Optimization of Catalytic Properties of Natural Pyrite by Calcination Heat Treatment: Mechanism and Efficacy of Fenton-like Reaction for Degradation of Organic Pollutants.

IF 3.9 2区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
Mengxia Ma,Hepeng Zhou,Xuekun Tang,Muyuan Chang,Xianping Luo
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Abstract

In this study, the catalytic performance of natural pyrite was increased through thermal activation. The degradation efficacy of the PY-250/H2O2 system on Rhodamine B (RhB) was systematically investigated. The results showed that the degradation rate of RhB at 50 mg·L-1 reached 96.4% in 2 min under the combined effect of 0.3 g·L-1 PY-250 and 2.0 mM H2O2, and the apparent rate constant (kobs) was 5.22-fold in comparison with the pyrite/H2O2 system. The PY-250 exhibited excellent adaptability under a broad pH range and effectively mitigated interference from anions and humic acids. Radical scavenging experiments revealed that the reactive oxygen species (ROS) generated within the PY-250/H2O2 system included •OH, 1O2, and •O2-, of which •OH and 1O2 played a primary role in RhB degradation. The excellent catalytic activity of PY-250 is intimately associated with two factors: first, the thermal activation formed surface sulfate, which caused ferrous ions to be induced to dissolve, facilitated the activation of H2O2, and promoted the degradation of RhB via ROS. Second, thermal activation treatment could increase the sulfur vacancies (SVs) on the pyrite, which promotes the cycling of Fe(III)/Fe(II), significantly delaying the deactivation of the catalyst. Therefore, this study provides new material options for the development of green low-cost catalysts to promote the widespread application of Fenton-like catalytic reactions in practical wastewater treatment.
煅烧热处理优化天然黄铁矿的催化性能:类芬顿反应降解有机污染物的机理及效果
本研究通过热活化提高天然黄铁矿的催化性能。系统研究了PY-250/H2O2体系对罗丹明B (Rhodamine B, RhB)的降解效果。结果表明,在0.3 g·L-1 PY-250和2.0 mM H2O2的共同作用下,50 mg·L-1条件下,2 min内RhB的降解率达到96.4%,表观速率常数(kobs)是黄铁矿/H2O2体系的5.22倍。PY-250在较宽的pH范围内表现出良好的适应性,并能有效地减轻阴离子和腐植酸的干扰。自由基清除实验表明,PY-250/H2O2体系中产生的活性氧(ROS)包括•OH、1O2和•O2-,其中•OH和1O2在RhB降解中起主要作用。PY-250优异的催化活性与两个因素密切相关:一是热活化形成表面硫酸盐,诱导亚铁离子溶解,促进H2O2的活化,通过ROS促进RhB的降解。其次,热活化处理增加了黄铁矿上的硫空位(SVs),促进了Fe(III)/Fe(II)的循环,显著延缓了催化剂的失活。因此,本研究为开发绿色低成本催化剂提供了新的材料选择,促进类芬顿催化反应在实际废水处理中的广泛应用。
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来源期刊
Langmuir
Langmuir 化学-材料科学:综合
CiteScore
6.50
自引率
10.30%
发文量
1464
审稿时长
2.1 months
期刊介绍: Langmuir is an interdisciplinary journal publishing articles in the following subject categories: Colloids: surfactants and self-assembly, dispersions, emulsions, foams Interfaces: adsorption, reactions, films, forces Biological Interfaces: biocolloids, biomolecular and biomimetic materials Materials: nano- and mesostructured materials, polymers, gels, liquid crystals Electrochemistry: interfacial charge transfer, charge transport, electrocatalysis, electrokinetic phenomena, bioelectrochemistry Devices and Applications: sensors, fluidics, patterning, catalysis, photonic crystals However, when high-impact, original work is submitted that does not fit within the above categories, decisions to accept or decline such papers will be based on one criteria: What Would Irving Do? Langmuir ranks #2 in citations out of 136 journals in the category of Physical Chemistry with 113,157 total citations. The journal received an Impact Factor of 4.384*. This journal is also indexed in the categories of Materials Science (ranked #1) and Multidisciplinary Chemistry (ranked #5).
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