Mechanochemical synthesis of Zn-bionanohybrids: size effect at the nanoscale to improve their enzyme-like activity†

Carla Garcia-Sanz, Laura Guijarro, Mirosława Pawlyta and Jose M. Palomo
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Abstract

The mechanochemical synthesis of nanomaterials for catalytic applications is a growing research field owing to its simplicity, scalability, and eco-friendliness. In this work, we synthesised new zinc bionanohybrids via a mechanochemical method involving a size effect at the nanoscale and microscale levels of the final nanostructure. This effect translates into an improvement in the catalytic properties of this nanomaterial, such as enzyme-like activities, compared to that synthesized in an aqueous media. One-pot synthesis was performed by combining Candida antarctica lipase B (CALB) solution, solid zinc salts and phosphate or bicarbonate salts using the ball-milling approach, where overall reaction times were drastically reduced in comparison with the traditional aqueous method. The reaction was carried out at r.t. and the synthesis process was evaluated by considering the use of steel balls with different sizes, completely dry conditions or in the presence of a very small amount of water as an additive (2 mL), and incubation methods (planetary or horizontal ball milling). The final nanostructure of the Zn biohybrids was determined using XRD, FT-IR, TEM and SEM analysis, demonstrating changes in metal species and drastic changes in the nanostructure conformation of the biohybrids obtained through the mechanical approach compared to those obtained through the aqueous method. The size effect at the nanoscale was also demonstrated in the final species, showing a reduced size. This nanoscale effect of the material had a positive impact on the catalytic properties of the materials, in some cases showing up to 2000 times greater activity compared to the counterpart synthesised under aqueous conditions.

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Zn 生物杂化物的机械化学合成:通过纳米尺度的尺寸效应提高其酶样活性†。
用于催化应用的纳米材料的机械化学合成因其简便性、可扩展性和生态友好性而成为一个不断发展的研究领域。在这项工作中,我们通过一种机械化学方法合成了新的锌仿生杂化物,这种方法涉及最终纳米结构的纳米级和微米级尺寸效应。与在水介质中合成的纳米材料相比,这种效应提高了这种纳米材料的催化特性,如类似酶的活性。采用球磨法将白色念珠菌脂肪酶 B(CALB)溶液、固体锌盐和磷酸盐或碳酸氢盐结合在一起进行了单锅合成,与传统的水溶液法相比,整个反应时间大大缩短。反应是在恒温条件下进行的,并通过考虑使用不同大小的钢球、完全干燥条件或在有极少量水作为添加剂(2 mL)的情况下,以及培养方法(行星式或水平式球磨)对合成过程进行了评估。通过 XRD、FT-IR、TEM 和 SEM 分析测定了锌生物混合物的最终纳米结构,结果表明,与水溶液法相比,通过机械法获得的生物混合物的金属种类发生了变化,纳米结构的构象也发生了巨大变化。纳米尺度的尺寸效应也体现在最终产品上,显示出尺寸的缩小。材料的这种纳米级效应对材料的催化特性产生了积极影响,在某些情况下,材料的活性比在水溶液条件下合成的材料高出多达 2000 倍。
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