Fe-based
MOFs (Fe-MOFs) are deemed promising Fenton-like catalysts
due to their well-developed pores and accessible active sites. However,
their inferior catalytic activity, iron leaching, and low H2O2 utilization always hinder their application as Fe-based
MOF catalysts. In this work, we manipulated the structure of Fe-oxo
nodes in MIL-88B(Fe) via a CuI species substitution method,
affording a mixed-valence (Cu-incorporated Fe-MOFs) with highly improved
Fenton-like performance. It is found that the CuI serves
as a shuttle to promote transfer between FeII/FeIII, inducing the formation of a larger amount of stable FeII sites, which was proven by experimental and DFT calculation results.
A linear relationship was observed for the Fenton-like performance
and the amount of CuI species for the catalysts. The corresponding
value of the •OH formation is 2.17 eV for Cu-incorporated
MIL-88B(Fe), which is significantly lower than that of MIL-88B(Fe)
(2.69 eV). Meanwhile, the enriched CuI species suppress
Fe species leaching during the catalytic reaction. The Fe-ion leakage
of 0.4Cu@MIL-88B is very tiny (0.01–0.03 mg/L), significantly
less than that of MIL-88B (2.00–3.02 mg/L). At the same time,
H2O2 utilization for 0.4Cu@ MIL-88B(Fe) is 88%,
which is almost 4.4 times that of pure MIL-88B(Fe). This work provides
insights into the rational design of Fe-MOFs as promising Fenton-like
catalysts for wastewater treatment.