Electrochemical oxygen reduction catalysed by Ni3(hexaiminotriphenylene)2

Miner, Elise M.; Fukushima, Tomohiro; Sheberla, Dennis; Sun, Lei; Surendranath, Yogesh; Dincă, Mircea

doi:10.1038/ncomms10942

Cited by 637 publications

(536 citation statements)

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“…ChemSusChem 2017, 10,4374 -4392 www.chemsuschem.org lysts. [116] NiCo-based thin MOF nanosheets, [108] aN iFe MOF array, [109] and an iron-cobalt carboxylate framework (Fe 3 -Co 2 ) [110] exhibit highere lectrocatalytic OER activity than commercial RuO 2 and IrO 2 .T hese examples demonstrate the viability of MOFs as alternatives to precious-metal-based heterogeneous electrocatalysts.…”

Section: Discussionmentioning

confidence: 99%

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Electrocatalytic Metal–Organic Frameworks for Energy Applications

2017

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With the global energy demand expected to increase drastically over the next several decades, the development of a sustainable energy system to meet this increase is paramount. Renewable energy sources can be coupled with electrochemical conversion processes to store energy in chemical bonds. To promote these difficult transformations, electrocatalysts that operate at high conversion rates and efficiency are required. Metal–organic frameworks (MOFs) have emerged as a promising class of materials; however, the insulating nature of MOFs has limited their application as electrocatalysts. The recent development of conductive MOFs has led to several electrocatalytic MOFs that display activity comparable to that of the best‐performing heterogeneous catalysts. Although many electrocatalytic MOFs exhibit low activity and stability, the few successful examples highlight the possibility of MOF electrocatalysts as replacements for noble‐metal‐based catalysts in commercial energy‐converting devices. We review herein the use of pristine MOFs as electrocatalysts to facilitate important energy‐related reactions.

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Section: Discussionmentioning

confidence: 99%

“…[116] ICP-MSa nd atomic absorption spectroscopy (AAS) measurements of the films after potentiostatic measurements revealed the same Ni contentb efore and after electrolysis. XPS after electrolysis showed a + 1.0 eV increase in the bindinge nergy (BE) of the Ni 2p feature.…”

Section: Electrocatalytic Mofs For the Orrmentioning

confidence: 91%

Electrocatalytic Metal–Organic Frameworks for Energy Applications

2017

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“…[280] The polarization curve depicts that an onset potential of 0.82 V (vs RHE) was achieved for Ni 3 (HITP) 2 electrode measured in the O 2 -saturated solution, which is competitive with most of nonprecious metal catalysts. For example, Dinca and coworkers reported a conductive 2D layered MOF, i.e., Ni 3 (2,3, 6,7,10,11-hexaiminotriphenylene (HITP)) 2 , and then used as catalyst for ORR in alkaline electrolyte.…”

Section: Electrocatalysismentioning

confidence: 94%

Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications

et al. 2019

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Low‐dimensional metal–organic frameworks (LD MOFs) have attracted increasing attention in recent years, which successfully combine the unique properties of MOFs, e.g., large surface area, tailorable structure, and uniform cavity, with the distinctive physical and chemical properties of LD nanomaterials, e.g., high aspect ratio, abundant accessible active sites, and flexibility. Significant progress has been made in the morphological and structural regulation of LD MOFs in recent years. It is still of great significance to further explore the synthetic principles and dimensional‐dependent properties of LD MOFs. In this review, recent progress in the synthesis of LD MOF‐based materials and their applications are summarized, with an emphasis on the distinctive advantages of LD MOFs over their bulk counterparties. First, the unique physical and chemical properties of LD MOF‐based materials are briefly introduced. Synthetic strategies of various LD MOFs, including 1D MOFs, 2D MOFs, and LD MOF‐based composites, as well as their derivatives, are then summarized. Furthermore, the potential applications of LD MOF‐based materials in catalysis, energy storage, gas adsorption and separation, and sensing are introduced. Finally, challenges and opportunities of this fascinating research field are proposed.

