Liquid marbles: review of recent progress in physical properties, formation techniques, and lab-in-a-marble applications in microreactors and biosensors

Tenjimbayashi, Mizuki; Mouterde, Timothée; Roy, Pritam Kumar; Uto, Koichiro

doi:10.1039/d3nr04966c

Cited by 11 publications

(7 citation statements)

References 158 publications

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“…Liquid marbles were first discovered and proposed by Aussillous and Quéré, which are nonwetting droplets that are wrapped by hydrophobic powder particles . The process of preparing liquid marbles is simple, and the special structure of liquid marbles shows typical properties such as nonadhesion, − elasticity, , mechanical stability, , and divisibility properties, − which are widely used in the fields of droplet microfluidics, , controlled release, − microreactors, − granulation and energy storage. − …”

Section: Introductionmentioning

confidence: 99%

“…However, the existing process of preparing the anisotropic superhydrophobic surface is complex, expensive, and challenging to implement on an industrial scale. − Moreover, the anisotropy depends mainly on the specific arrangement of micronano structures on the surface, limiting its ability to control the directional movement of larger droplets. , For “droplets” with significant particle size, the influence of particle size becomes paramount, where the kinetic energy arising from solid/solid contact surpasses the energy barrier imposed by the micronano architecture. − Consequently, the anisotropic superhydrophobic surface prepared by the traditional method is unsuitable for the batch-directional transportation of large-sized liquid/melt marbles.…”

Section: Introductionmentioning

confidence: 99%

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Preparation of Oriented Superhydrophobic Surface to Reduce Agglomeration in Preparing Melt Marbles

He,

Huang,

Liu

et al. 2024

Langmuir

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Numerous innovative granulation techniques utilizing the concept of liquid marbles have been proposed before. However, these processes frequently encounter issues such as collisions, aggregation, and fragmentation of liquid/melt marble during the granulation process. In this study, the oriented superhydrophobic surface (OSS) was successfully prepared by utilizing copper wire to solve the above problem, facilitating efficient batch production and guided transportation of uniform marbles. The parameters and mechanisms of this process were thoroughly studied. The optimized structure is that the copper wire spacing (d) and height (h) are set as 1.0 and 0.1 mm, respectively. This resulted in a surface contact angle (CA) of 156°and anisotropic sliding (ΔSA) of 16.3 ± 1.34°. Using the prepared substrate, high-quality urea products were successfully obtained through the controlled transport of urea melt marbles. The mechanism of guided and directional drag reduction, based on the solid/solid contact on the surface, is proposed. These findings in this study have significant implications for improving granulation processes.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Preparation of Oriented Superhydrophobic Surface to Reduce Agglomeration in Preparing Melt Marbles

He,

Huang,

Liu

et al. 2024

Langmuir

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“…Liquid marbles (LMs) are millimeter-sized liquid droplets stabilized by micro- or nanosized nonwetting hydrophobic particles that are spontaneously adsorbed at gas–liquid interfaces. − LMs are generally fabricated by rolling liquid droplets on a hydrophobic powder bed. The particles form a porous shell encapsulating the droplet, which behaves as a barrier between the liquid inside and the supporting substrates of the LMs to prevent the liquid from contacting the substrates.…”

Section: Introductionmentioning

confidence: 99%

pH-Responsive Liquid Marbles Stabilized with Chitosan-Stearic Acid-Conjugated Particles

Kunanopparatn,

Hayashi,

Atsuta

et al. 2024

ACS Sustainable Chem. Eng.

