Liao Weixiang, Lyu Lai, Wang Di, Hu Chun, Li Tong
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China.
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China; School of Energy and Environmental Engineering, University of Science and Technology Beijing, Beijing 100083, China.
J Environ Sci (China). 2023 Apr;126:565-574. doi: 10.1016/j.jes.2022.05.022. Epub 2022 May 22.
Excessive consumption of energy and resources is a major challenge in wastewater treatment. Here, a novel heterogeneous Fenton-like catalyst consisting of Cu-doped graphene-like catalysts (Cu-GCD NSs) was first synthesized by an enhanced carbothermal reduction of β-cyclodextrin (β-CD). The catalyst exhibits excellent Fenton-like catalytic activity for the degradation of various pollutants under neutral conditions, accompanied by low HO consumption. The results of structural characterization and theoretical calculations confirmed that the dual reaction centers (DRCs) were constructed on Cu-GCD NSs surface through C-O-Cu bonds supported on zero-valent copper species, which play a significant role in the high-performance Fenton-like reaction. The pollutants that served as electron donors were decomposed in the electron-poor carbon centers, whereas HO and dissolved oxygen obtained these electrons in the electron-rich Cu centers through C-O-Cu bonds, thereby producing more active species. This study demonstrates that the electrons of pollutants can be efficiently utilized in Fenton-like reactions by DRCs on the catalyst surface, which provides an effective strategy to improve Fenton-like reactivity and reduce HO consumption.
能源和资源的过度消耗是废水处理中的一项重大挑战。在此,首次通过β-环糊精(β-CD)的强化碳热还原合成了一种由铜掺杂类石墨烯催化剂(Cu-GCD NSs)组成的新型非均相类芬顿催化剂。该催化剂在中性条件下对各种污染物的降解表现出优异的类芬顿催化活性,同时HO消耗量较低。结构表征和理论计算结果证实通过负载在零价铜物种上的C-O-Cu键在Cu-GCD NSs表面构建了双反应中心(DRCs),这在高性能类芬顿反应中发挥了重要作用。作为电子供体的污染物在缺电子的碳中心分解,而HO和溶解氧通过C-O-Cu键在富电子的铜中心获得这些电子,从而产生更多活性物种。本研究表明,催化剂表面的DRCs可在类芬顿反应中有效利用污染物的电子,这为提高类芬顿反应活性和减少HO消耗提供了一种有效策略。