Electrocatalytic Upcycling of Biomass and Plastic Wastes to Biodegradable Polymer Monomers and Hydrogen Fuel at High Current Densities

被引:198
|
作者
Yan, Yifan [1 ]
Zhou, Hua [1 ,3 ]
Xu, Si-Min [1 ]
Yang, Jiangrong [1 ]
Hao, Pengjie [1 ]
Cai, Xi [1 ]
Ren, Yue [1 ]
Xu, Ming [1 ]
Kong, Xianggui [1 ]
Shao, Mingfei [1 ]
Li, Zhenhua [1 ]
Duan, Haohong [2 ,3 ,4 ]
机构
[1] Beijing Univ Chem Technol, Coll Chem, State Key Lab Chem Resource Engn, Beijing 100029, Peoples R China
[2] Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
[3] Haihe Lab Sustainable Chem Transformat, Tianjin 300192, Peoples R China
[4] Tsinghua Univ, Engn Res Ctr Adv Rare Earth Mat, Dept Chem, Minist Educ, Beijing 100084, Peoples R China
基金
国家重点研发计划; 中国国家自然科学基金; 北京市自然科学基金;
关键词
ETHYLENE-GLYCOL; GLYCEROL ELECTROOXIDATION; ELECTROCHEMICAL VALORIZATION; ETHANOL OXIDATION; REACTION-PRODUCTS; LACTIC-ACID; AT-PD; GOLD; AU; NANOPARTICLES;
D O I
10.1021/jacs.2c11861
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Transformation of biomass and plastic wastes to value-added chemicals and fuels is considered an upcycling process that is beneficial to resource utilization. Electrocatalysis offers a sustainable approach; however, it remains a huge challenge to increase the current density and deliver market-demanded chemicals with high selectivity. Herein, we demonstrate an electrocatalytic strategy for upcycling glycerol (from biodiesel byproduct) to lactic acid and ethylene glycol (from polyethylene terephthalate waste) to glycolic acid, with both products being as valuable monomers for biodegradable polymer production. By using a nickel hydroxide-supported gold electrocatalyst (Au/ Ni(OH)2), we achieve high selectivities of lactic acid and glycolic acid (77 and 91%, respectively) with high current densities at moderate potentials (317.7 mA/cm2 at 0.95 V vs RHE and 326.2 mA/ cm2 at 1.15 V vs RHE, respectively). We reveal that glycerol and ethylene glycol can be enriched at the Au/Ni(OH)2 interface through their adjacent hydroxyl groups, substantially increasing local concentrations and thus high current densities. As a proof of concept, we employed a membrane-free flow electrolyzer for upcycling triglyceride and PET bottles, attaining 11.2 g of lactic acid coupled with 9.3 L of H2 and 13.7 g of glycolic acid coupled with 9.4 L of H2, respectively, revealing the potential of coproduction of valuable chemicals and H2 fuel from wastes in a sustainable fashion.
引用
收藏
页码:6144 / 6155
页数:12
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