Nitrogen-doped carbon materials, including nitrogen-doped carbon nanotubes (NCNTs) and nitrogen-doped graphene (NG), have attracted increasing attention for oxygen reduction reaction (ORR) in metal-air batteries and fuel cell applications, due to their optimal properties including excellent electronic conductivity, 4e − transfer and superb mechanical properties. Here, the recent progress of NCNTs-and NG-based catalysts for ORR is reviewed. Firstly, the general preparation routes of these two N-doped carbon-allotropes are introduced briefly, and then a special emphasis is placed on the developments of both NCNTs and NG as promising metal-free catalysts and/or catalyst support materials for ORR. All these efficient ORR electrocatalysts feature a low cost, high durability and excellent performance, and are thus the key factors in accelerating the widespread commercialization of metal-air battery and fuel cell technologies.
OPEN ACCESSCatalysts 2015, 5 1575
Nanostructures constituted of Pt nanoparticles (NPs) supported on carbon materials are considered to be among the most active oxygen reduction reaction (ORR) catalysts for fuel cells. However, in practice, the usage of such ORR catalysts is limited by their insufficient durability caused by the low physical and chemical stability of Pt NPs during the reaction. We herein present a strategy to synthesize highly durable and active electrocatalysts composed of Pt NPs supported on carbon nanotubes (CNTs) and covered with an ultrathin layer of graphitic carbon. Such hybrid ORR catalysts were obtained by an interfacial in situ polymer encapsulation− graphitization method, where a glucose-containing polymer was grown directly on the surface of Pt/CNTs. The thickness of the carbon-coating layer can be precisely tuned between 0.5 nm and several nanometers by simply programming the polymer growth on Pt/CNTs. The resulting Pt/CNTs@C with a carbon layer thickness of ∼0.8 nm (corresponding to ∼2−3 graphene layers) showed high activity, and excellent durability, with no noticeable activity loss, even after 20 000 cycles of accelerated durability tests. These ultrathin carbon coatings not only act as a protective layer to prevent aggregation of Pt NPs but they also lead to better sample dispersion in solvent which are devoid of aggregates, resulting in a better utilization of Pt. We envision that this polymeric nanoencapsulation strategy is a promising technique for the production of highly active and stable ORR catalysts for fuel cells and metal−air batteries.
Graphene family materials, including graphene quantum dots (GQDs), graphene nanoribbons (GNRs) and 3D graphene (3D-G), have attracted much research interest for the oxygen reduction reaction (ORR) in fuel cells and metal-air batteries, due to their unique structural characteristics, such as abundant activate sites, edge effects and the interconnected network. In this review, we summarize recent developments in fabricating various new graphene family materials and their applications for use as ORR electrocatalysts. These new graphene family materials play an important role in improving the ORR performance, thus promoting the practical use in metal-air batteries and fuel cells.
Nitrogen and phosphorus-codoped graphene dots supported on nitrogen-doped three-dimensional graphene (N, P-GDs/N-3DG) have been synthesized by a facile freeze-annealing process. On the surface of the 3D interconnected porous structure, the N, P-GDs are uniformly dispersed. The as-prepared N, P-GDs/ N-3DG material served as a metal-free catalyst for oxygen reduction reaction (ORR) in an alkaline medium and evaluated by a rotating ring-disk electrode. The N, P-GDs/N-3DG catalyst exhibits excellent ORR activity, which is comparable to that of the commercial Pt/C catalyst. Furthermore, it exhibits a higher tolerance to methanol and better stability than the Pt/C. This enhanced electrochemical catalytic performance can be ascribed to the presence of abundant functional groups and edge defects. This study indicates that P−N bonded structures play a vital role as the active sites in ORR.
The photoelectric
properties of multiferroic double-perovskite Bi2FeCrO6 (BFCO), such as above-band gap photovoltages, switchable
photocurrents, and bulk photovoltaic effects, have recently been explored
for potential applications in solar technology. Here, we report the
fabrication of photoelectrodes based on n-type ferroelectric (FE)
semiconductor BFCO heterojunctions coated with p-type transparent
conducting oxides (TCOs) by pulsed laser deposition and their application
for photoelectrochemical (PEC) water oxidation. The photocatalytic
properties of the bare BFCO photoanodes can be improved by controlling
the FE polarization state. However, the charge recombination as well
as the limited charge transfer kinetics in the photoanode/electrolyte
cause major energy loss and thus hinder the PEC performance. We show
that this problem may be addressed by the deposition of an ultrathin
p-type NiO layer on the photoanode to enhance the charge transport
kinetics and reduce charge recombination at surface-trapped states
for increased surface band bending. A fourfold enhancement of photocurrent
density, up to 0.4 mA cm–2 (at +1.23 V vs RHE),
a best performance of stability over 4 h, and a high incident photon-to-current
efficiency (∼3.7%) were achieved under 1 sun illumination in
such p-NiO/n-BFCO heterojunction photoanodes. These studies reveal the
optimization of PEC performance by polarization switching of BFCO
and the successful achievement of p-TCOs/n-FE heterojunction photoanodes
that are able to sustain water oxidation that is stable for many hours.
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