葡萄糖氧化酶与金纳米粒子在葡萄糖顺序氧化制糖酸中的催化协同作用,Green Chemistry

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葡萄糖氧化酶与金纳米粒子在葡萄糖顺序氧化制糖酸中的催化协同作用
Green Chemistry ( IF 9.3 ) Pub Date : 2022-06-03 , DOI: 10.1039/d1gc03453g
Joseph S. Brindle ₁ , Patrick S. Nelson ₁ , Rashmi P. Charde ₁ , Sayed Abu Sufyan ₁ , Michael M. Nigra ₁

Affiliation

将异质金属纳米颗粒活性位点和酶活性位点组合起来用于顺序催化的化学转化具有巨大的潜力。该研究提供了一个说明性系统，其中葡萄糖氧化酶和金纳米颗粒成功地结合成混合催化材料。这种多点催化剂用于将葡萄糖转化为更有价值的糖酸产品，而无需外部添加强氧化剂如 H ₂ O ₂、次氯酸盐或硝酸。我们合成了一种能够将葡萄糖氧化成葡萄糖酸和用葡萄糖氧化酶将 H ₂ O ₂氧化成的杂化材料，而金催化进一步氧化成糖酸。H的原位生成₂ O₂为进一步氧化提供近端的稀释氧化剂。观察到较高的pH促进了由金纳米颗粒催化的_{H 2} O_{2分解和糖酸生成。}在不添加硝酸、强氧化剂、高于环境温度或高氧气压力的情况下，观察到 90 分钟内的糖精收率为 33%。结果表明，协同反应级联系统为金属纳米颗粒-酶杂化材料开辟了新的可能性，可应用于温和反应条件下的催化生物质转化。

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Catalytic cooperativity between glucose oxidase and gold nanoparticles in the sequential oxidation of glucose to saccharic acid

There exists great potential in combining heterogeneous metallic nanoparticle active sites and enzymatic active sites for sequentially catalysed chemical transformations. This study provides an illustrative system where glucose oxidase and gold nanoparticles are successfully combined into a hybrid catalytic material. This multi-site catalyst is used to convert glucose to a more valuable saccharic acid product without the need for a strong oxidant such as H₂O₂, hypochlorite, or nitric acid to be externally added. We synthesise a hybrid material that is able to oxidise glucose to gluconic acid and H₂O₂ with glucose oxidase, and gold catalyses the further oxidation to saccharic acid. The in situ generation of H₂O₂ provides a proximal, dilute oxidizing agent for further oxidation. It is observed that higher pH promotes H₂O₂ decomposition and saccharic acid generation catalysed by the gold nanoparticles. A 33% yield of saccharic acid in 90 minutes is observed without the addition of nitric acid, harsh oxidants, above ambient temperatures, or high oxygen pressures. The results demonstrate a cooperative reaction cascade system that opens new possibilities for metal nanoparticle–enzyme hybrid materials that can be applied to catalytic biomass conversion in mild reaction conditions.

更新日期：2022-06-03

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