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合成一种 Zn(II)-2-氨基咪唑骨架作为高效碳酸酐酶模拟物。

Synthesis of a Zn(II)-2-aminoimidazole Framework as an Efficient Carbonic Anhydrase Mimic.

机构信息

State Key Laboratory of Heavy Oil Processing and Center for Bioengineering and Biotechnology, College of Chemistry and Chemical Engineering, China University of Petroleum (East China), 66 Changjiang West Road, Qingdao 266580, China.

出版信息

Langmuir. 2024 Sep 17;40(37):19775-19786. doi: 10.1021/acs.langmuir.4c02563. Epub 2024 Sep 3.

Abstract

Carbonic anhydrase (CA) plays a crucial role in the CO capture processes by catalyzing the hydration of CO. In this study, we synthesized a bioinspired carbonic anhydrase Zn-MOF (metal-organic framework) incorporating 2-aminoimidazole and Zn as initial constituents. The synthesized Zn-MOF exhibited promising potential for efficiently catalyzing the CO hydration. Structural analyses such as SEM, XRD, and BET confirmed that the Zn-MOF crystal consisted of stacked grains with an average size of approximately 36 nm, forming a micron-sized spherical structure. Functionally, Zn-MOF exhibited effective catalytic activity toward both CO hydration and ester hydrolysis. The introduction of amino groups significantly enhanced the esterase activity of Zn-MOF to 0.28 U/mg at ambient temperature, which was twice that of ZIF-8. Furthermore, the introduction of amino groups resulted in remarkable hydrothermal stability, with the esterase activity reaching 0.72 U/mg after undergoing hydrothermal treatment at 80 °C for 12 h. Additionally, Zn-MOF exhibited enhanced capability in CO hydration at a pH value exceeding 8.5. After six repeated uses, ZIF-8 and Zn-MOF retained approximately 68 and 65% of their initial enzyme activity, respectively, underscoring the potential practical applicability of Zn-MOF in industrial CO capture processes. This work showcases the development of a novel Zn-MOF crystal as an efficient CA mimic, effectively emulating the active sites of natural CA using 2-aminoimidazole as a coordinating ligand for Zn coordination. These findings not only advance the field of innovative enzyme mimics but also pave the way for further exploration of industrial CO capture catalysts.

摘要

碳酸酐酶(CA)在 CO 捕获过程中通过催化 CO 的水合反应发挥着关键作用。在这项研究中,我们合成了一种仿生碳酸酐酶 Zn-MOF(金属有机骨架),其包含 2-氨基咪唑和 Zn 作为初始成分。合成的 Zn-MOF 表现出高效催化 CO 水合反应的潜力。结构分析,如 SEM、XRD 和 BET,证实了 Zn-MOF 晶体由堆叠的晶粒组成,平均粒径约为 36nm,形成了微米级的球形结构。在功能方面,Zn-MOF 对 CO 水合和酯水解均表现出有效的催化活性。引入氨基基团显著提高了 Zn-MOF 的酯酶活性,在环境温度下达到 0.28U/mg,是 ZIF-8 的两倍。此外,引入氨基基团还赋予了 Zn-MOF 显著的热稳定性,经过 80°C 12 小时的水热处理后,酯酶活性达到 0.72U/mg。此外,Zn-MOF 在 pH 值超过 8.5 的条件下表现出增强的 CO 水合能力。经过六次重复使用,ZIF-8 和 Zn-MOF 分别保留了约 68%和 65%的初始酶活性,这表明 Zn-MOF 在工业 CO 捕获过程中具有潜在的实际应用价值。这项工作展示了一种新型 Zn-MOF 晶体的开发,作为一种高效的 CA 模拟物,有效地模拟了天然 CA 的活性位点,使用 2-氨基咪唑作为 Zn 配位的配位体。这些发现不仅推动了创新酶模拟物领域的发展,也为进一步探索工业 CO 捕获催化剂铺平了道路。

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