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Pinpointing the Onset of Water Harvesting in Reticular Frameworks from Structure 从结构上确定网状框架中集水的开始
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-17 DOI: 10.1021/acscentsci.4c0187810.1021/acscentsci.4c01878
Ha L. Nguyen, Andrea Darù, Saumil Chheda, Ali H. Alawadhi, S. Ephraim Neumann, Lifen Wang, Xuedong Bai, Majed O. Alawad, Christian Borgs, Jennifer T. Chayes, Joachim Sauer*, Laura Gagliardi* and Omar M. Yaghi*, 
{"title":"Pinpointing the Onset of Water Harvesting in Reticular Frameworks from Structure","authors":"Ha L. Nguyen,&nbsp;Andrea Darù,&nbsp;Saumil Chheda,&nbsp;Ali H. Alawadhi,&nbsp;S. Ephraim Neumann,&nbsp;Lifen Wang,&nbsp;Xuedong Bai,&nbsp;Majed O. Alawad,&nbsp;Christian Borgs,&nbsp;Jennifer T. Chayes,&nbsp;Joachim Sauer*,&nbsp;Laura Gagliardi* and Omar M. Yaghi*,&nbsp;","doi":"10.1021/acscentsci.4c0187810.1021/acscentsci.4c01878","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01878https://doi.org/10.1021/acscentsci.4c01878","url":null,"abstract":"<p >Covalent organic frameworks (COFs) have emerged as promising atmospheric water harvesters, offering a potential solution to the pressing global issue of water scarcity, which threatens millions of lives worldwide. This study presents a series of 2D COFs, including HCOF-3, HCOF-2, and a newly developed structure named COF-309, designed for optimized water harvesting performance with a high working capacity at low relative humidity. To elucidate their water sorption behavior, we introduce a hydrophilicity index directly linked to intrinsic properties, such as the strength and spatial density of adsorptive sites. This index is mathematically correlated to the step of water adsorption isotherms. Our correlation provides a predictive tool that extends to other microporous COFs and metal–organic frameworks, significantly enhancing the ability to predict their onset positions of water adsorption isotherms based on structural characteristics. This advancement holds the potential to guide the development of more efficient materials for atmospheric water harvesting.</p><p >HCOF-3, HCOF-2, and COF-309 excel in atmospheric water harvesting. A novel hydrophilicity index links adsorptive site properties to water isotherms, aiding efficient reticular structure design.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 5","pages":"665–671 665–671"},"PeriodicalIF":12.7,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01878","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144146438","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Pinpointing the Onset of Water Harvesting in Reticular Frameworks from Structure. 从结构上确定网状框架中集水的开始。
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-17 eCollection Date: 2025-05-28 DOI: 10.1021/acscentsci.4c01878
Ha L Nguyen, Andrea Darù, Saumil Chheda, Ali H Alawadhi, S Ephraim Neumann, Lifen Wang, Xuedong Bai, Majed O Alawad, Christian Borgs, Jennifer T Chayes, Joachim Sauer, Laura Gagliardi, Omar M Yaghi
{"title":"Pinpointing the Onset of Water Harvesting in Reticular Frameworks from Structure.","authors":"Ha L Nguyen, Andrea Darù, Saumil Chheda, Ali H Alawadhi, S Ephraim Neumann, Lifen Wang, Xuedong Bai, Majed O Alawad, Christian Borgs, Jennifer T Chayes, Joachim Sauer, Laura Gagliardi, Omar M Yaghi","doi":"10.1021/acscentsci.4c01878","DOIUrl":"10.1021/acscentsci.4c01878","url":null,"abstract":"<p><p>Covalent organic frameworks (COFs) have emerged as promising atmospheric water harvesters, offering a potential solution to the pressing global issue of water scarcity, which threatens millions of lives worldwide. This study presents a series of 2D COFs, including HCOF-3, HCOF-2, and a newly developed structure named COF-309, designed for optimized water harvesting performance with a high working capacity at low relative humidity. To elucidate their water sorption behavior, we introduce a hydrophilicity index directly linked to intrinsic properties, such as the strength and spatial density of adsorptive sites. This index is mathematically correlated to the step of water adsorption isotherms. Our correlation provides a predictive tool that extends to other microporous COFs and metal-organic frameworks, significantly enhancing the ability to predict their onset positions of water adsorption isotherms based on structural characteristics. This advancement holds the potential to guide the development of more efficient materials for atmospheric water harvesting.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 5","pages":"665-671"},"PeriodicalIF":12.7,"publicationDate":"2025-02-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12123544/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144197696","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Direct (LC-)MS Identification of Regioisomers from C-H Functionalization by Partial Isotopic Labeling. 部分同位素标记法直接(LC-)质谱鉴定碳氢功能化区域异构体。
