Modulating electronic structure of NiFe layered double hydroxide membrane by interlayer-confinement for enhanced water decontamination

Herein, the role of nanoconfinement on modulating the electronic structure of the catalyst that influences the efficiency of advanced oxidation processes (AOPs) was investigated. Peroxymonosulfate (PMS)-based AOP was conducted within the nanoconfined sub-nanometer interlayer channels of a 2D NiFe layered double hydroxide membrane (NiFeM). The interlayer-confined NiFeM exhibited complete removal of sulfamethoxazole, with a degradation rate constant of 211.67 s −1 that was 2.6–946.2 times higher than previously reported nanoconfined AOPs systems, and also demonstrated broad pH working range and anti-interference ability with excellent catalytic stability in 25 h. Theoretical calculations suggested such interlayer confinement upshifted the catalyst metal d-band center, accounting for strengthened PMS adsorption and electron transfer from catalyst to PMS molecules. This work embodies the interlayer confinement effect on modulating the electronic structure of catalyst and provides insights for designing catalysts with excellent capability for environmental remediation, energy conversion and chemical synthesis.