DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Harnessing liquid-in-liquid printing and micropatterned substrates to fabricate 3-dimensional all-liquid fluidic devices

Abstract

Systems comprised of immiscible liquids held in non-equilibrium shapes by the interfacial assembly and jamming of nanoparticle-polymer surfactants have crucial potential to advance catalysis, chemical separations, energy storage and conversion. Spatially directing functionality within them and coupling processes in both phases remains a challenge. In this work, we exploit nanoclay-polymer surfactant assemblies at an oil-water interface to produce a semi-permeable membrane between the liquids, and from them all-liquid fluidic devices with bespoke properties. Flow channels are fabricated using micropatterned 2D substrates and liquid-in-liquid 3D printing. The anionic walls of the device can be functionalized with cationic small molecules, enzymes, and colloidal nanocrystal catalysts. Multi-step chemical transformations can be conducted within the channels under flow, as can selective mass transport across the liquid-liquid interface for in-line separations. These all-liquid systems become automated using pumps, detectors, and control systems, revealing a latent ability for chemical logic and learning.

Authors:
ORCiD logo [1];  [2];  [1]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [2]
  1. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
  2. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  4. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division; Univ. of Massachusetts, Amherst, MA (United States). Dept. of Polymer Science and Engineering, Conte Research Center; Beijing Univ. of Chemical Technology (China); Tohoku Univ., Sendai (Japan). WPI-Advanced Inst. for Materials Research
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1542387
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Feng, Wenqian, Chai, Yu, Forth, Joe, Ashby, Paul D., Russell, Thomas P., and Helms, Brett A. Harnessing liquid-in-liquid printing and micropatterned substrates to fabricate 3-dimensional all-liquid fluidic devices. United States: N. p., 2019. Web. doi:10.1038/s41467-019-09042-y.
Feng, Wenqian, Chai, Yu, Forth, Joe, Ashby, Paul D., Russell, Thomas P., & Helms, Brett A. Harnessing liquid-in-liquid printing and micropatterned substrates to fabricate 3-dimensional all-liquid fluidic devices. United States. https://doi.org/10.1038/s41467-019-09042-y
Feng, Wenqian, Chai, Yu, Forth, Joe, Ashby, Paul D., Russell, Thomas P., and Helms, Brett A. Wed . "Harnessing liquid-in-liquid printing and micropatterned substrates to fabricate 3-dimensional all-liquid fluidic devices". United States. https://doi.org/10.1038/s41467-019-09042-y. https://www.osti.gov/servlets/purl/1542387.
@article{osti_1542387,
title = {Harnessing liquid-in-liquid printing and micropatterned substrates to fabricate 3-dimensional all-liquid fluidic devices},
author = {Feng, Wenqian and Chai, Yu and Forth, Joe and Ashby, Paul D. and Russell, Thomas P. and Helms, Brett A.},
abstractNote = {Systems comprised of immiscible liquids held in non-equilibrium shapes by the interfacial assembly and jamming of nanoparticle-polymer surfactants have crucial potential to advance catalysis, chemical separations, energy storage and conversion. Spatially directing functionality within them and coupling processes in both phases remains a challenge. In this work, we exploit nanoclay-polymer surfactant assemblies at an oil-water interface to produce a semi-permeable membrane between the liquids, and from them all-liquid fluidic devices with bespoke properties. Flow channels are fabricated using micropatterned 2D substrates and liquid-in-liquid 3D printing. The anionic walls of the device can be functionalized with cationic small molecules, enzymes, and colloidal nanocrystal catalysts. Multi-step chemical transformations can be conducted within the channels under flow, as can selective mass transport across the liquid-liquid interface for in-line separations. These all-liquid systems become automated using pumps, detectors, and control systems, revealing a latent ability for chemical logic and learning.},
doi = {10.1038/s41467-019-09042-y},
journal = {Nature Communications},
number = 1,
volume = 10,
place = {United States},
year = {Wed Mar 06 00:00:00 EST 2019},
month = {Wed Mar 06 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 72 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

Organic synthesis in a modular robotic system driven by a chemical programming language
journal, November 2018


Colloidosomes: Selectively Permeable Capsules Composed of Colloidal Particles
journal, November 2002

  • Dinsmore, A. D.; Hsu, M. F.; Nikolaides, M. G.
  • Science, Vol. 298, Issue 5595, p. 1006-1009
  • DOI: 10.1126/science.1074868

