Investigation of Oxygen Reduction Activity of Catalysts Derived from Co and Co/Zn Methyl‐Imidazolate Frameworks in Proton Exchange Membrane Fuel Cells

Chong, Lina; Goenaga, Gabriel A.; Williams, Kia; Barkholtz, Heather M.; Grabstanowicz, Lauren R.; Brooksbank, Jeremy; Papandrew, Alexander B.; Elzein, Radwan; Schlaf, Rudiger; Zawodzinski, Thomas A.; Zou, Jianxin; Ma, Shengqian; Liu, Di-Jia

doi:10.1002/celc.201600163

Cited by 50 publications

(28 citation statements)

References 25 publications

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“…In addition to the Co@NC core–shell architectures, presence of both M–N–C and M–N active sites (CoN x C y and CoN x species), as observed from XPS analysis (Figure d), is also responsible factors for the enhanced ORR activity of Co@NC–MOF–2–900 catalyst . In view of the durability of Co@NC–MOF–2–900 electrocatalyst, N‐doped carbon shells greatly protect the Co nanoparticles, and hence preserve them from leaching out under highly oxidative alkaline and acidic environments . Though isolating the effect of individual factors responsible for the enhanced ORR activity is not possible at this stage, we believe that the synergistic effect of all factors are responsible for the ORR activity and excellent durability of Co@NC–MOF–2–900 electrocatalyst.…”

Section: Resultsmentioning

confidence: 95%

Sustainable Synthesis of Co@NC Core Shell Nanostructures from Metal Organic Frameworks via Mechanochemical Coordination Self‐Assembly: An Efficient Electrocatalyst for Oxygen Reduction Reaction

Peera

Balamurugan

Lee

2018

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Herein, a new type of cobalt encapsulated nitrogen-doped carbon (Co@NC) nanostructure employing Zn Co (C H N ) metal-organic framework (MOF) as precursor is developed, by a simple, ecofriendly, solvent-free approach that utilizes a mechanochemical coordination self-assembly strategy. Possible evolution of Zn Co (C H N ) MOF structures and their conversion to Co@NC nanostructures is established from an X-ray diffraction technique and transmission electron microscopy analysis, which reveal that MOF-derived Co@NC core-shell nanostructures are well ordered and highly crystalline in nature. Co@NC-MOF core-shell nanostructures show excellent catalytic activity for the oxygen reduction reaction (ORR), with onset potential of 0.97 V and half-wave potential of 0.88 V versus relative hydrogen electrode in alkaline electrolyte, and excellent durability with zero degradation after 5000 potential cycles; whereas under similar experimental conditions, the commonly utilized Pt/C electrocatalyst degrades. The Co@NC-MOF electrocatalyst also shows excellent tolerance to methanol, unlike the Pt/C electrocatalyst. X-ray photoelectron spectroscopy (XPS) analysis shows the presence of ORR active pyridinic-N and graphitic-N species, along with CoN C and CoN ORR active (M-N-C) sites. Enhanced electron transfer kinetics from nitrogen-doped carbon shell to core Co nanoparticles, the existence of M-N-C active sites, and protective NC shells are responsible for high ORR activity and durability of the Co@NC-MOF electrocatalyst.

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Section: Resultsmentioning

confidence: 95%

Sustainable Synthesis of Co@NC Core Shell Nanostructures from Metal Organic Frameworks via Mechanochemical Coordination Self‐Assembly: An Efficient Electrocatalyst for Oxygen Reduction Reaction

Peera

Balamurugan

Lee

2018

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“…Apart from highly electrical conductive nanocarbon supports, non-carbon supports were also studied to template MOF crystals for catalyst preparation. Co/Zn-ZIF crystals are arrayed onto the surface of cobalt aluminum layered double hyroxide (CoAl-LDH) microplates to assemble two dimensional MOF hybrid precursors (Figure 13) [100,112]. Reprinted with permission from Ref.…”

