We report selective photocatalytic partial oxidation of glycerol on bimetallic formate oxidase mimicking AuPt/TiO, with a unique self-accelerating reaction kinetics discovered for the first time. Systematic investigation on the glycerol oxidation in the presence of externally added formic acid and various scavengers reveals a positive correlation between photocatalytic activity and solution HO level. A reaction mechanism has been put forward, where the in situ generated formic acid consumes photogenerated holes, and enables on-site HO production on AuPt/TiO, resulting in accelerated glycerol oxidation and improved C3 product selectivity. In pH 9 borate buffer solution, C3 products selectivity of 72% (60% for glyceric acid) has been achieved at 90% glycerol conversion under AM 1.5 G irradiation for 4 h, at ambient conditions. Our findings presented here may help guiding catalyst design for the photocatalytic biomass valorization in the future.

中文翻译：

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模拟 AuPt/TiO2 的甲酸氧化酶上阳光驱动的甘油选择性氧化

我们报道了模仿 AuPt/TiO 的双金属甲酸氧化酶对甘油的选择性光催化部分氧化，并首次发现了独特的自加速反应动力学。对外部添加甲酸和各种清除剂存在下甘油氧化的系统研究表明，光催化活性与溶液 H2O 水平之间呈正相关。提出了一种反应机理，其中原位产生的甲酸消耗光生空穴，并能够在 AuPt/TiO 上现场生成 H2O，从而加速甘油氧化并提高 C3 产物选择性。在 pH 9 硼酸盐缓冲溶液中，在环境条件下，AM 1.5 G 照射 4 小时，甘油转化率为 90%，C3 产物选择性为 72%（甘油酸为 60%）。我们在此提出的研究结果可能有助于指导未来光催化生物质增值的催化剂设计。