Mechanistic insights of evaporation-induced actuation in supramolecular crystals

Roxana PIOTROWSKA; Travis HESKETH; Haozhen WANG; Alan R.G. MARTIN; Deborah BOWERING; Chunqiu ZHANG; Chunhua T. HU; Scott A. MCPHEE; Tong WANG; Yaewon PARK; Pulkit SINGLA; Thomas MCGLONE; Alastair FLORENCE; Tell TUTTLE; Rein V. ULIJN; Xi CHEN

doi:10.1038/s41563-020-0799-0

Mechanistic insights of evaporation-induced actuation in supramolecular crystals

Roxana PIOTROWSKA, Travis HESKETH, Haozhen WANG, Alan R.G. MARTIN, Deborah BOWERING, Chunqiu ZHANG, Chunhua T. HU, Scott A. MCPHEE, Tong WANG, Yaewon PARK, Pulkit SINGLA, Thomas MCGLONE, Alastair FLORENCE, Tell TUTTLE^*, Rein V. ULIJN^*, Xi CHEN^*

^*Corresponding author for this work

Research output: Journal Publications › Journal Article (refereed) › peer-review

34 Citations (Scopus)

Abstract

Water-responsive materials undergo reversible shape changes upon varying humidity levels. These mechanically robust yet flexible structures can exert substantial forces and hold promise as efficient actuators for energy harvesting, adaptive materials and soft robotics. Here we demonstrate that energy transfer during evaporation-induced actuation of nanoporous tripeptide crystals results from the strengthening of water hydrogen bonding that drives the contraction of the pores. The seamless integration of mobile and structurally bound water inside these pores with a supramolecular network that contains readily deformable aromatic domains translates dehydration-induced mechanical stresses through the crystal lattice, suggesting a general mechanism of efficient water-responsive actuation. The observed strengthening of water bonding complements the accepted understanding of capillary-force-induced reversible contraction for this class of materials. These minimalistic peptide crystals are much simpler in composition compared to natural water-responsive materials, and the insights provided here can be applied more generally for the design of high-energy molecular actuators.

Original language	English
Pages (from-to)	403-409
Number of pages	7
Journal	Nature Materials
Volume	20
Issue number	3
Early online date	14 Sept 2020
DOIs	https://doi.org/10.1038/s41563-020-0799-0
Publication status	Published - Mar 2021
Externally published	Yes

Bibliographical note

Funding Information:
This work was supported in part by the Office of Naval Research (ONR; N00014-18-1-2492), the Air Force Office of Scientific Research (AFOSR; FA9550-19-1-0111), the National Science Foundation (NSF; CHE-1808143), the EPSRC-funded ARCHIE-WeSt High Performance Computer (www.archie-west.ac.uk) for computational resources via EPSRC grant no. EP/K000586/1 and the CUNY/Strathclyde partnership. We acknowledge that the powder X-ray diffraction and DVS experiments were carried out in the CMAC National Facility, housed within the University of Strathclyde’s Technology and Innovation Centre, and funded with a UKRPIF (UK Research Partnership Institute Fund) capital award, SFC ref. H13054, from the Higher Education Funding Council for England (HEFCE). C.T.H. acknowledges the support of the National Science Foundation (NSF) Chemistry Research Instrumentation and Facilities Program (CHE-0840277) and Materials Research Science and Engineering Center (MRSEC) Program (DMR-1420073).

Publisher Copyright:
© 2020, The Author(s), under exclusive licence to Springer Nature Limited.

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10.1038/s41563-020-0799-0

https://strathprints.strath.ac.uk/id/eprint/73907

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PIOTROWSKA, R., HESKETH, T., WANG, H., MARTIN, A. R. G., BOWERING, D., ZHANG, C., HU, C. T., MCPHEE, S. A., WANG, T., PARK, Y., SINGLA, P., MCGLONE, T., FLORENCE, A., TUTTLE, T., ULIJN, R. V., & CHEN, X. (2021). Mechanistic insights of evaporation-induced actuation in supramolecular crystals. Nature Materials, 20(3), 403-409. Advance online publication. https://doi.org/10.1038/s41563-020-0799-0

