Premium
Isolating the Electrocatalytic Activity of a Confined NiFe Motif within Zirconium Phosphate
Author(s) -
Sanchez Joel,
Stevens Michaela Burke,
Young Alexandra R.,
Gallo Alessandro,
Zhao Meng,
Liu Yunzhi,
RamosGarcés Mario V.,
BenNaim Micha,
Colón Jorge L.,
Sinclair Robert,
King Laurie A.,
Bajdich Michal,
Jaramillo Thomas F.
Publication year - 2021
Publication title -
advanced energy materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 10.08
H-Index - 220
eISSN - 1614-6840
pISSN - 1614-6832
DOI - 10.1002/aenm.202003545
Subject(s) - catalysis , intercalation (chemistry) , zirconium , materials science , oxygen evolution , zirconium phosphate , phosphate , chemical engineering , nickel , transition metal , electrocatalyst , density functional theory , inorganic chemistry , chemistry , electrochemistry , organic chemistry , computational chemistry , metallurgy , electrode , engineering
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.