Malaria, caused by protozoan parasite Plasmodium falciparum, has long been a major global health problem. In 2016, there were an estimated 216 million cases of malaria, and at least 445, 000 deaths. Substantial funding, over US$ 19 billion since 2010, has been invested in the elimination and prevention of malaria, according to World Malaria Report 2017. The World Health Organization recommends artemisinin-based combination therapies (ACTs) as first-line drugs due to the fact that sesquiterpene endoperoxide artemisinin is currently the most effective treatment against malaria. Conventional photo- and acid catalysts usually suffer from problems such as active-site accessibility and precise tailorability over reaction environment.<br/>Porous catalysts with tailored pore environments are highly desired in hetergenous catalysis due to the high tunability of pore size and functionalization. Among them, metal-organic frameworks (MOFs) are a series of crystalline frameworks with designable topology, adjustable porosity, tunable functionality, and variable surface moieties. Synergistic effects originating from the precisely controlled apportionment of specific functional groups in the proper proximity are expected to benefit the overall efficiency of cascade catalysis.<br/>Herein, we demonstrate that a highly porous dual-function solid acid/photocatalyst, sulfated porphyrinic metal-organic frameworks (MOFs), can be prepared by a post-synthetic sulfation approach. Accordingly, it could further be utilized for tandem semisynthesis of artemisinin from dihydroartemisinic acid, and function as the most efficient catalyst among all homogenous and heterogenous photocatalysts for artemisinin production. This facile heterogenous catalytic system can be efficiently recycled and shows enhanced stability compared to the traditional homogeneous catalysts. This result highlights the advantage of the hierarchically porous MOF catalysts with tailed functionalities and cooperative motifs as highly accessible and recyclable heterogeneous catalysts, providing a more efficient, recyclable, cost-effective approach to this important drug production.

Construction of highly efficient and recyclable metal-organic framework catalysts for artemisinin production

2019 Spring National Meeting

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