Synthesis and Characterization of Stimuli-Responsive Polymer Brushes in Nanofluidic Channels
Source abstract
Abstract
Nanochannels with controllable gating behavior are attractive features in a wide range of nanofluidic applications including viral detection, particle sorting, and flow regulation. Here, we use selective sidewall functionalization of nanochannels with a polyelectrolyte brush to investigate the channel gating response to variations in solution pH and ionic strength. The conformational and structural changes of the interfacial brush layer within the channels are interrogated by specular and off-specular neutron reflectometry. Simultaneous fits of the specular and off-specular signals, using a dynamical theory model and a fitting optimization protocol, enable detailed characterization of the brush conformations and corresponding channel geometry under different solution conditions. Our results indicate a collapsed brush state under basic pH, equivalent to an open gate, and an expanded brush state representing a partially closed gate upon decreasing the pH and salt concentration. These findings open new possibilities in noninvasive in situ characterization of tunable nanofluidics and lab-on-chip devices with advanced designs and improved functionality.
Source: openalex_inverted_index · Quality: baseline
Research context
OpenAlex topics: Nanopore and Nanochannel Transport Studies · Polymer Surface Interaction Studies · Microfluidic and Capillary Electrophoresis Applications
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Department of Physics, Virginia Tech, Blacksburg, Virginia 24061, United States
Center for Soft Matter and Biological Physics, Virginia Tech, Blacksburg, Virginia 24061, United States
Department of Physics, The University of Sheffield, Sheffield S3 7RH, U.K.
Department of Material Science and Engineering, University of Pennsylvania, Philadelphia, Pennsylvania 19104, United States
Department of Material Science and Engineering, Cornell University, Ithaca, New York 14850, United States
Department of Chemical and Biological Engineering, The University of Sheffield, Sheffield S1 3JD, U.K.
Second Target Station, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37830, United States
Department of Chemistry, The University of Sheffield, Sheffield S3 7HF, U.K.
Macromolecular Innovation Institute, Virginia Tech, Blacksburg, Virginia 24061, United States
Funding
Division of Chemistry · Oak Ridge National Laboratory · Basic Energy Sciences
References (69)
Show source-provided references
1. 10.1039/b917759k10.1039/b917759k ↗
2. Abgrall P. · 2009
3. 10.1088/0957-4484/15/10/01510.1088/0957-4484/15/10/015 ↗
4. 10.1038/s42003-018-0034-610.1038/s42003-018-0034-6 ↗
5. 10.1007/s00216-004-2526-010.1007/s00216-004-2526-0 ↗
6. 10.1016/j.gpb.2015.01.00910.1016/j.gpb.2015.01.009 ↗
7. 10.1038/nbt.295010.1038/nbt.2950 ↗
8. 10.1109/JSEN.2008.91875810.1109/JSEN.2008.918758 ↗
9. 10.1016/j.snb.2011.12.00410.1016/j.snb.2011.12.004 ↗
10. 10.1007/s10404-010-0614-310.1007/s10404-010-0614-3 ↗
11. 10.1021/ma060628f10.1021/ma060628f ↗
12. 10.3390/jfb302023910.3390/jfb3020239 ↗
13. 10.1021/acsami.1c0197510.1021/acsami.1c01975 ↗
14. 10.1021/acs.macromol.5b0128910.1021/acs.macromol.5b01289 ↗
15. 10.1021/acs.macromol.7b0045010.1021/acs.macromol.7b00450 ↗
16. 10.1039/C0SM00035C10.1039/C0SM00035C ↗
17. 10.1039/D0TB00570C10.1039/D0TB00570C ↗
18. 10.1021/acs.langmuir.7b0294510.1021/acs.langmuir.7b02945 ↗
19. 10.1038/nmat256410.1038/nmat2564 ↗
20. 10.1002/adfm.20050070210.1002/adfm.200500702 ↗
21. 10.1039/B920870D10.1039/B920870D ↗
22. 10.1016/B978-0-08-101995-5.00014-310.1016/B978-0-08-101995-5.00014-3 ↗
23. 10.1038/2161910.1038/21619 ↗
24. 10.3109/10717544.2014.94009110.3109/10717544.2014.940091 ↗
25. 10.1016/j.snb.2005.06.00310.1016/j.snb.2005.06.003 ↗
26. 10.1007/s00216-013-7090-z10.1007/s00216-013-7090-z ↗
27. 10.1021/la063450z10.1021/la063450z ↗
28. 10.1021/am101250x10.1021/am101250x ↗
29. Ashkar, R. Dynamical theory applications to neutron scattering from periodic nanostructures. Ph.D. thesis, Indiana University, 2012.
