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1.
Langmuir ; 36(50): 15309-15318, 2020 Dec 22.
Artículo en Inglés | MEDLINE | ID: mdl-33306912

RESUMEN

The introduction of the self-healing function into superhydrophobic surfaces has recently raised increasing attention because it can renew the feature of the surface iteratively to a large extent to extend the service life span of the surface in practical applications. However, it still faces a great challenge on how to achieve this unique surface with a tunable self-healing function via an easy and effective way. Here, we propose a general, yet easily implemented strategy to endow a diversity of commercial substrates with self-healable superhydrophobic surfaces mainly relying on the collective use of the polydopamine (PDA) chemistry with a hydrophobic silane-octadecyltrimethoxysilane (ODTMS). Upon applying ultrasonication for 30 min to an alkaline aqueous solution comprising dopamine hydrochloride (DA) and ODTMS, ODTMS disperses into the aqueous phase as microdroplets, while DA polymerizes into PDA exclusively onto the micro-sized oil droplets, forming capsules with nanoroughness. In the presence of substrates, PDA also anchors these composite capsules onto substrates, resulting in hierarchical surfaces. ODTMS is detected abundantly on the hierarchical surfaces, leading to superhydrophobic surfaces. Remarkably, this superhydrophobicity is self-restorable at room temperature (e.g., days) once it is deteriorated by the air plasma or extremely acid/alkali treatment, and this self-restoration can be significantly accelerated via the heating (2 h) or rubbing (5 min) treatment. Generally, heating and rubbing are the valid ways to induce self-healing, which is speculated to accelerate the migration of hidden ODTMS from the capsules to the surfaces because of the minimization of the global surface-free energy. Benefiting from the self-healing superhydrophobicity, we devise oil/water separation using various surface-modified commercial fabrics, which exhibit a prolonged life span in applications and may further facilitate other usage in environmental remediation and water purification.

2.
Nat Commun ; 12(1): 2305, 2021 Apr 16.
Artículo en Inglés | MEDLINE | ID: mdl-33863884

RESUMEN

The selective hydrogenation of CO2 to value-added chemicals is attractive but still challenged by the high-performance catalyst. In this work, we report that gallium nitride (GaN) catalyzes the direct hydrogenation of CO2 to dimethyl ether (DME) with a CO-free selectivity of about 80%. The activity of GaN for the hydrogenation of CO2 is much higher than that for the hydrogenation of CO although the product distribution is very similar. The steady-state and transient experimental results, spectroscopic studies, and density functional theory calculations rigorously reveal that DME is produced as the primary product via the methyl and formate intermediates, which are formed over different planes of GaN with similar activation energies. This essentially differs from the traditional DME synthesis via the methanol intermediate over a hybrid catalyst. The present work offers a different catalyst capable of the direct hydrogenation of CO2 to DME and thus enriches the chemistry for CO2 transformations.

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