Structured Liquids with pH-Triggered Reconfigurability
journal, May 2016


Electrotunable nanoplasmonic liquid mirror
journal, September 2017

  • Montelongo, Yunuen; Sikdar, Debabrata; Ma, Ye
  • Nature Materials, Vol. 16, Issue 11
  • DOI: 10.1038/nmat4969

Suspended microfluidics
journal, May 2013

  • Casavant, B. P.; Berthier, E.; Theberge, A. B.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 25
  • DOI: 10.1073/pnas.1302566110

Wrinkling of an elastic sheet under tension
journal, October 2002

  • Cerda, E.; Ravi-Chandar, K.; Mahadevan, L.
  • Nature, Vol. 419, Issue 6907
  • DOI: 10.1038/419579b

Elastometry of Deflated Capsules: Elastic Moduli from Shape and Wrinkle Analysis
journal, September 2013

  • Knoche, Sebastian; Vella, Dominic; Aumaitre, Elodie
  • Langmuir, Vol. 29, Issue 40
  • DOI: 10.1021/la402322g

Rational Design of Amyloid Binding Agents Based on the Molecular Rotor Motif
journal, January 2010

  • Sutharsan, Jeyanthy; Dakanali, Marianna; Capule, Christina C.
  • ChemMedChem, Vol. 5, Issue 1
  • DOI: 10.1002/cmdc.200900440

Stabilization of the tetramethylbenzidine (TMB) reaction product: application for retrograde and anterograde tracing, and combination with immunohistochemistry.
journal, November 1984

  • Rye, D. B.; Saper, C. B.; Wainer, B. H.
  • Journal of Histochemistry & Cytochemistry, Vol. 32, Issue 11
  • DOI: 10.1177/32.11.6548485

Single-file electrophoretic transport and counting of individual DNA molecules in surfactant nanotubes
journal, June 2005

  • Tokarz, M.; Akerman, B.; Olofsson, J.
  • Proceedings of the National Academy of Sciences, Vol. 102, Issue 26
  • DOI: 10.1073/pnas.0500081102

Controlled microfluidic interfaces
journal, September 2004


Stabilizing Liquid Drops in Nonequilibrium Shapes by the Interfacial Jamming of Nanoparticles
journal, October 2013


Three-dimensional surface microfluidics enabled by spatiotemporal control of elastic fluidic interface
journal, January 2010


Nanocrystal bilayer for tandem catalysis
journal, April 2011

  • Yamada, Yusuke; Tsung, Chia-Kuang; Huang, Wenyu
  • Nature Chemistry, Vol. 3, Issue 5
  • DOI: 10.1038/nchem.1018

Propagation of a topological transition: The Rayleigh instability
journal, May 1998

  • Powers, Thomas R.; Zhang, Dengfu; Goldstein, Raymond E.
  • Physics of Fluids, Vol. 10, Issue 5
  • DOI: 10.1063/1.869650

Bicontinuous Macroporous Materials from Bijel Templates
journal, September 2010


Fine-Tuning Nanoparticle Packing at Water–Oil Interfaces Using Ionic Strength
journal, September 2017


Tunable Substrate Wettability by Thin Water Layer
journal, October 2016

  • Jiménez-Ángeles, Felipe; Firoozabadi, Abbas
  • The Journal of Physical Chemistry C, Vol. 120, Issue 43
  • DOI: 10.1021/acs.jpcc.6b06054

Surface-Directed Liquid Flow Inside Microchannels
journal, February 2001


Nanoparticle Assembly and Transport at Liquid-Liquid Interfaces
journal, January 2003


Heme Protein−Clay Films:  Direct Electrochemistry and Electrochemical Catalysis
journal, January 2002

  • Zhou, Yinglin; Hu, Naifei; Zeng, Yonghuai
  • Langmuir, Vol. 18, Issue 1
  • DOI: 10.1021/la010834a

Elastic membranes of close-packed nanoparticle arrays
journal, July 2007

  • Mueggenburg, Klara E.; Lin, Xiao-Min; Goldsmith, Rodney H.
  • Nature Materials, Vol. 6, Issue 9
  • DOI: 10.1038/nmat1965

Reconfigurable Printed Liquids
journal, March 2018


Reconfigurable Microfluidic Droplets Stabilized by Nanoparticle Surfactants
journal, February 2018


High-throughput discovery of organic cages and catenanes using computational screening fused with robotic synthesis
journal, July 2018


Liquid Tubule Formation and Stabilization Using Cellulose Nanocrystal Surfactants
journal, September 2017

  • Liu, Xubo; Shi, Shaowei; Li, Yanan
  • Angewandte Chemie International Edition, Vol. 56, Issue 41
  • DOI: 10.1002/anie.201706839

