English
 
User Manual Privacy Policy Disclaimer Contact us
  Advanced SearchBrowse

Item

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

Liu, Y., Turunen, P., de Waal, B. F. M., Blank, K. G., Rowan, A. E., Palmans, A. R. A., et al. (2018). Catalytic single-chain polymeric nanoparticles at work: from ensemble towards single-particle kinetics. Molecular Systems Design & Engineering, 3(4), 609-618. doi:10.1039/C8ME00017D.

Item is

Basic

show hide
Item Permalink: http://hdl.handle.net/21.11116/0000-0001-9256-9 Version Permalink: http://hdl.handle.net/21.11116/0000-0002-06F9-F
Genre: Journal Article

Files

show Files
hide Files
:
Article.pdf (Publisher version), 6MB
Name:
Article.pdf
Description:
-
Visibility:
Public
MIME-Type / Checksum:
application/pdf / [MD5]
Technical Metadata:
Copyright Date:
-
Copyright Info:
-

Locators

show

Creators

show
hide
 Creators:
Liu, Yiliu, Author
Turunen, Petri, Author
de Waal, Bas F. M., Author
Blank, Kerstin G.1, Author              
Rowan, Alan E., Author
Palmans, Anja R. A., Author
Meijer, E. W., Author
Affiliations:
1Kerstin Blank, Mechano(bio)chemie, Max Planck Institute of Colloids and Interfaces, Max Planck Society, ou_2301698              

Content

show
hide
Free keywords: -
 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.

Details

show
hide
Language(s):
 Dates: 2018-06-192018
 Publication Status: Published in print
 Pages: -
 Publishing info: -
 Table of Contents: -
 Rev. Method: -
 Identifiers: DOI: 10.1039/C8ME00017D
 Degree: -

Event

show

Legal Case

show

Project information

show

Source 1

show
hide
Title: Molecular Systems Design & Engineering
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: London, UK : The Royal Society of Chemistry
Pages: - Volume / Issue: 3 (4) Sequence Number: - Start / End Page: 609 - 618 Identifier: ISSN: 2058-9689