Louvain Institute of Biomolecular Science and Technology, UCLouvain, Place Croix du Sud 4-5, 1348, Louvain-la-Neuve, Belgium.
Department of Biochemistry, University of Cambridge, 80 Tennis Court Road, Cambridge, CB2 1GA, UK.
Sci Rep. 2024 Jun 18;14(1):13999. doi: 10.1038/s41598-024-64806-x.
Penicillin binding proteins (PBPs) are involved in biosynthesis, remodeling and recycling of peptidoglycan (PG) in bacteria. PBP-A from Thermosynechococcus elongatus belongs to a cyanobacterial family of enzymes sharing close structural and phylogenetic proximity to class A β-lactamases. With the long-term aim of converting PBP-A into a β-lactamase by directed evolution, we simulated what may happen when an organism like Escherichia coli acquires such a new PBP and observed growth defect associated with the enzyme activity. To further explore the molecular origins of this harmful effect, we decided to characterize deeper the activity of PBP-A both in vitro and in vivo. We found that PBP-A is an enzyme endowed with DD-carboxypeptidase and DD-endopeptidase activities, featuring high specificity towards muropeptides amidated on the D-iso-glutamyl residue. We also show that a low promiscuous activity on non-amidated peptidoglycan deteriorates E. coli's envelope, which is much higher under acidic conditions where substrate discrimination is mitigated. Besides expanding our knowledge of the biochemical activity of PBP-A, this work also highlights that promiscuity may depend on environmental conditions and how it may hinder rather than promote enzyme evolution in nature or in the laboratory.
青霉素结合蛋白(PBPs)参与细菌中肽聚糖(PG)的生物合成、重塑和再循环。来自 elongatus 嗜热蓝藻的 PBP-A 属于一种与 A 类β-内酰胺酶具有密切结构和系统发育相似性的蓝藻酶家族。我们的长期目标是通过定向进化将 PBP-A 转化为β-内酰胺酶,为此我们模拟了大肠杆菌等生物体获得这种新 PBP 时可能发生的情况,并观察到与酶活性相关的生长缺陷。为了进一步探讨这种有害影响的分子起源,我们决定更深入地研究 PBP-A 的体外和体内活性。我们发现 PBP-A 是一种具有 DD-羧肽酶和 DD-内肽酶活性的酶,对 D-异谷氨酰残基上酰胺化的肽聚糖具有很高的特异性。我们还表明,在酸性条件下,非酰胺化肽聚糖的低混杂活性会使大肠杆菌的包膜恶化,而在酸性条件下,这种混杂活性会降低底物的辨别能力。除了扩展我们对 PBP-A 的生化活性的了解外,这项工作还强调了混杂性可能取决于环境条件,以及它如何在自然界或实验室中阻碍而不是促进酶的进化。