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A Molybdenum Trioxide Hybrid Decorated by 3-(1,2,4-Triazol-4-yl)adamantane-1-carboxylic Acid: A Promising Reaction-Induced Self-Separating (RISS) Catalyst.
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2019-11-25 , DOI: 10.1021/acs.inorgchem.9b02137 Andrey B Lysenko 1 , Ganna A Senchyk 1 , Konstantin V Domasevitch 1 , Stefan Henfling 2 , Oliver Erhart 2 , Harald Krautscheid 2 , Patrícia Neves 3 , Anabela A Valente 3 , Martyn Pillinger 3 , Isabel S Gonçalves 3
Inorganic Chemistry ( IF 4.3 ) Pub Date : 2019-11-25 , DOI: 10.1021/acs.inorgchem.9b02137 Andrey B Lysenko 1 , Ganna A Senchyk 1 , Konstantin V Domasevitch 1 , Stefan Henfling 2 , Oliver Erhart 2 , Harald Krautscheid 2 , Patrícia Neves 3 , Anabela A Valente 3 , Martyn Pillinger 3 , Isabel S Gonçalves 3
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3-(1,2,4-Triazol-4-yl)adamantane-1-carboxylic acid (tradcH), a heterobifunctional organic ligand in which carboxylic acid and 1,2,4-triazole groups are united through a rigid 1,3-adamantanediyl spacer, was employed for the synthesis of a MoVI oxide organic hybrid. The ligand crystallized from water as tradcH·H2O (1), possessing a two-dimensional hydrogen-bonding network, and from ethanol as a cyclic molecular solvate with the composition (tradcH)3·2EtOH (2). Treatment of tradcH with MoO3 under hydrothermal conditions afforded a new Mo trioxide hybrid, [MoO3(tradcH)]·H2O (3), which was structurally characterized. In 3, the molybdenum atoms form a polymeric zigzag chain of {μ2-O-MoO2}n which is supported by double triazole bridges, while the carboxylic acid termini are left uncoordinated. The coordination environment of the Mo centers appears as distorted cis-{MoN2O4} octahedra. The hybrid exhibits high thermal stability (up to 270 °C) and was employed for a relatively broad scope of catalytic oxidation reactions in the liquid phase. Its catalytic behavior may be compared to a reversible mutation, featuring the best sides of homogeneous and heterogeneous catalysis. The original solid material converts into soluble active species, and the latter revert to the original material upon completion of the catalytic reaction, precipitating and allowing straightforward catalyst separation/reuse (like a heterogeneous catalyst). This catalyst was explored for a chemical reaction scope covering sulfoxidation, oxidative alcohol dehydrogenation, aldehyde oxidation, and olefin epoxidation, using hydrogen peroxide as an eco-friendly oxidant that gives water as a coproduct.
中文翻译：
3-（1,2,4-三唑-4-基）金刚烷-1-羧酸修饰的三氧化钼杂化物：有希望的反应诱导自分离（RISS）催化剂。
3-（1,2,4-三唑-4-基）金刚烷-1-羧酸（tradcH），一种杂双功能有机配体，其中羧酸和1,2,4-三唑基通过刚性的1,3相连-金刚烷二烯基间隔基用于合成MoVI氧化物有机杂化物。配体从水中结晶为tradcH·H2O（1），具有二维氢键网络，从乙醇中结晶为环状分子溶剂化物（tradcH）3·2EtOH（2）。在水热条件下用MoO3处理tradcH得到了一种新的三氧化钼杂化物[MoO3（tradcH）]·H2O（3），其结构经过了表征。在图3中，钼原子形成{μ2 -O-MoO 2} n的聚合物之字形链，该链由双三唑桥支撑，而羧酸末端未配位。Mo中心的配位环境显示为扭曲的顺式{MoN2O4}八面体。该杂化物表现出高的热稳定性（高达270°C），并被用于液相中相对较宽的催化氧化反应范围。可以将其催化行为与可逆突变进行比较，该突变具有均相和异相催化的最佳方面。原始固体物质转化为可溶性活性物质，而催化反应完成后，后者又恢复为原始物质，沉淀并允许直接进行催化剂分离/重复使用（如非均相催化剂）。对该催化剂的化学反应范围进行了探索，涉及的范围包括磺化氧化，氧化性醇脱氢，醛氧化和烯烃环氧化，
更新日期：2019-11-28
中文翻译：
3-（1,2,4-三唑-4-基）金刚烷-1-羧酸修饰的三氧化钼杂化物：有希望的反应诱导自分离（RISS）催化剂。
3-（1,2,4-三唑-4-基）金刚烷-1-羧酸（tradcH），一种杂双功能有机配体，其中羧酸和1,2,4-三唑基通过刚性的1,3相连-金刚烷二烯基间隔基用于合成MoVI氧化物有机杂化物。配体从水中结晶为tradcH·H2O（1），具有二维氢键网络，从乙醇中结晶为环状分子溶剂化物（tradcH）3·2EtOH（2）。在水热条件下用MoO3处理tradcH得到了一种新的三氧化钼杂化物[MoO3（tradcH）]·H2O（3），其结构经过了表征。在图3中，钼原子形成{μ2 -O-MoO 2} n的聚合物之字形链，该链由双三唑桥支撑，而羧酸末端未配位。Mo中心的配位环境显示为扭曲的顺式{MoN2O4}八面体。该杂化物表现出高的热稳定性（高达270°C），并被用于液相中相对较宽的催化氧化反应范围。可以将其催化行为与可逆突变进行比较，该突变具有均相和异相催化的最佳方面。原始固体物质转化为可溶性活性物质，而催化反应完成后，后者又恢复为原始物质，沉淀并允许直接进行催化剂分离/重复使用（如非均相催化剂）。对该催化剂的化学反应范围进行了探索，涉及的范围包括磺化氧化，氧化性醇脱氢，醛氧化和烯烃环氧化，
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