Abigail A Whittington, Alison R Keimowitz, Joseph M Tanski
{"title":"从水力压裂液中结晶出的三种铀酰-乙酸盐-联吡啶复合物的晶体结构。","authors":"Abigail A Whittington, Alison R Keimowitz, Joseph M Tanski","doi":"10.1107/S2053229623010288","DOIUrl":null,"url":null,"abstract":"<p><p>Hydraulic fracking exposes shale plays to acidic hydraulic fracking fluid (HFF), releasing toxic uranium (U) along with the desired oil and gas. With no existing methods to ensure U remains sequestered in the shale, this study sought to add organic ligands to HFF to explore potential U retention in shale plays. To test this possibility, incubations were set up in which uranyl acetate and one organic bipyridine ligand (either 2,2'-, 2,3'-, 2,4'-, or 4,4'-bipyridine) were added to pristine HFF as the crystallization medium. After several months and complete evaporation of all volatiles, bulk yellow crystalline material was obtained from the incubations, three of which yielded crystals suitable for single-crystal analysis, resulting in two novel structures and a high-quality structure of a previously described compound. The UO<sub>2</sub><sup>VI</sup> acetate complexes bis(acetato-κ<sup>2</sup>O,O')(2,2'-bipyridine-κ<sup>2</sup>N,N')dioxidouranium(VI), [U(C<sub>2</sub>H<sub>3</sub>O<sub>2</sub>)<sub>2</sub>O<sub>2</sub>(C<sub>10</sub>H<sub>8</sub>N<sub>2</sub>)<sub>2</sub>] or [2,2'-bipyridine]U<sup>VI</sup>O<sub>2</sub>(CH<sub>3</sub>CO<sub>2</sub>)<sub>2</sub>, (I), and bis(acetato-κ<sup>2</sup>O,O')(2,4'-bipyridine-κN<sup>1'</sup>)dioxidouranium(VI), [U(C<sub>2</sub>H<sub>3</sub>O<sub>2</sub>)<sub>2</sub>O<sub>2</sub>(C<sub>10</sub>H<sub>8</sub>N<sub>2</sub>)<sub>2</sub>] or [2,4'-bipyridine]<sub>2</sub>U<sup>VI</sup>O<sub>2</sub>(CH<sub>3</sub>CO<sub>2</sub>)<sub>2</sub>, (III), contain eight-coordinate U<sup>VI</sup> in a pseudo-hexagonal bipyramidal coordination geometry and are molecular, packing via weak C-H...O/N interactions, whereas catena-poly[bis(2,3'-bipyridinium) [di-μ-acetato-μ<sub>3</sub>-hydroxido-μ-hydroxido-di-μ<sub>3</sub>-oxido-hexaoxidotriuranium(VI)]-2,3'-bipyridine-water (1/1/1)], (C<sub>10</sub>H<sub>9</sub>N<sub>2</sub>)<sub>2</sub>[U<sub>3</sub>(C<sub>2</sub>H<sub>3</sub>O<sub>2</sub>)<sub>2</sub>O<sub>8</sub>(OH)<sub>2</sub>]·C<sub>10</sub>H<sub>8</sub>N<sub>2</sub>·H<sub>2</sub>O or {[2,3'-bipyridinium]<sub>2</sub>[2,3'-bipyridine][(U<sup>VI</sup>O<sub>2</sub>)<sub>3</sub>(O)<sub>2</sub>(OH)<sub>2</sub>(CH<sub>3</sub>CO<sub>2</sub>)<sub>2</sub>·H<sub>2</sub>O]}<sub>n</sub>, (II), forms an ionic one-dimensional polymer with seven-coordinate pentagonal bipyramidal U<sup>VI</sup> centers and hydrogen-bonding interactions within each chain. The formation of these crystals could indicate the potential for bipyridine to bind with U in shale during fracking, which will be explored in a future study via ICP-MS (inductively coupled plasma mass spectrometry) analyses of U concentration in HFF/bipyridine/shale incubations. The variation seen here between the molecular structures may indicate variance in the ability of bipyridine isomers to form complexes with U, which could impact their ability to retain U within shale in the context of fracking.</p>","PeriodicalId":7115,"journal":{"name":"Acta Crystallographica Section C Structural Chemistry","volume":null,"pages":null},"PeriodicalIF":0.7000,"publicationDate":"2024-01-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Crystal structures of three uranyl-acetate-bipyridine complexes crystallized from hydraulic fracking fluid.