Metal–organic framework-induced construction of actiniae-like carbon nanotube assembly as advanced multifunctional electrocatalysts for overall water splitting and Zn-air batteries
TL;DR: In this article, a novel and simple MOF-induced strategy is developed to construct three-dimensional actiniae-like carbon nanotube assembly (3D-CNTA) as effective and low-cost multifunctional electrocatalysts for overall water splitting and Zn-air batteries.
About: This article is published in Nano Energy.The article was published on 2017-09-01. It has received 232 citations till now. The article focuses on the topics: Carbon nanotube & Water splitting.
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TL;DR: A wide range of applications based on these materials for ORR, OER, HER and multifunctional electrocatalysis are discussed, with an emphasis on the required features of MOF-derived carbon-based materials for the Electrocatalysis of corresponding reactions.
Abstract: Oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are three key reactions for the development of green and sustainable energy systems. Efficient electrocatalysts for these reactions are highly desired to lower their overpotentials and promote practical applications of related energy devices. Metal–organic frameworks (MOFs) have recently emerged as precursors to fabricate carbon-based electrocatalysts with high electrical conductivity and uniformly distributed active sites. In this review, the current progress of MOF-derived carbon-based materials for ORR/OER/HER electrocatalysis is presented. Materials design strategies of MOF-derived carbon-based materials are firstly summarized to show the rich possibilities of the morphology and composition of MOF-derived carbon-based materials. A wide range of applications based on these materials for ORR, OER, HER and multifunctional electrocatalysis are discussed, with an emphasis on the required features of MOF-derived carbon-based materials for the electrocatalysis of corresponding reactions. Finally, perspectives on the development of MOF-derived carbon-based materials for ORR, OER and HER electrocatalysis are provided.
970 citations
TL;DR: In this paper, a spontaneous gas-foaming method was used to prepare nitrogen doped ultrathin carbon nanosheets (NCNs) by simply pyrolysing a mixture of citric acid and NH4Cl.
Abstract: Rational design and facile preparation of non-noble trifunctional electrocatalysts with high performance, low cost and strong durability for the oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) are highly demanded, but remain as a big challenge. Herein, we report a spontaneous gas-foaming method to prepare nitrogen doped ultrathin carbon nanosheets (NCNs) by simply pyrolysing a mixture of citric acid and NH4Cl. Under the optimized pyrolysis temperature (carbonized at 1000 °C) and mass ratio of precursors (1 : 1), the synthesized NCN-1000-5 sample possesses an ultrathin sheet structure, an ultrahigh specific surface area (1793 m2 g−1), and rich edge defects, and exhibits low overpotential and robust stability for the ORR, OER and HER. By means of density functional theory (DFT) computations, we revealed that the intrinsic active sites for the ORR, OER and HER are the carbon atoms located at the armchair edge and adjacent to the graphitic N dopants. When practically used as a catalyst in rechargeable Zn–air batteries, a high energy density (806 W h kg−1), a low charge/discharge voltage gap (0.77 V) and an ultralong cycle life (over 330 h) were obtained at 10 mA cm−2 for NCN-1000-5. This work not only presents a versatile strategy to develop advanced carbon materials with ultrahigh specific surface area and abundant edge defects, but also provides useful guidance for designing and developing multifunctional metal-free catalysts for various energy-related electrocatalytic reactions.
955 citations
TL;DR: This work has prepared a series of Fe/Ni-based trimetallic MOFs (Fe/Ni/Co(Mn)-MIL-53 accordingly to the Material of Institute Lavoisier) by solvothermal synthesis, which can be directly adopted as highly efficient electrocatalysts.
Abstract: Metal-organic frameworks (MOFs) are a class of promising materials for diverse catalysis, but they are usually not directly employed for oxygen evolution electrocatalysis. Most reports focus on using MOFs as templates to in-situ create efficient electrocatalysts via annealing. Herein, we prepared a series of Fe/Ni/-based trimetallic MOFs (Fe/Ni/Co(Mn)-Material of Institute Lavoisier (MIL-53)) by solvothermal synthesis, which can be directly adopted as electrocatalysts. It was revealed that the Fe/Ni/Co(Mn)-MIL-53 exhibited volcano-type oxygen evolution reaction (OER) activity as a function of compositions. The optimized Fe/Ni2.4/Co0.4-MIL-53 can reach the current density of 20 mA*cm-2 at low overpotential of 236 mV with small Tafel slope of 52.2 mV*dec-1. The OER performance of these MOFs can be further enhanced by directly being grown on nickel foam (NF), in which the optimized Fe/Ni/Mn0.4-MIL-53/NF exhibits low overpotential of 290 mV at 500 mA*cm-2 as well as high durability.
524 citations
01 May 2020
TL;DR: In this paper, the authors present a critical overview on the recent progress of the use of MOF-based materials for gaseous fuel storage, chemical hydrogen storage, solar and electrochemical energy storage and conversion.
Abstract: Metal–organic frameworks (MOFs), an emerging class of porous materials, have shown intriguing and promising properties in a wide range of applications due to their versatile structures, large surface areas, tunable porosity and tailorable chemistry. In recent years one of the most active research fields is to explore energy applications of MOF-based materials. In this review, we present a critical overview on the recent progress of the use of MOF-based materials for gaseous fuel storage, chemical hydrogen storage, solar and electrochemical energy storage and conversion. The challenges and opportunities towards advanced energy technologies with the MOF-based materials are discussed.
