Cobalt Nanoparticles Embedded into N-Doped Carbon from Metal Organic Frameworks as Highly Active Electrocatalyst for Oxygen Evolution Reaction

Lü, Jitao; Zeng, Yue; Ma, Xiumei; Wang, Huiqin; Gao, Linna; Zhong, Hua; Meng, Qingguo

doi:10.3390/polym11050828

Cited by 41 publications

(26 citation statements)

References 49 publications

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“…Zeng et al theoretically predicted that the SACs with a Co-pyrrole-N4 center could efficiently catalyze OER compared with pyridine nitrogen coordination 22 . Lu et al found that cobalt nanoparticles@N-doped carbon composite exhibited a low onset overpotential of 300 mV for OER, which is similar to the performance of reported single-atom Co-N-C catalysts 23 . Therefore, the Co-N-C structure is chosen as an example system in this work to study the structure-activity relationship 12,[24][25][26] .…”

Section: Introductionsupporting

confidence: 63%

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

Wu¹,

Zhang²,

Fu³

et al. 2022

Acta Physico Chimica Sinica

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Understanding the origin of the active site activity in the oxygen evolution reaction (OER) electrocatalysts is key for developing efficient electrocatalysts. However, crucial challenges remain due to the complexity of catalyst structure-activity relationships. Herein, various Co-N-C configurations, including single atoms, diatoms, and clusters, were designed to establish structure-activity relationships by first-principles calculations. It was revealed that the Co-N4 exhibited the best reactivity due to the high coordination number of the metal center and moderate adsorption energies for all reaction intermediates. The diatom and cluster activities originate from the highly coordinated structures formed with reaction intermediates, which serve as coordination ligands. Furthermore, other factors influencing the OER activity based on the Co-N4 configuration are discussed. For example, the weak metal-metal interaction can further optimize the adsorption of oxygen-containing intermediates by tuning antibonding energy levels of Co-O. Subsequently, an ultralow overpotential of 0.23 V for the OER in CoNi-type4 systems can be obtained by extrapolation of the volcano plot derived from the established structure-adsorption-activity relationships. This work uncovers the underlying OER activity mechanisms of Co-N-C catalysts, which helps to further understanding of high-performance of M-N-C base catalysts and will aid in the future design of high-efficiency OER catalysts.

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Section: Introductionsupporting

confidence: 63%

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

Wu¹,

Zhang²,

Fu³

et al. 2022

Acta Physico Chimica Sinica

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“…At present, proper regulation of the chemical composition is one effective approach to improve the electrocatalytic activity toward HER. − Bimetal (M–Mo, M = Co and Ni) sulfide hybrids have richer active sites because of chemical environment changes compared with single-metal sulfide compositions. , What’s more, by reconfiguring electronic structure of MoS 2 , designing Co–Mo–S based hybrid electrocatalysts could provide synergistic advantages to enhance the reaction rate of the Volmer step and promote the electrocatalytic process from kinetic aspects. In the meantime, Co sites have an optimum binding strength for H 2 O, which could effectively bind and dissociate H 2 O species. , The Mo site has superior generation and adsorption capabilities toward H ads , which could facilitate H ads reactions in the electrolyte and accelerate the hydrogen release process .…”

Section: Introductionmentioning

confidence: 99%

Defect-Rich Porous CoS_1.097/MoS₂ Hybrid Microspheres as Electrocatalysts for pH-Universal Hydrogen Evolution

Sun

Huang

et al. 2019

ACS Appl. Energy Mater.

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As a clean and promising hydrogen production process, the electrochemical hydrogen evolution reaction (HER) is particularly important. However, its electrocatalytic activity is usually limited by the acid or base environment of the electrolyte. To achieve efficient conversion in energy storage, developing cost-effective nonprecious HER electrocatalysts at all pH values is highly required. Herein, defect-rich porous CoS 1.097 /MoS 2 hybrid microspheres are synthesized via a one-step sulfurization method. As expected, the optimal pH-universal CoS 1.097 /MoS 2 HER electrocatalyst shows overpotentials of 228, 249, and 341 mV at −10 mA cm −2 and small Tafel slopes of 59, 75, and 85 mV dec −1 in 0.5 M H 2 SO 4 , 1.0 M KOH, and 0.1 M PBS electrolyte, respectively. Furthermore, the CoS 1.097 /MoS 2 also presents outstanding HER catalytic stability in a 21 h stability test. The outstanding performance of CoS 1.097 /MoS 2 can be ascribed to the synergetic interplay of CoS 1.097 and MoS 2 , with abundant defects and a hierarchically ordered interconnected micro/mesoporous structure.

