Chemical and Electrochemical Stability of Nitrogen and Sulphur Doped Mesoporous Carbons

Perazzolo, Valentina; Grądzka, Emilia; Durante, Christian; Pilot, Roberto; Vicentini, Nicola; Rizzi, Gian Andrea; Granozzi, Gaetano; Gennaro, Armando

doi:10.1016/j.electacta.2016.02.025

Cited by 57 publications

(36 citation statements)

References 65 publications

(88 reference statements)

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“…The XPS peaks of carbon, oxygen, nitrogen, and iron were separated into single components by using symmetrical Voigt functions; the χ 2 was minimized by using a nonlinear least squares routine. The sample preparation for XPS analysis was performed as previously reported …”

Section: Methodssupporting

confidence: 90%

“…Among the different available supports, carbon materials represent a versatile platform for Pt NPs loading because they are good electronic conductors, possess good chemical and thermal stability, and can be easily functionalized, and their pore structure and surface area can be opportunely tuned by employing templating agents . The functionalization of the carbon support consists of the introduction of heteroatoms such as nitrogen, boron, phosphorus, and sulfur, a process that is commonly known as doping.…”

Section: Introductionmentioning

confidence: 99%

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Mesoporous Carbon with Different Density of Thiophenic‐Like Functional Groups and Their Effect on Oxygen Reduction

et al. 2019

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The metal–support interactions between sulfur‐doped carbon supports (SMCs) and Pt nanoparticles (NPs) were investigated, aiming at verifying how sulfur functional groups can improve the electrocatalytic performance of Pt NPs towards the oxygen reduction reaction (ORR). SMCs were synthetized, tailoring the density of sulfur functional groups, and Pt NPs were deposited by thermal reduction of Pt(acac)2. The extent of the metal–support interaction was proved by X‐ray photoelectron spectroscopy (XPS) analysis, which revealed a strong electronic interaction, proportional to the density of sulfur defects, whereas XRD spectra provided evidence of higher strain in Pt NPs loaded on SMC. DFT simulations confirmed that the metal–support interaction was strongest in the presence of a high density of sulfur defects. The combination of microstrain and electronic effects resulted in a high catalytic activity of supported Pt NPs towards ORR, with linear correlations of the half‐wave potential E1/2 or the kinetic current jk with the sulfur content in the support. Furthermore, a mass activity value (550 A g−1) well above the United States Department of Energy target of 440 A g−1 at 0.9 V (vs. reversible hydrogen electrode, RHE), was determined.

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Section: Methodssupporting

confidence: 90%

Section: Introductionmentioning

confidence: 99%

Mesoporous Carbon with Different Density of Thiophenic‐Like Functional Groups and Their Effect on Oxygen Reduction

et al. 2019

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“…are the most commonly investigated materials for application in catalysis, and in separation technology . In addition, because of their good conductivity, combined with mechanical, chemical and electrochemical stability, they are widely used in electrocatalysis as well as in energy storage and generation systems . In recent years, there has been a growing interest in the synthesis of porous carbon materials with well controlled and uniform pore sizes, which confer high surface area and large pore volume to the material .…”

Section: Introductionmentioning

confidence: 99%

Nitrogen and Sulfur Doped Mesoporous Carbons, Prepared from Templating Silica, as Interesting Material for Supercapacitors

et al. 2017

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Highly accessible surface area and heteroatom-doping are desired properties for carbon electrode materials to be used in electrochemical supercapacitors. In this paper, nitrogen and sulfur doped carbon materials with wide mesopores (13-14 nm) were synthetized according to a hard template approach by pyrolysis of sucrose, 1,10-phenanthroline or dibenzothiophene as carbon, nitrogen-carbon or sulfur-carbon precursors, respectively. The morphology and dimension of mesopores were induced by sacrificial SiO2 nanoparticles (10-20 nm), which are removed at the end of synthesis by an etching solution to reveal a network of hemispherical pores. The interconnected pore structure was confirmed by scanning electron microscopy and transmission electron microscopy. X-ray photoemission spectroscopy and elemental analysis confirmed the presence of nitrogen and sulfur functional groups. The prepared materials were fully characterized by cyclic voltammetry, chronopotentiometry and electrochemical impedance spectroscopy in 0.5 M H2SO4. Notwithstanding the small surface (200 m2g-1) determined by BET method, the nitrogen doped mesoporous carbon showed high specific gravimetric (∼170 F g-1) and surface (∼835 F m-2) capacitances that are comparable to those of materials with much higher surface area (5-10-fold higher)

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“…CoO/NC catalysts experience substantial weight losses above 250 °C, with the expectation that the Ketjenblack and other carbon materials from PVP and urea are decomposed or thermally oxidized, accompanying breakage of the C−C and C−N bonds . In addition, significant mass losses begin at different temperatures, probably due to the difference in the binding energies or thermal stabilities of the catalysts originating from the different ratios of urea and PVP . It is believed that the nitrogen doping in the carbon structure decreases the thermal stability due to the reduced conjugation of the graphitic structure of NC .…”

Section: Resultsmentioning

confidence: 99%

Enhanced Oxygen Reduction Stability and Activity by Co and N (or O) Interaction in CoO on N‐Doped Carbon Prepared through Spray Pyrolysis

2018

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Although the development of a highly active and cost‐effective electrocatalyst for the oxygen reduction reaction (ORR) is necessary, it is a challenging issue for commercially viable energy conversion applications such as fuel cells or metal‐air batteries. In this study, we synthesize nitrogen‐doped, carbon‐supported CoO catalysts (denoted as CoO/NCs) with high stability and activity. The CoO/NC is prepared by one‐pot spray pyrolysis, which is simple and has an easily scalable synthetic route. In an effort to find a better catalyst composition for ORR activity, several catalysts are synthesized by controlling the concentrations of the solutions that contain carbon, urea as the nitrogen source, and a cobalt precursor. The catalysts are then characterized using various methods to comprehensively study their properties coupled with ORR kinetics and stability. The CoO/NC2 catalyst shows higher catalytic activity towards ORR than the other in‐house prepared catalysts. It is comparable to commercial Pt/C and has very high stability for 80 h in an alkaline medium. Systematic analyses clarify that the superior electrocatalytic performance of CoO/NC2 stems mainly from its enhanced electron density and pathway by heteroatom doping and its modified carbon nature during spray pyrolysis.

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Chemical and Electrochemical Stability of Nitrogen and Sulphur Doped Mesoporous Carbons

Cited by 57 publications

References 65 publications

Mesoporous Carbon with Different Density of Thiophenic‐Like Functional Groups and Their Effect on Oxygen Reduction

Mesoporous Carbon with Different Density of Thiophenic‐Like Functional Groups and Their Effect on Oxygen Reduction

Nitrogen and Sulfur Doped Mesoporous Carbons, Prepared from Templating Silica, as Interesting Material for Supercapacitors

Enhanced Oxygen Reduction Stability and Activity by Co and N (or O) Interaction in CoO on N‐Doped Carbon Prepared through Spray Pyrolysis

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