Modulating the Reactivity of Liquid Ga Nanoparticle Inks by Modifying Their Surface Chemistry

Castilla-Amorós, Laia; Chien, Tzu-Chin Chang; Pankhurst, James R.; Buonsanti, Raffaella

doi:10.1021/jacs.1c12880

Cited by 23 publications

(20 citation statements)

References 73 publications

(197 reference statements)

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“…Figure A reports a representative TEM image illustrating the uniformity of the Ga NPs, which possess a diameter of 26 nm with a particle size distribution of less than 10% (Figure S1). Scanning transmission electron microscopy (STEM) imaging (Figure B) along with EDXS elemental mapping of O and Ga and the line profile over one Ga NP (Figure C–E) evidence the presence of a native oxide skin around 2.6 nm thick on the Ga NPs, which is consistent with previous studies. ,, …”

Section: Resultsmentioning

confidence: 63%

“…Ga NPs were synthesized by means of colloidal chemistry, following a previously reported protocol. ,, This wet chemistry approach provides the uniform size distribution that is essential when investigating eventual size and morphology changes of the catalysts during operation. Figure A reports a representative TEM image illustrating the uniformity of the Ga NPs, which possess a diameter of 26 nm with a particle size distribution of less than 10% (Figure S1).…”

Section: Resultsmentioning

confidence: 99%

“…Scanning transmission electron microscopy (STEM) imaging (Figure 1B) along with EDXS elemental mapping of O and Ga and the line profile over one Ga NP (Figure 1C−E) evidence the presence of a native oxide skin around 2.6 nm thick on the Ga NPs, which is consistent with previous studies. 29,30,34 Electrochemical CO 2 Reduction. Bulk Ga electrodes were reported to be selective for CO 2 RR with a faradaic efficiency (FE) for CO of around 20%, the rest being H 2 from the competing hydrogen evolution reaction (HER).…”

Section: ■ Introductionmentioning

confidence: 99%

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The Native Oxide Skin of Liquid Metal Ga Nanoparticles Prevents Their Rapid Coalescence during Electrocatalysis

et al. 2022

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Liquid metals (LMs) have been used in electrochemistry since the 19th century, but it is only recently that they have emerged as electrocatalysts with unique properties, such as inherent resistance to coke poisoning, which derives from the dynamic nature of their surface. The use of LM nanoparticles (NPs) as electrocatalysts is highly desirable to enhance any surface-related phenomena. However, LM NPs are expected to rapidly coalesce, similarly to liquid drops, which makes their implementation in electrocatalysis hard to envision. Herein, we demonstrate that liquid Ga NPs (18 nm, 26 nm, 39 nm) drive the electrochemical CO2 reduction reaction (CO2RR) while remaining well-separated from each other. CO is generated with a maximum faradaic efficiency of around 30% at −0.7 VRHE, which is similar to that of bulk Ga. The combination of electrochemical, microscopic, and spectroscopic techniques, including operando X-ray absorption, indicates that the native oxide skin of the Ga NPs is still present during CO2RR and provides a barrier to coalescence during operation. This discovery provides an avenue for future development of Ga-based LM NPs as a new class of electrocatalysts.

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Section: Resultsmentioning

confidence: 63%

Section: Resultsmentioning

confidence: 99%

Section: ■ Introductionmentioning

confidence: 99%

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The Native Oxide Skin of Liquid Metal Ga Nanoparticles Prevents Their Rapid Coalescence during Electrocatalysis

et al. 2022

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“…As a result, the interface interaction between LMs and functionalized molecules deserves further exploration, thereby achieving a better modification of LM and facilitating the optimization of synthetic strategies. [ 135,136 ] Although LM‐based materials have made progress in targeted therapy, better modification of LM by biomolecules such as proteins and genes to achieve more efficient targeted therapy is still expected. Besides, improving the stability of LM‐based materials for long‐term storage is crucial for further biomedical applications.…”

