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通过工程蚀刻策略制备的Co@C多刺纳米盒活化单过硫酸盐促进水中防晒剂二苯甲酰甲烷(BP-2)的去除:一项比较和机理研究

Boosting elimination of sunscreen, Tetrahydroxybenzophenone (BP-2), from water using monopersulfate activated by thorny NanoBox of Co@C prepared via the engineered etching strategy: A comparative and mechanistic investigation.

作者信息

Khiem Ta Cong, Huy Nguyen Nhat, Trang Tran Doan, Wen Jet-Chau, Kwon Eilhann, Chang Hou-Chien, Hu Chechia, Duan Xiaoguang, Lin Kun-Yi Andrew

机构信息

Department of Environmental Engineering & Innovation and Development Center of Sustainable Agriculture, National Chung Hsing University, Taichung, 402, Taiwan.

Faculty of Environment and Natural Resources, Ho Chi Minh City University of Technology (HCMUT), Ho Chi Minh City, 700000, Viet Nam; Vietnam National University Ho Chi Minh City, Ho Chi Minh City, 700000, Viet Nam.

出版信息

Chemosphere. 2023 Jun;327:138469. doi: 10.1016/j.chemosphere.2023.138469. Epub 2023 Mar 22.

Abstract

As sunscreens, benzophenones (BPs), are regarded as emerging contaminants, most of studies are focused on removal of 2-hydroxy-4-methoxybenzophenone (BP-3), which, however, has been employed for protecting skin. Another major class of BPs, which is used to prevent UV-induce degradation in various products, is completely neglected. Thus, this present study aims to develop a useful advanced oxidation process (AOP) for the first time to eliminate such a class of BP sunscreens from contaminated water. Specifically, 2,2',4,4'-Tetrahydroxybenzophenone (BP-2) would be focused here as BP-2 is intensively used in perfumes, lipsticks, and plastics for preventing the UV-induced degradation. As monopersulfate (MPS)-based AOP is practical for degrading emerging contaminants, a facile nanostructured cobalt-based material is then developed for maximizing catalytic activities of MPS activation by immobilizing Co nanoparticles onto carbon substrates. In particular, ZIF-67 is employed as a template, followed by the etching and carbonization treatments to afford the thorny nanobox of Co@C (TNBCC) with the hollow-nanostructure. In comparison to the solid (non-hollow) nanocube of Co@C (NCCC) from the direct carbonization of ZIF-67, TNBCC possesses not only the excellent textural features, but also superior electrochemical properties and highly reactive surfaces, making TNBCC exhibit the significantly higher catalytic activity than NCCC as well as CoO in activating MPS to degrade BP-2. Mechanisms of BP-2 degradation are also elucidated and ascribed to both radical and non-radical routes. These advantageous features make TNBCC a useful catalyst of activating MPS in BP-2 degradation.

摘要

作为防晒剂,二苯甲酮(BPs)被视为新兴污染物,大多数研究都集中在去除2-羟基-4-甲氧基二苯甲酮(BP-3)上,然而,BP-3已被用于保护皮肤。另一类主要的二苯甲酮用于防止各种产品中的紫外线诱导降解,但却完全被忽视了。因此,本研究旨在首次开发一种有效的高级氧化工艺(AOP),以从受污染的水中去除这类二苯甲酮防晒剂。具体来说,这里将重点研究2,2',4,4'-四羟基二苯甲酮(BP-2),因为BP-2被广泛用于香水、口红和塑料中以防止紫外线诱导的降解。由于基于单过硫酸盐(MPS)的AOP在降解新兴污染物方面具有实用性,因此开发了一种简便的纳米结构钴基材料,通过将钴纳米颗粒固定在碳基底上来最大化MPS活化的催化活性。特别地,采用ZIF-67作为模板,随后进行蚀刻和碳化处理,以得到具有中空纳米结构的Co@C刺状纳米盒(TNBCC)。与通过ZIF-67直接碳化得到的Co@C实心(非中空)纳米立方体(NCCC)相比,TNBCC不仅具有优异的结构特征,还具有优异的电化学性能和高反应性表面,使得TNBCC在活化MPS降解BP-2方面表现出比NCCC以及CoO更高的催化活性。还阐明了BP-2降解的机制,并将其归因于自由基和非自由基途径。这些有利特性使TNBCC成为BP-2降解中活化MPS的有用催化剂。

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