Journal
NANO LETTERS
Volume 22, Issue 6, Pages 2529-2537Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.nanolett.2c00446
Keywords
Redox-active metal-organic frameworks; Noble metal nanodots; Interfacial reduction nucleation; Electrochemical nitrate reduction
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Funding
- National Key RAMP
- D Program of China [2017YFA0208200]
- National Natural Science Foundation of China [22022505, 21872069, 21875099]
- Fundamental Research Funds for the Central Universities [0205-14380266]
- Suzhou Gusu Leading Talents of Science and Technology Innovation and Entrepreneurship in Wujiang District
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This study reports the construction of stable and redox-active zirconium metal-organic frameworks (Zr-MOFs) for electrochemically converting nitrate to ammonia. By utilizing the Zr-MOFs as catalysts, noble metal nanodots could be uniformly nucleated, leading to highly efficient electrocatalytic activity. The PdNDs/Zr-MOF catalyst exhibits the highest electrocatalytic activity.
Electrochemically converting nitrate to ammonia is a promising route to realize artificial nitrogen recycling. However, developing highly efficient electrocatalysts is an ongoing challenge. Herein, we report the construction of stable and redox-active zirconium metal-organic frameworks (Zr-MOFs) based on Zr-6 nanoclusters and redox-reversible tetrathiafulvalene (TTF) derivatives as inorganic nodes and organic linkers, respectively. The redox-active Zr-MOF can facilitate the in situ reduction of noble metal precursors free of external reductants and realize the uniform nucleation of noble metal nanodots (NDs) on Zr-MOF, achieving the preparation of M-NDs/Zr-MOF (M = Pd, Ag, or Au). The highly porous Zr-MOF with good conductivity can facilitate the mass transfer process. Among the M-NDs/Zr-MOF catalysts, PdNDs/Zr-MOF exhibits the highest electrocatalytic activity, delivering a NH3 yield of 287.31 mmol center dot h(-1)center dot g(-1)cat. and a Faradaic efficiency of 58.1%. The proposed interfacial reduction nucleation strategy for anchoring M NDs on Zr-MOFs can be applied to other challenging energy conversion reactions.
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