Hintersatz Christian, Tsushima Satoru, Kaufer Tobias, Kretzschmar Jerome, Thewes Angela, Pollmann Katrin, Jain Rohan
Helmholtz Institute Freiberg for Resource Technology, Department of Biotechnology, Helmholtz-Zentrum Dresden-Rossendorf, Bautzner Landstraße 400, 01328 Dresden, Germany.
Institute of Resource Ecology, Department of Biophysics, Helmholtz-Zentrum Dresden-Rossendorf, Bautzner Landstraße 400, 01328 Dresden, Germany.
J Hazard Mater. 2024 Oct 5;478:135523. doi: 10.1016/j.jhazmat.2024.135523. Epub 2024 Aug 19.
Siderophores are promising ligands for application in novel recycling and bioremediation technologies, as they can selectively complex a variety of metals. However, with over 250 known siderophores, the selection of suiting complexants in the wet lab is impractical. Thus, this study established a density functional theory (DFT) based approach to efficiently identify siderophores with increased selectivity towards target metals on the example of germanium and indium. Considering 239 structures, chemically similar siderophores were clustered, and their complexation reactions modeled utilizing DFT. The calculations revealed siderophores with, compared to the reference siderophore desferrioxamine B (DFOB), up to 128 % or 48 % higher selectivity for indium or germanium, respectively. Experimental validation of the method was conducted with fimsbactin A and agrobactin, demonstrating up to 40 % more selective indium binding and at least sevenfold better germanium binding than DFOB, respectively. The results generated in this study open the door for the utilization of siderophores in eco-friendly technologies for the recovery of many different critical metals from various industry waters and leachates or bioremediation approaches. This endeavor is greatly facilitated by applying the herein-created database of geometry-optimized siderophore structures as de novo modeling of the molecules can be omitted.
铁载体是应用于新型回收和生物修复技术的有前景的配体，因为它们可以选择性地络合多种金属。然而，已知的铁载体超过250种，在湿实验室中选择合适的络合剂是不切实际的。因此，本研究以锗和铟为例，建立了一种基于密度泛函理论（DFT）的方法，以有效地识别对目标金属具有更高选择性的铁载体。考虑到239种结构，将化学相似的铁载体聚类，并利用DFT对它们的络合反应进行建模。计算结果表明，与参考铁载体去铁胺B（DFOB）相比，某些铁载体对铟或锗的选择性分别高出128%或48%。用铁杆菌素A和土壤杆菌素对该方法进行了实验验证，结果表明，它们对铟的结合选择性分别比DFOB高40%，对锗的结合能力至少是DFOB的7倍。本研究产生的结果为在环保技术中利用铁载体从各种工业用水、渗滤液或生物修复方法中回收许多不同的关键金属打开了大门。应用本文创建的几何优化铁载体结构数据库可以省略分子的从头建模，极大地促进了这一努力。
