Thiele Grace A R, Friedman Connie P, Tsai Kathleen J S, Beld Joris, Londergan Casey H, Charkoudian Louise K
Department of Chemistry, Haverford College , Haverford, Pennsylvania 19041-1392, United States.
Department of Microbiology and Immunology, Drexel University College of Medicine , 245 North 15th Street, Philadelphia, Pennsylvania 19102, United States.
Biochemistry. 2017 May 23;56(20):2533-2536. doi: 10.1021/acs.biochem.7b00219. Epub 2017 May 8.
Acyl carrier proteins (ACPs) are central hubs in polyketide and fatty acid biosynthetic pathways, but the fast motions of the ACP's phosphopantetheine (Ppant) arm make its conformational dynamics difficult to capture using traditional spectroscopic approaches. Here we report that converting the terminal thiol of Escherichia coli ACP's Ppant arm into a thiocyanate activates this site to form a selective cross-link with the active site cysteine of its partner ketoacyl synthase (FabF). The reaction releases a cyanide anion, which can be detected by infrared spectroscopy. This represents a practical and generalizable method for obtaining and visualizing ACP-protein complexes relevant to biocatalysis and will be valuable in future structural and engineering studies.
酰基载体蛋白(ACPs)是聚酮化合物和脂肪酸生物合成途径的核心枢纽,但ACP的磷酸泛酰巯基乙胺(Ppant)臂的快速运动使得使用传统光谱方法难以捕捉其构象动力学。在此,我们报告将大肠杆菌ACP的Ppant臂的末端硫醇转化为硫氰酸盐会激活该位点,从而与它的伴侣酮酰基合酶(FabF)的活性位点半胱氨酸形成选择性交联。该反应会释放出一个氰化物阴离子,可通过红外光谱进行检测。这代表了一种获取和可视化与生物催化相关的ACP-蛋白质复合物的实用且可推广的方法,在未来的结构和工程研究中将具有重要价值。