Zlotnikov Igor D, Kudryashova Elena V
Faculty of Chemistry, Lomonosov Moscow State University, Leninskie Gory, 1/3, 119991 Moscow, Russia.
Int J Mol Sci. 2025 May 29;26(11):5227. doi: 10.3390/ijms26115227.
Majority of commercial L-asparaginase (L-ASNase) activity assays are based on coupled enzymatic reaction, which converts aspartate into pyruvate, subsequently reacting with the probe to form a stable chromophore, which can be detected spectrophotometrically. However, in complex biological samples this method can be inaccurate due to poor optical transparency or presence of compounds interfering with the coupled enzyme reaction-for this kind of cases alternative methods have been suggested. Here we suggest a strategy to rationally pick a method of choice in a variety of situations, taking into consideration the upsides and downsides of each method. A high-throughput fluorometric assay employing the substrate Asp-AMC was rigorously validated for L-ASPNase activity screening. Aassay performance is evaluated in complex biological matrices, including bovine serum, whole and diluted human blood, and finally the mouse blood and liver homogenates samples obtained from pharmacokinetic studies. This comprehensive validation process ensures the reliability and applicability of the assay for assessing L-asparaginase activity in diverse and physiologically relevant environments. Potential interfering factors and matrix effects were addressed, and assay conditions were optimized for each matrix. The optimized assay was employed to screen various L-asparaginase types (intracellular L-ASNases type I RrA, periplasmic L-ASNases type II EcA and EwA) and ASPNase formulations (conjugates with polyamines or polyelectrolyte complexes), comparing their kinetic parameters and stability. Fourier-transform infrared (FTIR) spectroscopy was further employed to investigate the fine features of molecular mechanisms of L-asparaginase catalysis. FTIR spectra of Asn during hydrolysis were analyzed in buffer solutions and in complex biological matrices, such as blood sample or liver homogenates which is crucial in the context of pharmacokinetic research. This combined fluorometric and FTIR approach provides a powerful platform for optimizing L-ASNase formulations and therapeutic strategies for ALL. Based on the results obtained we have developed a strategy to choose an approach for L-Asparaginase activity assessment for a variety of difficult situations when dealing with complex biological samples.
大多数商业L-天冬酰胺酶(L-ASNase)活性测定基于偶联酶反应,该反应将天冬氨酸转化为丙酮酸,随后与探针反应形成稳定的发色团,可通过分光光度法进行检测。然而,在复杂生物样品中,由于光学透明度差或存在干扰偶联酶反应的化合物,这种方法可能不准确——针对此类情况,已提出了替代方法。在此,我们提出一种策略,在考虑每种方法优缺点的基础上,合理选择在各种情况下的首选方法。一种采用底物Asp-AMC的高通量荧光测定法已针对L-ASPNase活性筛选进行了严格验证。在复杂生物基质中评估测定性能,包括牛血清、全血和稀释的人血,最后是从小鼠药代动力学研究中获得的小鼠血液和肝脏匀浆样品。这一全面的验证过程确保了该测定法在评估不同生理相关环境中L-天冬酰胺酶活性时的可靠性和适用性。解决了潜在干扰因素和基质效应,并针对每种基质优化了测定条件。采用优化后的测定法筛选各种L-天冬酰胺酶类型(细胞内I型RrA L-ASNases、周质II型EcA和EwA L-ASNases)和ASPNase制剂(与多胺或聚电解质复合物的缀合物),比较它们的动力学参数和稳定性。进一步采用傅里叶变换红外(FTIR)光谱研究L-天冬酰胺酶催化分子机制的精细特征。在缓冲溶液以及复杂生物基质(如血液样本或肝脏匀浆)中分析天冬酰胺水解过程中的FTIR光谱,这在药代动力学研究背景下至关重要。这种荧光法和FTIR法相结合的方法为优化L-ASNase制剂和急性淋巴细胞白血病的治疗策略提供了一个强大的平台。基于所获得的结果,我们制定了一种策略,用于在处理复杂生物样品的各种困难情况下选择L-天冬酰胺酶活性评估方法。