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Mechanochemically engineered defect-rich Zn/Co-ZIF-8 solid solutions for enhanced electrochemical water splitting
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DOI：10.1039/d6ta00038j.png)
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Abstract
En 中文
Zeolitic imidazolate frameworks (ZIFs), a subclass of porous MOFs, have attracted significant attention due to their high crystallinity and exceptional thermal and chemical stability. The synthetic protocols of Zn-ZIF-8 and Co-ZIF-8 strongly influence their thermodynamic and kinetic properties. Room-temperature (RT) aqueous synthesis yields less crystalline phases (pZn-ZIF-8-RT and pCo-ZIF-8-RT) compared to high-temperature (HT) solvothermal synthesis in DMF/DEF (pZn-ZIF-8-HT and pCo-ZIF-8-HT). Mechanical milling of equimolar RT-synthesized phases produces a highly disordered amorphous solid solution, a-Zn50Co50ZIF8-RT, which upon water/methanol vapor exposure at 25 degrees C transforms into a crystalline counterpart (c-Zn50Co50ZIF8-RT). Following the same protocol, milling of HT-synthesized precursors yields a more ordered amorphous phase, a-Zn50Co50ZIF8-HT. Comprehensive characterization using DFT, Raman spectroscopy, FE-SEM, and HR-TEM reveals that a-Zn50Co50ZIF8-RT possesses abundant active sites, enhanced electron density, and a less ordered structure, making it an efficient electrocatalyst. Consequently, it exhibits superior performance towards electrocatalytic water splitting with low overpotentials of 301 mV (OER) and 437 mV (HER) at 10 mA cm-2, outperforming that of a-Zn50Co50ZIF8-HT, c-Zn50Co50ZIF8-RT and c-Zn50Co50ZIF8-HT.
Keywords:
ZEOLITIC IMIDAZOLATE FRAMEWORKS
EFFICIENT ELECTROCATALYST
HYDROGEN GENERATION
OXYGEN REDUCTION
ZIF-8
PERFORMANCE
CATALYST
NANOPARTICLES
MEMBRANES
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9.5
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3.3W
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21.7W
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