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1.
ACS Nano ; 12(11): 10764-10771, 2018 Nov 27.
Artigo em Inglês | MEDLINE | ID: mdl-30335961

RESUMO

Hexagonal boron nitride (h-BN) and graphene have emerged as promising materials for proton exchange membranes because of their high proton conductivity and chemical stability. However, the defects and grain boundaries generated during the growth and transfer of two-dimensional materials limit their practical applicability. Here, we report the fabrication of membrane electrode assemblies using large-area single-oriented AA'-stacked trilayer h-BN (3L-BN), which exhibits very few defects during the growth and transfer, as a proton exchange membrane for use in fuel cell systems. The fuel cell based on AA'-stacked 3L-BN showed a H2 permeation current density as low as 2.69 mA cm-2 and an open circuit voltage (OCV) as high as 0.958 V; this performance is much superior to those for cells based on Nafion (3.7 mA cm-2 and 0.942 V, respectively) and single-layer h-BN (10.08 mA cm-2 and 0.894 V, respectively). Furthermore, the fuel cell with the AA'-stacked 3L-BN membrane almost maintained its original performance (OCV, maximum power density, and H2 permeation current density) even after 100 h of an accelerated stress test at 30% RH and 90 °C, while the fuel cells with the Nafion and single-layer BN membranes exhibited severely deteriorated performances. The stability of the cell based on the AA'-stacked 3L-BN membrane was better because the membrane prevented gas crossover and suppressed the generation of reactive radicals during cell operation.

2.
Nanoscale ; 9(22): 7373-7379, 2017 Jun 08.
Artigo em Inglês | MEDLINE | ID: mdl-28405666

RESUMO

In this study, we report self-assembled nitrogen-doped fullerenes (N-fullerene) as non-precious catalysts, which are active for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER), and thus applicable for energy conversion and storage devices such as fuel cells and metal-air battery systems. We screen the best N-fullerene catalyst at the nitrogen doping level of 10 at%, not at the previously known doping level of 5 or 20 at% for graphene. We identify that the compressive surface strain induced by doped nitrogen plays a key role in the fine-tuning of catalytic activity.

3.
Nanoscale ; 6(20): 12111-9, 2014 Oct 21.
Artigo em Inglês | MEDLINE | ID: mdl-25196022

RESUMO

A critical issue for maintaining long-term applications of polymer electrolyte fuel cells (PEFCs) is the development of an innovative technique for the functionalization of a carbon support that preserves their exceptional electrical conductivity and robustly enriches their durability. Here, we report for the first time how the formation of a partially coated, ultrathin, hydrophobic silica layer around the surfaces of the carbon nanofiber (CNF) helps improve the durability of the CNF without decreasing the significant electrical conductivity of the virgin CNF. The synthesis involved the adsorption of polycarbomethylsilane (PS) on the CNF's sidewalls, followed by high temperature pyrolysis of PS, resulting in a highly durable, conductive carbon support in PEFCs. The Pt nanoparticles are in direct contact with the surface of the carbon in the empty spaces between unevenly coated silica layers, which are not deposited directly onto the silica layer. The presence of a Pt nanoparticle layer that was thicker than the silica layer would be a quite advantageous circumstance that provides contact with other neighboring CNFs without having a significant adverse effect that deeply damages the electrical conductivity of the neighboring CNF composites with the silica layer. Furthermore, the ultrathin, hydrophobic silica layer around the surfaces of the CNF provides great potential to reduce the presence of water molecules in the vicinity of the carbon supports and the ˙OH radicals formed on the surface of the Pt catalyst. As a result, the CNF with a 5 wt% silica layer that we prepared has had extremely high initial performance and durability under severe carbon corrosion conditions, starting up with 974 mA cm(-2) at 0.6 V and ending up with more than 58% of the initial performance (i.e., 569 mA cm(-2) at 0.6 V) after a 1.6 V holding test for 6 h. The beginning-of-life and end-of-life performances based on the virgin CNF without the silica layer were 981 and 340 mA cm(-2) at 0.6 V, respectively. The CNF having a silica layer had long-term durability which was superior to that of the virgin CNF.

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