Abstract
Chemical and morphological traits of natural substrates that can propel and transport fluids over their surfaces have long provided inspiration for the engineering of artificial materials that can harvest and collect water from aerial humidity. Here we report that the gradual widening of parallel microchannels on a surface of a slowly subliming hexachlorobenzene crystal can promote the autonomous and bidirectional transduction of condensed aerial water. Driven by topology changes on the surface of the crystal and water exchange with the gas phase, droplets of condensed water migrate over the crystal. These droplets are also able to transport silver particles and other particulate matter, such as dust. The velocity of the particles was shown to be dependent on both the sublimation rate of the crystal and the relative humidity of its environment. This example of a sublimation-powered water flow demonstrates that topological surface changes accompanying crystal phase transitions can be harnessed to transport liquid and solid matter over surfaces.

This is a preview of subscription content, access via your institution
Access options
Access Nature and 54 other Nature Portfolio journals
Get Nature+, our best-value online-access subscription
$29.99 / 30 days
cancel any time
Subscribe to this journal
Receive 12 print issues and online access
$259.00 per year
only $21.58 per issue
Rent or buy this article
Get just this article for as long as you need it
$39.95
Prices may be subject to local taxes which are calculated during checkout




Data availability
Unprocessed images and raw data have been uploaded to the data repository site Zenodo at https://doi.org/10.5281/zenodo.7457189. Source data are provided with this paper.
References
Park, Y. & Chen, X. Water-responsive materials for sustainable energy applications. J. Mater. Chem. A 8, 15227–15244 (2020).
Zhang, J. et al. Fundamentals and applications of inertial microfluidics: a review. Lab Chip 16, 10–34 (2016).
Lv, J.-A. et al. Photocontrol of fluid slugs in liquid crystal polymer microactuators. Nature 537, 179–184 (2016).
Psaltis, D., Quake, S. R. & Yang, C. Developing optofluidic technology through the fusion of microfluidics and optics. Nature 442, 381–386 (2006).
Venancio-Marques, A., Barbaud, F. & Baigl, D. Microfluidic mixing triggered by an external LED illumination. J. Am. Chem. Soc. 135, 3218–3223 (2013).
Ichimura, K., Oh, S. & Nakagawa, M. Light-driven motion of liquids on a photoresponsive surface. Science 288, 1624–1626 (2000).
Gao, C. et al. Droplets manipulated on photothermal organogel surfaces. Adv. Funct. Mater. 28, 1803072 (2018).
Feng, S. et al. Radial wettable gradient of hot surface to control droplets movement in directions. Sci. Rep. 5, 10067 (2015).
Seo, S., Ha, D. & Kim, T. Evaporation-driven transport-control of small molecules along nanoslits. Nat. Commun. 12, 1336–1339 (2021).
Fan, J. C., Wu, H. A. & Wang, F. C. Evaporation-driven liquid flow through nanochannels. Phys. Fluids 32, 012001 (2020).
Randall, G. C. & Doyle, P. S. Permeation-driven flow in poly (dimethylsiloxane) microfluidic devices. Proc. Natl Acad. Sci. USA 102, 10813–10818 (2005).
Pamme, N. Magnetism and microfluidics. Lab Chip 6, 24–38 (2006).
Linke, H. et al. Self-propelled Leidenfrost droplets. Phys. Rev. Lett. 96, 154502 (2006).
Shang, L., Cheng, Y. & Zhao, Y. Emerging droplet microfluidics. Chem. Rev. 117, 7964–8040 (2017).
Soltani, M. & Golovin, K. Anisotropy-induced directional self-transportation of low surface tension liquids: a review. RSC Adv. 10, 40569–40581 (2020).
Chu, K.-H., Xiao, R. & Wang, E. N. Uni-directional liquid spreading on asymmetric nanostructured surfaces. Nat. Mater. 9, 413–417 (2010).
Marangoni, C. Sul principio della viscosita' superficiale dei liquidi stabilito dal sig. J. Plateau. Il Nuovo Cimento 5, 239–273 (1871).
Nelson, W. C. & Kim, C.-J. Droplet actuation by electrowetting-on-dielectric (EWOD): a review. J. Adhes. Sci. Technol. 26, 1747–1771 (2012).
Wang, D., Zhu, L., Chen, J. F. & Dai, L. Liquid marbles based on magnetic upconversion nanoparticles as magnetically and optically responsive miniature reactors for photocatalysis and photodynamic therapy. Angew. Chem. Int. Ed. 55, 10795–10799 (2016).
Chen, H. et al. Continuous directional water transport on the peristome surface of Nepenthes alata. Nature 532, 85–89 (2016).
Malik, F. T., Clement, R. M., Gethin, D. T., Krawszik, W. & Parker, A. R. Nature’s moisture harvesters: a comparative review. Bioinspir. Biomim. 9, 031002 (2014).
Zheng, Y. et al. Directional water collection on wetted spider silk. Nature 463, 640–643 (2010).
