Zhang Chun, Yang Xiaolan, Gao Ang, Hu Xiaolei, Pu Jun, Liu Hongbo, Feng Juan, Liao Juan, Li Yuanli, Liao Fei
Unit for Analytical Probes and Protein Biotechnology, Key Laboratory of Clinical Laboratory Diagnostics of the Education Ministry, College of Laboratory Medicine, Chongqing Medical University, Chongqing, People's Republic of China.
Biotechnol Appl Biochem. 2014 Nov-Dec;61(6):683-90. doi: 10.1002/bab.1215. Epub 2014 Mar 28.
Uricase after modification with monomethoxy poly(ethylene glycol) (mPEG) is currently the sole agent to treat refractory gout. For formulating Bacillus fastidious uricase, succinimidyl carbonate of mPEG-5000 (SC-mPEG5k) and succinimidyl succinate of mPEG-5000 (SS-mPEG5k) were compared. SC-mPEG5k possessed higher purity, comparable reaction rate constant with glycine but lower hydrolysis rate, and stronger effectiveness to modify amino groups. The uricase possessed two types of amino groups bearing a 25-fold difference in reactivity with SC-mPEG5k or SS-mPEG5k at pH 9.2. Oxonate and xanthine concentration-dependently protected the bacterial uricase from inactivation during PEGylation. With SC-mPEG5k at a molar ratio of 200 to uricase subunits and oxonate of 50 µM, the PEGylated uricase (1) retained about 73% of the original activity, (2) displayed about 10% reactivity to rabbit anti-sera recognizing the native uricase, (3) elicited IgG in rats accounting for about 5% of that by the native uricase, (4) exhibited circulation half-life time of about 25 H in cock plasma in vivo, and (5) concurrently maintained uric acid at lowered levels for over 20 H. Hence, PEGylation with SC-mPEG under the protection of a competitive inhibitor was a practical approach to formulation of the bacterial uricase; protection of enzymes by competitive inhibitors during PEGylation may have universal significance.
用单甲氧基聚(乙二醇)(mPEG)修饰后的尿酸酶是目前治疗难治性痛风的唯一药物。为了制备苛求芽孢杆菌尿酸酶,比较了mPEG-5000的琥珀酰碳酸酯(SC-mPEG5k)和mPEG-5000的琥珀酰琥珀酸酯(SS-mPEG5k)。SC-mPEG5k具有更高的纯度,与甘氨酸相当的反应速率常数但更低的水解速率,以及更强的氨基修饰效果。在pH 9.2时,尿酸酶具有两种类型的氨基,它们与SC-mPEG5k或SS-mPEG5k的反应性相差25倍。氧嗪酸盐和黄嘌呤浓度依赖性地保护细菌尿酸酶在聚乙二醇化过程中不被灭活。在尿酸酶亚基与SC-mPEG5k的摩尔比为200以及50 μM氧嗪酸盐的条件下,聚乙二醇化尿酸酶(1)保留了约73%的原始活性,(2)对识别天然尿酸酶的兔抗血清显示约10%的反应性,(3)在大鼠中引发的IgG约占天然尿酸酶的5%,(4)在鸡血浆中的体内循环半衰期约为25小时,(5)同时在20多个小时内将尿酸维持在较低水平。因此,在竞争性抑制剂保护下用SC-mPEG进行聚乙二醇化是制备细菌尿酸酶的一种实用方法;聚乙二醇化过程中用竞争性抑制剂保护酶可能具有普遍意义。