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-14 eCollection Date: 2025-02-26 DOI: 10.1021/acscentsci.4c01765
Christopher A Sojdak, David A Polefrone, Hriday M Shah, Cassandra D Vu, Brandon J Orzolek, Pedro M Jimenez Antenucci, Micah Valadez Bush, Marisa C Kozlowski
{"title":"Direct (LC-)MS Identification of Regioisomers from C-H Functionalization by Partial Isotopic Labeling.","authors":"Christopher A Sojdak, David A Polefrone, Hriday M Shah, Cassandra D Vu, Brandon J Orzolek, Pedro M Jimenez Antenucci, Micah Valadez Bush, Marisa C Kozlowski","doi":"10.1021/acscentsci.4c01765","DOIUrl":"10.1021/acscentsci.4c01765","url":null,"abstract":"<p><p>C-H functionalization of complex substrates is highly enabling in total synthesis and in the development of late-stage drug candidates. Much work has been dedicated to developing new methods as well as predictive modeling to accelerate route scouting. However, workflows to identify regioisomeric products are arduous, typically requiring chromatographic separation and/or nuclear magnetic resonance spectroscopy analysis. In addition, most reports focus on major products or do not assign regioisomeric products, which biases predictive models constructed from such data. Herein, we present a novel approach to complex reaction analysis utilizing partial deuterium labels, which enables direct product identification via liquid chromatography-mass spectrometry. When combined with spectral deconvolution, the method generates product ratios while circumventing chromatography altogether. Competitive kinetic isotope effects can also be determined. The resultant data are expected to be useful in the construction of predictive models across several dimensions including reaction selectivity, the impact of structure on mechanism, and mass spectral ionization patterns and expedite the identification of drug metabolites.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 2","pages":"272-278"},"PeriodicalIF":12.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11868960/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539545","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Direct (LC-)MS Identification of Regioisomers from C–H Functionalization by Partial Isotopic Labeling 部分同位素标记法直接(LC-)质谱鉴定碳氢功能化区域异构体
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-14 DOI: 10.1021/acscentsci.4c0176510.1021/acscentsci.4c01765
Christopher A. Sojdak, David A. Polefrone, Hriday M. Shah, Cassandra D. Vu, Brandon J. Orzolek, Pedro M. Jimenez Antenucci, Micah Valadez Bush and Marisa C. Kozlowski*, 
{"title":"Direct (LC-)MS Identification of Regioisomers from C–H Functionalization by Partial Isotopic Labeling","authors":"Christopher A. Sojdak,&nbsp;David A. Polefrone,&nbsp;Hriday M. Shah,&nbsp;Cassandra D. Vu,&nbsp;Brandon J. Orzolek,&nbsp;Pedro M. Jimenez Antenucci,&nbsp;Micah Valadez Bush and Marisa C. Kozlowski*,&nbsp;","doi":"10.1021/acscentsci.4c0176510.1021/acscentsci.4c01765","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01765https://doi.org/10.1021/acscentsci.4c01765","url":null,"abstract":"<p >C–H functionalization of complex substrates is highly enabling in total synthesis and in the development of late-stage drug candidates. Much work has been dedicated to developing new methods as well as predictive modeling to accelerate route scouting. However, workflows to identify regioisomeric products are arduous, typically requiring chromatographic separation and/or nuclear magnetic resonance spectroscopy analysis. In addition, most reports focus on major products or do not assign regioisomeric products, which biases predictive models constructed from such data. Herein, we present a novel approach to complex reaction analysis utilizing partial deuterium labels, which enables direct product identification via liquid chromatography–mass spectrometry. When combined with spectral deconvolution, the method generates product ratios while circumventing chromatography altogether. Competitive kinetic isotope effects can also be determined. The resultant data are expected to be useful in the construction of predictive models across several dimensions including reaction selectivity, the impact of structure on mechanism, and mass spectral ionization patterns and expedite the identification of drug metabolites.