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Side Chain Induced Self-Assembly and Selective Catalytic Oxidation Activity of Copper(I)–Copper(II)-N4 Complexes
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2020-01-15 , DOI: 10.1021/acs.cgd.9b01499 Yun-Long Hou 1 , Yun-Lei Peng 2 , Yingxue Diao 3 , Jie Liu 4 , Lizhuang Chen 1 , Dan Li 2
Crystal Growth & Design ( IF 3.2 ) Pub Date : 2020-01-15 , DOI: 10.1021/acs.cgd.9b01499 Yun-Long Hou 1 , Yun-Lei Peng 2 , Yingxue Diao 3 , Jie Liu 4 , Lizhuang Chen 1 , Dan Li 2
Affiliation
Crystalline coordination architectures with coordinatively unsaturated metal sites are of great importance for their attractive properties. Tunable side chains of the 4-formylimidazole here were employed for directing the subcomponent self-assembly of (CuIIN4)2(CuII)2 (1), {(CuIIN4)(CuII)2}n (2), and {L(CuII)2}n (3) under the same solvothermal conditions, giving the structural diversity. The unique square-planar CuII/NiIIN4 units with open metal sites can not only be in situ embedded in 1 and 2, but also be successfully immobilized in {(NiIIN4)2(CuICN)9}n (4) and {(CuIIN4)2(CuICN)9}n (5), through the metalloligand strategy. Enzyme-like substrate-specific activity was observed by employing 5 as a heterogeneous catalyst, which exhibits increased activity and high selectivity toward the catalytic oxidation of 1-phenylethyl alcohol derivatives. This work presents two promising methodologies for the introduction of controllable open metal sites in versatile crystalline coordination complexes and their application in the substrate-selective catalytic oxidation reaction.
中文翻译:
侧链诱导的铜(I)-铜(II)-N 4配合物的自组装和选择性催化氧化活性
具有不饱和配位金属位点的晶体配位结构对于其吸引人的性能非常重要。4-甲酰基咪唑这里被用于引导副成分的自组装的可调谐侧链(铜II Ñ 4)2(铜我I)2(1),{(铜II Ñ 4)(铜我I)2 } n(2)和{ L(Cu I I)2 } n(3)在相同的溶剂热条件下,给出了结构多样性。具有开放金属位点的独特方形平面Cu II / Ni II N 4单元不仅可以原位嵌入1和2中,而且还可以成功地固定在{(Ni II N 4)2(Cu I CN)9 }中n(4)和{(Cu II N 4)2(Cu I CN)9 } n(5),通过金属配体策略。通过使用5作为非均相催化剂,可以观察到酶样底物的特定活性,该催化剂显示出更高的活性和对1-苯乙醇衍生物的催化氧化的高选择性。这项工作提出了两种有前途的方法学,用于在通用的晶体配位络合物中引入可控的开放金属位点,并将其应用在底物选择性催化氧化反应中。
更新日期:2020-01-16
中文翻译:
侧链诱导的铜(I)-铜(II)-N 4配合物的自组装和选择性催化氧化活性
具有不饱和配位金属位点的晶体配位结构对于其吸引人的性能非常重要。4-甲酰基咪唑这里被用于引导副成分的自组装的可调谐侧链(铜II Ñ 4)2(铜我I)2(1),{(铜II Ñ 4)(铜我I)2 } n(2)和{ L(Cu I I)2 } n(3)在相同的溶剂热条件下,给出了结构多样性。具有开放金属位点的独特方形平面Cu II / Ni II N 4单元不仅可以原位嵌入1和2中,而且还可以成功地固定在{(Ni II N 4)2(Cu I CN)9 }中n(4)和{(Cu II N 4)2(Cu I CN)9 } n(5),通过金属配体策略。通过使用5作为非均相催化剂,可以观察到酶样底物的特定活性,该催化剂显示出更高的活性和对1-苯乙醇衍生物的催化氧化的高选择性。这项工作提出了两种有前途的方法学,用于在通用的晶体配位络合物中引入可控的开放金属位点,并将其应用在底物选择性催化氧化反应中。