Key Laboratory of Microorganism Application and Risk Control of Shenzhen, Guangdong Provincial Engineering Research Center for Urban Water Recycling and Environmental Safety, Shenzhen Key Laboratory of Ecological Remediation and Carbon Sequestration, Institute of Environment and Ecology, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, China.
Division of Chemical Research, National Institute of Environmental Research, Incheon 22689, Republic of Korea.
Water Res. 2024 Dec 1;267:122505. doi: 10.1016/j.watres.2024.122505. Epub 2024 Sep 23.
The KrCl* excimer lamp (UV222) is a promising alternative of low-pressure mercury lamp (UV254) for UV-based advanced oxidation processes (UV-AOPs), because it is mercury-free and has high photon energy. But there lacks a comprehensive assessment of UV222-AOPs based on different radicals. Herein, the properties (e.g., oxidant decay and innate radical quantum yield), and micropollutant degradation, were comprehensively studied for representative oxidants (i.e., hydrogen peroxide, persulfate (PDS), monochloramine, and free active chlorine (FAC)) under UV222 irradiation. UV222 outperformed UV254 for the activation of oxidants with 2.6-14.4 times fluence-based kinetic constant (k). The main reason of enhanced activation varied with oxidants: higher UV absorbance for HO, higher innate quantum yield for monochloramine and FAC, and both reasons for PDS. Overall, PDS was the optimum oxidant under UV222 for the degradation of 8 representative micropollutants because of effective promotion of radical formation, as confirmed by radical competitive kinetics and modeling simulations. In real water, UV222/PDS still show advantages than UV254/PDS in terms of micropollutant elimination efficacy (3.2-5.3 times) and energy consumption (33.9 %-57.6 % lower) though it was more inhibited by water constituents via competing for UV222 photons. This study fills gaps in photochemistry knowledge and will facilitate engineering practice of UV222-AOPs.
KrCl* 准分子灯(UV222)是一种很有前途的低压汞灯(UV254)替代品,可用于基于紫外线的高级氧化工艺(UV-AOPs),因为它不含汞且具有高光子能量。但目前缺乏基于不同自由基的 UV222-AOPs 的综合评估。在此,针对代表性氧化剂(即过氧化氢、过硫酸盐(PDS)、一氯胺和游离活性氯(FAC)),在 UV222 辐照下,从性质(如氧化剂衰减和固有自由基量子产率)和微污染物降解两方面对其进行了综合研究。与 UV254 相比,UV222 辐照下的氧化剂的激活具有 2.6-14.4 倍的基于辐照量的动力学常数(k)。增强激活的主要原因因氧化剂而异:HO 的 UV 吸光度更高,一氯胺和 FAC 的固有量子产率更高,而 PDS 则兼具两者的原因。总体而言,由于自由基形成的有效促进,PDS 是 UV222 下 8 种代表性微污染物降解的最佳氧化剂,这一点得到了自由基竞争动力学和模拟模拟的证实。在实际水体中,尽管 UV222 会因与 UV222 光子竞争而受到更多抑制,但与 UV254/PDS 相比,UV222/PDS 在微污染物去除效率(高 3.2-5.3 倍)和能耗(低 33.9%-57.6%)方面仍具有优势。本研究填补了光化学知识的空白,将有助于促进 UV222-AOPs 的工程实践。