Yan Yifan, Zhou Hua, Xu Si-Min, Yang Jiangrong, Hao Pengjie, Cai Xi, Ren Yue, Xu Ming, Kong Xianggui, Shao Mingfei, Li Zhenhua, Duan Haohong
State Key Laboratory of Chemical Resource Engineering, College of Chemistry, Beijing University of Chemical Technology, Beijing 100029, China.
Haihe Laboratory of Sustainable Chemical Transformations, Tianjin 300192, China.
J Am Chem Soc. 2023 Mar 22;145(11):6144-6155. doi: 10.1021/jacs.2c11861. Epub 2023 Feb 17.
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)), we achieve high selectivities of lactic acid and glycolic acid (77 and 91%, respectively) with high current densities at moderate potentials (317.7 mA/cm at 0.95 V vs RHE and 326.2 mA/cm at 1.15 V vs RHE, respectively). We reveal that glycerol and ethylene glycol can be enriched at the Au/Ni(OH) 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 H and 13.7 g of glycolic acid coupled with 9.4 L of H, respectively, revealing the potential of coproduction of valuable chemicals and H fuel from wastes in a sustainable fashion.
将生物质和塑料废物转化为高附加值化学品和燃料被认为是一种有利于资源利用的升级回收过程。电催化提供了一种可持续的方法;然而,提高电流密度并以高选择性生产市场所需的化学品仍然是一个巨大的挑战。在此,我们展示了一种电催化策略,即将甘油(来自生物柴油副产品)升级回收为乳酸,将乙二醇(来自聚对苯二甲酸乙二酯废料)升级回收为乙醇酸,这两种产物都是用于生产可生物降解聚合物的有价值单体。通过使用氢氧化镍负载的金电催化剂(Au/Ni(OH)),我们在中等电位下(相对于可逆氢电极,在0.95 V时为317.7 mA/cm²,在1.15 V时为326.2 mA/cm²)实现了乳酸和乙醇酸的高选择性(分别为77%和91%)以及高电流密度。我们发现甘油和乙二醇可以通过其相邻的羟基在Au/Ni(OH)界面处富集,从而大幅提高局部浓度并进而提高电流密度。作为概念验证,我们采用了无膜流动电解槽来升级回收甘油三酯和PET瓶,分别获得了11.2 g乳酸和9.3 L氢气以及13.7 g乙醇酸和9.4 L氢气,揭示了以可持续方式从废物中共生产有价值化学品和氢气燃料的潜力。