Fabrication of Novel MOF/HOF Composite for Efficient Degradation of Methylene Blue via Photo-Fenton-like Process

The photo-Fenton process is an advanced oxidation method widely employed in environmental remediation. Herein, we developed a novel metal–organic framework@hydrogen-bonded organic framework (MOF/HOF) composite with excellent photo-Fenton-like activity for the efficient degradation of organic dye methylene blue (MB). Cu-based MOF (CuBTC) was firstly prepared via the solvothermal method, then melamine (MA) and trimesic acid (TMA)-based HOF (MA-TMA) was grown in situ on CuBTC with hydrogen bonding interactions to produce the MOF/HOF composite CuBTC-MA. The CuBTC-MA composite could catalyze H2O2 to produce active substances for efficient MB degradation. The degradation rate constant of the CuBTC-MA composite was 4.4 times and 16.7 times higher than that of CuBTC and MA-TMA. The remarkably enhanced performance was attributed to the synergistic effect between the efficient separation of electron–holes supported by the type-II heterojunction structure of the CuBTC-MA composite and the Cu(I)/Cu(II) inter-conversion. The CuBTC-MA composite demonstrated exceptional repeatability and maintained a stable performance across a broad pH range. This study provided a novel paradigm for engineering heterogeneous MOF/HOF heterostructures, demonstrating significant potential in advancing photo-Fenton-like catalytic systems for the efficient environmental remediation of organic pollutants through synergistic charge separation and radical generation mechanisms.