Facile Method To Prepare a Novel Biological HKUST-1@CMCS with Macroscopic Shape Control for the Long-Acting and Sustained Release

We have developed a green and versatile method to prepare hierarchically porous Cu3(BTC)2@carboxymethyl chitosan (HKUST-1@CMCS) with a macroscopic shape control and designable performance via the cross-linking of Cu(II) ions with CMCS. Furthermore, atomic force microscopy, scanning electron microscopy, powder X-ray diffraction, Brunauer–Emmett–Teller, and X-ray photoelectron spectroscopy analyses showed that the morphology of HKUST-1 could be controlled and changed by tailoring the surface roughness (Rq) of polymer matrix. For the ball-like, fiberlike, and membrane-like composites, the matrix Rq values were 887, 88.4, and 18.2 nm and the average sizes of HKUST-1 crystals were about 10.2, 5.9, and 1.7 μm, respectively. It was found that the larger the Rq of the polymer matrix, the higher the drug payload. The results of drug release showed that the release percentage of dimethyl fumarate from HKUST-1@CMCS was 66% in 326 h, whereas that of Cu@CMCS was only 12 h. Obviously, the HKUST-1@CMCS had a long-acting and sustained release property compared to that of Cu@CMCS due to its complementary advantages of metal–organic frameworks (MOFs) and polymers. Therefore, this study not only provided an interesting way to make up for the shortcomings of MOFs and natural polymer but also developed a long-acting delivery system for a huge potential application prospect.