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“…We previously showed that the electrically conductive MOF Ni 3 (HITP) 2 (HITP = 2,3,6,7,10, (Figure 1) functions as …”

Section: ■ Introductionmentioning

confidence: 99%

Mechanistic Evidence for Ligand-Centered Electrocatalytic Oxygen Reduction with the Conductive MOF Ni₃(hexaiminotriphenylene)₂

et al. 2017

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Establishing catalytic structure−function relationships introduces the ability to optimize the catalyst structure for enhanced activity, selectivity, and durability against reaction conditions and prolonged catalysis. Here we present experimental and computational data elucidating the mechanism for the O 2 reduction reaction with a conductive nickel-based metal−organic framework (MOF). Elucidation of the O 2 reduction electrokinetics, understanding the role of the extended MOF structure in providing catalytic activity, observation of how the redox activity and pK a of the organic ligand influences catalysis, and identification of the catalyst active site yield a detailed O 2 reduction mechanism where the ligand, rather than the metal, plays a central role. More generally, familiarization with how the structural and electronic properties of the MOF influence reactivity may provide deeper insight into the mechanisms by which less structurally defined nonplatinum group metal electrocatalysts reduce O 2 . KEYWORDS: O 2 reduction, electrocatalysis, metal−organic framework, porous catalysts, 2D materials ■ INTRODUCTIONUnderstanding catalytic kinetics and thermodynamics to construct a reasonable reaction mechanism is central for both elucidating the behavior of a given catalyst and gaining predictive power over structure−function relationships. This predictive power aids in efficiently optimizing catalyst performance by systematically tuning the structural and electronic properties of the catalyst. One class of materials that could benefit from mechanism-guided optimization is nonplatinum group metal (non-PGM) electrocatalysts for the O 2 reduction reaction (ORR) to water (4e − reduction) and/or hydrogen peroxide (2e − reduction). Such catalysts typically include abundant transition metals and/or heteroatoms such as N, O, and S doped into a carbonaceous matrix.1−6 Although quite active and stable during ORR, previously reported non-PGM catalysts often consist of amorphous carbon mechanically blended with transition metal macrocycles or other metal and main group heteroatomic sources. These relatively poorly defined materials do not lend themselves to facile mechanistic studies; the inhomogeneous dispersion and irregular orientation of the dopants throughout the carbon matrix engenders structural ambiguity that makes identification, experimental probing, and computational modeling of active sites difficult.Conversely, highly ordered metal−organic frameworks (MOFs) containing well-defined, spatially isolated active sites present an attractive platform for experimental and computational correlation between the chemical and electronic structure of a given catalyst and the electrocatalytic activity and mechanism, a feat that is traditionally restricted to homogeneous molecular systems. We previously showed that the electrically conductive MOF Ni 3 (HITP) 2 (HITP = 2,3,6,7,10, (Figure 1) functions as

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Electrochemical oxygen reduction catalysed by Ni3(hexaiminotriphenylene)2

Cited by 637 publications

References 50 publications

Electrocatalytic Metal–Organic Frameworks for Energy Applications

Electrocatalytic Metal–Organic Frameworks for Energy Applications

Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications

Mechanistic Evidence for Ligand-Centered Electrocatalytic Oxygen Reduction with the Conductive MOF Ni₃(hexaiminotriphenylene)₂

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Electrochemical oxygen reduction catalysed by Ni3(hexaiminotriphenylene)2

Cited by 637 publications

References 50 publications

Electrocatalytic Metal–Organic Frameworks for Energy Applications

Electrocatalytic Metal–Organic Frameworks for Energy Applications

Structural Engineering of Low‐Dimensional Metal–Organic Frameworks: Synthesis, Properties, and Applications

Mechanistic Evidence for Ligand-Centered Electrocatalytic Oxygen Reduction with the Conductive MOF Ni3(hexaiminotriphenylene)2

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Mechanistic Evidence for Ligand-Centered Electrocatalytic Oxygen Reduction with the Conductive MOF Ni₃(hexaiminotriphenylene)₂