New Deoxyenhygrolides from Plesiocystis pacifica Provide Insights into Butenolide Core Biosynthesis

Marine myxobacteria present a virtually unexploited reservoir for the discovery of natural products with diverse biological functions and novel chemical scaffolds. We report here the isolation and structure elucidation of eight new deoxyenhygrolides (1–8) from the marine myxobacterium Plesiocystis pacifica DSM 14875T. The herein described deoxyenhygrolides C–J (1–8) feature a butenolide core with an ethyl residue at C-3 of the γ-lactone in contrast to the previously described derivatives, deoxyenhygrolides A and B, which feature an isobutyl residue at this position. The butenolide core is 2,4-substituted with a benzyl (1, 2 and 7), benzoyl (3 and 4) or benzyl alcohol (5, 6 and 8) moiety in the 2-position and a benzylidene (1–6) or benzylic hemiketal (7 and 8) in the 4-position. The description of these new deoxyenhygrolide derivatives, alongside genomic in silico investigation regarding putative biosynthetic genes, provides some new puzzle pieces on how this natural product class might be formed by marine myxobacteria.

High specific surface CeO2-NPs doped loose porous C3N4 for enhanced photocatalytic oxidation ability

Porous C3N4 (PCN) is favored by researchers because it has more surface active sites, higher specific surface area and stronger light absorption ability than traditional g-C3N4. In this study, cerium dioxide nanoparticles (CeO2-NPs) with mixed valence state of Ce3+ and Ce4+ were doped into the PCN framework by a two-step method. The results indicate that CeO2-NPs are highly dispersed in the PCN framework, which leads to a narrower band gap, a wider range of the light response and an improved the separation efficiency of photogenerated charge in PCN. Moreover, the specific surface area (145.69 m2•g-1) of CeO2-NPs doped PCN is a 25.5 % enhancement than that of PCN (116.13 m2•g-1). In the experiment of photocatalytic selective oxidation of benzyl alcohol, CeO2-NPs doped porous C3N4 exhibits excellent photocatalytic activity, especially Ce-PCN-30. The conversion rate of benzyl alcohol reaches 74.9 % using Ce-PCN-30 as photocatalyst by 8 hours of illumination, which is 25.7 % higher than that of pure porous C3N4. Additionally, CeO2-NPs doped porous C3N4 also exhibits better photocatalytic efficiency for other aromatic alcohols.

Alcohols electrooxidation coupled with H2 production at high current densities promoted by a cooperative catalyst

Electrochemical alcohols oxidation offers a promising approach to produce valuable chemicals and facilitate coupled H2 production. However, the corresponding current density is very low at moderate cell potential that substantially limits the overall productivity. Here we report the electrooxidation of benzyl alcohol coupled with H2 production at high current density (540 mA cm−2 at 1.5 V vs. RHE) over a cooperative catalyst of Au nanoparticles supported on cobalt oxyhydroxide nanosheets (Au/CoOOH). The absolute current can further reach 4.8 A at 2.0 V in a more realistic two-electrode membrane-free flow electrolyzer. Experimental combined with theoretical results indicate that the benzyl alcohol can be enriched at Au/CoOOH interface and oxidized by the electrophilic oxygen species (OH*) generated on CoOOH, leading to higher activity than pure Au. Based on the finding that the catalyst can be reversibly oxidized/reduced at anodic potential/open circuit, we design an intermittent potential (IP) strategy for long-term alcohol electrooxidation that achieves high current density (>250 mA cm−2) over 24 h with promoted productivity and decreased energy consumption.