School of Chemistry and Chemical Engineering, Wuhan Textile University, Wuhan 430200, China; 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.
J Environ Sci (China). 2024 Mar;137:567-579. doi: 10.1016/j.jes.2023.01.028. Epub 2023 Feb 8.
The design of efficient heterogeneous catalysts in bicarbonate-activated hydrogen peroxide systems (BAP) is a hot topic in wastewater treatment. In this work, CuO nanoparticles with different morphologies including cubic shape (c-CuO), octahedron shape (o-CuO) and spherical shape (s-CuO), were applied in BAP for the first time to degrade tetracycline hydrochloride (TC). Compared with Cu ions and CuO, TC degradation was boosted in the presence of CuO in the BAP system, with the degradation rate following the order c-CuO > o-CuO > s-CuO. The morphology-dependent effects could be linearly correlated with the ratio of surface oxygen species (O), but not with the surface area or Cu(I) ratio. The c-CuO catalyst with exposure of (100) facets contained 76.6% O as the active site for HO adsorption and activation, while the value was much lower for o-CuO and s-CuO with dominant (111) facets. The presence of HCO enhanced the interactions among CuO, HO and TC, leading to facile oxidation of Cu(I) to Cu(II) by HO, and the formation of various reactive species such as hydroxyl radicals and Cu(III) contributed to TC degradation. This work provides a new method for enhancing HO activation with heterogeneous catalysts by crystal facet engineering.
在碳酸氢盐活化过氧氢体系 (BAP) 中设计高效的多相催化剂是废水处理领域的一个热点。本工作首次将具有不同形貌的氧化铜纳米粒子(包括立方体形(c-CuO)、八面体形(o-CuO)和球形(s-CuO))应用于 BAP 中,用于降解盐酸四环素(TC)。与 Cu 离子和 CuO 相比,BAP 体系中存在 CuO 时可促进 TC 的降解,降解速率顺序为 c-CuO > o-CuO > s-CuO。形貌依赖性效应与表面氧物种(O)的比例呈线性相关,而与比表面积或 Cu(I) 比例无关。暴露(100)面的 c-CuO 催化剂含有 76.6%的 O 作为 HO 吸附和活化的活性位,而具有主导(111)面的 o-CuO 和 s-CuO 的 O 含量要低得多。HCO 的存在增强了 CuO、HO 和 TC 之间的相互作用,使得 HO 容易将 Cu(I)氧化为 Cu(II),形成各种活性物质,如羟基自由基和 Cu(III),从而促进 TC 的降解。本工作为通过晶体面工程增强多相催化剂对 HO 的活化提供了一种新方法。