</p><p >Partial isotopic labels allow direct identification of regioisomers via their distinct isotopic distributions. Alternately, spectral deconvolution of unseparated mixtures delivers regioisomer ratios.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 2","pages":"272–278 272–278"},"PeriodicalIF":12.7,"publicationDate":"2025-02-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01765","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486659","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Stars by the Pocketful. 星星的口袋。
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-12 eCollection Date: 2025-02-26 DOI: 10.1021/acscentsci.5c00223
Clara E Lavis, Luke D Lavis
{"title":"Stars by the Pocketful.","authors":"Clara E Lavis, Luke D Lavis","doi":"10.1021/acscentsci.5c00223","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00223","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 2","pages":"183-186"},"PeriodicalIF":12.7,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11868956/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539465","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Stars by the Pocketful 星星的口袋
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-12 DOI: 10.1021/acscentsci.5c0022310.1021/acscentsci.5c00223
Clara E. Lavis,  and , Luke D. Lavis​, 
{"title":"Stars by the Pocketful","authors":"Clara E. Lavis,&nbsp; and ,&nbsp;Luke D. Lavis​,&nbsp;","doi":"10.1021/acscentsci.5c0022310.1021/acscentsci.5c00223","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00223https://doi.org/10.1021/acscentsci.5c00223","url":null,"abstract":"<p >SWIR dyes─The Eras Tour. This love story between chemistry and biology shines.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 2","pages":"183–186 183–186"},"PeriodicalIF":12.7,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.5c00223","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486979","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Pumping Iron for Tuberculosis Diagnostics 为肺结核诊断抽铁
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-11 DOI: 10.1021/acscentsci.5c0013310.1021/acscentsci.5c00133
Abdulai Zigli,  and , Benjamin M. Swarts​, 
{"title":"Pumping Iron for Tuberculosis Diagnostics","authors":"Abdulai Zigli,&nbsp; and ,&nbsp;Benjamin M. Swarts​,&nbsp;","doi":"10.1021/acscentsci.5c0013310.1021/acscentsci.5c00133","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00133https://doi.org/10.1021/acscentsci.5c00133","url":null,"abstract":"<p >Synthetic mycobactin−fluorophore conjugates exploit the mycobacterial iron acquisition pathway to enable sensitive fluorogenic detection of <i>Mycobacterium tuberculosis</i>.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 2","pages":"190–192 190–192"},"PeriodicalIF":12.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.5c00133","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143486822","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Scaling Organic Electrosynthesis: The Crucial Interplay between Mechanism and Mass Transport. 标度有机电合成:机制与质量传递之间的关键相互作用。
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-11 eCollection Date: 2025-04-23 DOI: 10.1021/acscentsci.4c01733
Zachary J Oliver, Dylan J Abrams, Luana Cardinale, Chih-Jung Chen, Gregory L Beutner, Seb Caille, Benjamin Cohen, Lin Deng, Moiz Diwan, Michael O Frederick, Kaid Harper, Joel M Hawkins, Dan Lehnherr, Christine Lucky, Alex Meyer, Seonmyeong Noh, Diego Nunez, Kyle Quasdorf, Jaykumar Teli, Shannon S Stahl, Marcel Schreier
{"title":"Scaling Organic Electrosynthesis: The Crucial Interplay between Mechanism and Mass Transport.","authors":"Zachary J Oliver, Dylan J Abrams, Luana Cardinale, Chih-Jung Chen, Gregory L Beutner, Seb Caille, Benjamin Cohen, Lin Deng, Moiz Diwan, Michael O Frederick, Kaid Harper, Joel M Hawkins, Dan Lehnherr, Christine Lucky, Alex Meyer, Seonmyeong Noh, Diego Nunez, Kyle Quasdorf, Jaykumar Teli, Shannon S Stahl, Marcel Schreier","doi":"10.1021/acscentsci.4c01733","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01733","url":null,"abstract":"<p><p>Organic electrosynthesis opens new avenues of reactivity and promises more sustainable practices in the preparation of fine chemicals and pharmaceuticals. The full value of this approach will be realized by taking these processes to the production scale; however, achieving this goal