Liquid Letters
journal, January 2018


Dynamically reconfigurable complex emulsions via tunable interfacial tensions
journal, February 2015

  • Zarzar, Lauren D.; Sresht, Vishnu; Sletten, Ellen M.
  • Nature, Vol. 518, Issue 7540
  • DOI: 10.1038/nature14168

Designing Algorithms To Aid Discovery by Chemical Robots
journal, July 2018


Machine-learning-assisted materials discovery using failed experiments
journal, May 2016

  • Raccuglia, Paul; Elbert, Katherine C.; Adler, Philip D. F.
  • Nature, Vol. 533, Issue 7601
  • DOI: 10.1038/nature17439

Bicontinuous structured liquids with sub-micrometre domains using nanoparticle surfactants
journal, September 2017


Elasticity of an interfacial particle raft
journal, October 2004


Jamming is not just cool any more
journal, November 1998

  • Liu, Andrea J.; Nagel, Sidney R.
  • Nature, Vol. 396, Issue 6706
  • DOI: 10.1038/23819

A passive pumping method for microfluidic devices
journal, January 2002

  • Walker, Glenn M.; Beebe, David J.
  • Lab on a Chip, Vol. 2, Issue 3
  • DOI: 10.1039/b204381e

The Matter Simulation (R)evolution
journal, February 2018


Nanoparticle Polymer Composites: Where Two Small Worlds Meet
journal, November 2006

  • Balazs, A. C.; Emrick, T.; Russell, T. P.
  • Science, Vol. 314, Issue 5802, p. 1107-1110
  • DOI: 10.1126/science.1130557

Microfluidics with fluid walls
journal, October 2017

  • Walsh, Edmond J.; Feuerborn, Alexander; Wheeler, James H. R.
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/s41467-017-00846-4

Surface Patterning via Thiol-Yne Click Chemistry: An Extremely Fast and Versatile Approach to Superhydrophilic-Superhydrophobic Micropatterns
journal, July 2014

  • Feng, Wenqian; Li, Linxian; Ueda, Erica
  • Advanced Materials Interfaces, Vol. 1, Issue 7
  • DOI: 10.1002/admi.201400269

Systems of mechanized and reactive droplets powered by multi-responsive surfactants
journal, January 2018

  • Yang, Zhijie; Wei, Jingjing; Sobolev, Yaroslav I.
  • Nature, Vol. 553, Issue 7688
  • DOI: 10.1038/nature25137

Enzymatic Determination of Total Serum Cholesterol
journal, April 1974


Liquid Tubule Formation and Stabilization Using Cellulose Nanocrystal Surfactants
journal, September 2017


Tunable Substrate Wettability by Thin Water Layer
journal, September 2016


Improving reaction prediction
journal, May 2020


The Matter Simulation (R)evolution
text, January 2018


Elasticity of an interfacial particle raft
text, January 2004


Bicontinuous Macroporous Materials from Bijel Templates
journal, September 2010


Structured Liquids with pH-Triggered Reconfigurability
journal, May 2016


Liquid Letters
journal, January 2018


Reconfigurable Printed Liquids
journal, March 2018


Liquid Tubule Formation and Stabilization Using Cellulose Nanocrystal Surfactants
journal, September 2017

  • Liu, Xubo; Shi, Shaowei; Li, Yanan
  • Angewandte Chemie International Edition, Vol. 56, Issue 41
  • DOI: 10.1002/anie.201706839

Rational Design of Amyloid Binding Agents Based on the Molecular Rotor Motif
journal, January 2010

  • Sutharsan, Jeyanthy; Dakanali, Marianna; Capule, Christina C.
  • ChemMedChem, Vol. 5, Issue 1
  • DOI: 10.1002/cmdc.200900440

Tunable Substrate Wettability by Thin Water Layer
journal, October 2016

  • Jiménez-Ángeles, Felipe; Firoozabadi, Abbas
  • The Journal of Physical Chemistry C, Vol. 120, Issue 43
  • DOI: 10.1021/acs.jpcc.6b06054

Fine-Tuning Nanoparticle Packing at Water–Oil Interfaces Using Ionic Strength
journal, September 2017


Designing Algorithms To Aid Discovery by Chemical Robots
journal, July 2018


Reconfigurable Microfluidic Droplets Stabilized by Nanoparticle Surfactants
journal, February 2018


Controlled microfluidic interfaces
journal, September 2004


Dynamically reconfigurable complex emulsions via tunable interfacial tensions
journal, February 2015

