Supramolecular purification of mono-adamantane mixtures by enhanced stability in three-shell Matryoshka-type assemblies

The adamantane (Ad) core is widely spread in the pharmaceutical realm since it is considered a lipophilic bullet that boosts the bioactivity of Ad-bearing drugs. However, little is known about the precise recognition modes in confined enzymatic active sites, and poor chromatographic strategies are reported for the purification of mixtures of Ad-derivatives. Here we report on the exquisite supramolecular purification of mono-adamantane mixtures by the development of three-shell supramolecular Matryoshkas featuring an adamantane-cycloparaphenylene (CPP) host-guest adduct encapsulated in a tetragonal prismatic nanocage. The three-shell assembly features an all-in-one strategy, since the encapsulation is inefficient for either [8]CPP or diamondoids alone, and is only formed efficiently when the three components are present. A straightforward solid-state filtration-redissolution protocol allows the purification of diamondoid mixtures, with enhanced preference to amine-bearing adamantane derivatives. This level of supramolecular selectivity among diamondoid complex mixtures is unprecedented, surpassing chromatographic techniques. This deposit includes parameter files of the nanocapsule and the guests studied (diamontoides and CPP rings), output files of the simulations without solvent of the different systems and files releated to the well-tempered metadynamics carried out.金刚烷（adamantane, Ad）核心因其被视作可提升含金刚烷药物生物活性的亲脂性弹头，而在制药领域得到广泛应用。然而，人们对其在受限酶活性位点中的精准识别模式知之甚少，且目前鲜有针对金刚烷衍生物混合物纯化的高效色谱策略报道。本工作开发了以金刚烷-环对苯撑（cycloparaphenylene, CPP）主客体加合物为内核、封装于四方棱柱形纳米笼中的三层超分子俄罗斯套娃结构，实现了单金刚烷混合物的精准超分子纯化。该三层组装体采用一体化策略：单独使用[8]CPP或金刚石烷类（diamondoids）时包封效率低下，仅当三种组分同时存在时才能高效形成。通过简便的固态过滤-再溶解操作流程，即可实现金刚石烷类混合物的纯化，且对含胺基的金刚烷衍生物具有更优的选择性偏好。这种针对复杂金刚石烷混合物的超分子选择性水平前所未有，其性能远超传统色谱技术。 本数据集包含纳米笼及所研究客体（金刚石烷类与CPP环）的参数文件、不同体系无溶剂模拟的输出文件，以及与所开展的温控元动力学（well-tempered metadynamics）相关的各类文件。