3D Nitrogen-doped graphene prepared by pyrolysis of graphene oxide with polypyrrole for electrocatalysis of oxygen reduction reaction
TL;DR: In this paper, a low-cost, scalable, synthetic method for preparation of NG via pyrolysis of graphene oxide with a rationally selected N source polypyrrole is presented.
About: This article is published in Nano Energy.The article was published on 2013-03-01. It has received 355 citations till now. The article focuses on the topics: Electrocatalyst & Polypyrrole.
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TL;DR: This paper presents a probabilistic procedure for estimating the polymethine content of carbon dioxide using a straightforward two-step procedure, and shows good results in both the stationary and the liquid phase.
Abstract: Liming Dai,*,†,‡ Yuhua Xue,†,‡ Liangti Qu,* Hyun-Jung Choi, and Jong-Beom Baek* †Center of Advanced Science and Engineering for Carbon (Case4Carbon), Department of Macromolecular Science and Engineering, Case Western Reserve University, 10900 Euclid Avenue, Cleveland, Ohio 44106, United States Key Laboratory of Cluster Science, Ministry of Education of China, Beijing Key Laboratory of Photoelectronic/Electrophotonic Conversion Materials, Department of Chemistry, School of Science, Beijing Institute of Technology, Beijing 100081, People’s Republic of China School of Energy and Chemical Engineering/Center for Dimension-Controllable Covalent Organic Frameworks, Ulsan National Institute of Science and Technology (UNIST), 100 Banyeon, Ulsan, 689-798, South Korea
1,967 citations
TL;DR: The fundamental relationships between electronic structure, adsorption energy, and apparent activity for a wide variety of 2D electrocatalysts are described with the goal of providing a better understanding of these emerging nanomaterials at the atomic level.
Abstract: Over the past few decades, the design and development of advanced electrocatalysts for efficient energy conversion technologies have been subjects of extensive study. With the discovery of graphene, two-dimensional (2D) nanomaterials have emerged as some of the most promising candidates for heterogeneous electrocatalysts due to their unique physical, chemical, and electronic properties. Here, we review 2D-nanomaterial-based electrocatalysts for selected electrocatalytic processes. We first discuss the unique advances in 2D electrocatalysts based on different compositions and functions followed by specific design principles. Following this overview, we discuss various 2D electrocatalysts for electrocatalytic processes involved in the water cycle, carbon cycle, and nitrogen cycle from their fundamental conception to their functional application. We place a significant emphasis on different engineering strategies for 2D nanomaterials and the influence these strategies have on intrinsic material performance, ...
1,363 citations
TL;DR: In this paper, a review article summarizes the very recent efforts in the field of OER electrocatalysis along with the faced challenges and solutions to these challenges also outline with appropriate examples of scientific literatures.
1,121 citations
856 citations
TL;DR: It is reported that nitrogen and sulfur co-doping leads to high catalytic activity of nanoporous graphene in HER at low operating potential, comparable to the best Pt-free HER catalyst, 2D MoS2 .
Abstract: Chemical doping has been demonstrated to be an effective way to realize new functions of graphene as metal-free catalyst in energy-related electrochemical reactions. Although efficient catalysis for the oxygen reduction reaction (ORR) has been achieved with doped graphene, its performance in the hydrogen evolution reaction (HER) is rather poor. In this study we report that nitrogen and sulfur co-doping leads to high catalytic activity of nanoporous graphene in HER at low operating potential, comparable to the best Pt-free HER catalyst, 2D MoS2 . The interplay between the chemical dopants and geometric lattice defects of the nanoporous graphene plays the fundamental role in the superior HER catalysis.
795 citations
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TL;DR: It is reported that vertically aligned nitrogen-containing carbon nanotubes (VA-NCNTs) can act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction in alkaline fuel cells.
