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1.
Sci Total Environ ; 912: 169342, 2024 Feb 20.
Article in English | MEDLINE | ID: mdl-38123093

ABSTRACT

The substantial production of polyethylene terephthalate (PET) products, coupled with high abandonment rates, results in significant environmental pollution and resource wastage. This has prompted global attention to the development of rational strategies for PET waste treatment. In the context of renewability and sustainability, catalytic chemical technology provides an effective means to recycle and upcycle PET waste into valuable resources. In this review, we initially provide an overview of strategies employed in the thermocatalytic process to recycle PET waste into valuable carbon materials, fuels and typical refined chemicals. The effect of catalysts on the quality and quantity of specific products is highlighted. Next, we introduce the development of renewable-energy-driven electrocatalytic and photocatalytic systems for sustainable PET waste upcycling, focusing on rational catalysts, innovative catalytic system design, and corresponding underlying catalytic mechanisms. Moreover, we discuss advantages and disadvantages of three chemical catalytic strategies. Finally, existing limitations and outlook toward controllable selectivity and yield enhancement of value-added products and PET upvaluing technology for scale-up applications are proposed. This review aims to inspire the exploration of waste-to-treasure technologies for renewable-energy-driven waste management toward a circular economy.

2.
Adv Mater ; 35(41): e2304130, 2023 Oct.
Article in English | MEDLINE | ID: mdl-37403556

ABSTRACT

The selective hydrogenation of alkynes is an important reaction; however, the catalytic activity and selectivity in this reaction are generally conflicting. In this study, ultrafine Pd nanoparticles (NPs) loaded on a graphite-like C3 N4 structure with nitrogen defects (Pd/DCN) are synthesized. The resulting Pd/DCN exhibits excellent photocatalytic performance in the transfer hydrogenation of alkynes with ammonia borane. The reaction rate and selectivity of Pd/DCN are superior to those of Pd/BCN (bulk C3 N4 without nitrogen defects) under visible-light irradiation. The characterization results and density functional theory calculations show that the Mott-Schottky effect in Pd/DCN can change the electronic density of the Pd NPs, and thus enhances the hydrogenation selectivity toward phenylacetylene. After 1 h, the hydrogenation selectivity of Pd/DCN reaches 95%, surpassing that of Pd/BCN (83%). Meanwhile, nitrogen defects in the supports improve the visible-light response and accelerate the transfer and separation of photogenerated charges to enhance the catalytic activity of Pd/DCN. Therefore, Pd/DCN exhibits higher efficiency under visible light, with a turnover frequency (TOF) of 2002 min-1 . This TOF is five times that of Pd/DCN under dark conditions and 1.5 times that of Pd/BCN. This study provides new insights into the rational design of high-performance photocatalytic transfer hydrogenation catalysts.

3.
Phys Rev Lett ; 122(1): 016804, 2019 Jan 11.
Article in English | MEDLINE | ID: mdl-31012640

ABSTRACT

Distinct from all the existing methods for determining the spin Hall angle with bilayers, we have developed a new approach based on the mesoscopic H-shaped structure, which generates and detects pure spin current in a single metal. Using this approach we have unequivocally addressed the long-standing controversy of the magnitude of the spin Hall angle of gold. By exploiting the long spin diffusion length of Cu and the large spin-orbit coupling of Bi, we have realized a very large spin Hall effect in 10 nm Cu films delta doped with 0.15 nm of Bi. This new artificial material can generate a large spin-orbit torque to switch an adjacent Fe layer. We have thus demonstrated new artificial materials with a simultaneously large spin Hall angle and long spin diffusion length.

4.
Sci Adv ; 3(3): e1602579, 2017 Mar.
Article in English | MEDLINE | ID: mdl-28435865

ABSTRACT

Superconductivity that spontaneously breaks time-reversal symmetry (TRS) has been found, so far, only in a handful of three-dimensional (3D) crystals with bulk inversion symmetry. We report an observation of spontaneous TRS breaking in a 2D superconducting system without inversion symmetry: the epitaxial bilayer films of bismuth and nickel. The evidence comes from the onset of the polar Kerr effect at the superconducting transition in the absence of an external magnetic field, detected by the ultrasensitive loop-less fiber-optic Sagnac interferometer. Because of strong spin-orbit interaction and lack of inversion symmetry in a Bi/Ni bilayer, superconducting pairing cannot be classified as singlet or triplet. We propose a theoretical model where magnetic fluctuations in Ni induce the superconducting pairing of the [Formula: see text] orbital symmetry between the electrons in Bi. In this model, the order parameter spontaneously breaks the TRS and has a nonzero phase winding number around the Fermi surface, thus making it a rare example of a 2D topological superconductor.

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