Travis K. Deason, Hunter B. Tisdale, Adrian T. Hines, Gregory Morrison, Yunping Zhoujin, Mark D. Smith, Theodore M. Besmann, Amir M. Mofrad, Shanna L. Estes, Jake W. Amoroso, David P. DiPrete and Hans-Conrad zur Loye*,
{"title":"高温助熔剂晶体生长法合成含镅磷酸盐、硅酸盐、硼酸盐、钼酸盐和氟化物的研究","authors":"Travis K. Deason, Hunter B. Tisdale, Adrian T. Hines, Gregory Morrison, Yunping Zhoujin, Mark D. Smith, Theodore M. Besmann, Amir M. Mofrad, Shanna L. Estes, Jake W. Amoroso, David P. DiPrete and Hans-Conrad zur Loye*, ","doi":"10.1021/jacs.5c03457","DOIUrl":null,"url":null,"abstract":"<p >The crystal chemistry of americium-containing extended structures was investigated, and several classes of americium-containing solid-state oxide materials were obtained in single-crystal form via high-temperature flux crystal growth. This enabled the structural characterization of rare examples of ternary, quaternary, and penternary americium-containing silicates K<sub>3</sub>Am (Si<sub>2</sub>O<sub>7</sub>) and Cs<sub>6</sub>Am<sub>2</sub>Si<sub>21</sub>O<sub>48</sub>, phosphates Na<sub>3</sub>Am (PO<sub>4</sub>)<sub>2</sub> and K<sub>3</sub>Am (PO<sub>4</sub>)<sub>2</sub>, borates Ba<sub>3</sub>Am<sub>2</sub>(BO<sub>3</sub>)<sub>4</sub> and AmBO<sub>3</sub>, borate halides Ca<sub>5</sub>Am(BO<sub>3</sub>)<sub>4</sub>Cl, molybdates Li<sub>0.5</sub>Am<sub>0.5</sub>MoO<sub>4</sub>, and fluorides CsAm<sub>2</sub>F<sub>7</sub>. Using these crystallographic data, the ionic radii of Am<sup>3+</sup> with coordination numbers of six (0.975 Å), seven (1.052 Å), and nine (1.162 Å) were established. A maximum entropy method (MEM) analysis was performed on the single-crystal X-ray diffraction data that were collected for K<sub>3</sub>Nd(PO<sub>4</sub>)<sub>2</sub>/K<sub>3</sub>Am(PO<sub>4</sub>)<sub>2</sub>, K<sub>3</sub>NdSi<sub>2</sub>O<sub>7</sub>/K<sub>3</sub>AmSi<sub>2</sub>O<sub>7</sub>, and NdBO<sub>3</sub>/AmBO<sub>3</sub>, to qualitatively compare the ionicities of the Nd–O and Am–O bonds. Raman spectroscopy data were collected on single crystals of K<sub>3</sub>Am(PO<sub>4</sub>)<sub>2</sub> and compared to the calculated Raman spectrum of K<sub>3</sub>Am(PO<sub>4</sub>)<sub>2</sub> obtained from DFT calculations.</p>","PeriodicalId":49,"journal":{"name":"Journal of the American Chemical Society","volume":"147 25","pages":"21659–21671"},"PeriodicalIF":15.6000,"publicationDate":"2025-06-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Investigation of Americium-Containing Phosphates, Silicates, Borates, Molybdates, and Fluorides Synthesized via High-Temperature Flux Crystal Growth\",\"authors\":\"Travis K. Deason, Hunter B. Tisdale, Adrian T. Hines, Gregory Morrison, Yunping Zhoujin, Mark D. Smith, Theodore M. Besmann, Amir M. Mofrad, Shanna L. Estes, Jake W. Amoroso, David P. DiPrete and Hans-Conrad zur Loye*, \",\"doi\":\"10.1021/jacs.5c03457\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >The crystal chemistry of americium-containing extended structures was investigated, and several classes of americium-containing solid-state oxide materials were obtained in single-crystal form via high-temperature flux crystal growth. This enabled the structural characterization of rare examples of