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1.
Dalton Trans ; 53(6): 2762-2769, 2024 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-38226665

RESUMO

The hydrogen oxidation reaction is an important process in anion exchange membrane fuel cells with alkaline solutions. The pursuit of efficient catalysts for alkaline hydrogen oxidation has attracted considerable attention. In this study, we present a precursor route for the synthesis of a new Ir-based catalyst (Ir-Ni/NiO/C), in which Ir nanoclusters were immobilized on the generated Ni/NiO/C support derived from a metal-organic framework. The small size of Ir clusters facilitates the exposure of catalytically active sites. The electronic interplay between the Ir nanoclusters and the Ni/NiO/C support optimized the hydrogen binding energy (HBE) and hydroxide binding energy (OHBE) on the surface, which is unattainable on the contrasting Ir-C, Ir-Ni/C, and Ir-NiO/C products. The optimized catalyst shows excellent mass activity for alkaline hydrogen oxidation, which is 3.1 times that of the Pt/C catalyst. This study presents a promising pathway for the development of advanced HOR catalysts.

2.
ACS Mater Lett ; 5(9): 2508-2517, 2023 Sep 04.
Artigo em Inglês | MEDLINE | ID: mdl-37680546

RESUMO

Delivering heat in vivo could enhance a wide range of biomedical therapeutic and diagnostic technologies, including long-term drug delivery devices and cancer treatments. To date, providing thermal energy is highly power-intensive, rendering it oftentimes inaccessible outside of clinical settings. We developed an in vivo heating method based on the exothermic reaction between liquid-metal-activated aluminum and water. After establishing a method for consistent activation, we characterized the heat generation capabilities with thermal imaging and heat flux measurements. We then demonstrated one application of this reaction: to thermally actuate a gastric resident device made from a shape-memory alloy called Nitinol. Finally, we highlight the advantages and future directions for leveraging this novel in situ heat generation method beyond the showcased example.

3.
Dalton Trans ; 52(30): 10323-10331, 2023 Aug 01.
Artigo em Inglês | MEDLINE | ID: mdl-37448344

RESUMO

Design and fabrication of cost-effective (pre-)catalysts are important for water splitting and metal-air batteries. In this direction, various metal-organic frameworks (MOFs) have been investigated as pre-catalysts for oxygen evolution. However, the activation process and the complex reconstruction behaviour of these MOFs are not well understood. Herein, square-like MOF nanosheets in which carbon nanotubes were embedded were prepared by introducing an amine ligand to coordinate with Ni ions and then reacting with [Fe(CN)6]3-. The formed MOF nanosheets containing nickel and iron species were then activated by NaBH4, inducing the leaching of ligands and the formation of tiny active species in situ loaded on carbon nanotubes. The prepared catalyst shows superior oxygen evolution performance with an ultralow overpotential of 231 mV for 10 mA cm-2, a fast reaction kinetics with a small Tafel slope of 52.3 mV dec-1, and outstanding catalysis stability. The excellent electrocatalytic performance for oxygen evolution can be attributed to the structural advantage of in situ derived small sized active species and one-dimensional conductive networks. This work provides a new thought for the enhancement of the electrocatalytic performance of MOF materials.

4.
Dalton Trans ; 51(40): 15467-15474, 2022 Oct 18.
Artigo em Inglês | MEDLINE | ID: mdl-36156615

RESUMO

The development of hydrogen-oxygen fuel cells with an alkaline electrolyte was highly limited by the sluggish kinetics of the hydrogen oxidation reaction (HOR). Here, with a pyrolysis-reduction route, a new RuNi-based electrocatalyst was prepared, which presents an ultrathin nanowire-like structure. In alkaline media, this catalyst shows an excellent catalytic performance with an exchange current density of 1.10 mA cm-2disk for hydrogen oxidation. The exchange current density and mass activity of this catalyst are much higher than those of its single-metal counterparts and even the commercial Pt/C catalyst containing 20% Pt. Such a remarkable catalytic activity can be explained by the interaction between Ru and Ni; the incorporation of Ni may induce an electronic effect on the optimization of the Ru-Had strength and provide a functional surface that can absorb OH species, thus boosting the catalytic activity. These findings may cast a new light on the exploration of low-cost but high-efficiency catalysts for fuel cells.