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“…The peaks at 284.7, 285.5, 286.1, 288.0, 289.1, and 290.5 eV in the C 1 s XPS spectra corresponded to sp 2 –C, sp 3 –C, C–O, CO, OC–O, and π–π* transition, respectively, whereas those at 530.3, 532.0, and 532.8 eV in the O 1 s XP spectra corresponded to Co–O, CO, and C–O. , The peaks at 398.7, 400.4, and 402.2 eV were attributed to pyridinic-N, pyrrolic-N, and graphitic-N, respectively, and could be fitted to the model of perfect dodecahedral carbons . The peaks at 779.8 and 782.0 eV in the Co 2p 1/2 XPS spectra corresponded to Co 3+ and Co 2+ , respectively, and the signal at 786.1 eV was a satellite peak . The Co 3+ /Co 2+ ratio, as calculated from the Co 2p XPS spectra (Figure D), was 3:2.…”

Section: Resultsmentioning

confidence: 96%

Synthesis of Carbon Nanoparticles with Cobalt-Rich Shell via Pyrolysis of Zn-ZIF@Co/Zn-ZIF: Relevance of Co(III) Precursors

Ohata

Fukuda

et al. 2022

Inorg. Chem.

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To the best of our knowledge, this is the first report on the rapid one-pot synthesis of a unique core−shell-structured zeolitic imidazolate framework (ZIF) using Co(III) and Zn(II) precursors. The key to obtaining this unique structure is the use of a Co(III) precursor as the starting material. Transmission electron microscopy (TEM) reveals that Co was present within a 30-nmthick shell layer of the ZIF material. Thermal decomposition of the ZIF material affords core−shell-structured carbon nanoparticles that have Co on the external surface of the carbon grain. We have previously demonstrated that this carbonaceous material obtained by thermal decomposition exhibited high performance as an adsorbent for nitric oxide, even in the presence of excess oxygen and water vapor, and therefore, it was a suitable material for NO x elimination at low temperatures. The growth mechanism of the synthesized ZIF particles and the differences between synthesized ZIF and conventional Co(II)-ZIF-67 are discussed. The reactivity of the Co(III) precursor is much lower than that of the Co(II) species, leading to slower precipitation of Co(III) than that of Zn(II), thus forming the core−shell structure.

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Cobalt Nanoparticles Embedded into N-Doped Carbon from Metal Organic Frameworks as Highly Active Electrocatalyst for Oxygen Evolution Reaction

Cited by 41 publications

References 49 publications

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

Defect-Rich Porous CoS_1.097/MoS₂ Hybrid Microspheres as Electrocatalysts for pH-Universal Hydrogen Evolution

Synthesis of Carbon Nanoparticles with Cobalt-Rich Shell via Pyrolysis of Zn-ZIF@Co/Zn-ZIF: Relevance of Co(III) Precursors

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Cobalt Nanoparticles Embedded into N-Doped Carbon from Metal Organic Frameworks as Highly Active Electrocatalyst for Oxygen Evolution Reaction

Cited by 41 publications

References 49 publications

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

Structure-Activity Relationship of Atomic-Scale Cobalt-Based N-C Catalysts in the Oxygen Evolution Reaction

Defect-Rich Porous CoS1.097/MoS2 Hybrid Microspheres as Electrocatalysts for pH-Universal Hydrogen Evolution

Synthesis of Carbon Nanoparticles with Cobalt-Rich Shell via Pyrolysis of Zn-ZIF@Co/Zn-ZIF: Relevance of Co(III) Precursors

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Defect-Rich Porous CoS_1.097/MoS₂ Hybrid Microspheres as Electrocatalysts for pH-Universal Hydrogen Evolution