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1.
Small ; 13(25)2017 07.
Artículo en Inglés | MEDLINE | ID: mdl-28509363

RESUMEN

Obtaining bifunctional electrocatalysts with high activity for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is a main hurdle in the application of rechargeable metal-air batteries. Earth-abundant 3d transition metal-based catalysts have been developed for the OER and ORR; however, most of these are based on oxides, whose insulating nature strongly restricts their catalytic performance. This study describes a metallic Ni-Fe nitride/nitrogen-doped graphene hybrid in which 2D Ni-Fe nitride nanoplates are strongly coupled with the graphene support. Electronic structure of the Ni-Fe nitride is changed by hybridizing with the nitrogen-doped graphene. The unique heterostructure of this hybrid catalyst results in very high OER activity with the lowest onset overpotential (150 mV) reported, and good ORR activity comparable to that for commercial Pt/C. The high activity and durability of this bifunctional catalyst are also confirmed in rechargeable zinc-air batteries that are stable for 180 cycles with an overall overpotential of only 0.77 V at 10 mA-2 .

2.
ChemSusChem ; 16(4): e202201639, 2023 Feb 20.
Artículo en Inglés | MEDLINE | ID: mdl-36504341

RESUMEN

As part of the concerted effort for development of energy storage technologies, dual-ion batteries (DIBs) or dual-carbon batteries (DCBs) are attracting interest, owing primarily to their eco-friendly active materials. The use of carbon as the active materials of DCBs brings about several challenges involving capacity and stability. This contribution aims to provide an in-depth understanding of the structural and electronic properties of Ge-doped graphene (Germagraphene) as a novel cathode material for DCBs. Density functional theory (DFT) calculations are combined with the effective screening medium (ESM) method for analyzing the electronic and band structure of PF6 - anion-adsorbed Germagraphene under a potential bias. These theoretical investigations indicate that the use of Ge as a dopant for graphene has a positive impact on the adsorption of the anion on the cathode under both neutral and electrically biased conditions.

3.
J Phys Chem Lett ; 10(11): 2998-3005, 2019 Jun 06.
Artículo en Inglés | MEDLINE | ID: mdl-31095396

RESUMEN

Solar water splitting to produce hydrogen is a promising solution for global energy issues. One of the main bottlenecks in this technology is the spontaneous fast backward reaction (2H2 + O2 → H2O, Δ G < 0), limiting the solar energy conversion efficiency. How to suppress backward reaction is vitally important but rarely reported. Here we found that single-electron-trapped oxygen vacancy (Vo·) can suppress spontaneous backward reaction in pure water splitting. Taking WO3·0.33H2O catalyst as an example, ultrathin WO3·0.33H2O {100} facets with large amount of surface Vo· realized a continuous H2 evolution from pure water splitting with a productivity of 9.9 µmol/g·h without the assistance of any sacrifice agent and noble metal cocatalyst. Quantum chemical calculations revealed that the backward-reaction suppression ability of Vo· is attributed to the high concentration of localized electrons around Vo·, stimulating unidirectional simultaneous water dissociation into H and OH under light irradiation.

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