A highly efficient streamlined chemoenzymatic strategy for total synthesis of four prioritized ganglioside cancer antigens GD2, GD3, fucosyl GM1, and GM3 from commercially available lactose and phytosphingosine is demonstrated. Lactosyl sphingosine (LacβSph) was chemically synthesized (on a 13 g scale), subjected to sequential one-pot multienzyme (OPME) glycosylation reactions with facile C18-cartridge purification, followed by improved acylation conditions to form target gangliosides, including fucosyl GM1 which has never been synthesized before.
The temperature and pressure of the hydrothermal process occurring in a batch reactor are typically coupled. Herein, we develop a decoupled temperature and pressure hydrothermal system that can heat the cellulose at a constant pressure, thus lowering the degradation temperature of cellulose significantly and enabling the fast production of carbon sub-micron spheres. Carbon sub-micron spheres can be produced without any isothermal time, much faster compared to the conventional hydrothermal process. High-pressure water can help to cleave the hydrogen bonds in cellulose and facilitate dehydration reactions, thus promoting cellulose carbonization at low temperatures. A life cycle assessment based on a conceptual biorefinery design reveals that this technology leads to a substantial reduction in carbon emissions when hydrochar replacing fuel or used for soil amendment. Overall, the decoupled temperature and pressure hydrothermal treatment in this study provides a promising method to produce sustainable carbon materials from cellulose with a carbon-negative effect.
A sensitive turn-on fluorescent sensor based on single-layer MnO2 nanosheet-quenched fluorescent carbon quantum dots has been developed for rapid and selective sensing of glutathione in aqueous solutions, as well as in living cells.
A high-content bioorthogonal prodrug with multiple outputs using the "click, cyclize, and release" concept is described. The proof of concept is established by the co-delivery of a gasotransmitter carbon monoxide, an anticancer drug floxuridine, and an in situ generated fluorescent reporter molecule for real-time monitoring of the prodrug activation. Bioorthogonal prodrugs as such are invaluable tools for the co-delivery of other drug payloads for multimodal therapy.
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