will require a better understanding of the influence of mass transport on reaction behavior and the interactions between reactive species and electrodes inherent to organic electrosynthesis. The limited options for cell geometries used on small scale limit elucidation of these features. Here, we show how advanced cell geometries allow us to control the interplay between reaction mechanism and mass transport, leading to improved performance of three modern organic electrosynthetic reactions. Each reaction shows a unique relationship with mass transport, highlighting the importance of understanding this relationship further to maximize the utility of organic electrosynthesis at scale.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"528-538"},"PeriodicalIF":12.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC12022915/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143951145","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Pumping Iron for Tuberculosis Diagnostics. 泵铁用于结核病诊断。
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-11 eCollection Date: 2025-02-26 DOI: 10.1021/acscentsci.5c00133
Abdulai Zigli, Benjamin M Swarts
{"title":"Pumping Iron for Tuberculosis Diagnostics.","authors":"Abdulai Zigli, Benjamin M Swarts","doi":"10.1021/acscentsci.5c00133","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00133","url":null,"abstract":"","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 2","pages":"190-192"},"PeriodicalIF":12.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11869129/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143539345","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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
Scaling Organic Electrosynthesis: The Crucial Interplay between Mechanism and Mass Transport 标度有机电合成:机制与质量传递之间的关键相互作用
IF 12.7 1区 化学
ACS Central Science Pub Date : 2025-02-11 DOI: 10.1021/acscentsci.4c0173310.1021/acscentsci.4c01733
Zachary J. Oliver, Dylan J. Abrams, Luana Cardinale, Chih-Jung Chen, Gregory L. Beutner, Seb Caille, Benjamin Cohen, Lin Deng, Moiz Diwan, Michael O. Frederick, Kaid Harper, Joel M. Hawkins, Dan Lehnherr, Christine Lucky, Alex Meyer, Seonmyeong Noh, Diego Nunez, Kyle Quasdorf, Jaykumar Teli, Shannon S. Stahl* and Marcel Schreier*, 
{"title":"Scaling Organic Electrosynthesis: The Crucial Interplay between Mechanism and Mass Transport","authors":"Zachary J. Oliver,&nbsp;Dylan J. Abrams,&nbsp;Luana Cardinale,&nbsp;Chih-Jung Chen,&nbsp;Gregory L. Beutner,&nbsp;Seb Caille,&nbsp;Benjamin Cohen,&nbsp;Lin Deng,&nbsp;Moiz Diwan,&nbsp;Michael O. Frederick,&nbsp;Kaid Harper,&nbsp;Joel M. Hawkins,&nbsp;Dan Lehnherr,&nbsp;Christine Lucky,&nbsp;Alex Meyer,&nbsp;Seonmyeong Noh,&nbsp;Diego Nunez,&nbsp;Kyle Quasdorf,&nbsp;Jaykumar Teli,&nbsp;Shannon S. Stahl* and Marcel Schreier*,&nbsp;","doi":"10.1021/acscentsci.4c0173310.1021/acscentsci.4c01733","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01733https://doi.org/10.1021/acscentsci.4c01733","url":null,"abstract":"<p >Organic electrosynthesis opens new avenues of reactivity and promises more sustainable practices in the preparation of fine chemicals and pharmaceuticals. The full value of this approach will be realized by taking these processes to the production scale; however, achieving this goal will require a better understanding of the influence of mass transport on reaction behavior and the interactions between reactive species and electrodes inherent to organic electrosynthesis. The limited options for cell geometries used on small scale limit elucidation of these features. Here, we show how advanced cell geometries allow us to control the interplay between reaction mechanism and mass transport, leading to improved performance of three modern organic electrosynthetic reactions. Each reaction shows a unique relationship with mass transport, highlighting the importance of understanding this relationship further to maximize the utility of organic electrosynthesis at scale.</p><p >In this work, we systematically investigate the relationship between mass transport and reaction mechanism, enabling the scale-up of organic electrosynthesis.</p>","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"528–538 528–538"},"PeriodicalIF":12.7,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01733","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858706","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"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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