Finley Stacey D, Broadbelt Linda J, Hatzimanikatis Vassily
Department of Chemical and Biological Engineering, McCormick School of Engineering and Applied Sciences, Northwestern University, Evanston, Illinois 60208, USA.
Biotechnol Bioeng. 2009 Jun 15;103(3):532-41. doi: 10.1002/bit.22285.
Microorganisms provide a wealth of biodegradative potential in the reduction and elimination of xenobiotic compounds in the environment. One useful metric to evaluate potential biodegradation pathways is thermodynamic feasibility. However, experimental data for the thermodynamic properties of xenobiotics is scarce. The present work uses a group contribution method to study the thermodynamic properties of the University of Minnesota Biocatalysis/Biodegradation Database. The Gibbs free energies of formation and reaction are estimated for 914 compounds (81%) and 902 reactions (75%), respectively, in the database. The reactions are classified based on the minimum and maximum Gibbs free energy values, which accounts for uncertainty in the free energy estimates and a feasible concentration range relevant to biodegradation. Using the free energy estimates, the cumulative free energy change of 89 biodegradation pathways (51%) in the database could be estimated. A comparison of the likelihood of the biotransformation rules in the Pathway Prediction System and their thermodynamic feasibility was then carried out. This analysis revealed that when evaluating the feasibility of biodegradation pathways, it is important to consider the thermodynamic topology of the reactions in the context of the complete pathway. Group contribution is shown to be a viable tool for estimating, a priori, the thermodynamic feasibility and the relative likelihood of alternative biodegradation reactions. This work offers a useful tool to a broad range of researchers interested in estimating the feasibility of the reactions in existing or novel biodegradation pathways.
微生物在环境中还原和消除外源化合物方面具有丰富的生物降解潜力。评估潜在生物降解途径的一个有用指标是热力学可行性。然而,关于外源化合物热力学性质的实验数据却很匮乏。本研究采用基团贡献法来研究明尼苏达大学的生物催化/生物降解数据库的热力学性质。分别估算了该数据库中914种化合物(占81%)和902个反应(占75%)的生成吉布斯自由能和反应吉布斯自由能。这些反应根据吉布斯自由能的最小值和最大值进行分类,这考虑了自由能估算中的不确定性以及与生物降解相关的可行浓度范围。利用自由能估算值,可以估算该数据库中89条生物降解途径(占51%)的累积自由能变化。随后对途径预测系统中的生物转化规则的可能性及其热力学可行性进行了比较。该分析表明,在评估生物降解途径的可行性时,在完整途径的背景下考虑反应的热力学拓扑结构很重要。基团贡献法被证明是一种可行的工具,可用于先验地估算替代生物降解反应的热力学可行性和相对可能性。这项工作为广泛的研究人员提供了一个有用的工具,这些研究人员对估算现有或新的生物降解途径中反应的可行性感兴趣。