Ju, J. et al. A multi-structural and multi-functional integrated fog collection system in cactus. Nat. Commun. 3, 1247 (2012).
Parker, A. R. & Lawrence, C. R. Water capture by a desert beetle. Nature 414, 33–34 (2001).
Feng, S., Wang, Q., Xing, Y., Hou, Y. & Zheng, Y. Continuous directional water transport on integrating tapered surfaces. Adv. Mater. Interf. 7, 2000081 (2020).
Li, C. et al. Bioinspired inner microstructured tube controlled capillary rise. Proc. Natl Acad. Sci. USA 116, 12704–12709 (2019).
Chen, H. et al. Uni-directional liquid spreading control on a bio-inspired surface from the peristome of Nepenthes alata. J. Mater. Chem. A 5, 6914–6920 (2017).
Si, Y. & Dong, Z. Bioinspired smart liquid directional transport control. Langmuir 36, 667–681 (2020).
Ju, J., Xiao, K., Yao, X., Bai, H. & Jiang, L. Bioinspired conical copper wire with gradient wettability for continuous and efficient fog collection. Adv. Mater. 25, 5937–5942 (2013).
Hu, B. et al. Ultrafast self-propelled directional liquid transport on the pyramid-structured fibers with concave curved surfaces. J. Am. Chem. Soc. 142, 6111–6116 (2020).
Daniel, S., Chaudhury, M. K. & Chen, J. C. Fast drop movements resulting from the phase change on a gradient surface. Science 291, 633–636 (2001).
Taylor, B. Concerning the ascent of water between two glass plates. Phil. Trans. R. Soc. Lond. 27, 538 (1712).
Higuera, F. J., Medina, A. & Liñán, A. Capillary rise of a liquid between two vertical plates making a small angle. Phys. Fluids 20, 102102 (2008).
Ponomarenko, A., Quere, D. & Clanet, C. A universal law for capillary rise in corners. J. Fluid Mech. 666, 146–154 (2011).
Panda, M. K. et al. Spatially resolved analysis of short-range structure perturbations in a plastically bent molecular crystal. Nat. Chem. 7, 65–72 (2015).
Pejov, L., Panda, M. K., Moriwaki, T. & Naumov, P. Probing structural perturbation in a bent molecular crystal with synchrotron infrared microspectroscopy and periodic density functional theory calculations. J. Am. Chem. Soc. 139, 2318–2328 (2017).
Hirai, Y., Mayama, H., Matsuo, Y. & Shimomura, M. Uphill water transport on a wettability-patterned surface: experimental and theoretical results. ACS Appl. Mater. Interf. 9, 15814–15821 (2017).
Chaudhury, M. K. & Whitesides, G. M. How to make water run uphill. Science 256, 1539–1541 (1992).
Fang, G., Li, W., Wang, X. & Qiao, G. Droplet motion on designed microtextured superhydrophobic surfaces with tunable wettability. Langmuir 24, 11651–11660 (2008).
Zhang, P., Zhang, L., Chen, H., Dong, Z. & Zhang, D. Surfaces inspired by the Nepenthes peristome for unidirectional liquid transport. Adv. Mater. 29, 1702995 (2017).
Prakash, M., Quéré, D. & Bush, J. W. M. Surface tension transport of prey by feeding shorebirds: the capillary ratchet. Science 320, 931–934 (2008).
Renvoisé, P., Bush, J. W. M., Prakash, M. & Quéré, D. Drop propulsion in tapered tubes. EPL 86, 64003 (2009).
Chen, H. et al. Ultrafast water harvesting and transport in hierarchical microchannels. Nat. Mater. 17, 935–942 (2018).
Greenspan, L. Humidity fixed points of binary saturated aqueous solutions. J. Res. Natl Bur. Stand. 81, 89–96 (1977).
Commins, P., Hara, H. & Naumov, P. Self-healing molecular crystals. Angew. Chem. Int. Ed. 55, 13028–13032 (2016).
Kaupp, G. & Naimi-Jamal, M. R. Mechanically induced molecular migrations in molecular crystals. CrystEngComm 7, 402–409 (2005).
Groom, C. R., Bruno, I. J., Lightfoot, M. P. & Ward, S. C. The Cambridge Structural Database. Acta Cryst. B 72, 171–179 (2016).
Schindelin, J. et al. Fiji: an open-source platform for biological-image analysis. Nat. Methods 9, 676–682 (2012).
Nečas, D. & Klapetek, P. Gwyddion: an open-source software for SPM data analysis. Cent. Eur. J. Phys. 10, 181–188 (2012).
Bückmann, T. et al. Tailored 3D mechanical metamaterials made by dip-in direct-laser-writing optical lithography. Adv. Mater. 24, 2710–2714 (2012).
Acknowledgements
We thank New York University Abu Dhabi for the financial support of this work. We also thank Q. Zhang for help with printing the model surfaces. This research was partially carried out using the Core Technology Platform resources at New York University Abu Dhabi.
