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1.
ACS Catal ; 13(15): 10457-10467, 2023 Aug 04.
Artículo en Inglés | MEDLINE | ID: mdl-37564127

RESUMEN

Copper-based hydrogen evolution electrocatalysts are promising materials to scale-up hydrogen production due to their reported high current densities; however, electrode durability remains a challenge. Here, we report a facile, cost-effective, and scalable synthetic route to produce Cu2-xS electrocatalysts, exhibiting hydrogen evolution rates that increase for ∼1 month of operation. Our Cu2-xS electrodes reach a state-of-the-art performance of ∼400 mA cm-2 at -1 V vs RHE under mild conditions (pH 8.6), with almost 100% Faradaic efficiency for hydrogen evolution. The rise in current density was found to scale with the electrode electrochemically active surface area. The increased performance of our Cu2-xS electrodes correlates with a decrease in the Tafel slope, while analyses by X-ray photoemission spectroscopy, operando X-ray diffraction, and in situ spectroelectrochemistry cooperatively revealed the Cu-centered nature of the catalytically active species. These results allowed us to increase fundamental understanding of heterogeneous electrocatalyst transformation and consequent structure-activity relationship. This facile synthesis of highly durable and efficient Cu2-xS electrocatalysts enables the development of competitive electrodes for hydrogen evolution under mild pH conditions.

2.
Environ Technol ; 43(13): 1988-2001, 2022 May.
Artículo en Inglés | MEDLINE | ID: mdl-33308050

RESUMEN

Acid mine drainage (AMD) is the major effluent generated from metal and coal mines, causing serious ecological risks and degradation of aquatic habitats and surrounding soil quality. Biochemical passive reactors (BPRs) are an option for improving AMD affected water. This study investigates the effect of the size and concentration of zerovalent iron nanoparticles (nZVI) on the efficiency of batch BPRs during AMD remediation. Atomic force microscopy (AFM) and transmission electron microscopy (TEM) were also used as complementary techniques for the investigation of the changes in microbial cells and nZVI properties after the AMD remediation. The results from the batch experiment showed that the concentration of nZVI increases the pH and decreases ORP during AMD treatment, thus favouring the removal of metals. The results also suggest that metal sulfide precipitation occurred in all the batch with reactive mixture but was greater in reactors amended with nZVI of larger size. This study revealed that the presence of nZVI in the BPR leads to metal removal as well as the inhibition of sulfate-reducing bacteria (SRB) activity. Microscopy study indicated that the addition of nZVI creates a morphological change on certain microorganisms in which the cellular membrane was fully covered with nZVI, inducing cell lysis process. These results show that nZVI is a promising reactive material for the treatment of AMD in BPR systems.


Asunto(s)
Nanopartículas , Contaminantes Químicos del Agua , Ácidos/química , Hierro/química , Metales , Minería , Contaminantes Químicos del Agua/química
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