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Liquid marbles (LMs) are liquid droplets covered by hydrophobic solid particles adsorbed at liquid−gas interfaces. In this study, we designed pH-responsive LMs by using chitosan (CS) particles conjugated with stearic acid (SA) as a stabilizer, both of which are natural materials. Micrometer-sized CS-SA-conjugated particles were synthesized via a sustainable route based on solvent-free and one-pot thermal amidation between CS and SA. The resulting particles were extensively characterized on multiple scales by determining their sizes, shapes, morphologies, bulk/ surface chemical compositions, hydrophilic−hydrophobic balances, and pHresponsive behaviors. The heterogeneous reactions only occurred near the particle surface, and the CS-SA-conjugated particles showed hydrophobic surfaces and pH-responsive cores. Millimeter-and centimeter-sized LMs with liquid contents ranging between 15 μL and 1.0 mL were readily prepared by rolling water droplets over a dried CS-SA particle powder bed. Stereomicroscopy studies confirmed that the CS-SA particles were adsorbed at the surfaces of the water droplets as mono-and bilayers, resulting in stable LMs. These LMs showed long-term stability (>2 h) under a water vapor atmosphere but were disrupted immediately (<2 min) when exposed to HCl vapor, with wetting of the particles by the inner aqueous solution. Here, acid vaporinduced disruption was realized with the "response cascade" concept: the initial pH stimulus led to disruption via intermediate wetting responses. We also demonstrated the use of LMs as colorimetric sensors for amines generated during food spoilage.

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“…Liquid marbles (LMs) are prepared by the adsorption of hydrophobic particles, ranging from micrometer to submicrometer sizes, at the air–liquid interface of a liquid droplet. − These have been studied for applications such as microliquid transfer, detectors, − and microreaction fields. − The constituents for LMs encompass diverse materials such as hydrophobic silica particles, , carbon nanotubes, small organic powders, , and polymer particles. − Typically, LMs are prepared by rolling a water droplet on hydrophobic powder. Recently, stimuli-responsive LMs have been prepared using hydrophobic powder that can change from hydrophobic to hydrophilic in response to pH, − temperature, electric and magnetic fields, − and light …”

Section: Introductionmentioning

confidence: 99%

pH- and Photoresponsive Liquid Plasticine

Onodera,

Usuda,

Hara

et al. 2024

Langmuir

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Liquid marbles (LMs) can be prepared by adsorption of hydrophobic particles at the air–liquid interface of a water droplet. LMs have been studied for their application as microreaction vessels. However, their opaqueness poses challenges for internal observation. Liquid plasticines (LPs), akin to LMs, can be prepared by the adsorption of hydrophobic particles with a diameter of 50 nm or less, at the air–liquid interface of a water droplet. Unlike LMs, LPs are transparent, allowing for internal observation, thus presenting promising applications as reactors and culture vessels on a microliter scale. In this study, the surface of silica particles, approximately 20 nm in diameter, was rendered hydrophobic to prepare hydrophobic silica particles (SD0). A small amount of poly(2-(diisopropylamino)ethyl methacrylate) (PDPA) was then grafted onto the surface of SD0, yielding SD1. SD0 particles exhibited consistent hydrophobicity irrespective of the environmental pH atmosphere. Under acidic conditions, SD1 became hydrophilic due to the protonation of pendant tertiary amines in the grafted PDPA chains. However, SD1 alone was unsuitable for LP preparation due to its high surface wettability regardless of atmospheric pH, attributable to the presence of PDPA-grafted chains. Therefore, to prepare pH-responsive LP, SD1 and SD0 were mixed (SD1/SD0 = 3/7). Upon exposure to HCl gas, these LPs ruptured, with the leaked water from the LPs being absorbed by adjacent paper. Moreover, clear LPs, prepared using an aqueous solution containing a water-soluble photoacid generator (PAG), disintegrated upon exposure to light as PAG generated acid, leading to LP breakdown. In summary, pH-responsive LPs, capable of disintegration under acidic conditions and upon light irradiation, were successfully prepared in this study.

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Liquid marbles: review of recent progress in physical properties, formation techniques, and lab-in-a-marble applications in microreactors and biosensors

Abstract: This review summarises the fundamental properties of liquid marbles, the recent advances in the concept of liquid marbles, physical properties, formation methods, liquid marble-templated material design, and biochemical applications.

Cited by 11 publications

References 158 publications

Preparation of Oriented Superhydrophobic Surface to Reduce Agglomeration in Preparing Melt Marbles

Preparation of Oriented Superhydrophobic Surface to Reduce Agglomeration in Preparing Melt Marbles

pH-Responsive Liquid Marbles Stabilized with Chitosan-Stearic Acid-Conjugated Particles

pH- and Photoresponsive Liquid Plasticine

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