The curious chemistry observed in microdroplets has captivated chemists in recent years and has led to an investigation into their ability to drive seemingly impossible chemistries. One particularly interesting capability of these microdroplets is their ability to accelerate reactions by several orders of magnitude. While there have been many investigations into which reactions can be accelerated by confinement within microdroplets, no study has directly compared reaction acceleration at the liquid|liquid and gas|liquid interfaces. Here, we confine glucose oxidase, one of life’s most important enzymes, to microdroplets and monitor the turnover rate of glucose by the electroactive cofactor, hexacyanoferrate (III). We use stochastic electrochemistry to monitor the collision of single femtoliter water droplets on an ultramicroelectrode. We also develop a measurement modality to robustly quantify reaction rates for femtoliter liquid aerosol droplets, where the majority of the interface is gas|liquid. We demonstrate that the gas|liquid interface accelerates enzyme turnover by over an order of magnitude over the liquid|liquid interface. This is the first apples-to-apples comparison of reaction acceleration at two distinct interfaces that indicates that the gas|liquid interface plays a central role in driving curious chemistry.
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Interfacial Dynamics in Dual Channels: Inspired by Cuttlebone
The cuttlebone, a chambered gas-filled structure found in cuttlefish, serves a crucial role in buoyancy control for the animal. This study investigates the motion of liquid-gas interfaces within cuttlebone-inspired artificial channels. The cuttlebone’s unique microstructure, characterized by chambers divided by vertical pillars, exhibits interesting fluid dynamics at small scales while pumping water in and out. Various channels were fabricated with distinct geometries, mimicking cuttlebone features, and subjected to different pressure drops. The behavior of the liquid-gas interface was explored, revealing that channels with pronounced waviness facilitated more non-uniform air-water interfaces. Here, Lyapunov exponents were employed to characterize interface separation, and they indicated more differential motions with increased pressure drops. Channels with greater waviness and amplitude exhibited higher Lyapunov exponents, while straighter channels exhibited slower separation. This is potentially aligned with cuttlefish’s natural adaptation to efficient water transport near the membrane, where more straight channels are observed in real cuttlebone.
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- Award ID(s):
- 2042740
- PAR ID:
- 10494862
- Publisher / Repository:
- MDPI
- Date Published:
- Journal Name:
- Biomimetics
- Volume:
- 8
- Issue:
- 6
- ISSN:
- 2313-7673
- Page Range / eLocation ID:
- 466
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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