Dataset Information

Direct Pyrolysis of a Manganese-Triazolate Metal-Organic Framework into Air-Stable Manganese Nitride Nanoparticles.

ABSTRACT: Although metal-organic frameworks (MOFs) are being widely used to derive functional nanomaterials through pyrolysis, the actual mechanisms involved remain unclear. In the limited studies to date, elemental metallic species are found to be the initial products, which limits the variety of MOF-derived nanomaterials. Here, the pyrolysis of a manganese triazolate MOF is examined carefully in terms of phase transformation, reaction pathways, and morphology evolution in different conditions. Surprisingly, the formation of metal is not detected when manganese triazolate is pyrolyzed in an oxygen-free environment. Instead, a direct transformation into nanoparticles of manganese nitride, Mn₂N _x embedded in N-doped graphitic carbon took place. The electrically conductive Mn₂N _x nanoparticles show much better air stability than bulk samples and exhibit promising electrocatalytic performance for the oxygen reduction reaction. The findings on pyrolysis mechanisms expand the potential of MOF as a precursor to derive more functional nanomaterials.

SUBMITTER: Hu Y

PROVIDER: S-EPMC7887590 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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Direct Pyrolysis of a Manganese-Triazolate Metal-Organic Framework into Air-Stable Manganese Nitride Nanoparticles.

Hu Yating Y Li Changjian C Xi Shibo S Deng Zeyu Z Liu Ximeng X Cheetham Anthony K AK Wang John J

Advanced science (Weinheim, Baden-Wurttemberg, Germany) 20210104 4

Although metal-organic frameworks (MOFs) are being widely used to derive functional nanomaterials through pyrolysis, the actual mechanisms involved remain unclear. In the limited studies to date, elemental metallic species are found to be the initial products, which limits the variety of MOF-derived nanomaterials. Here, the pyrolysis of a manganese triazolate MOF is examined carefully in terms of phase transformation, reaction pathways, and morphology evolution in different conditions. Surprisin ...[more]

PMID: 33643801

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Project description:Zeolites, silica-supported amines, and metal-organic frameworks (MOFs) have been demonstrated as promising adsorbents for direct air CO2 capture (DAC), but the shaping and structuring of these materials into sorbent modules for practical processes have been inadequately investigated compared to the extensive research on powder materials. Furthermore, there have been relatively few studies reporting the DAC performance of sorbent contactors under cold, subambient conditions (temperatures below 20 °C). In this work, we demonstrate the successful fabrication of adsorbent monoliths composed of cellulose acetate (CA) and adsorbent particles such as zeolite 13X and MOF MIL-101(Cr) by a 3D printing technique: solution-based additive manufacturing (SBAM). These monoliths feature interpenetrated macroporous polymeric frameworks in which microcrystals of zeolite 13X or MIL-101(Cr) are evenly distributed, highlighting the versatility of SBAM in fabricating monoliths containing sorbents with different particle sizes and density. Branched poly(ethylenimine) (PEI) is successfully loaded into the CA/MIL-101(Cr) monoliths to impart CO2 uptakes of 1.05 mmol gmonolith-1 at -20 °C and 400 ppm of CO2. Kinetic analysis shows that the CO2 sorption kinetics of PEI-loaded MIL-101(Cr) sorbents are not compromised in the monoliths compared to the powder sorbents. Importantly, these monoliths exhibit promising working capacities (0.95 mmol gmonolith-1) over 14 temperature swing cycles with a moderate regeneration temperature of 60 °C. Dynamic breakthrough experiments at 25 °C under dry conditions reveal a CO2 uptake capacity of 0.60 mmol gmonolith-1, which further increases to 1.05 and 1.43 mmol gmonolith-1 at -20 °C under dry and humid (70% relative humidity) conditions, respectively. Our work showcases the successful implementation of SBAM in making DAC sorbent monoliths with notable CO2 capture performance over a wide range of sorption temperatures, suggesting that SBAM can enable the preparation of efficient sorbent contactors in various form factors for other important chemical separations.

Dataset Information

Direct Pyrolysis of a Manganese-Triazolate Metal-Organic Framework into Air-Stable Manganese Nitride Nanoparticles.

Publications

Direct Pyrolysis of a Manganese-Triazolate Metal-Organic Framework into Air-Stable Manganese Nitride Nanoparticles.

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