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1.
Proc Natl Acad Sci U S A ; 121(13): e2317192121, 2024 Mar 26.
Artigo em Inglês | MEDLINE | ID: mdl-38507451

RESUMO

Photothermal heating and photocatalytic treatment are two solar-driven water processing approaches by harnessing NIR and UV-vis light, respectively, which can fully utilize solar energy if integrated. However, it remains a challenge to achieve high performance in both approaches when integrated in a material due to uncontrollable heat diffusion. Here, we report a demonstration of heat confinement on photothermal sites and fluid cooling on photocatalysis sites at the nanoscale, within a well-designed heat and fluid confinement nanofiber reactor. Photothermal and photocatalytic nanostructures were alternatively aligned in electrospun nanofibers for on-demand nanofluidic thermal management as well as easy folding into 3D structures with enhanced light utilization and mass transfer. Such a design showed simultaneously high photothermal evaporation rate (2.59 kg m-2 h-1, exceeding the limit rate) and efficient photocatalytic upcycling of microplastics pollutant into valued products. Enabled by controlled photothermal heating, the valued main product (i.e., methyl acetate) can be evaporated out with 100% selectivity by in situ separation.

2.
Artigo em Inglês | MEDLINE | ID: mdl-39136725

RESUMO

Ultrafine noble metals have emerged as advanced nanocatalysts in modern society but still suffer from unavoidable sintering at temperatures above 250 °C (e.g., Pt). In this work, closely packed CeO2 grains were confined elegantly in fibrous nanostructures and served as a porous support for stabilizing sub-3 nm Pt clusters. Through precisely manipulating the asymmetry of obtained nanofibers, uneven strain was induced within C-shaped CeO2 nanofibers with tensile strain at the outer side and compressive strain at the inner side. As a result, the enriched oxygen vacancies significantly improved adhesion of Pt to CeO2, thereby boosting the sinter-resistance of ultraclose sub-3 nm Pt clusters. Notably, no aggregation was observed even after exposure to humid air at 750 °C for 12 h, which is far beyond their Tammann temperature (sintering onset temperature, below 250 °C). In situ HAADF-STEM observation revealed a unique sintering mechanism, wherein Pt clusters initially migrate toward the grain boundaries with concentrated stain and undergo slight coalescence, followed by subsequent Ostwald ripening at higher temperatures. Moreover, the sinter-resistant Pt/C-shaped CeO2 effectively catalyzed soot combustion (over 700 °C) in a durable manner. This work provides a new insight for developing sinter-resistant catalysts from the perspective of strain engineering within nano-oxides.

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