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首页> 外文期刊>Catalysis science & technology >Efficient nitrogen-13 radiochemistry catalyzed by a highly stable immobilized biocatalyst
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Efficient nitrogen-13 radiochemistry catalyzed by a highly stable immobilized biocatalyst

机译：高度稳定的固定生物催化剂催化的有效氮-13放射化学

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摘要

The continuous progress of nuclear imaging techniques demands the development and implementation of efficient, clean and sustainable synthetic routes for the preparation of novel radiotracers. This is especially challenging in the context of radiotracers labelled with short-lived positron emitters such as nitrogen-13. Biocatalysis can offer attractive alternatives to conventional chemistry, because enzymes present exquisite chemical selectivity and high turnover numbers. However, enzymes have been poorly exploited in the area of radiochemistry. Herein, we present the design and fabrication of a heterogeneous biocatalyst suitable for the reduction of [N-13] NO3- to [N-13] NO2-. A eukaryotic nitrate reductase from Aspergillus niger was immobilized on different carriers and immobilization parameters were determined. Optimal results were obtained for agarose beads activated with a positively charged tertiary amino group (Ag-DEAE). The immobilized preparation was 12-fold more thermostable than the soluble enzyme. Biochemical characterization of the immobilized enzyme showed interesting thermally-induced hyperactivation driven by the interaction between the enzyme and the carrier. The heterogeneous biocatalyst could be re-used up to 7 reaction cycles while preserving its initial activity. Finally, to demonstrate the potential of this heterogeneous biocatalyst in the context of radiochemistry, radiosynthesis of S-[N-13] nitrosoglutathione was carried out using the enzymatically produced [N-13] NO (-)(2) as the labelling agent.
机译：核成像技术的持续进展需要开发和实施高效，清洁和可持续的合成途径，以制备新型的放射性示意剂。在用短寿命正电子发射器（如氮13）标记的放射性示例的背景下，这尤其具有挑战性。生物催化可以为常规化学提供有吸引力的替代品，因为酶具有精致的化学选择性和高的周转率。但是，在放射化学领域，酶的利用很差。本文中，我们介绍了适用于[N-13] NO3-至[N-13] NO2-的异质生物催化剂的设计和制造。固定在不同的载体上，并确定了固定参数。对于用正电荷氨基氨基（AG-DEAE）激活的琼脂糖珠获得的最佳结果。固定的制剂比可溶性酶高12倍。固定酶的生化表征显示出有趣的热诱导的过度激活，这是由酶与载体之间的相互作用驱动的。在保留其初始活性的同时，可以将异质性生物催化剂重新使用多达7个反应周期。最后，为了证明这种异质性生物催化剂在放射化学的背景下，使用酶促产生的[n-13] no（ - ）（2）作为标记剂，使用了s- [n-13]硝基谷氨酸的放射性合成。

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