ternary, quaternary, and penternary americium-containing silicates K<sub>3</sub>Am (Si<sub>2</sub>O<sub>7</sub>) and Cs<sub>6</sub>Am<sub>2</sub>Si<sub>21</sub>O<sub>48</sub>, phosphates Na<sub>3</sub>Am (PO<sub>4</sub>)<sub>2</sub> and K<sub>3</sub>Am (PO<sub>4</sub>)<sub>2</sub>, borates Ba<sub>3</sub>Am<sub>2</sub>(BO<sub>3</sub>)<sub>4</sub> and AmBO<sub>3</sub>, borate halides Ca<sub>5</sub>Am(BO<sub>3</sub>)<sub>4</sub>Cl, molybdates Li<sub>0.5</sub>Am<sub>0.5</sub>MoO<sub>4</sub>, and fluorides CsAm<sub>2</sub>F<sub>7</sub>. Using these crystallographic data, the ionic radii of Am<sup>3+</sup> with coordination numbers of six (0.975 Å), seven (1.052 Å), and nine (1.162 Å) were established. A maximum entropy method (MEM) analysis was performed on the single-crystal X-ray diffraction data that were collected for K<sub>3</sub>Nd(PO<sub>4</sub>)<sub>2</sub>/K<sub>3</sub>Am(PO<sub>4</sub>)<sub>2</sub>, K<sub>3</sub>NdSi<sub>2</sub>O<sub>7</sub>/K<sub>3</sub>AmSi<sub>2</sub>O<sub>7</sub>, and NdBO<sub>3</sub>/AmBO<sub>3</sub>, to qualitatively compare the ionicities of the Nd–O and Am–O bonds. Raman spectroscopy data were collected on single crystals of K<sub>3</sub>Am(PO<sub>4</sub>)<sub>2</sub> and compared to the calculated Raman spectrum of K<sub>3</sub>Am(PO<sub>4</sub>)<sub>2</sub> obtained from DFT calculations.</p>\",\"PeriodicalId\":49,\"journal\":{\"name\":\"Journal of the American Chemical Society\",\"volume\":\"147 25\",\"pages\":\"21659–21671\"},\"PeriodicalIF\":15.6000,\"publicationDate\":\"2025-06-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of the American Chemical Society\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/jacs.5c03457\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of the American Chemical Society","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/jacs.5c03457","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Investigation of Americium-Containing Phosphates, Silicates, Borates, Molybdates, and Fluorides Synthesized via High-Temperature Flux Crystal Growth
The crystal chemistry of americium-containing extended structures was investigated, and several classes of americium-containing solid-state oxide materials were obtained in single-crystal form via high-temperature flux crystal growth. This enabled the structural characterization of rare examples of ternary, quaternary, and penternary americium-containing silicates K3Am (Si2O7) and Cs6Am2Si21O48, phosphates Na3Am (PO4)2 and K3Am (PO4)2, borates Ba3Am2(BO3)4 and AmBO3, borate halides Ca5Am(BO3)4Cl, molybdates Li0.5Am0.5MoO4, and fluorides CsAm2F7. Using these crystallographic data, the ionic radii of Am3+ with coordination numbers of six (0.975 Å), seven (1.052 Å), and nine (1.162 Å) were established. A maximum entropy method (MEM) analysis was performed on the single-crystal X-ray diffraction data that were collected for K3Nd(PO4)2/K3Am(PO4)2, K3NdSi2O7/K3AmSi2O7, and NdBO3/AmBO3, to qualitatively compare the ionicities of the Nd–O and Am–O bonds. Raman spectroscopy data were collected on single crystals of K3Am(PO4)2 and compared to the calculated Raman spectrum of K3Am(PO4)2 obtained from DFT calculations.
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