Crystal structures of three uranyl-acetate-bipyridine complexes crystallized from hydraulic fracking fluid.

IF 0.7 4区化学 Q4 CHEMISTRY, MULTIDISCIPLINARY

Acta Crystallographica Section C Structural Chemistry Pub Date : 2024-01-01 DOI:10.1107/S2053229623010288

Abigail A Whittington, Alison R Keimowitz, Joseph M Tanski

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Abstract

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 UO₂^VI acetate complexes bis(acetato-κ²O,O')(2,2'-bipyridine-κ²N,N')dioxidouranium(VI), [U(C₂H₃O₂)₂O₂(C₁₀H₈N₂)₂] or [2,2'-bipyridine]U^VIO₂(CH₃CO₂)₂, (I), and bis(acetato-κ²O,O')(2,4'-bipyridine-κN^1')dioxidouranium(VI), [U(C₂H₃O₂)₂O₂(C₁₀H₈N₂)₂] or [2,4'-bipyridine]₂U^VIO₂(CH₃CO₂)₂, (III), contain eight-coordinate U^VI 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][(U^VIO₂)₃(O)₂(OH)₂(CH₃CO₂)₂·H₂O]}_n, (II), forms an ionic one-dimensional polymer with seven-coordinate pentagonal bipyramidal U^VI 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.

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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。

水力压裂法将页岩地层暴露在酸性水力压裂液（HFF）中，从而将有毒的铀（U）与所需的石油和天然气一起释放出来。由于没有现成的方法可以确保铀被封存在页岩中，本研究试图在水力压裂液中添加有机配体，以探索在页岩区保留铀的可能性。为了测试这种可能性，研究人员在原始 HFF 中添加了乙酸铀酰和一种有机联吡啶配体（2,2'-、2,3'-、2,4'- 或 4,4'- 联吡啶）作为结晶介质，并进行了培养。经过数月并完全蒸发掉所有挥发物后，从培养液中获得了大量黄色结晶物质，其中有三种结晶适合进行单晶分析，产生了两种新结构和一种以前描述过的化合物的高质量结构。醋酸 UO2VI 复合物双（醋酸-κ2O,O'）（2,2'-联吡啶-κ2N,N'）二氧化铀（VI），[U(C2H3O2)2O2(C10H8N2)2] 或 [2、2'-联吡啶]UVIO2(CH3CO2)2，(I)，以及双(乙酰氧基κO,O')(2,4'-联吡啶-κN1')二氧化硼(VI)、U(C2H3O2)2O2(C10H8N2)2]或[2,4'-联吡啶]2UVIO2(CH3CO2)2，(III)，含有八配位的 UVI，呈假六角双锥配位几何形状，是分子，通过弱 C-H...O/N相互作用，而双[双(2,3'-联吡啶鎓)[二-μ-乙酰氧基-μ-3-羟基-μ-羟基-二-μ-3-氧化-六氧化三铀(VI)]-2,3'-联吡啶-水 (1/1/1)]、(C10H9N2)2[U3(C2H3O2)2O8(OH)2]-C10H8N2-H2O或{[2、3'-联吡啶鎓]2[2,3'-联吡啶][(UVIO2)3(O)2(OH)2(CH3CO2)2-H2O]}n，(II)，形成一种离子型一维聚合物，具有七个配位的五角双锥 UVI 中心，每个链内都有氢键相互作用。这些晶体的形成可能表明联吡啶有可能在压裂过程中与页岩中的铀结合，这将在今后的研究中通过 ICP-MS（电感耦合等离子体质谱法）分析 HFF/联吡啶/页岩培养液中的铀浓度进行探讨。分子结构之间的差异可能表明联吡啶异构体与铀形成复合物的能力存在差异，这可能会影响它们在压裂过程中将铀保留在页岩中的能力。

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来源期刊

Acta Crystallographica Section C Structural Chemistry CHEMISTRY, MULTIDISCIPLINARYCRYSTALLOGRAPH-CRYSTALLOGRAPHY

CiteScore

1.60

自引率

12.50%

发文量

148

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.