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Title: Harnessing surface-bound enzymatic reactions to organize microcapsules in solution

Abstract

By developing new computational models, we examine how enzymatic reactions on an underlying surface can be harnessed to direct the motion and organization of reagent-laden microcapsules in a fluid-filled microchannel. In the presence of appropriate reagents, surface-bound enzymes can act as pumps, which drive large-scale fluid flows. When the reagents diffuse through the capsules’ porous shells, they can react with enzymatic sites on the bottom surface. The ensuing reaction generates fluid density variations, which result in fluid flows. These flows carry the suspended microcapsules and drive them to aggregate into “colonies” on and near the enzyme-covered sites. This aggregation continues until the reagent has been depleted and the convection stops. Here, we show that the shape of the assembled colonies can be tailored by patterning the distribution of enzymes on the surface. This fundamental physicochemical mechanism could have played a role in the self-organization of early biological cells (protocells) and can be used to regulate the autonomous motion and targeted delivery of microcarriers in microfluidic devices.

Authors:
 [1];  [1];  [2];  [1]
  1. Univ. of Pittsburgh, PA (United States). Dept. of Chemical Engineering
  2. Pennsylvania State Univ., University Park, PA (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Northwestern Univ., Evanston, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Kaufman Foundation
OSTI Identifier:
1466570
Grant/Contract Number:  
SC0000989
Resource Type:
Accepted Manuscript
Journal Name:
Science Advances
Additional Journal Information:
Journal Volume: 2; Journal Issue: 3; Journal ID: ISSN 2375-2548
Publisher:
AAAS
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; Collective behavior; microcapsules; self-organization; protocell aggregation; colloidal transport; enzymatic chemical; micropumps; computational modeling

Citation Formats

Shklyaev, Oleg E., Shum, Henry, Sen, Ayusman, and Balazs, Anna C. Harnessing surface-bound enzymatic reactions to organize microcapsules in solution. United States: N. p., 2016. Web. doi:10.1126/sciadv.1501835.
Shklyaev, Oleg E., Shum, Henry, Sen, Ayusman, & Balazs, Anna C. Harnessing surface-bound enzymatic reactions to organize microcapsules in solution. United States. doi:10.1126/sciadv.1501835.
Shklyaev, Oleg E., Shum, Henry, Sen, Ayusman, and Balazs, Anna C. Fri . "Harnessing surface-bound enzymatic reactions to organize microcapsules in solution". United States. doi:10.1126/sciadv.1501835. https://www.osti.gov/servlets/purl/1466570.
@article{osti_1466570,
title = {Harnessing surface-bound enzymatic reactions to organize microcapsules in solution},
author = {Shklyaev, Oleg E. and Shum, Henry and Sen, Ayusman and Balazs, Anna C.},
abstractNote = {By developing new computational models, we examine how enzymatic reactions on an underlying surface can be harnessed to direct the motion and organization of reagent-laden microcapsules in a fluid-filled microchannel. In the presence of appropriate reagents, surface-bound enzymes can act as pumps, which drive large-scale fluid flows. When the reagents diffuse through the capsules’ porous shells, they can react with enzymatic sites on the bottom surface. The ensuing reaction generates fluid density variations, which result in fluid flows. These flows carry the suspended microcapsules and drive them to aggregate into “colonies” on and near the enzyme-covered sites. This aggregation continues until the reagent has been depleted and the convection stops. Here, we show that the shape of the assembled colonies can be tailored by patterning the distribution of enzymes on the surface. This fundamental physicochemical mechanism could have played a role in the self-organization of early biological cells (protocells) and can be used to regulate the autonomous motion and targeted delivery of microcarriers in microfluidic devices.},
doi = {10.1126/sciadv.1501835},
journal = {Science Advances},
number = 3,
volume = 2,
place = {United States},
year = {2016},
month = {3}
}

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Cited by: 2 works
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