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基于氮化碳的两亲性 Janus 型 N 掺杂碳/ MoS2 纳米片的设计与制备及其用于界面酶纳米反应器。

Design and Preparation of Carbon Nitride-Based Amphiphilic Janus N-Doped Carbon/MoS Nanosheets for Interfacial Enzyme Nanoreactor.

机构信息

Hubei Key Laboratory of Lipid Chemistry and Nutrition, Key Laboratory of Oilseeds Processing, Ministry of Agriculture and Rural Affairs, Oil Crops Research Institute, Chinese Academy of Agricultural Sciences, Wuhan 430062, China.

College of Chemistry, Chemical Engineering and Materials Science, Key Laboratory of Molecular and Nano Probes, Ministry of Education, Shandong Normal University, Jinan 250014, China.

出版信息

ACS Appl Mater Interfaces. 2020 Mar 11;12(10):12227-12237. doi: 10.1021/acsami.9b18735. Epub 2020 Feb 27.

Abstract

Janus amphiphilic particles have gained much attention for their important application value in areas as diverse as interfacial modification, sensors, drug delivery, optics, and actuators. In this work, we prepared Janus amphiphilic nanosheets composed of nitrogen-doped stratiform meso-macroporous carbons (NMC) and molybdenum sulfide (MoS) for hydrophilic and hydrophobic sides, respectively. The dicyandiamide and glucose were used as precursors for synthesizing two-dimensional nitrogen-doped meso-macroporous carbons, and the molybdate could be anchored by the functional groups on the surface of carbon layers and then transform into uniformly MoS to form the Janus amphiphilic layer by layer NMC/MoS support. Transmission electron microscopy, scanning electron microscopy, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy are used to demonstrate the successful preparation of Janus materials. As the typical interfacial enzyme, lipase (CRL) immobilized on the Janus amphiphilic NMC/MoS support brought forth to improvement of its performance because the Janus nanosheets can be easily attached on the oil-aqueous interface for better catalytic activity (interfacial activation of lipases). The obtained immobilized lipase (NMC/MoS@CRL) exhibited satisfactory lipase loading (193.1 mg protein per g), specific hydrolytic activity (95.76 U g), thermostability (at 55 °C, 84% of the initial activity remained after 210 min), pH flexibility, and recyclability (60% of the initial activity remained after nine runs). In terms of its application, the esterification rate of using NMC/MoS@CRL (75%) is higher than those of NMC@CRL (20%) and MoS@CRL (11.8%) in the "oil-water" biphase and CRL as well as NMC/MoS@CRL in the one-phase. Comparing with the free CRL, NMC@CRL, and MoS@CRL, the Janus amphiphilic NMC/MoS served as a carrier that exhibited more optimal performance and practicability.

摘要

Janus 两亲粒子因其在界面改性、传感器、药物输送、光学和致动器等领域的重要应用价值而备受关注。在这项工作中,我们制备了由氮掺杂层状介孔大孔碳 (NMC) 和硫化钼 (MoS) 组成的 Janus 两亲性纳米片,分别作为亲水和疏水侧。双氰胺和葡萄糖被用作合成二维氮掺杂介孔大孔碳的前体,而钼酸盐可以通过碳层表面的官能团固定,并进一步转化为均匀的 MoS,通过层层自组装形成 Janus 两亲性 NMC/MoS 载体。透射电子显微镜、扫描电子显微镜、X 射线光电子能谱和傅里叶变换红外光谱用于证明 Janus 材料的成功制备。作为典型的界面酶,脂肪酶 (CRL) 固定在 Janus 两亲性 NMC/MoS 载体上,提高了其性能,因为 Janus 纳米片可以很容易地附着在油-水界面上,从而获得更好的催化活性(脂肪酶的界面激活)。所获得的固定化脂肪酶 (NMC/MoS@CRL) 表现出令人满意的脂肪酶负载量(每克 193.1 毫克蛋白质)、比水解活性(95.76 U/g)、热稳定性(在 55°C 下,210 分钟后仍保持初始活性的 84%)、pH 灵活性和可回收性(经过 9 次运行后仍保持初始活性的 60%)。在应用方面,使用 NMC/MoS@CRL(75%)的酯化率高于 NMC@CRL(20%)和 MoS@CRL(11.8%)在“油-水”两相以及 CRL 和 NMC/MoS@CRL 单相中的酯化率。与游离 CRL、NMC@CRL 和 MoS@CRL 相比,Janus 两亲性 NMC/MoS 作为载体表现出更优的性能和实用性。

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