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1.
Proc Natl Acad Sci U S A ; 121(9): e2319286121, 2024 Feb 27.
Artigo em Inglês | MEDLINE | ID: mdl-38394244

RESUMO

Hydrogen (H2) and hydrogen peroxide (H2O2) play crucial roles as energy carriers and raw materials for industrial production. However, the current techniques for H2 and H2O2 production rely on complex catalysts and involve multiple intermediate steps. In this study, we present a straightforward, environmentally friendly, and highly efficient laser-induced conversion method for overall water splitting to simultaneously generate H2 and H2O2 at ambient conditions without any catalysts. The laser direct overall water splitting approach achieves an impressive light-to-hydrogen energy conversion efficiency of 2.1%, with H2 production rates of 2.2 mmol/h and H2O2 production rates of 65 µM/h in a limited reaction area (1 mm2) within a short real reaction time (0.36 ms/h). Furthermore, we elucidate the underlying physics and chemistry behind the laser-induced water splitting to produce H2 and H2O2. The laser-induced cavitation bubbles create an optimal microenvironment for water-splitting reactions because of the transient high temperatures (104 K) surpassing the chemical barrier required. Additionally, their rapid cooling rate (1010 K/s) hinders reverse reactions and facilitates H2O2 retention. Finally, upon bubble collapse, H2 is released while H2O2 remains dissolved in the water. Moreover, a preliminary amplification experiment demonstrates the potential industrial applications of this laser chemistry. These findings highlight that laser-based production of H2 and H2O2 from water holds promise as a straightforward, environmentally friendly, and efficient approach on an industrial scale beyond conventional chemical catalysis.

2.
J Phys Chem Lett ; 14(51): 11735-11741, 2023 Dec 28.
Artigo em Inglês | MEDLINE | ID: mdl-38113518

RESUMO

Macroscopically, the traditional Young-Lippmann equation is used to describe the water contact angle under a weak electric field. Here we report a new wetting mechanism of deionized water under a strong electric field that defies the conventional Young-Lippmann equation. The contact angle of the deionized water droplet on a model hexagonal lattice with a different initial wettability is extensively modulated by the vertical electric field. The cosine of water contact angle on a hydrophilic substrate displays an anomalous linear relationship with the field, in contrast to the hydrophobic case, which shows an inverse parabolic relationship. Such anomalous wetting is verified by experimental measurements of water droplets on a pyroelectric substrate. Moreover, we identify that this anomaly arises from the linear modulation of the solid-liquid interfacial tension of hydrophilic substrates by the electric field. Our findings provide atomistic insight into the fundamental laws and new phenomena of water-surface interactions under extreme electric fields.

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