Artificial synthesis of polyesters at ambient condition via consecutive CO_(2)electrolysis and fermentation  

作　　者：Guiru Zhang Ning Ji Shiheng Lyu Baoxin Ni Peng Shen Ke Ye Yuting Wang Xuheng Jiang Hai Zhang Xi Liu Yongcheng Wang Kun Jiang 

机构地区：[1]Department of Laboratory Medicine of The First Affiliated Hospital&Liangzhu Laboratory,Zhejiang University School of Medicine,Hangzhou 310058,China [2]Interdisciplinary Research Center,School of Mechanical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China [3]In-situ Centre for Physical Sciences,Frontiers Science Center for Transformative Molecules,School of Chemistry and Chemical Engineering,Shanghai Jiao Tong University,Shanghai 200240,China

出　　处：《Nano Research》2024年第7期6016-6025,共10页纳米研究（英文版）

基　　金：supported by the National Key Research and Development Program of China(Nos.2022YFB4102000 and 2022YFA1505100);the National Natural Science Foundation of China(No.22002088);the Shanghai Sailing Program(No.20YF1420500);the Leading Innovative and Entrepreneur Team Introduction Program of Zhejiang(No.2021R01012);the Shanghai Science and Technology Innovation Action Plan(No.22dz1205500).

摘　　要：Electrochemically converting CO_(2)into value-added chemicals is a promising approach to mitigate anthropogenic carbon emissions,yet largely limited to short-chained C_(1)–C_(3)products.Herein,we demonstrate a tandem artificial synthesis of biodegradable polyhydroxybutyrate(PHB)plastic from CO_(2)building blocks.Batch synthesis of defects-enriched Bi catalyst is firstly demonstrated by plasma bombardment and following in situ electrochemical reduction,which delivers a HCOOH Faradaic efficiency above 80%at tunable concentration from 2 to 250 mM,an energy efficiency up to 41%,and a single-pass carbon conversion efficiency up to 60%.Annular dark field and second electron microscopic analysis,density functional theory(DFT)calcualtions,coupled with H-type and solid-state electrolyzer assessments,point out the vital role of defective and/or stepped Bi surface sites in promoting CO_(2)-to-HCOOH conversion.Thereafter,as-synthesized high-purity HCOOH is used as the sole carbon source for C-chain growth within microbial fermentation reactor with Ralstonia eutropha,where activated formate dehydrogenase and increased metabolites related to Calvin–Benson–Bassham cycle are found to be responsible for the enhanced polyester accumulation.

关 键 词：CO_(2)electrolysis Bi catalyst vacancy site formic acid FERMENTATION 

分 类 号：O64[理学—物理化学]