\",\"authors\":\"Abigail A Whittington, Alison R Keimowitz, Joseph M Tanski\",\"doi\":\"10.1107/S2053229623010288\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Hydraulic fracking exposes shale plays to acidic hydraulic fracking fluid (HFF), releasing toxic uranium (U) along with the desired oil and gas. With no existing methods to ensure U remains sequestered in the shale, this study sought to add organic ligands to HFF to explore potential U retention in shale plays. To test this possibility, incubations were set up in which uranyl acetate and one organic bipyridine ligand (either 2,2'-, 2,3'-, 2,4'-, or 4,4'-bipyridine) were added to pristine HFF as the crystallization medium. After several months and complete evaporation of all volatiles, bulk yellow crystalline material was obtained from the incubations, three of which yielded crystals suitable for single-crystal analysis, resulting in two novel structures and a high-quality structure of a previously described compound. The UO<sub>2</sub><sup>VI</sup> acetate complexes bis(acetato-κ<sup>2</sup>O,O')(2,2'-bipyridine-κ<sup>2</sup>N,N')dioxidouranium(VI), [U(C<sub>2</sub>H<sub>3</sub>O<sub>2</sub>)<sub>2</sub>O<sub>2</sub>(C<sub>10</sub>H<sub>8</sub>N<sub>2</sub>)<sub>2</sub>] or [2,2'-bipyridine]U<sup>VI</sup>O<sub>2</sub>(CH<sub>3</sub>CO<sub>2</sub>)<sub>2</sub>, (I), and bis(acetato-κ<sup>2</sup>O,O')(2,4'-bipyridine-κN<sup>1'</sup>)dioxidouranium(VI), [U(C<sub>2</sub>H<sub>3</sub>O<sub>2</sub>)<sub>2</sub>O<sub>2</sub>(C<sub>10</sub>H<sub>8</sub>N<sub>2</sub>)<sub>2</sub>] or [2,4'-bipyridine]<sub>2</sub>U<sup>VI</sup>O<sub>2</sub>(CH<sub>3</sub>CO<sub>2</sub>)<sub>2</sub>, (III), contain eight-coordinate U<sup>VI</sup> in a pseudo-hexagonal bipyramidal coordination geometry and are molecular, packing via weak C-H...O/N interactions, whereas catena-poly[bis(2,3'-bipyridinium) [di-μ-acetato-μ<sub>3</sub>-hydroxido-μ-hydroxido-di-μ<sub>3</sub>-oxido-hexaoxidotriuranium(VI)]-2,3'-bipyridine-water (1/1/1)], (C<sub>10</sub>H<sub>9</sub>N<sub>2</sub>)<sub>2</sub>[U<sub>3</sub>(C<sub>2</sub>H<sub>3</sub>O<sub>2</sub>)<sub>2</sub>O<sub>8</sub>(OH)<sub>2</sub>]·C<sub>10</sub>H<sub>8</sub>N<sub>2</sub>·H<sub>2</sub>O or {[2,3'-bipyridinium]<sub>2</sub>[2,3'-bipyridine][(U<sup>VI</sup>O<sub>2</sub>)<sub>3</sub>(O)<sub>2</sub>(OH)<sub>2</sub>(CH<sub>3</sub>CO<sub>2</sub>)<sub>2</sub>·H<sub>2</sub>O]}<sub>n</sub>, (II), forms an ionic one-dimensional polymer with seven-coordinate pentagonal bipyramidal U<sup>VI</sup> centers and hydrogen-bonding interactions within each chain. The formation of these crystals could indicate the potential for bipyridine to bind with U in shale during fracking, which will be explored in a future study via ICP-MS (inductively coupled plasma mass spectrometry) analyses of U concentration in HFF/bipyridine/shale incubations. The variation seen here between the molecular structures may indicate variance in the ability of bipyridine isomers to form complexes with U, which could impact their ability to retain U within shale in the context of fracking.</p>\",\"PeriodicalId\":7115,\"journal\":{\"name\":\"Acta Crystallographica Section C Structural Chemistry\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.7000,\"publicationDate\":\"2024-01-01\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Acta Crystallographica Section C Structural Chemistry\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1107/S2053229623010288\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q4\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Acta Crystallographica Section C Structural Chemistry","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1107/S2053229623010288","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q4","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
Crystal structures of three uranyl-acetate-bipyridine complexes crystallized from hydraulic fracking fluid.