516 citations
TL;DR: In this article, a multilevel architecture optimization of Co-based nanoparticles (NPs) embedded in hollow N-doped carbon polyhedra for boosting the ORR and OER was reported.
Abstract: Emerging clean energy technologies such as regenerative fuel cells and rechargeable metal–air batteries have attracted increasing global interest because of their high efficiency and environmental benignity, but the lack of highly active bifunctional electrocatalysts at low cost for both oxygen reduction and evolution reactions (ORR and OER) greatly hinders their commercial applications. Here, we report the multilevel architecture optimization of Co-based nanoparticles (NPs) embedded in hollow N-doped carbon polyhedra for boosting the ORR and OER, which are fabricated by a two-step pyrolysis–oxidation strategy with a Co-based MOF (ZIF-67) as precursor. The key for this strategy lies in the precise and effective control of the oxidation processes of Co NPs, which enables the synthesis of a series of Co–Co3O4-based nanoarchitectures that are embedded in hollow nitrogen-doped carbon polyhedra (HNCP), including core–shell Co/Co3O4, yolk@shell Co@Co3O4, and hollow Co3O4 NPs. Benefiting from its abundant oxygen...
359 citations
References
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TL;DR: This work shows that graphene's electronic structure is captured in its Raman spectrum that clearly evolves with the number of layers, and allows unambiguous, high-throughput, nondestructive identification of graphene layers, which is critically lacking in this emerging research area.
Abstract: Graphene is the two-dimensional building block for carbon allotropes of every other dimensionality We show that its electronic structure is captured in its Raman spectrum that clearly evolves with the number of layers The D peak second order changes in shape, width, and position for an increasing number of layers, reflecting the change in the electron bands via a double resonant Raman process The G peak slightly down-shifts This allows unambiguous, high-throughput, nondestructive identification of graphene layers, which is critically lacking in this emerging research area
13,474 citations
TL;DR: Taking the step towards successful commercialization requires oxygen reduction electrocatalysts that meet exacting performance targets, and these catalyst systems will need to be highly durable, fault-tolerant and amenable to high-volume production with high yields and exceptional quality.
Abstract: Fuel cells powered by hydrogen from secure and renewable sources are the ideal solution for non-polluting vehicles, and extensive research and development on all aspects of this technology over the past fifteen years has delivered prototype cars with impressive performances. But taking the step towards successful commercialization requires oxygen reduction electrocatalysts--crucial components at the heart of fuel cells--that meet exacting performance targets. In addition, these catalyst systems will need to be highly durable, fault-tolerant and amenable to high-volume production with high yields and exceptional quality. Not all the catalyst approaches currently being pursued will meet those demands.
4,538 citations
TL;DR: This review highlights the recent research efforts toward the synthesis of noble metal-free electrocatalysts, especially at the nanoscale, and their catalytic properties for the hydrogen evolution reaction (HER), and summarizes some important examples showing that non-Pt HER electrocatsalysts could serve as efficient cocatalysts for promoting direct solar-to-hydrogen conversion in both photochemical and photoelectrochemical water splitting systems, when combined with suitable semiconductor photocatalyst.
Abstract: Sustainable hydrogen production is an essential prerequisite of a future hydrogen economy. Water electrolysis driven by renewable resource-derived electricity and direct solar-to-hydrogen conversion based on photochemical and photoelectrochemical water splitting are promising pathways for sustainable hydrogen production. All these techniques require, among many things, highly active noble metal-free hydrogen evolution catalysts to make the water splitting process more energy-efficient and economical. In this review, we highlight the recent research efforts toward the synthesis of noble metal-free electrocatalysts, especially at the nanoscale, and their catalytic properties for the hydrogen evolution reaction (HER). We review several important kinds of heterogeneous non-precious metal electrocatalysts, including metal sulfides, metal selenides, metal carbides, metal nitrides, metal phosphides, and heteroatom-doped nanocarbons. In the discussion, emphasis is given to the synthetic methods of these HER electrocatalysts, the strategies of performance improvement, and the structure/composition-catalytic activity relationship. We also summarize some important examples showing that non-Pt HER electrocatalysts could serve as efficient cocatalysts for promoting direct solar-to-hydrogen conversion in both photochemical and photoelectrochemical water splitting systems, when combined with suitable semiconductor photocatalysts.
4,351 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: In this paper, the oxygen reduction reaction (ORR) active site was characterized by using newly designed graphite (highly oriented pyrolitic graphite) model catalysts with well-defined π conjugation and well-controlled doping of N species.
Abstract: Nitrogen (N)-doped carbon materials exhibit high electrocatalytic activity for the oxygen reduction reaction (ORR), which is essential for several renewable energy systems. However, the ORR active site (or sites) is unclear, which retards further developments of high-performance catalysts. Here, we characterized the ORR active site by using newly designed graphite (highly oriented pyrolitic graphite) model catalysts with well-defined π conjugation and well-controlled doping of N species. The ORR active site is created by pyridinic N. Carbon dioxide adsorption experiments indicated that pyridinic N also creates Lewis basic sites. The specific activities per pyridinic N in the HOPG model catalysts are comparable with those of N-doped graphene powder catalysts. Thus, the ORR active sites in N-doped carbon materials are carbon atoms with Lewis basicity next to pyridinic N.
3,201 citations