Key Laboratory of Jiangxi Province for Persistent Pollutants Control and Resources Recycle, Nanchang Hangkong University, Nanchang, 330063, PR China.
Brook Byers Institute for Sustainable Systems and School of Civil and Environmental Engineering, Georgia Institute of Technology, Atlanta, GA, 30332, United States.
Water Res. 2019 Mar 1;150:330-339. doi: 10.1016/j.watres.2018.11.077. Epub 2018 Nov 30.
A novel electrocatalytic system was developed to realize one-pot conversion of organic pollutants into liquid fuels such as methanol (CHOH) and ethanol (CHOH). The process combines the catalytic oxidation of organic pollutants with electrocatalytic reduction of CO. We first coupled the electrocatalytic process with SO-based advanced oxidation processes (AOPs) for the degradation of 4-nitrophenol (4-NP) using a 3D-hexagonal CoO anode. In this step, 4-NP was mineralized to CO, and then the CO was converted to CHOH and CHOH by electrocatalytic reduction using a flower-like CuO cathode. The experimental results show the destruction of 4-NP (60 mL, 10 mg/L) can be as high as 99%. In addition, the yields of CHOH and CHOH were 98.29 μmol/L and 40.95 μmol/L, respectively, which represents a conversion of 41.8% of 4-NP into liquid fuels; the electron efficiency was 73.1%. In addition, we found that 3D-hexagonal arrays of CoO with different morphologies can be obtained by adding different amounts of urea. We also investigated the formation mechanism of novel 3D-hexagonal CoO arrays for the first time. A mechanism was proposed to explain the electrocatalytic steps involved in the conversion of 4-NP to CHOH and CHOH and the synergetic effects between AOPs and electrocatalysis.
开发了一种新型电催化体系，实现了将有机污染物一锅转化为甲醇（CHOH）和乙醇（CHOH）等液体燃料。该过程将有机污染物的催化氧化与 CO 的电催化还原相结合。我们首先将电催化过程与基于 SO 的高级氧化工艺（AOP）耦合，使用 3D 六方 CoO 阳极降解 4-硝基苯酚（4-NP）。在这一步中，4-NP 被矿化为 CO，然后使用花状 CuO 阴极通过电催化还原将 CO 转化为 CHOH 和 CHOH。实验结果表明，4-NP（60mL，10mg/L）的破坏率可高达 99%。此外，CHOH 和 CHOH 的产率分别为 98.29μmol/L 和 40.95μmol/L，这代表 4-NP 中有 41.8%转化为液体燃料；电子效率为 73.1%。此外，我们发现通过添加不同量的尿素可以获得具有不同形态的 3D 六方 CoO 阵列。我们还首次研究了新型 3D 六方 CoO 阵列的形成机制。提出了一种机制来解释 4-NP 转化为 CHOH 和 CHOH 的电催化步骤以及 AOPs 和电催化之间的协同作用。