Section: Non-carbon Templatesmentioning

confidence: 99%

Engineering nanostructures of PGM-free oxygen-reduction catalysts using metal-organic frameworks

et al. 2017

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Oxygen reduction reaction (ORR) is one of the essential electrochemical reactions for the energy conversion and storage devices such as fuel cells and metal-air batteries. However, a large amount of Pt is required for catalyzing the kinetically sluggish ORR at the air cathode, therefore greatly limiting their large scale implementation. Development of high-performance platinum group-metal (PGM)-free ORR catalysts has been a long-term goal for such clean energy technologies. However, current PGM-free catalysts are still significantly suffering from insufficient activity and limited durability especially in more challenging acidic media, such as proton exchange membranes (PEM) fuel cells. Recently, metal-organic frameworks (MOFs), constructed from bridging metal ions and ligands, have emerged as a new type of attractive precursors for the synthesis of PGM-free catalysts, which has led to encouraging performance improvement. Compared to other catalyst precursors, MOFs have well-defined crystal structure with tunable chemistry and contain all required elements (e.g., carbon, nitrogen, and metal). Here, we provide an account of recent innovative PGM-free catalyst design and synthesis derived from the unique MOF precursors with special emphasis on engineering nanostructure and morphology of catalysts. We aim to provide new insights into the design and synthesis of advanced PGM-free

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“…Bimetallic (Co/Zn) ZIF precursor‐based Co−N−C catalyst derived utilizing Pluronic F‐127 surfactant (Co−N−C@F‐127) showed j l of ∼−3.9 mA cm −2 [6a] . Another bimetallic ZIF precursor derived Co−N−C catalyst achieved after post acid‐washing (Co/Zn(mIm) 2 ‐P) exhibited j l of ∼−4.8 mA cm −2 utilizing two heat treatment process under Ar and NH 3 atmosphere [38] . These comparisons demonstrate the efficacy and simplicity of the employed synthesis route utilizing dual ZIF precursor approach without usage of any additional surfactant, template and/or post acid‐treatment steps to prepare high performing CoNC catalyst.…”

Section: Resultsmentioning

confidence: 99%

Robust Co‐Embedded Nitrogen Doped Carbon Catalyst for Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cell

Bharti

Natarajan

2021

ChemistrySelect

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This work reports non‐noble, cobalt embedded nitrogen doped carbon (CoNC) catalysts for oxygen reduction reaction (ORR) in Nafion‐based acidic proton exchange membrane fuel cells (PEMFCs). CoNC catalysts are synthesized through direct pyrolysis of two different zeolitic imidazolate framework (ZIF) precursors, Zn‐ZIF and Co‐ZIF. Profiting from two different precursor approach, appropriate assimilation of metal, nitrogen and carbon components is achieved which boosts oxygen reduction. Electrochemical results exemplified CoNC 3–1 catalyst derived from Zn‐ZIF:Co‐ZIF precursor in the weight ratio of 3 : 1 as the better ORR catalyst. CoNC 3–1 catalyst exhibited the highest electrochemical surface area (ECSA) (570 cm2), highest limiting current density (‐5.14 mA cm−2) and followed near 4e− reduction of oxygen revealing superior ORR activity. The catalyst also demonstrated remarkable durability with loss of only 6 % of ECSA after 30,000 cycles of accelerated durability test. The enhanced ORR activity and durability is attributed to optimal balance of Co−Nx active sites along with appropriate N contents and graphitic carbon framework.

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Investigation of Oxygen Reduction Activity of Catalysts Derived from Co and Co/Zn Methyl‐Imidazolate Frameworks in Proton Exchange Membrane Fuel Cells

Abstract: This is the author manuscript accepted for publication and has undergone full peer review but has not been through the copyediting, typesetting, pagination and proofreading process, which may lead to differences between this version and the Version of Record.

Cited by 50 publications

References 25 publications

Sustainable Synthesis of Co@NC Core Shell Nanostructures from Metal Organic Frameworks via Mechanochemical Coordination Self‐Assembly: An Efficient Electrocatalyst for Oxygen Reduction Reaction

Sustainable Synthesis of Co@NC Core Shell Nanostructures from Metal Organic Frameworks via Mechanochemical Coordination Self‐Assembly: An Efficient Electrocatalyst for Oxygen Reduction Reaction

Engineering nanostructures of PGM-free oxygen-reduction catalysts using metal-organic frameworks

Robust Co‐Embedded Nitrogen Doped Carbon Catalyst for Oxygen Reduction Reaction in Proton Exchange Membrane Fuel Cell

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