A rational synthesis of hierarchically porous, N-doped carbon from Mg-based MOFs: understanding the link between nitrogen content and oxygen reduction electrocatalysis

Eisenberg, David; Stroek, Wowa; Geels, Norbert J.; Tanase, Stéfania; Ferbinţeanu, Marilena; Teat, Simon J.; Mettraux, P.; Yan, Ning; Rothenberg, Gadi

doi:10.1039/c6cp04132a

Cited by 42 publications

(43 citation statements)

References 48 publications

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“…However, metals/metal oxides incorporated in these nanocatalysts vulnerable to aggregation and dissolution in practical fuel cell operation. In this case, metals with low evaporation temperature are used to synthesize MOF precursors, such as Al, Zn and Mg. [43,45,62,63] For example, Zn-containing MOFs (e.g., MOF-5, ZIF-7 and ZIF-8) have been widely used to synthesize metal-free catalysts for ORR. [61] These drawbacks can be overcome by developing metal-free nanocatalysts.…”

Section: Mof-derived Metal-free Nanocatalystsmentioning

confidence: 99%

Metal‐Organic Framework‐Derived Non‐Precious Metal Nanocatalysts for Oxygen Reduction Reaction

Zhu

Song

et al. 2017

Advanced Energy Materials

326

167

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By virtue of diverse structures and tunable properties, metal‐organic frameworks (MOFs) have presented extensive applications including gas capture, energy storage, and catalysis. Recently, synthesis of MOFs and their derived nanomaterials provide an opportunity to obtain competent oxygen reduction reaction (ORR) electrocatalysts due to their large surface area, controllable composition and pore structure. This review starts with the introduction of MOFs and current challenges of ORR, followed by the discussion of MOF‐based non‐precious metal nanocatalysts (metal‐free and metal/metal oxide‐based carbonaceous materials) and their application in ORR electrocatalysis. Current issues in MOF‐derived ORR catalysts and some corresponding strategies in terms of composition and morphology to enhance their electrocatalytic performance are highlighted. In the last section, a perspective for future development of MOFs and their derivatives as catalysts for ORR is discussed.

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Section: Mof-derived Metal-free Nanocatalystsmentioning

confidence: 99%

Metal‐Organic Framework‐Derived Non‐Precious Metal Nanocatalysts for Oxygen Reduction Reaction

Zhu

Song

et al. 2017

Advanced Energy Materials

326

167

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“…Indeed, the mesopore volume rises from 137 to 205 mm 3 g À1 after washing (Table S5). [24][25][26] Thee lectrical wiring of the active sites to the external circuit is linked to the graphitic content of the carbon matrix. [24][25][26] Thee lectrical wiring of the active sites to the external circuit is linked to the graphitic content of the carbon matrix.…”

Section: Angewandte Chemiementioning

confidence: 99%

A Multi‐Doped Electrocatalyst for Efficient Hydrazine Oxidation

et al. 2018

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We report an efficient electrocatalyst for the oxidation of hydrazine,apromising fuel for fuel cells and an important analyte for health and environmental monitoring. To design this material, we emulated natural nitrogen-cycle enzymes,f ocusing on designing ac ooperative,m ulti-doped active site.T he catalytic oxidation occurs on Fe 2 MoC nanoparticles and on edge-positioned nitrogen dopants,a ll welldispersed on ah ierarchically porous,g raphitic carbon matrix that provides active site exposure to mass-transfer and charge flow. The new catalyst is the first carbide with HzOR activity.It operates at the most negative onset potentials reported for carbon-based HzOR catalysts at pH 14 (0.28 Vvs. RHE), and has good-to-excellent activity at pH values down to 0. It shows high faradaic efficiency for oxidation to N 2 (3.6 e À /N 2 H 4 ), and is perfectly stable for at least 2000 cycles. Conflict of interestTheauthors declare no conflict of interest.

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“…For even larger particles (>100 nm), as in the case of our metal oxide on nitrogen‐doped carbon catalysts, the active doughnut volume is smaller still, relative to the particle. Here, the nitrogen‐doped carbon surface is responsible for oxygen activation, while metal oxide particles (such as CoO x and CuO x ) catalyse the alcohol oxidation (see illustration in Figure ). This reaction requires the transfer of two protons from the alcohol to the oxygen.…”

Section: Case Studiesmentioning

confidence: 99%

Cooperative Surface‐Particle Catalysis: The Role of the “Active Doughnut” in Catalytic Oxidation

2018

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We consider the factors that govern the activity of bifunctional catalysts comprised of active particles supported on active surfaces. Such catalysts are interesting because the adsorption and diffusion steps, which are often discounted in “conventional” catalytic scenarios, play a key role here. We present an intuitive model, the so‐called “active doughnut” concept, defining an active catalytic region around the supported particles. This simple model explains the role of adsorption and diffusion steps in cascade catalytic cycles for active particles supported on active surfaces. The concept has two important practical implications. First, the reaction rate is no longer proportional to the number of active sites, but rather to the number of “communicative” active sites—those available to the reaction intermediates during their respective lifetimes. Second, it generates an important testable prediction concerning the dependence of the total reaction rate on the particle size. With these tools at hand, we examine six experimental examples of catalytic oxidation from the literature, and show that the active doughnut concept gives valuable insight even when detailed mechanistic information is hard to come by.

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A rational synthesis of hierarchically porous, N-doped carbon from Mg-based MOFs: understanding the link between nitrogen content and oxygen reduction electrocatalysis

Cited by 42 publications

References 48 publications

Metal‐Organic Framework‐Derived Non‐Precious Metal Nanocatalysts for Oxygen Reduction Reaction

Metal‐Organic Framework‐Derived Non‐Precious Metal Nanocatalysts for Oxygen Reduction Reaction

A Multi‐Doped Electrocatalyst for Efficient Hydrazine Oxidation

Cooperative Surface‐Particle Catalysis: The Role of the “Active Doughnut” in Catalytic Oxidation

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