30. 10.1007/s00396-014-3330-910.1007/s00396-014-3330-9 ↗
31. 10.1016/j.coal.2018.02.00210.1016/j.coal.2018.02.002 ↗
32. Rahmaninejad, H.; Ashkar, R. Polymer-Based Nanoscale Materials for Surface Coatings; Thomas, S., George, J. S., Eds. Elsevier, 2023; pp 349–381.10.1016/B978-0-32-390778-1.00024-4 ↗
33. 10.1021/ma201839y10.1021/ma201839y ↗
34. 10.1039/B611847J10.1039/B611847J ↗
35. 10.1107/S002188981001064210.1107/S0021889810010642 ↗
36. 10.1103/PhysRevB.67.22420110.1103/PhysRevB.67.224201 ↗
37. 10.1021/ma990443r10.1021/ma990443r ↗
38. 10.1021/la101550w10.1021/la101550w ↗
39. 10.1126/science.251.4996.90510.1126/science.251.4996.905 ↗
40. 10.1051/jphys:0197700380809830010.1051/jphys:01977003808098300 ↗
41. 10.1021/ma60077a00910.1021/ma60077a009 ↗
42. 10.1063/1.149092410.1063/1.1490924 ↗
43. 10.1051/jp2:199211310.1051/jp2:1992113 ↗
44. 10.1021/ma950795810.1021/ma9507958 ↗
45. 10.1021/acs.langmuir.7b0139510.1021/acs.langmuir.7b01395 ↗
46. Rühe, J. Polyelectrolytes with Defined Molecular Architecture I; Schmidt, M., Ed. Springer Berlin Heidelberg: Berlin, Heidelberg, 2004; Vol. 165, pp 79–150.
47. 10.1002/adma.20110112010.1002/adma.201101120 ↗
48. 10.1021/la404727510.1021/la4047275 ↗
49. 10.1021/jp809814j10.1021/jp809814j ↗
50. 10.1021/ma00089a02810.1021/ma00089a028 ↗
51. 10.1063/1.48001910.1063/1.480019 ↗
52. 10.1103/PhysRevLett.98.01830210.1103/PhysRevLett.98.018302 ↗
53. 10.1021/ma00114a00910.1021/ma00114a009 ↗
54. 10.1021/ma00109a02110.1021/ma00109a021 ↗
55. 10.1002/bbpc.1996100064010.1002/bbpc.19961000640 ↗
56. 10.1021/ma071017610.1021/ma0710176 ↗
57. 10.1021/la991528o10.1021/la991528o ↗
58. 10.1016/j.polymer.2008.11.05110.1016/j.polymer.2008.11.051 ↗
59. 10.1021/ma047501f10.1021/ma047501f ↗
60. Koepsel, R. T. R. R.; Russell, A. J. Methods, Devices and Systems for Biocidal Surface Activity. U. S. Patent 0,090,074,709 A1, 2002.
61. 10.1002/1521-3927(20020701)23:10/11<612::AID-MARC612>3.0.CO;2-910.1002/1521-3927(20020701)23:10/11<612::AID-MARC612>3.0.CO;2-9 ↗
62. 10.1107/S002188980600507310.1107/S0021889806005073 ↗
63. 10.1021/acsami.5b0145310.1021/acsami.5b01453 ↗
64. 10.1063/1.366116210.1063/1.3661162 ↗
65. 10.1107/S002188981103273010.1107/S0021889811032730 ↗
66. Hansen, N.; Akimoto, Y.; Baudis, P. CMA-ES/pycma on Github; Zenodo, 2019.
67. Sattler K. D. · 202010.1201/9780429347313 ↗
68. 10.1039/b921218c10.1039/b921218c ↗
69. 10.1016/0370-1573(94)00110-O10.1016/0370-1573(94)00110-O ↗