Hubei Key Laboratory of Biomass Fibers and Eco-dyeing and Finishing, Wuhan Textile University, Wuhan 430200, China; School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430200, China.
School of Environmental Engineering, Wuhan Textile University, Wuhan 430200, China.
J Environ Sci (China). 2023 Feb;124:350-359. doi: 10.1016/j.jes.2021.09.035. Epub 2022 Feb 3.
Sulfite (SO) activation is one of the most potential sulfate-radical-based advanced oxidation processes, and the catalysts with high efficiency and low-cost are greatly desired. In this study, the cobalt nanoparticles embedded in nitrogen-doped graphite layers (Co@NC), were used to activate SO for removal of Methyl Orange in aqueous solution. The Co@NC catalysts were synthesized via pyrolysis of Co-based metal-organic framework (Co-MOF), where CoO was firstly formed at 400℃ and then partially reduced to Co nanoparticles embedded in carbon layers at 800℃. The Co@NC catalysts were more active than other cobalt-based catalysts such as Co, CoO and CoFeO, due to the synergistic effect of metallic Co and CoO. A series of chain reaction between Co species and dissolved oxygen was established, with the production and transformation of SO, SO, and subsequent active radicals SO and HO•. In addition, HCO was found to play a key role in the reaction by complexing with Co species on the surface of the catalysts. The results provide a new promising strategy by using the Co@NC catalyst for SO oxidation to promote organic pollutants degradation.
亚硫酸盐(SO)活化是最具潜力的硫酸盐自由基类高级氧化工艺之一,因此需要开发高效、低成本的催化剂。本研究采用氮掺杂石墨层中嵌入钴纳米颗粒(Co@NC)作为催化剂,用于活化 SO 去除水溶液中的甲基橙。Co@NC 催化剂通过钴基金属有机骨架(Co-MOF)的热解合成得到,其中 CoO 首先在 400℃下形成,然后在 800℃下部分还原为嵌入碳层的 Co 纳米颗粒。由于金属 Co 和 CoO 的协同作用,Co@NC 催化剂比其他钴基催化剂(如 Co、CoO 和 CoFeO)具有更高的活性。一系列 Co 物种与溶解氧之间的链式反应建立起来,产生并转化了 SO、SO、随后的活性自由基 SO 和 HO•。此外,发现 HCO 通过与催化剂表面的 Co 物种络合,在反应中起着关键作用。该结果为利用 Co@NC 催化剂氧化 SO 以促进有机污染物降解提供了一种有前景的新策略。