Hydraulic fracking exposes shale plays to acidic hydraulic fracking fluid (HFF), releasing toxic uranium (U) along with the desired oil and gas. With no existing methods to ensure U remains sequestered in the shale, this study sought to add organic ligands to HFF to explore potential U retention in shale plays. To test this possibility, incubations were set up in which uranyl acetate and one organic bipyridine ligand (either 2,2'-, 2,3'-, 2,4'-, or 4,4'-bipyridine) were added to pristine HFF as the crystallization medium. After several months and complete evaporation of all volatiles, bulk yellow crystalline material was obtained from the incubations, three of which yielded crystals suitable for single-crystal analysis, resulting in two novel structures and a high-quality structure of a previously described compound. The UO2VI acetate complexes bis(acetato-κ2O,O')(2,2'-bipyridine-κ2N,N')dioxidouranium(VI), [U(C2H3O2)2O2(C10H8N2)2] or [2,2'-bipyridine]UVIO2(CH3CO2)2, (I), and bis(acetato-κ2O,O')(2,4'-bipyridine-κN1')dioxidouranium(VI), [U(C2H3O2)2O2(C10H8N2)2] or [2,4'-bipyridine]2UVIO2(CH3CO2)2, (III), contain eight-coordinate UVI in a pseudo-hexagonal bipyramidal coordination geometry and are molecular, packing via weak C-H...O/N interactions, whereas catena-poly[bis(2,3'-bipyridinium) [di-μ-acetato-μ3-hydroxido-μ-hydroxido-di-μ3-oxido-hexaoxidotriuranium(VI)]-2,3'-bipyridine-water (1/1/1)], (C10H9N2)2[U3(C2H3O2)2O8(OH)2]·C10H8N2·H2O or {[2,3'-bipyridinium]2[2,3'-bipyridine][(UVIO2)3(O)2(OH)2(CH3CO2)2·H2O]}n, (II), forms an ionic one-dimensional polymer with seven-coordinate pentagonal bipyramidal UVI centers and hydrogen-bonding interactions within each chain. The formation of these crystals could indicate the potential for bipyridine to bind with U in shale during fracking, which will be explored in a future study via ICP-MS (inductively coupled plasma mass spectrometry) analyses of U concentration in HFF/bipyridine/shale incubations. The variation seen here between the molecular structures may indicate variance in the ability of bipyridine isomers to form complexes with U, which could impact their ability to retain U within shale in the context of fracking.
期刊介绍：
Acta Crystallographica Section C: Structural Chemistry is continuing its transition to a journal that publishes exciting science with structural content, in particular, important results relating to the chemical sciences. Section C is the journal of choice for the rapid publication of articles that highlight interesting research facilitated by the determination, calculation or analysis of structures of any type, other than macromolecular structures. Articles that emphasize the science and the outcomes that were enabled by the study are particularly welcomed. Authors are encouraged to include mainstream science in their papers, thereby producing manuscripts that are substantial scientific well-rounded contributions that appeal to a broad community of readers and increase the profile of the authors.
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