Tailorable synthesis of heterogeneous enzyme–copper nanobiohybrids and their application in the selective oxidation of benzene to phenol,Catalysis Science & Technology

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Tailorable synthesis of heterogeneous enzyme–copper nanobiohybrids and their application in the selective oxidation of benzene to phenol
Catalysis Science & Technology ( IF 4.4 ) Pub Date : 2019-11-27 , DOI: 10.1039/c9cy02091h
Noelia Losada-García _{1,

2,

3,

4} , Alba Rodríguez-Otero _{1,

2,

3,

4} , Jose M. Palomo _{1,

2,

3,

4}

Affiliation

A protein-direct synthetic route to make nanobiohybrids containing copper nanoparticles (CuNPs) using an enzyme in combination with copper sulfate in aqueous media at room temperature is described. Enzyme–Cu(II) intermediates, rapidly generated in aqueous media, are transformed, induced by the enzyme structure, to facilitate the formation of a particular Cu species, tailoring the size of the nanoparticles formed depending on the experimental conditions, e.g. the pH, reducing step, amount of enzyme or incubation time. This controlled synthesis allows the preparation of tailor-made nanobiohybrids of Cu(0)NPs, Cu(0)/Cu₂ONPs, Cu₂ONPs or Cu₃(PO₄)₂NPs on the multimilligram scale. The catalytic performance of the novel CuNPs nanobiohybrids was evaluated in relation to the selective C–H functionalization of benzene via direct monohydroxylation using hydrogen peroxide as a green oxidant under mild conditions, in aqueous media and at moderate temperature. Optimization of the amount of hydrogen peroxide, the co-solvent, and the temperature was performed, resulting in the production of 17 mM phenol with 83% selectivity using the Cu-CALB-PHOS-NR nanobiohybrid as a catalyst.

中文翻译：

异质酶-铜纳米生物杂化体的可定制合成及其在苯选择性氧化为苯酚中的应用

描述了在室温下使用酶结合硫酸铜在水性介质中制备含铜纳米颗粒（CuNPs）的纳米生物杂化物的蛋白质直接合成途径。在水介质中快速生成的酶–Cu（II）中间体通过酶结构被转化，以促进特定Cu物种的形成，根据实验条件（例如pH值）调整所形成的纳米颗粒的尺寸，还原步骤，酶量或孵育时间。这种受控的合成方法可以制备定制的Cu（0）NPs，Cu（0）/ Cu ₂ ONPs，Cu ₂ ONPs或Cu ₃（PO ₄）₂纳米生物杂化物毫克级的NP。通过在温和的条件下，在水性介质中和在中等温度下，使用过氧化氢作为绿色氧化剂，通过直接单羟基化直接通过单羟基化作用，对新型CuNPs纳米生物杂化物的催化性能进行了评估。使用Cu-CALB-PHOS-NR纳米生物混合物作为催化剂，对过氧化氢，助溶剂和温度进行了优化，以17％的选择性生产了17 mM苯酚。

更新日期：2019-11-27

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