a Peptide-Based Pd2L4X4 Cage (ChemistryEurope 1/2025)","authors":"Dr. Dominic F. Brightwell,&nbsp;Dr. Kushal Samanta,&nbsp;Dr. Jimmy Muldoon,&nbsp;Dr. Patricia C. Fleming,&nbsp;Dr. Yannick Ortin,&nbsp;Dr. Lina Mardiana,&nbsp;Dr. Paul G. Waddell,&nbsp;Dr. Michael J. Hall,&nbsp;Dr. Ewan R. Clark,&nbsp;Dr. Felipe Fantuzzi,&nbsp;Dr. Aniello Palma","doi":"10.1002/ceur.202580102","DOIUrl":"https://doi.org/10.1002/ceur.202580102","url":null,"abstract":"<p><b>The Cover Feature</b> celebrates the stereoselective synthesis of a peptide-based palladium cage. The chiral, low-symmetry peptide-based ligand used to generate this Pd cage could theoretically yield up to four structural isomers. Remarkably, only a single isomeric cage is formed in solution, the thermodynamically stable one. The image represents the single isomer emerging into the spotlight from all the possible isomers, shown in different colours in the background. More information can be found in the Research Article by A. Palma and co-workers (DOI: 10.1002/ceur.202400050).\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure>\u0000 </p>","PeriodicalId":100234,"journal":{"name":"ChemistryEurope","volume":"3 1","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ceur.202580102","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143114459","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","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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