Preparation, characterization and activity of CuZn and Cu2 superoxide dismutase mimics encapsulated in mesoporous silica.,Journal of Inorganic Biochemistry

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Preparation, characterization and activity of CuZn and Cu2 superoxide dismutase mimics encapsulated in mesoporous silica.
Journal of Inorganic Biochemistry ( IF 3.8 ) Pub Date : 2020-02-24 , DOI: 10.1016/j.jinorgbio.2020.111050
Matías Patriarca ₁ , Verónica Daier ₁ , Gerardo Camí ₁ , Eric Rivière ₂ , Christelle Hureau ₃ , Sandra Signorella ₁

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Encapsulation of three superoxide dismutase (SOD) functional mimics, [CuZn(dien)2(μ-Im)(ClO4)2]ClO4 (1), [Cu2(dien)2(μ-Im)(ClO4)2]ClO4 (2) (Im = imidazolate, dien = diethylenetriamine), and [CuZn(salpn)Cl2] (3) (H2salpn = 1,3-bis(salicylideneamino)propane) in mesoporous MCM-41 silica afforded three hybrid catalysts 1@MCM-41, 2@MCM-41 and 3@MCM-41. Spectroscopic and magnetic analyses of these materials confirmed the metal centers of the complexes keep the coordination sphere after insertion into the MCM-41 silica matrix. For the imidazolate-bridged complexes the silica channels restraint the relative orientation of the two metal ions. While 3@MCM-41 shows SOD activity significantly lower than the host-free complex, insertion of the imidazolate-bridged CuZn or Cu2 complexes by ion exchange onto mesoporous MCM-41 silica affords durable and recoverable supported catalysts with much better SOD activity than the free complexes. For confined imidazolate-bridged complexes, 1@MCM-41 and 2@MCM-41, the small pore size of the silica matrix improves the SOD activity more than a host with larger pores. This high SOD activity is attributed to the close-fitting of the complexes into the nanochannels of MCM-41 silica that favors the Cu active site and HImZn(or Cu) group stay in close proximity during catalysis.

中文翻译：

包埋在介孔二氧化硅中的CuZn和Cu2超氧化物歧化酶模拟物的制备，表征和活性。

封装的三种超氧化物歧化酶（SOD）功能模拟物[CuZn（dien）2（μ-Im）（ClO4）2] ClO4（1），[Cu2（dien）2（μ-Im）（ClO4）2] ClO4（ 2）在中孔MCM-41二氧化硅中的（Im =咪唑酸酯，dien =二亚乙基三胺）和[CuZn（salpn）Cl2]（3）（H2salpn = 1,3-双（水杨基亚氨基）丙烷）在硅胶中提供了三种杂化催化剂1 @ MCM- 41、2 @ MCM-41和3 @ MCM-41。这些材料的光谱和磁学分析证实，配合物的金属中心插入MCM-41二氧化硅基质后，保持了配位球。对于咪唑化物桥联的配合物，二氧化硅通道限制了两种金属离子的相对取向。尽管3 @ MCM-41显示SOD活性明显低于无宿主复合物，通过离子交换将咪唑化物桥联的CuZn或Cu2配合物插入介孔MCM-41二氧化硅，可提供耐用且可回收的负载型催化剂，其SOD活性比游离配合物好得多。对于局限的咪唑基桥联络合物1 @ MCM-41和2 @ MCM-41，二氧化硅基质的小孔径比具有较大孔的主体更能提高SOD活性。这种高的SOD活性归因于配合物紧密配合到MCM-41二氧化硅的纳米通道中，这有利于Cu活性位点，并且HImZn（或Cu）基团在催化过程中紧密相邻。

更新日期：2020-02-25

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