Catalytic single-chain polymeric nanoparticles at work: from ensemble towards single-particle kinetics

作者: Yiliu Liu , Petri Turunen , Bas F. M. de Waal , Kerstin G. Blank , Alan E. Rowan

DOI: 10.1039/C8ME00017D

关键词: CatalysisSelectivityLigandFluorescenceCombinatorial chemistryRhodamineChemistryKineticsMoleculeFluorescence correlation spectroscopy

摘要: Folding a single polymer chain around catalytically active sites to construct catalytic polymeric nanoparticles (SCPNs) is novel approach mimic the activity and selectivity of enzymes. In order relate efficiency SCPNs their three-dimensional structure, better understanding at an individual level, rather than ensemble highly desirable. this work, we present design preparation family fluorogenic substrates, characterization level as well our progress towards analyzing with single-molecule fluorescence microscopy (SMFM). Firstly, organocopper-based together rhodamine-based substrates were designed synthesized. The catalyze carbamate cleavage reaction mono-protected rhodamines, dimethylpropargyloxycarbonyl protecting group being cleaved most efficiently. A systematic study focusing on conditions during catalysis revealed that ligand acceleration effect accumulation in significantly promote performance. Secondly, streptavidin–biotin based strategy was developed immobilize surface glass coverslips. Fluorescence correlation spectroscopy experiments confirmed remained after immobilization. Finally, single-SCPN measurements performed. results qualitatively indicated fluorescent product molecules formed result could be detected. So far, no evidence for strongly different behaviors has been observed when comparing SCPNs.

参考文章(58)
Zhi-Qiang Wang, Jinfang Liao, Zhenjun Diwu, N-DEVD-N'-morpholinecarbonyl-rhodamine 110: novel caspase-3 fluorogenic substrates for cell-based apoptosis assay. Bioorganic & Medicinal Chemistry Letters. ,vol. 15, pp. 2335- 2338 ,(2005) , 10.1016/J.BMCL.2005.02.081
Paul Zhu, Harold G. Craighead, Zero-mode waveguides for single-molecule analysis. Annual Review of Biophysics. ,vol. 41, pp. 269- 293 ,(2012) , 10.1146/ANNUREV-BIOPHYS-050511-102338
Johannes Willenbacher, Ozcan Altintas, Vanessa Trouillet, Nicolai Knöfel, Michael J. Monteiro, Peter W. Roesky, Christopher Barner-Kowollik, Pd-complex driven formation of single-chain nanoparticles Polymer Chemistry. ,vol. 6, pp. 4358- 4365 ,(2015) , 10.1039/C5PY00389J
Nicholas E. Leadbeater, Maria Marco, Preparation of polymer-supported ligands and metal complexes for use in catalysis. Chemical Reviews. ,vol. 102, pp. 3217- 3273 ,(2002) , 10.1021/CR010361C
Davy Gérard, Jérôme Wenger, Nicolas Bonod, Evgeni Popov, Hervé Rigneault, Farhad Mahdavi, Steve Blair, José Dintinger, Thomas W. Ebbesen, Nanoaperture-enhanced fluorescence : Towards higher detection rates with plasmonic metals Physical Review B. ,vol. 77, pp. 045413- ,(2008) , 10.1103/PHYSREVB.77.045413
Takaya Terashima, Tristan Mes, Tom F. A. De Greef, Martijn A. J. Gillissen, Pol Besenius, Anja R. A. Palmans, E. W. Meijer, Single-Chain Folding of Polymers for Catalytic Systems in Water Journal of the American Chemical Society. ,vol. 133, pp. 4742- 4745 ,(2011) , 10.1021/JA2004494
Ozcan Altintas, Christopher Barner-Kowollik, Single Chain Folding of Synthetic Polymers by Covalent and Non-Covalent Interactions: Current Status and Future Perspectives Macromolecular Rapid Communications. ,vol. 33, pp. 958- 971 ,(2012) , 10.1002/MARC.201200049
Petri Turunen, Alan E. Rowan, Kerstin Blank, Single-enzyme kinetics with fluorogenic substrates: lessons learnt and future directions. FEBS Letters. ,vol. 588, pp. 3553- 3563 ,(2014) , 10.1016/J.FEBSLET.2014.06.021
Luke D. Lavis, Tzu-Yuan Chao, Ronald T. Raines, Fluorogenic Label for Biomolecular Imaging ACS Chemical Biology. ,vol. 1, pp. 252- 260 ,(2006) , 10.1021/CB600132M
Günter Wulff, Enzyme-like catalysis by molecularly imprinted polymers. Chemical Reviews. ,vol. 102, pp. 1- 27 ,(2002) , 10.1021/CR980039A