5.
Sci Robot ; 7(70): eabp9066, 2022 09 28.
Artigo em Inglês | MEDLINE | ID: mdl-36170378

RESUMO

Oral drug delivery of proteins is limited by the degradative environment of the gastrointestinal tract and poor absorption, requiring parenteral administration of these drugs. Luminal mucus represents the initial steric and dynamic barrier to absorption. To overcome this barrier, we report the development of the RoboCap, an orally ingestible, robotic drug delivery capsule that locally clears the mucus layer, enhances luminal mixing, and topically deposits the drug payload in the small intestine to enhance drug absorption. RoboCap's mucus-clearing and churning movements are facilitated by an internal motor and by surface features that interact with small intestinal plicae circulares, villi, and mucus. Vancomycin (1.4 kilodaltons of glycopeptide) and insulin (5.8 kilodaltons of peptide) delivery mediated by RoboCap resulted in enhanced bioavailability 20- to 40-fold greater in ex vivo and in vivo swine models when compared with standard oral delivery (P < 0.05). Further, insulin delivery via the RoboCap resulted in therapeutic hypoglycemia, supporting its potential to facilitate oral delivery of drugs that are normally precluded by absorption limitations.


Assuntos
Nanopartículas , Procedimentos Cirúrgicos Robóticos , Administração Oral , Animais , Trato Gastrointestinal/metabolismo , Insulina/metabolismo , Muco/metabolismo , Peptídeos/metabolismo , Suínos , Vancomicina/metabolismo
6.
Nat Rev Mater ; 7(11): 908-925, 2022.
Artigo em Inglês | MEDLINE | ID: mdl-36124042

RESUMO

The surface mucosa that lines many of our organs houses myriad biometric signals and, therefore, has great potential as a sensor-tissue interface for high-fidelity and long-term biosensing. However, progress is still nascent for mucosa-interfacing electronics owing to challenges with establishing robust sensor-tissue interfaces; device localization, retention and removal; and power and data transfer. This is in sharp contrast to the rapidly advancing field of skin-interfacing electronics, which are replacing traditional hospital visits with minimally invasive, real-time, continuous and untethered biosensing. This Review aims to bridge the gap between skin-interfacing electronics and mucosa-interfacing electronics systems through a comparison of the properties and functions of the skin and internal mucosal surfaces. The major physiological signals accessible through mucosa-lined organs are surveyed and design considerations for the next generation of mucosa-interfacing electronics are outlined based on state-of-the-art developments in bio-integrated electronics. With this Review, we aim to inspire hardware solutions that can serve as a foundation for developing personalized biosensing from the mucosa, a relatively uncharted field with great scientific and clinical potential.

7.
Inorg Chem ; 61(35): 14187-14194, 2022 Sep 05.
Artigo em Inglês | MEDLINE | ID: mdl-35998715

RESUMO

Development of effective electrocatalysts toward hydrogen oxidation with a low content of noble metals has attracted the attention of the catalytic community. In this work, a novel catalyst composed of nitrogen-doped carbon acting as the substrate and Ir nanoclusters as active species was prepared, which was then employed as an effective catalyst for the hydrogen oxidation reaction (HOR) in an alkaline electrolyte. In 0.1 M KOH, the optimized catalyst provides an exchange current density of 0.144 mA cmIr-2 for HOR that outperforms the catalytic activity of the commercial Pt/C catalyst with a Pt content of 20 wt %. The substrate induces highly active Ir sites that markedly boosted the electrocatalytic activity for HOR. The nitrogen-doped carbon substrate increases the stability of Ir nanoclusters and decreases the absorption energy of hydrogen on Ir sites; at the same time, the higher electrostatic potential around the adsorbed hydrogen on Ir/N-doped carbon also enables them to be easily attracted by OH- species, both of which enhanced the catalytic activity. The excellent catalytic activity and the understanding shown here will give some hints for the development of HOR catalysts used in alkaline electrolytes.

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