Abstract: The large-scale practical application of fuel cells will be difficult to realize if the expensive platinum-based electrocatalysts for oxygen reduction reactions (ORRs) cannot be replaced by other efficient, low-cost, and stable electrodes. Here, we report that vertically aligned nitrogen-containing carbon nanotubes (VA-NCNTs) can act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction in alkaline fuel cells. In air-saturated 0.1 molar potassium hydroxide, we observed a steady-state output potential of –80 millivolts and a current density of 4.1 milliamps per square centimeter at –0.22 volts, compared with –85 millivolts and 1.1 milliamps per square centimeter at –0.20 volts for a platinum-carbon electrode. The incorporation of electron-accepting nitrogen atoms in the conjugated nanotube carbon plane appears to impart a relatively high positive charge density on adjacent carbon atoms. This effect, coupled with aligning the NCNTs, provides a four-electron pathway for the ORR on VA-NCNTs with a superb performance.
6,370 citations
TL;DR: Batteries, fuel cells and supercapacitors belong to the same family of energy conversion devices and are needed to service the wide energy requirements of various devices and systems.
Abstract: Electrochemical energy conversion devices are pervasive in our daily lives. Batteries, fuel cells and supercapacitors belong to the same family of energy conversion devices. They are all based on the fundamentals of electrochemical thermodynamics and kinetics. All three are needed to service the wide energy requirements of various devices and systems. Neither batteries, fuel cells nor electrochemical capacitors, by themselves, can serve all applications.
6,230 citations
TL;DR: The resultant N-graphene was demonstrated to act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction via a four-electron pathway in alkaline fuel cells.
Abstract: Nitrogen-doped graphene (N-graphene) was synthesized by chemical vapor deposition of methane in the presence of ammonia. The resultant N-graphene was demonstrated to act as a metal-free electrode with a much better electrocatalytic activity, long-term operation stability, and tolerance to crossover effect than platinum for oxygen reduction via a four-electron pathway in alkaline fuel cells. To the best of our knowledge, this is the first report on the use of graphene and its derivatives as metal-free catalysts for oxygen reduction. The important role of N-doping to oxygen reduction reaction (ORR) can be applied to various carbon materials for the development of other metal-free efficient ORR catalysts for fuel cell applications, even new catalytic materials for applications beyond fuel cells.
3,604 citations
TL;DR: Electrical measurements show that the N-doped graphene exhibits an n-type behavior, indicating substitutional doping can effectively modulate the electrical properties of graphene.
Abstract: To realize graphene-based electronics, various types of graphene are required; thus, modulation of its electrical properties is of great importance. Theoretic studies show that intentional doping is a promising route for this goal, and the doped graphene might promise fascinating properties and widespread applications. However, there is no experimental example and electrical testing of the substitutionally doped graphene up to date. Here, we synthesize the N-doped graphene by a chemical vapor deposition (CVD) method. We find that most of them are few-layer graphene, although single-layer graphene can be occasionally detected. As doping accompanies with the recombination of carbon atoms into graphene in the CVD process, N atoms can be substitutionally doped into the graphene lattice, which is hard to realize by other synthetic methods. Electrical measurements show that the N-doped graphene exhibits an n-type behavior, indicating substitutional doping can effectively modulate the electrical properties of graphene. Our finding provides a new experimental instance of graphene and would promote the research and applications of graphene.
2,800 citations
TL;DR: In this paper, a microporous carbon-supported iron-based catalysts with active sites believed to contain iron cations coordinated by pyridinic nitrogen functionalities in the interstices of graphitic sheets within the micropores was produced.
Abstract: Iron-based catalysts for the oxygen-reduction reaction in polymer electrolyte membrane fuel cells have been poorly competitive with platinum catalysts, in part because they have a comparatively low number of active sites per unit volume. We produced microporous carbon-supported iron-based catalysts with active sites believed to contain iron cations coordinated by pyridinic nitrogen functionalities in the interstices of graphitic sheets within the micropores. We found that the greatest increase in site density was obtained when a mixture of carbon support, phenanthroline, and ferrous acetate was ball-milled and then pyrolyzed twice, first in argon, then in ammonia. The current density of a cathode made with the best iron-based electrocatalyst reported here can equal that of a platinum-based cathode with a loading of 0.4 milligram of platinum per square centimeter at a cell voltage of >/=0.9 volt.
2,762 citations