  • Zarzar, Lauren D.; Sresht, Vishnu; Sletten, Ellen M.
  • Nature, Vol. 518, Issue 7540
  • DOI: 10.1038/nature14168

Systems of mechanized and reactive droplets powered by multi-responsive surfactants
journal, January 2018

  • Yang, Zhijie; Wei, Jingjing; Sobolev, Yaroslav I.
  • Nature, Vol. 553, Issue 7688
  • DOI: 10.1038/nature25137

Nanocrystal bilayer for tandem catalysis
journal, April 2011

  • Yamada, Yusuke; Tsung, Chia-Kuang; Huang, Wenyu
  • Nature Chemistry, Vol. 3, Issue 5
  • DOI: 10.1038/nchem.1018

Elastic membranes of close-packed nanoparticle arrays
journal, July 2007

  • Mueggenburg, Klara E.; Lin, Xiao-Min; Goldsmith, Rodney H.
  • Nature Materials, Vol. 6, Issue 9
  • DOI: 10.1038/nmat1965

Electrotunable nanoplasmonic liquid mirror
journal, September 2017

  • Montelongo, Yunuen; Sikdar, Debabrata; Ma, Ye
  • Nature Materials, Vol. 16, Issue 11
  • DOI: 10.1038/nmat4969

Bicontinuous structured liquids with sub-micrometre domains using nanoparticle surfactants
journal, September 2017


A passive pumping method for microfluidic devices
journal, January 2002

  • Walker, Glenn M.; Beebe, David J.
  • Lab on a Chip, Vol. 2, Issue 3
  • DOI: 10.1039/b204381e

Three-dimensional surface microfluidics enabled by spatiotemporal control of elastic fluidic interface
journal, January 2010


Single-file electrophoretic transport and counting of individual DNA molecules in surfactant nanotubes
journal, June 2005

  • Tokarz, M.; Akerman, B.; Olofsson, J.
  • Proceedings of the National Academy of Sciences, Vol. 102, Issue 26
  • DOI: 10.1073/pnas.0500081102

Geometric Stability and Elastic Response of a Supported Nanoparticle Film
journal, July 2010


Geometry and Physics of Wrinkling
journal, February 2003


Colloidosomes: Selectively Permeable Capsules Composed of Colloidal Particles
journal, November 2002

  • Dinsmore, A. D.; Hsu, M. F.; Nikolaides, M. G.
  • Science, Vol. 298, Issue 5595, p. 1006-1009
  • DOI: 10.1126/science.1074868

Nanoparticle Assembly and Transport at Liquid-Liquid Interfaces
journal, January 2003


Nanoparticle Polymer Composites: Where Two Small Worlds Meet
journal, November 2006

  • Balazs, A. C.; Emrick, T.; Russell, T. P.
  • Science, Vol. 314, Issue 5802, p. 1107-1110
  • DOI: 10.1126/science.1130557

Stabilizing Liquid Drops in Nonequilibrium Shapes by the Interfacial Jamming of Nanoparticles
journal, October 2013


Elasticity of an interfacial particle raft
journal, October 2004


Elastometry of Deflated Capsules: Elastic Moduli from Shape and Wrinkle Analysis
text, January 2013


Propagation of a Topological Transition: the Rayleigh Instability
text, January 1997


Works referencing / citing this record:

Self‐Assembly of MXene‐Surfactants at Liquid–Liquid Interfaces: From Structured Liquids to 3D Aerogels
journal, October 2019


Self‐Assembly of MXene‐Surfactants at Liquid–Liquid Interfaces: From Structured Liquids to 3D Aerogels
journal, December 2019

  • Shi, Shaowei; Qian, Bingqing; Wu, Xinyu
  • Angewandte Chemie International Edition, Vol. 58, Issue 50
  • DOI: 10.1002/anie.201908402

Self‐Assembly of Nanoparticles in 2D and 3D: Recent Advances and Future Trends
journal, August 2019

  • Ghosh, Sujit Kumar; Böker, Alexander
  • Macromolecular Chemistry and Physics, Vol. 220, Issue 17
  • DOI: 10.1002/macp.201900196

Inner Surface Design of Functional Microchannels for Microscale Flow Control
journal, October 2019


Programmable unidirectional liquid transport on peristome-mimetic surfaces under liquid environments
journal, January 2019

  • Zhou, Shan; Yu, Cunlong; Li, Chuxin
  • Journal of Materials Chemistry A, Vol. 7, Issue 31
  • DOI: 10.1039/c9ta04770k

Controllable Liquid-Liquid Printing with Defect-free, Corrosion-Resistance, Unrestricted Wetting Condition
journal, September 2019