Queen Mary University of London, CSC-PhD recruit
伦敦玛丽皇后大学,生物化学学院,(Queen Mary University of London, School of Biological and Chemical Science), Dr. Rachel Crespo-Otero 招收Phd(最好是申请留学基金委奖学金China Scholarship Council (CSC)的)
物理、化学,材料背景均可。语言要求参考学院网站和CSC标准(一般是雅思6.5)。
联系人:Dr. Stellios Arseniyadis (s.arseniyadis@qmul.ac.uk, synthetic) & Dr. Rachel Crespo-Otero (r.crespo-otero@qmul.ac.uk, computational)
如有细节咨询可以先给我发邮件(请注明小木虫虫友):f.song@qmul.ac.uk
谢谢)
Understanding DNA-Ligand affinity to improve catalytic activity and selectivity
Bio-inspired catalysis has emerged as a particularly attractive tool, which combines homogeneous catalysis and biocatalysis. The field is now slowly transforming to take on new challenges. These include novel designs, novel catalytic reactions, some of which have no equivalent in both homogenous catalysis and biocatalysis. The challenge in DNA-based asymmetric catalysis is to perform the reaction in the vicinity of the helix, which provides the chiral information to the activated complex and enables chiral discrimination. The first DNA-based catalyst featuring a non‑chiral ligand bound to DNA in a non-covalent fashion was reported jointly by Roelfes and Feringa in 2005 and consisted of a catalytically active Cu(II) complex linked to a DNA-intercalating 9‑amino acridine via a spacer.[1] Following this study, we showed that dsDNA made from L nucleotides instead of the natural occurring D nucleotides could be used to control the selectivity outcome of a given reaction and thus allow a trivial and reliable access to both enantiomers.[2] Later, we reported the first generation of a DNA-based catalyst bound to a cellulose matrix. Interestingly, this commercially available, trivial to use and fully recyclable chiral bio-material produced high levels of enantioselectivity.[3] In addition to this supported DNA system, our group has also investigated a novel anchoring strategy based on the use of modified groove binder ligands, which offer interesting compartimentalization possibilities as well as promise in multi-catalysis. A better understanding of the mechanisms by which the chirality is transferred from the DNA to a given substrate is however necessary to design more efficient catalysts capable of promoting a wide variety of synthetic transformations.
We are looking for two motivated and talented candidates with two different profiles. One would have a synthetic background and will develop new DNA-based asymmetric transformations, the second one should be familiar with computational chemistry techniques as he/she will work on theoretical models to have a better understanding of the mechanisms that control the chirality transfer. This project will be a close collaboration between the Arseniyadis’ and Crespo-Otero’s groups both located at Queen Mary University of London (UK) as well as the Smietana group at the University of Montpellier (France).
If you are interested in this project, please contact Dr. Stellios Arseniyadis (s.arseniyadis@qmul.ac.uk, synthetic) and Dr. Rachel Crespo-Otero (r.crespo-otero@qmul.ac.uk, computational).
[1] Roelfes, G.; Feringa, B. L. Angew. Chem. Int. Ed. 2005, 44, 3230.
[2] Wang, J.; Benedetti, E.; Bethge, L.; Vonhoff, S.; Klussmann, S.; Vasseur, J.-J.; Cossy, J.; Smietana, M.; Arseniyadis, S. Angew. Chem. Int. Ed. Engl. 2013, 52, 11546.
[3] Benedetti, E.; Duchemin, N.; Bethge, L.; Vonhoff, S.; Klussmann, S.; Vasseur, J.-J.; Cossy, J.; Smietana, M.; Arseniyadis, S. Chem. Commun. 2015, 51, 6076-6079.
Amirbekyan, K.; Duchemin, N.; Benedetti, E.; Joseph, R.; Colon, A.; Markarian, S. A.; Bethge, L.; Vonhoff, S.; Klussmann, S.; Cossy, J.; Vasseur, J.‑J.; Arseniyadis, S.; Smietana, M. ACS Catal. 2016, 6, 3096.
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