Benchmarking Guanidinium Organosulfonate Hydrogen-Bonded Frameworks for Structure Determination of Encapsulated Guests
Benchmarking Guanidinium Organosulfonate Hydrogen-Bonded Frameworks for Structure Determination of Encapsulated Guests
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DOI：
10.1021/acsmaterialslett.4c00400
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发表时间：
2024-04-10
影响因子：
11.4
通讯作者：
Ward，Michael D.
中科院分区：
文献类型：
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作者：
Yusov，Anna;Dillon，Alexandra M.;Ward，Michael D.
单晶 X 射线衍射 (SCXRD) 可以说是确定分子结构的最权威的方法，但它经常受到室温下为液体或油或无法形成足以进行分析的晶体的化合物的挑战。我们的实验室之前报道了一种基于有机磺酸胍（GS）氢键框架的简单、经济有效的单步结晶方法，用于多种封装客体分子的结构测定，包括手性中心的绝对构型的分配。在此，我们扩展了这些结果，并报告了 GS 方法与金刚烷类“分子伴侣”的头对头比较，据报道，金刚烷类“分子伴侣”是结构测定的有用宿主。仅限于两种 GS 宿主的包合物的特点是 R1 值和 Flack 参数低，宿主和客体很少发生紊乱，并且当确实存在紊乱时可以控制。一些未使用金刚烷分子伴侣包含或解析的目标分子的结构被 GS 宿主成功包含和解析，反之亦然。在 GS 方法尝试的 32 种客体中，有 31 种包合物提供了成功的客体结构解决方案，成功率为 97%。 GS 宿主和金刚烷类伴侣在客体包含方面是互补的，认为两者都应该在结构测定方法库中使用。此外，有机磺酸盐主体成分的低成本为广大用户提供了一种确定分子结构的可行途径。
Single crystal X-ray diffraction (SCXRD) is arguably the most definitive method for molecular structure determination, but it is often challenged by compounds that are liquids or oils at room temperature or do not form crystals adequate for analysis. Our laboratory previously reported a simple, cost-effective, single-step crystallization method based on guanidinium organosulfonate (GS) hydrogen bonded frameworks for structure determination of a wide range of encapsulated guest molecules, including assignment of the absolute configuration of chiral centers. Herein, we expand on those results and report a head-to-head comparison of the GS method with adamantoid “molecular chaperones”, which have been reported to be useful hosts for structure determination. Inclusion compounds limited to only two GS hosts are characterized by lowR1values and Flack parameters, infrequent disorder of the host and guest, and manageable disorder when it does exist. The structures of some target molecules that were not included or resolved using the adamantoid chaperones were successfully included and resolved by the GS hosts, and vice versa. Of the 32 guests attempted by the GS method, 31 inclusion compounds afforded successful guest structure solutions, a 97% success rate. The GS hosts and adamantoid chaperones are complementary with respect to guest inclusion, arguing that both should be employed in the arsenal of methods for structure determination. Furthermore, the low cost of organosulfonate host components promises an accessible route to molecular structure determination for a wide range of users.