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abstract = "Water-responsive materials undergo reversible shape changes upon varying humidity levels. These mechanically robust yet flexible structures can exert substantial forces and hold promise as efficient actuators for energy harvesting, adaptive materials and soft robotics. Here we demonstrate that energy transfer during evaporation-induced actuation of nanoporous tripeptide crystals results from the strengthening of water hydrogen bonding that drives the contraction of the pores. The seamless integration of mobile and structurally bound water inside these pores with a supramolecular network that contains readily deformable aromatic domains translates dehydration-induced mechanical stresses through the crystal lattice, suggesting a general mechanism of efficient water-responsive actuation. The observed strengthening of water bonding complements the accepted understanding of capillary-force-induced reversible contraction for this class of materials. These minimalistic peptide crystals are much simpler in composition compared to natural water-responsive materials, and the insights provided here can be applied more generally for the design of high-energy molecular actuators.",

author = "Roxana PIOTROWSKA and Travis HESKETH and Haozhen WANG and MARTIN, {Alan R.G.} and Deborah BOWERING and Chunqiu ZHANG and HU, {Chunhua T.} and MCPHEE, {Scott A.} and Tong WANG and Yaewon PARK and Pulkit SINGLA and Thomas MCGLONE and Alastair FLORENCE and Tell TUTTLE and ULIJN, {Rein V.} and Xi CHEN",

note = "Funding Information: This work was supported in part by the Office of Naval Research (ONR; N00014-18-1-2492), the Air Force Office of Scientific Research (AFOSR; FA9550-19-1-0111), the National Science Foundation (NSF; CHE-1808143), the EPSRC-funded ARCHIE-WeSt High Performance Computer (www.archie-west.ac.uk) for computational resources via EPSRC grant no. EP/K000586/1 and the CUNY/Strathclyde partnership. We acknowledge that the powder X-ray diffraction and DVS experiments were carried out in the CMAC National Facility, housed within the University of Strathclyde{\textquoteright}s Technology and Innovation Centre, and funded with a UKRPIF (UK Research Partnership Institute Fund) capital award, SFC ref. H13054, from the Higher Education Funding Council for England (HEFCE). C.T.H. acknowledges the support of the National Science Foundation (NSF) Chemistry Research Instrumentation and Facilities Program (CHE-0840277) and Materials Research Science and Engineering Center (MRSEC) Program (DMR-1420073). Publisher Copyright: {\textcopyright} 2020, The Author(s), under exclusive licence to Springer Nature Limited.",

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AU - BOWERING, Deborah

AU - ZHANG, Chunqiu

AU - HU, Chunhua T.

AU - MCPHEE, Scott A.

AU - WANG, Tong

AU - PARK, Yaewon

AU - SINGLA, Pulkit

AU - MCGLONE, Thomas

AU - FLORENCE, Alastair

AU - TUTTLE, Tell

AU - ULIJN, Rein V.

AU - CHEN, Xi

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N2 - Water-responsive materials undergo reversible shape changes upon varying humidity levels. These mechanically robust yet flexible structures can exert substantial forces and hold promise as efficient actuators for energy harvesting, adaptive materials and soft robotics. Here we demonstrate that energy transfer during evaporation-induced actuation of nanoporous tripeptide crystals results from the strengthening of water hydrogen bonding that drives the contraction of the pores. The seamless integration of mobile and structurally bound water inside these pores with a supramolecular network that contains readily deformable aromatic domains translates dehydration-induced mechanical stresses through the crystal lattice, suggesting a general mechanism of efficient water-responsive actuation. The observed strengthening of water bonding complements the accepted understanding of capillary-force-induced reversible contraction for this class of materials. These minimalistic peptide crystals are much simpler in composition compared to natural water-responsive materials, and the insights provided here can be applied more generally for the design of high-energy molecular actuators.

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Mechanistic insights of evaporation-induced actuation in supramolecular crystals

Abstract

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Author Correction: Mechanistic insights of evaporation-induced actuation in supramolecular crystals (Nature Materials, (2021), 20, 3, (403-409), 10.1038/s41563-020-0799-0)

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