Author information
Authors and Affiliations
Contributions
P.C. and P.N. conceived of this work. P.C. performed the microscopy experiments and analysis. M.B.A.-H. performed the AFM measurements. R.R. assisted with the confocal microscopy. L.L. provided support with the crystallography. M.M. performed the video editing, tracking and AFM processing. P.N. supervised the work. P.C. and P.N. co-wrote the paper with contributions from all authors. All authors approved of the final version.
Corresponding author
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Chemistry thanks Huawei Chen, Lei Jiang, Taesung Kim and Yongmei Zheng for their contribution to the peer review of this work.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Supplementary Information
Supplementary Note 1, Figs. 1–13 and Tables 1–8.
Greyscale brightfield optical microscopy of dust particles moving on the (001) plane of an HCB crystal over 670 min. Images were acquired once every 10 min. The dimensions of the video are 616 μm × 416 μm.
Greyscale brightfield optical microscopy of AgMP 1–7 moving on the (001) plane of an HCB crystal over 800 min. Images were acquired once every 10 min. The dimensions of the video are 306 μm × 281 μm.
Greyscale brightfield optical microscopy of water moving downward though an HCB channel. Images were acquired once every 10 min. The dimensions of the video are 92 μm × 60 μm.
Optical images of a drop of water placed onto the (001) surface of an HCB crystal. The video is played in real time. The dimensions of the video are 2.87 mm × 1.55 mm.
Optical video of a drop of water placed onto the (001) surface of a prismatic HCB crystal. This crystal habit does not have channels on its (001) surface. The video is played at 10× speed and the drop is monitored for 3.5 min. The dimensions of the video are 2.87 mm × 1.55 mm.
Two-dimensional AFM images of the (001) face of the crystal monitored at 21 °C and 55% relative humidity for 27.5 h.
Two-dimensional AFM images of the (001) face of the crystal monitored at 21 °C and 55% relative humidity for 27.5 h to measure the rate of sublimation.
Greyscale brightfield optical microscopy of AgMPs a–ab moving on the (001) plane of an HCB crystal at 22.2–22.9, 27.9–36.0, 31.3–40.5 and 36.0–41.0 °C. Images were acquired once every 10 min.
Greyscale brightfield optical microscopy of AgNP 8–14 moving on the (001) plane of an HCB crystal at 34.73–41.49 °C over 1,000 min. Images were acquired once every 10 min. The dimensions of the video are 140 μm × 47 μm.
Greyscale brightfield optical microscopy of AgNP 14 being pushed by a water meniscus. Images were acquired once every 10 min. The dimensions of the video are 32 μm × 22 μm.
Greyscale brightfield optical microscopy of AgMP on the (001) plane of an HCB crystal under desiccation (~0% relative humidity) and under LiCl (saturated), CH3COOK (saturated), ambient and NaCl atmospheres (11, 22, 55 and 75% relative humidity, respectively) at 21 °C. The images were acquired over 1,000 min. The video is played at 30 frames per second and each image was acquired in 10-min intervals. The dimensions of the image in the video are 244 μm × 244 μm, 254 μm × 254 μm, 219 μm × 219 μm, 265 μm × 265 μm and 265 μm × 265 μm, respectively.
Greyscale brightfield optical microscopy of AgMPs tracked on the (001) plane of an HCB crystal under a methanol atmosphere. Particle movement was not observed. The dimensions of the video are 52 μm × 52 μm.
Greyscale brightfield optical microscopy of AgMP on the (001) plane of an HCB while being desiccated for 2,000 min and then rehydrated at 44% relative humidity for 1,000 min. A particle is being pulled by the receding water meniscus under desiccation and pushed by the advancing meniscus when rehydrated. The dimensions of the image in the video when the sample is being desiccated are 114 μm × 114 μm and when it is being rehydrated they are 112 μm × 112 μm. The video is played at 30 frames per second and each image was acquired in 10-min intervals.
Optical microscopy of a nanoscribed HCB simulated surface with AgNP on the surface being carried by evaporating water. The channels are 3 μm wide and 1 μm deep. The object is 1 mm long and 250 μm wide.
Source data
Source Data Fig. 1
Particle tracking data.
Source Data Fig. 2
AFM height map analysis.
Source Data Fig. 3
Particle tracking analysis at controlled temperatures and humidities.
Rights and permissions
Springer Nature or its licensor (e.g. a society or other partner) holds exclusive rights to this article under a publishing agreement with the author(s) or other rightsholder(s); author self-archiving of the accepted manuscript version of this article is solely governed by the terms of such publishing agreement and applicable law.
About this article
Cite this article
Commins, P., Al-Handawi, M.B., Rezgui, R. et al. Autonomous and directional flow of water and transport of particles across a subliming dynamic crystal surface. Nat. Chem. 15, 677–684 (2023). https://doi.org/10.1038/s41557-023-01158-5
Received:
Accepted:
Published:
Issue Date:
DOI: https://doi.org/10.1038/s41557-023-01158-5