Issue 4, 2018

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

Abstract

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

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

Supplementary files

Article information

Article type
Paper
Submitted
07 bal. 2018
Accepted
24 geg. 2018
First published
19 birž. 2018
This article is Open Access
Creative Commons BY-NC license

Mol. Syst. Des. Eng., 2018,3, 609-618

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

Y. Liu, P. Turunen, B. F. M. de Waal, K. G. Blank, A. E. Rowan, A. R. A. Palmans and E. W. Meijer, Mol. Syst. Des. Eng., 2018, 3, 609 DOI: 10.1039/C8ME00017D

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