Wang Ziqiang, Song Jiale, Zhang Hugang, Deng Kai, Yu Hongjie, Xu You, Wang Hongjing, Wang Liang
State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou, 310014, P. R. China.
Small. 2024 Nov;20(45):e2404124. doi: 10.1002/smll.202404124. Epub 2024 Jul 17.
Electrochemical upcycling of nitrate and polyester plastic into valuable products is an ideal solution to realize the resource utilization. Here, the co-production of ammonia (NH) and glycolic acid (GA) via electrochemical upcycling of nitrate and polyethylene terephthalate (PET) plastics over mesoporous PdAu film on Ni foam (mPdAu/NF), which is synthesized by micelle-assisted replacement method, is proposed. The mPdAu/NF with well-developed mesoporous structure provides abundant active sites and facilitated transfer channels and strong electronic effect. As such, the mPdAu/NF exhibits high Faraday efficiencies of 97.28% and 95.32% at 0.9 V for the formation of NH and GA, respectively. Theoretical results indicate that the synergistic effect of Pd and Au can optimize adsorption energy of key intermediates *NOH and *OCH-CHOH on active sites and increase bond energy of C─C band, thereby improving the activity and selectivity for the formation of NH and GA. This work proposes a promising strategy for the simultaneous conversation of nitrate and PET plastic into high-value NH and GA.
将硝酸盐和聚酯塑料电化学升级循环为有价值的产品是实现资源利用的理想解决方案。在此，提出了通过在泡沫镍上的介孔钯金薄膜（mPdAu/NF）上对硝酸盐和聚对苯二甲酸乙二酯（PET）塑料进行电化学升级循环来联产氨（NH₃）和乙醇酸（GA），该介孔钯金薄膜是通过胶束辅助置换法合成的。具有发达介孔结构的mPdAu/NF提供了丰富的活性位点、便利的传输通道和强大的电子效应。因此，mPdAu/NF在0.9 V时分别对NH₃和GA的生成表现出97.28%和95.32%的高法拉第效率。理论结果表明，Pd和Au的协同效应可以优化关键中间体NOH和OCH₂-CH₂OH在活性位点上的吸附能，并增加C─C键的键能，从而提高NH₃和GA生成的活性和选择性。这项工作为将硝酸盐和PET塑料同时转化为高价值的NH₃和GA提出了一种有前景的策略。
