当前位置: X-MOL 学术ACS Sustain. Chem. Eng. › 论文详情
Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)
Polymer Photocatalyst–Enzyme Coupled Artificial Photosynthesis System for CO2 Reduction into Formate Using Water as the Electron Donor
ACS Sustainable Chemistry & Engineering ( IF 7.1 ) Pub Date : 2022-09-06 , DOI: 10.1021/acssuschemeng.2c02199
Ya Tan 1 , Jun Ma 1 , Feng Zhang 1 , Song Wang 1 , Fang Lan 1 , Hongbo Liu 1 , Run Li 1
Affiliation  

Photocatalyst–biocatalyst coupled systems offer a sustainable approach for converting CO2 into high-value compounds. However, the usually excessive use of organic sacrificial electron donors often leads to undesired side products and toxic intermediates. Here, we report a complete artificial photosynthesis system for selective CO2 reduction into formate with simultaneous H2O2 formation using water as the electron donor. The photocatalyst consists of polymeric carbon nitride with implanted single cobalt atoms as oxidative sites, while formate dehydrogenase from Candida boidinii was employed as reductive sites via a coupled redox cycle of nicotinamide adenine dinucleotide as cofactor. The artificial photosynthesis system demonstrates a competitive catalytic formate production rate of 420 μmol gcat.–1 h–1. DFT calculations reveal that the presence of single cobalt atoms can significantly accelerate the water oxidation into H2O2. The result demonstrates a benchmark example of a polymeric artificial photosynthesis system with remarkable photostability and catalytic selectivity for high-value compound production directly from CO2 without using extra organic electron donors.

中文翻译:

聚合物光催化剂-酶耦合人工光合作用系统以水为电子供体将二氧化碳还原为甲酸盐

光催化剂-生物催化剂耦合系统为将 CO 2转化为高价值化合物提供了一种可持续的方法。然而,通常过度使用有机牺牲电子供体通常会导致不希望的副产物和有毒中间体。在这里,我们报告了一个完整的人工光合作用系统,用于选择性地将 CO 2还原为甲酸盐,同时使用水作为电子供体形成H 2 O 2 。光催化剂由聚合物氮化碳组成,其中植入单个钴原子作为氧化位点,而来自Candida boidinii的甲酸脱氢酶通过烟酰胺腺嘌呤二核苷酸作为辅因子的耦合氧化还原循环被用作还原位点。人工光合作用系统展示了 420 μmol g cat的竞争性催化甲酸盐生产速率。–1小时–1。DFT计算表明,单个钴原子的存在可以显着加速水氧化成H 2 O 2该结果展示了聚合人工光合作用系统的基准示例,该系统具有显着的光稳定性和催化选择性,可直接从 CO 2生产高价值化合物,而无需使用额外的有机电子供体。
更新日期:2022-09-06
down
wechat
bug