期刊
ADVANCED ENERGY MATERIALS
卷 11, 期 20, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/aenm.202003545
关键词
confinement; intercalation; metal‐ oxides; nanoenvironment; nickel iron; oxygen evolution reaction; zirconium phosphate
类别
资金
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division, Catalysis Science Program
- National Science Foundation Center for Chemical Innovation in Solar Fuels [CHE-1305124]
- Toyota Research Institute (TRI)
- TRI
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
- National Science Foundation [ECCS-1542152]
- Department of Defense (DoD) through the National Defense Science and Engineering Graduate Fellowship (NDSEG) Program
- Stanford University Diversifying Academia, Recruiting Excellence Doctoral Fellowship Program (DARE)
- NSF-PREM Center for Interfacial Electrochemistry of Energy Materials (CIE2M) [DMR-1827622]
A new catalyst motif has been engineered and isolated within a layered zirconium phosphate matrix for the oxygen evolution reaction (OER) using nickel-iron transition metal electrocatalysts. The confined NiFe catalysts demonstrate significantly improved mass activity compared to conventional surface-adsorbed systems under certain conditions. Intercalated Ni/Fe species within the layered structure serve as the active site during catalysis, and density functional theory shows correlation with experimental compositional trends, highlighting the potential for enhanced catalytic performance within unique nanoscale chemical environments.
Unique classes of active-site motifs are needed for improved electrocatalysis. Herein, the activity of a new catalyst motif is engineered and isolated for the oxygen evolution reaction (OER) created by nickel-iron transition metal electrocatalysts confined within a layered zirconium phosphate matrix. It is found that with optimal intercalation, confined NiFe catalysts have an order of magnitude improved mass activity compared to more conventional surface-adsorbed systems in 0.1 m KOH. Interestingly, the confined environments within the layered structure also stabilize Fe-rich compositions (90%) with exceptional mass activity compared to known Fe-rich OER catalysts. Through controls and by grafting inert molecules to the outer surface, it is evidenced that the intercalated Ni/Fe species stay within the interlayer during catalysis and serve as the active site. After determining a possible structure (wycherproofite), density functional theory is shown to correlate with the observed experimental compositional trends. It is further demonstrated that the improved activity of this motif is correlated to the Fe and water content/composition within the confined space. This work highlights the catalytic enhancement possibilities available through zirconium phosphate and isolates the activity from the intercalated species versus surface/edge ones, thus opening new avenues to develop and understand catalysts within unique nanoscale chemical environments.
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