Section: Discussionmentioning

confidence: 99%

Emerging Liquid Metal Biomaterials: From Design to Application

et al. 2022

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Liquid metals (LMs) as emerging biomaterials possess unique advantages including their favorable biosafety, high fluidity, and excellent electrical and thermal conductivities, thus providing a unique platform for a wide range of biomedical applications ranging from drug delivery, tumor therapy, and bioimaging to biosensors. The structural design and functionalization of LMs endow them with enhanced functions such as enhanced targeting ability and stimuli responsiveness, enabling them to achieve better and even multifunctional synergistic therapeutic effects. Herein, the advantages of LMs in biomedicine are presented. The design of LM‐based biomaterials with different scales ranging from micro‐/nanoscale to macroscale and various components is explored in‐depth to promote the understanding of structure–property relationships, guiding their performance optimization and applications. Furthermore, the related advanced progress in the development of LM‐based biomaterials in biomedicine is summarized. Current challenges and prospects of LMs in the biomedical field are also discussed.

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“…Thiol groups, hydroxyl groups, amine groups, carboxylic groups, and phosphate groups have been successfully grafted on EGaIn nanoparticles for different applications, mainly by sonicating EGaIn bulk alloys in aqueous and organic solutions containing the corresponding species in polymers to form multiple layers, − for example, sonication of EGaIn in a dopamine solution to prepare EGaIn nanoparticles wrapped with polydopamine . Sonicating the mixture of poly(1-octadecene- alt -maleic anhydride) (POMA) in toluene and mixing with deionized water in the presence of EGaIn resulted in the formation of POMA-coated EGaIn nanoparticles, which remain stable in biological buffers for at least 2 months without noticeable oxidation.…”

Section: Introductionmentioning

confidence: 99%

Surface Modification of Liquid Metal with p-Aniline Derivatives toward Bioapplications: Biosensing as an Example

Huang

Zou

Liu

2022

ACS Appl. Mater. Interfaces

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It is a long-lasting research topic to avoid the formation of oxidation layers on gallium-based liquid metals. This study has developed a simple general method for modification of the eutectic gallium−indium (EGaIn) surface with p-aniline derivatives to introduce a monolayer of organic molecules with versatile functional groups. The binding affinity of carboxylic acid groups, amine groups, or thiol groups with EGaIn is in the order SH > NH 2 > COOH. For the first time, it is evidenced that both NH 2 and SH groups can coexist on the EGaIn nanoparticle surface with the binding affinities of 30 and 70%, respectively. The formation of these organic molecules on the EGaIn surface antioxidizes and thus stabilizes the EGaIn nanoparticles, while increasing the conductivity of EGaIn significantly. The resulting EGaIn nanoparticles have very good distribution in both ethanol and aqueous solutions and rich surface chemistry, making them suitable for the following attachment of biomolecules such as aptamers, antibodies, or enzymes for biomedical applications. As an example, the EGaIn surface is successfully modified with p-aminobenzoic acid followed by the attachment of an insulin aptamer, which can be used for the electrochemical detection of insulin with the lowest detectable concentration limit of 1 pM. This study reveals the modification of EGaIn nanoparticles with p-aniline derivatives with versatile functional groups to antioxidize EGaIn in a biological environment, opening a door for gallium-based liquid metals toward biomedical applications.

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Modulating the Reactivity of Liquid Ga Nanoparticle Inks by Modifying Their Surface Chemistry

Cited by 23 publications

References 73 publications

The Native Oxide Skin of Liquid Metal Ga Nanoparticles Prevents Their Rapid Coalescence during Electrocatalysis

The Native Oxide Skin of Liquid Metal Ga Nanoparticles Prevents Their Rapid Coalescence during Electrocatalysis

Emerging Liquid Metal Biomaterials: From Design to Application

Surface Modification of Liquid Metal with p-Aniline Derivatives toward Bioapplications: Biosensing as an Example

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