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1.
Small ; : e2309252, 2024 Jan 12.
Artículo en Inglés | MEDLINE | ID: mdl-38217311

RESUMEN

The energy transition to renewables necessitates innovative storage solutions beyond the capacities of lithium-ion batteries. Aluminum-ion batteries (AIBs), particularly their aqueous variants (AAIBs), have emerged as potential successors due to their abundant resources, electrochemical advantages, and eco-friendliness. However, they grapple with achieving their theoretical voltage potential, often yielding less than expected. This perspective article provides a comprehensive examination of the voltage challenges faced by AAIBs, attributing gaps to factors such as the aluminum reduction potential, hydrogen evolution reaction, and aluminum's inherent passivation. Through a critical exploration of methodologies, strategies, such as underpotential deposition, alloying, interface enhancements, tailored electrolyte compositions, and advanced cathode design, are proposed. This piece seeks to guide researchers in harnessing the full potential of AAIBs in the global energy storage landscape.

2.
Chem Sci ; 15(21): 8204-8215, 2024 May 29.
Artículo en Inglés | MEDLINE | ID: mdl-38817556

RESUMEN

Electrocatalytic nitrate (NO3-) reduction reaction (eNO3-RR) to ammonia under ambient conditions is deemed a sustainable route for wastewater treatment and a promising alternative to the Haber-Bosch process. However, there is still a lack of efficient electrocatalysts to achieve high NH3 production performance at wastewater-relevant low NO3- concentrations. Herein, we report a Pd74Ru26 bimetallic nanocrystal (NC) electrocatalyst capable of exhibiting an average NH3 FE of ∼100% over a wide potential window from 0.1 to -0.3 V (vs. reversible hydrogen electrode, RHE) at a low NO3- concentration of 32.3 mM. The average NH3 yield rate at -0.3 V can reach 16.20 mg h-1 cm-2. Meanwhile, Pd74Ru26 also demonstrates excellent electrocatalytic stability for over 110 h. Experimental investigations and density functional theory (DFT) calculations suggest that the electronic structure modulation between Pd and Ru favors the optimization of NO3- transport with respect to single components. Along the *NO3 reduction pathway, the synergy between Pd and Ru can also lower the energy barrier of the rate-determining steps (RDSs) on Ru and Pd, which are the protonation of *NO2 and *NO, respectively. Finally, this unique alloying design achieves a high-level dynamic equilibrium of adsorption and coupling between *H and various nitrogen intermediates during eNO3-RR.

3.
ACS Nano ; 17(23): 23637-23648, 2023 Dec 12.
Artículo en Inglés | MEDLINE | ID: mdl-37979042

RESUMEN

Electrocatalytic nitrate (NO3-)/nitrite (NO2-) reduction reaction (eNOx-RR) to ammonia under ambient conditions presents a green and promising alternative to the Haber-Bosch process. Practically available NOx- sources, such as wastewater or plasma-enabled nitrogen oxidation reaction (p-NOR), typically have low NOx- concentrations. Hence, electrocatalyst engineering is important for practical eNOx-RR to obtain both high NH3 Faradaic efficiency (FE) and high yield rate. Herein, we designed balanced NOx- and proton adsorption by properly introducing Cu sites into the Fe/Fe2O3 electrocatalyst. During the eNOx-RR process, the H adsorption is balanced, and the good NOx- affinity is maintained. As a consequence, the designed Cu-Fe/Fe2O3 catalyst exhibits promising performance, with an average NH3 FE of ∼98% and an average NH3 yield rate of 15.66 mg h-1 cm-2 under the low NO3- concentration (32.3 mM) of typical industrial wastewater at an applied potential of -0.6 V versus reversible hydrogen electrode (RHE). With low-power direct current p-NOR generated NOx- (23.5 mM) in KOH electrolyte, the Cu-Fe/Fe2O3 catalyst achieves an FE of ∼99% and a yield rate of 15.1 mg h-1 cm-2 for NH3 production at -0.5 V (vs RHE). The performance achieved in this study exceeds industrialization targets for NH3 production by exploiting two available low-concentration NOx- sources.

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