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In-plane frost growth on chilled hydrophobic surfaces is an inter-droplet phenomenon, where frozen droplets harvest water from neighboring supercooled liquid droplets to grow ice bridges that propagate across the surface in a chain reaction. To date, no surface has been able to passively prevent the in-plane growth of ice bridges across the population of supercooled condensate. Here, we demonstrate that when the separation between adjacent nucleation sites for supercooled condensate is properly controlled with chemical micropatterns prior to freezing, inter-droplet ice bridging can be slowed and even halted entirely. Since the edge-to-edge separation between adjacent supercooled droplets decreases with growth time, deliberately triggering an early freezing event to minimize the size of nascent condensation was also necessary. These findings reveal that inter-droplet frost growth can be passively suppressed by designing surfaces to spatially control nucleation sites and by temporally controlling the onset of freezing events.
Frost inevitably forms on any subfreezing surface whose temperature is beneath the dew point. Water vapor can bypass the liquid phase and transform directly into ice, known as deposition or desublimation. However, in many cases the water vapor first condenses into supercooled liquid, which later freezes into ice. This indirect method of frost formation is known as condensation frosting and is more common than direct deposition in many cases, particularly at low supersaturation degrees and/or on hydrophobic surfaces1.
Until very recently, it was widely assumed that the primary mechanism of condensation frosting for surfaces promoting dropwise condensation was the heterogeneous nucleation of ice at the solid-liquid interface of each individual supercooled droplet2,3,4,5. Numerous reports have observed that heterogeneous nucleation can be delayed by minutes or even hours for supercooled droplets deposited on superhydrophobic surfaces compared to traditional surfaces, due to the hydrophobicity increasing the energy barrier for nucleation6,7,8 and because the air pockets trapped by a suspended Cassie droplet reduce the heat transfer rate8,9,10 and minimize the solid-liquid contact area where nucleation events can occur6,7,8,10,11,12. Condensed droplets can also grow in a Cassie state on nanostructured superhydrophobic surfaces13,14,15, such that supercooled condensate can exhibit delayed heterogeneous nucleation in the same manner as with deposited droplets3,4,5. Furthermore, the minimal contact angle hysteresis of Cassie droplets on superhydrophobic surfaces can be exploited to dynamically remove supercooled droplets before heterogeneous nucleation occurs at all. Examples include deposited droplets that were gravitationally removed by sliding9,11 or rebound16,17,18 and condensed droplets that were removed by gravity at millimetric length scales19,20 or by coalescence-induced jumping at micrometric length scales21,22,23. It would therefore seem that nanostructured superhydrophobic surfaces should be able to completely prevent the onset of condensation frosting, by delaying heterogeneous nucleation long enough to dynamically remove supercooled condensate from the surface.
Curiously, it was observed that even when supercooled condensate was continually removed from a superhydrophobic surface via coalescence-induced jumping before heterogeneous nucleation occurred, frost still grew over the surface21. This was attributed to an unexpected phenomenon where only a single droplet had to freeze due to heterogeneous nucleation (typically at edge defects where jumping did not occur), at which point the frozen droplet harvested water from nearby liquid droplets, growing ice bridges that connected across the forming condensate in an unstoppable chain reaction21,24. This source-sink vapor interaction between an evaporating liquid droplet and a bridging frozen droplet is most likely due to the higher water vapor pressure over liquid water compared to frozen water25,26,27. Since the mass of the ice bridge is harvested from the liquid droplet, it follows that the liquid droplet can completely evaporate before the ice bridge connects when the inter-droplet spacing is sufficiently large21,24. To date, no surface has been able to completely stop the inter-droplet growth of frost when a freezing event occurs near the population of supercooled condensate24,28,29,30,31; typically ice bridges connect for nearly every droplet on smooth hydrophobic surfaces and for approximately 1/3 of droplets on jumping-droplet superhydrophobic surfaces21.
Inspired by the Stenocara desert beetle32, the nucleation sites for condensation can be spatially controlled on engineered surfaces exhibiting chemical patterns of contrasting hydrophobic and hydrophilic regions, due to the dramatically lower energy barrier for nucleation on the hydrophilic features33,34,35,36,37,38. Chemically patterned substrates have been shown to enhance water harvesting39,40,41 and phase-change heat transfer42,43,44, and are also useful for controlling liquid morphology45,46, tuning droplet hysteresis47,48, controllably depositing micro/nano-materials49, and lab-on-a-chip applications50,51. Now that it is understood that condensation frosting is dependent upon the spatial distribution of droplets, the ability of a chemically patterned surface to control nucleation sites seems ideal for characterizing and controlling inter-droplet frost growth. However, to date there have been no reports using chemically patterned surfaces to characterize the spatial distribution of condensation or the related dynamics of inter-droplet frost growth.
Here, we demonstrate that chemical patterns can be used to tune the spatial distribution of supercooled condensation and subsequently control the geometry and speed of inter-droplet frost growth. The success and rate of inter-droplet frost growth was found to be dependent upon two primary factors: the extent of spacing between hydrophilic regions where liquid nucleation occurred and the time allowed for condensation growth prior to the initial freezing event. For the first time, inter-droplet ice bridging could be completely halted by utilizing sufficiently sparse hydrophilic patterns and by quickly triggering a freezing event near the patterned condensation.
Controlling condensation and frost growth with chemical micropatterns
Jonathan B. Boreyko,1,2,3 Ryan R. Hansen,2,3,4 Kevin R. Murphy,1 Saurabh Nath,1 Scott T. Retterer,2,3,5 and C. Patrick Colliera,2,3
Somatic component to myocardial infarction: three year follow up.
A S Nicholas, D A DeBias, and C H Greene
1991 Jun 29;
Within minutes of Bdellovibrio bacteriovorus attack on prey cells, such as Escherichia coli, the cytoplasmic membrane of the prey is altered. Sodium dodecyl sulfate-polyacrylamide gel electrophoresis of purified invaded prey cell (bdelloplast) membranes revealed the appearance of a noncytoplasmic membrane protein. This protein is not observed in preparations of noninvaded E. coli membranes and migrates in a manner similar to that of E. coli OmpF. Isoelectric focusing and two-dimensional gel electrophoresis of bdelloplast cytoplasmic membrane preparations also revealed the presence of a protein with electrophoretic properties similar to those of OmpF and the major Bdellovibrio outer membrane proteins. The protein appears in cytoplasmic membrane preparations within minutes of attack and persists throughout most of the intraperiplasmic developmental cycle. The appearance of this protein is consistent with our hypothesis that bdellovibrios translocate a pore protein into the bdelloplast cytoplasmic membrane to kill their prey and to gain access to the cytoplasmic contents for growth.
Translocation of an outer membrane protein into prey cytoplasmic membranes by bdellovibrios.
J J Tudor and M A Karp