Shanghai Key Lab of Chemical Assessment and Sustainability, School of Chemical Science and Engineering, Tongji University, 1239 Siping Road, Shanghai, 200092, China.
The institute of Scientific and Industrial Research, Osaka University, Mihogaoka 8-1, Ibaraki, Osaka, 567-0047, Japan.
Angew Chem Int Ed Engl. 2021 Apr 26;60(18):10375-10383. doi: 10.1002/anie.202101804. Epub 2021 Mar 22.
We reported the selective electrochemical reduction of oxygen (O ) to hydroxyl radicals ( OH) via 3-electron pathway with FeCo alloy encapsulated by carbon aerogel (FeCoC). The graphite shell with exposed -COOH is conducive to the 2-electron reduction pathway for H O generation stepped by 1-electron reduction towards to OH. The electrocatalytic activity can be regulated by tuning the local electronic environment of carbon shell with the electrons coming from the inner FeCo alloy. The new strategy of OH generation from electrocatalytic reduction O overcomes the rate-limiting step over electron transfer initiated by reduction-/oxidation-state cycle in Fenton process. Fast and complete removal of ciprofloxacin was achieved within 5 min in this proposed system, the apparent rate constant (k ) was up to 1.44±0.04 min , which is comparable with the state-of-the-art advanced oxidation processes. The degradation rate almost remains the same after 50 successive runs, suggesting the satisfactory stability for practical applications.
我们报道了通过碳气凝胶（FeCoC）封装的 FeCo 合金选择性地将氧气（O ）电化学还原为羟基自由基（OH ），通过 3 电子途径。具有暴露的-COOH 的石墨壳有利于 H O 通过 1 电子还原向 OH 生成的 2 电子还原途径。通过来自内 FeCo 合金的电子来调节碳壳的局部电子环境，可以调节电催化活性。通过电催化还原 O 生成 OH 的新策略克服了 Fenton 过程中由还原/氧化态循环引发的电子转移的限速步骤。在该提出的系统中，环丙沙星在 5 分钟内即可快速完全去除，表观速率常数（k ）高达 1.44±0.04 min ，与最先进的高级氧化工艺相当。在 50 次连续运行后，降解速率几乎保持不变，表明该系统具有良好的实际应用稳定性。
