According to the World Health Organization, cancer is currently the leading cause of global mortality, accounting for approximately 10 million deaths across the world in 2020. As a result, the development of novel oncologic treatment strategies have become a central topic of modern medicine. Despite the continuous effort, current clinical cancer treatment approaches still face several issues. Non-specificity associated with most current chemotherapy, for instance, along with their inability to deliver anti-cancer agents <i>via</i> a precise spatial-temporal controlled mechanism, often result in low therapeutic indices, as well as adverse side effects on healthy tissues. Metal-Organic Frameworks (MOFs) have become popular for applications in anti-cancer treatments, owing to their low cytotoxicity and high biodegradability as well as excellent chemical and physical stability. Moreover, the extensive variety of chemical and structural configurations arising from a library consisting of approximately 90,000 existing MOF compositions enable unlimited possibilities for their utilization in the rational design of hybrid systems with selective functionalities. Additive manufacturing, also known as three-dimensional (3D) printing, has revolutionized the biomedical industry, due to its ability to rapidly prototype complex 3D objects. Herein, we present the manufacturing of a scaffold-like multi-layered architecture composed of a graphene-based substrate interfaced with a Digital Light Processing (DLP)-printed hydrogel phase containing pH-responsive nanocarriers as a model system for cancer treatment <i>via</i> localized controlled release of chemotherapeutic agent. More specifically, the selected drug, curcumin, was encapsulated within Zeolitic Imidazolate Frameworks (ZIF-8) structures and subsequently dispersed into a photopolymerizable poly(ethylene glycol) diacrylate (PEGDA)-based hydrogel. Finally, DLP was applied to yield a multi-layered CCM-ZIF-8/Hydrogel phase, which was interfaced with a graphene-based substrate to produce the pH-responsive drug release system. Various characterizations revealed the effects of curcumin-encapsulated ZIF-8 (CCM-ZIF-8) addition. Furthermore, in vitro drug release tests were performed, confirming the pH-responsiveness of the ZIF-8 MOFs.

Digital light processing (DLP) printing of MOF-embedded multi-layered hydrogel for the localized controlled release of anti-cancer agents

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