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A new catalyst derived from the sulfur-doped metal-organic framework for Fenton-like reaction
Process Safety and Environmental Protection ( IF 6.9 ) Pub Date : 2024-09-21 , DOI: 10.1016/j.psep.2024.09.082 Jiawu Liu, Jianfeng Zhang, Shaofei Weng, Ziyue Xu, Yixin Zhang, Ting Hou, Weihuang Zhu
Process Safety and Environmental Protection ( IF 6.9 ) Pub Date : 2024-09-21 , DOI: 10.1016/j.psep.2024.09.082 Jiawu Liu, Jianfeng Zhang, Shaofei Weng, Ziyue Xu, Yixin Zhang, Ting Hou, Weihuang Zhu
Fenton-like reaction exhibits considerable advantages in the remediation of pollutants. To fabricate an efficient catalyst becomes an issue concerning the performance enhancement in Fenton-like reaction. Herein, S-Fe-MOF-400 which was derived from a sulfur-doped metal-organic framework (Fe-MOF), was newly prepared and exhibited high ability for H2 O2 activation during Fenton-like reaction. The results showed that the sulfurization effectively reduced the charge transfer resistance (R ct ) of S-Fe-MOF-400, and facilitated the charge transfer, consequently enhancing the catalytic performance of S-Fe-MOF-400 in the Fenton-like reaction. XRD analysis revealed that FeS2 was the predominant reactive component in S-Fe-MOF-400 with a regular cubic structure and pronounced crystallinity. Additionally, the presence of low-valent sulfur ensured the availability of Fe (II), thereby facilitating the occurrence of the Fenton reaction. Under optimal conditions, the removal efficiency of pollutants reached 86.7 % within 60 min, resulting in total organic carbon (TOC) removal efficiency at 40.6 %. Quenching experiments and electron paramagnetic resonance (EPR) detections revealed that • OH, 1 O2 , and O 2 • − synergistically participated in the Fenton-like reaction, with • OH being the primary active species. The activation process of H2 O2 induced by S-Fe-MOF-400 mainly yielded hydroxyl radicals and superoxide radicals. The 1 O2 was generated through two following pathways: (i) the transformation of superoxide and hydroxyl radicals, and (ii) the conversion of natural oxygen molecules (O2 ). This current study illustrated the significant potential for the application of sulfur-modified Fe-MOF in the Fenton-like reaction for pollutant removal.
中文翻译:
一种源自硫掺杂金属有机框架的新型催化剂,用于 Fenton 类反应
Fenton 样反应在污染物修复方面表现出相当大的优势。制备高效催化剂成为 Fenton 类反应性能增强的问题。本文新制备了源自硫掺杂金属有机框架 (Fe-MOF) 的 S-Fe-MOF-400,并在 Fenton 样反应中表现出很高的 H2O2 活化能力。结果表明,硫化作用有效降低了 S-Fe-MOF-400 的电荷转移电阻 (Rct),促进了电荷转移,从而提高了 S-Fe-MOF-400 在 Fenton 类反应中的催化性能。XRD 分析表明,FeS2 是 S-Fe-MOF-400 中的主要反应组分,具有规则的立方结构和明显的结晶度。此外,低价硫的存在确保了 Fe (II) 的可用性,从而促进了 Fenton 反应的发生。在最佳条件下,污染物去除效率在 60 分钟内达到 86.7 %,总有机碳 (TOC) 去除效率为 40.6 %。淬灭实验和电子顺磁共振 (EPR) 检测表明,•OH、1O2 和 O2•− 协同参与了 Fenton 样反应,•OH 是主要的活性物质。S-Fe-MOF-400 诱导的 H2O2 活化过程主要产生羟基自由基和超氧自由基。1O2 是通过以下两种途径产生的:(i) 超氧和羟基自由基的转化,以及 (ii) 天然氧分子 (O2) 的转化。目前的这项研究说明了硫改性的 Fe-MOF 在 Fenton 样反应中去除污染物的巨大应用潜力。
更新日期:2024-09-21
中文翻译:
一种源自硫掺杂金属有机框架的新型催化剂,用于 Fenton 类反应
Fenton 样反应在污染物修复方面表现出相当大的优势。制备高效催化剂成为 Fenton 类反应性能增强的问题。本文新制备了源自硫掺杂金属有机框架 (Fe-MOF) 的 S-Fe-MOF-400,并在 Fenton 样反应中表现出很高的 H2O2 活化能力。结果表明,硫化作用有效降低了 S-Fe-MOF-400 的电荷转移电阻 (Rct),促进了电荷转移,从而提高了 S-Fe-MOF-400 在 Fenton 类反应中的催化性能。XRD 分析表明,FeS2 是 S-Fe-MOF-400 中的主要反应组分,具有规则的立方结构和明显的结晶度。此外,低价硫的存在确保了 Fe (II) 的可用性,从而促进了 Fenton 反应的发生。在最佳条件下,污染物去除效率在 60 分钟内达到 86.7 %,总有机碳 (TOC) 去除效率为 40.6 %。淬灭实验和电子顺磁共振 (EPR) 检测表明,•OH、1O2 和 O2•− 协同参与了 Fenton 样反应,•OH 是主要的活性物质。S-Fe-MOF-400 诱导的 H2O2 活化过程主要产生羟基自由基和超氧自由基。1O2 是通过以下两种途径产生的:(i) 超氧和羟基自由基的转化,以及 (ii) 天然氧分子 (O2) 的转化。目前的这项研究说明了硫改性的 Fe-MOF 在 Fenton 样反应中去除污染物的巨大应用潜力。