Heat-fueled enzymatic cascade for selective oxyfunctionalization of hydrocarbons

• Published in: Nature communications Vol. 13; no. 1; pp. 3741 - 10
• Main Authors: Yoon, Jaeho, Jang, Hanhwi, Oh, Min-Wook, Hilberath, Thomas, Hollmann, Frank, Jung, Yeon Sik, Park, Chan Beum
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 29.06.2022; Nature Publishing Group; Nature Portfolio
• Subjects: 147/143; 147/28; 631/92/603; 639/301/299/2736; 639/4077/4072/4062; 639/4077/4107; 82/16; Biocatalysts; Bismuth tellurides; Chemical energy; Chemical reactions; Cyclohexane; Direct conversion; Energy; Enzymes; Epoxidation; Ethylbenzene; Heat; Heat sources; High temperature; Humanities and Social Sciences; Hydrogen peroxide; Hydroxylation; Low temperature; multidisciplinary; Propylbenzene; Room temperature; Science; Science (multidisciplinary); Substrates; Tetralin; Thermoelectric materials; Vehicle emissions; Waste heat
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-022-31363-8

Heat is a fundamental feedstock, where more than 80% of global energy comes from fossil-based heating process. However, it is mostly wasted due to a lack of proper techniques of utilizing the low-quality waste heat (<100 °C). Here we report thermoelectrobiocatalytic chemical conversion systems for heat-fueled, enzyme-catalyzed oxyfunctionalization reactions. Thermoelectric bismuth telluride (Bi 2 Te 3 ) directly converts low-temperature waste heat into chemical energy in the form of H 2 O 2 near room temperature. The streamlined reaction scheme (e.g., water, heat, enzyme, and thermoelectric material) promotes enantio- and chemo-selective hydroxylation and epoxidation of representative substrates (e.g., ethylbenzene, propylbenzene, tetralin, cyclohexane, cis -β-methylstyrene), achieving a maximum total turnover number of r Aae UPO (TTN r Aae UPO ) over 32000. Direct conversion of vehicle exhaust heat into the enantiopure enzymatic product with a rate of 231.4 μM h −1 during urban driving envisions the practical feasibility of thermoelectrobiocatalysis. Thermoelectric materials enable us to convert heat into electricity, but their application has been limited to high-temperature heat sources. Here, the authors show the direct conversion of low-grade waste heat into chemical energy via combining thermoelectric materials with biocatalysts below 100 °C.