ACS ES&T Engineering
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2023
·
IF 7.1
Dezhen Kong,Yumeng Zhao,Hongdi Guo,Mei Han,Xinru Fan,Jinkuo Li,Xu He,Jun Ma
The demands for high-efficient and green activation of peracetic acid (PAA) have triggered research in exploring carbon catalysis. Nevertheless, the efforts in designing reaction-oriented and high-performance carbon catalysts are largely impeded by an ambiguous understanding of the fundamental carbon structure–PAA activation performance relationship. Herein, we investigated the quantitative structure–activity relationship (QSAR) of carbon nanotubes (CNTs) for PAA activation and micropollutant (MP) removal, by tuning the physiochemical properties of CNT via thermal annealing. The CNT/PAA system was dominated by the nonradical direct electron transfer (DET) oxidation pathway, showing high MP removal rates under complex water matrices. By conducting QSAR analysis, improved catalytic efficacy of the surface-regulated CNTs was attributed to the reinforced DET via the elevated oxidative potential of the CNT–PAA complex and the enhanced electrical conductivity of CNT. Furthermore, the larger specific surface area and lower oxygen content of CNT gave rise to the elevated oxidative potential of the CNT–PAA complex, while the electrical conductivity of CNT was positively correlated with the graphitization degree of CNT. Overall, this work sheds light on the influence cascade of the physicochemical properties of CNT for MP removal and PAA activation, providing guidelines for the fit-for-purpose design of the DET-mediated carbon catalysts for PAA oxidation.
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Advanced Science
·
2023
·
IF 15.1
Yuqian Qiao,Shuilin Wu,Yufeng Zheng,Chaofeng Wang,Zhaoyang Li,Yu Zhang,Shengli Zhu,Hui Jiang,Zhenduo Cui,Xiangmei Liu
Microwave (MV)-trigged dynamic therapy based on MV-responsive materials is promising for treating deep infection diseases that cannot be effectively treated by antibiotics, like life-threatening osteomyelitis. Surface states of materials affect the generation of free charges under the excitation source with energy less than the band gap, consequently influencing the MV dynamic effects. Herein, an MV responsive system with interface confined 2D metal–organic framework (2D MOF) on oxidized carbon nanotube (CNT) is prepared, in which the ultrasmall Cu-based 2D MOF possesses sufficient surface/interface defects, endowing the system a large number of surface states. Under MV irradiation, the synthesized CNT-2D MOF not only efficiently absorbs and converts the microwave into heat for microwaveocaloric therapy (MCT) via enhanced hetero-interfacial polarization, but also generates excited electrons via surface state for microwave dynamic therapy (MDT). This biocompatible CNT-2D MOF exhibits highly effective broad-spectrum antimicrobial activity against seven pathogenic bacteria, including Gram-negative and Gram-positive pathogens, under 7 min MV irradiation. And this system is proven to efficiently eradicate Staphylococcus aureus infected rabbit tibia osteomyelitis. Significantly, MV-excited MCT and MDT of CNT-CuHHTP developed in this study makes a major step forward in antibiotic-free MV therapy in deep tissue bacterial infection diseases.
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npj Clean Water
·
2023
·Vol. 6
·期 1
·1-10
·
IF 11.4
Li Meng,Song Jiayu,Han Wei,Yeung King Lun,Zhou Shaoqi,Mo Ce-Hui
Although Fenton-like reactions have been extensively used to treat various organic contaminants in wastewaters (oily wastewaters, landfill leachate, denitrification with Fenton oxidized non-degradable large molecular organic pollutants, and removal of phosphorus, etc.), the difficulty in catalyst recovery and the instability of catalytic activity limit their practical application. Herein, iron atoms were inserted in a metal-organic framework (FeNC) with dual reaction sites as highly reactive and stable electro-Fenton-like catalysts for the catalytic oxidation of organic pollutants via the electro-Fenton-like activation reaction of peroxymonosulfate (PMS) with fractional leaching of metal ions. Experiments and density functional theory (DFT) calculations indicate that FeNC with FeN 4 and Fe–Fe active sites can rapidly deliver electrons for PMS dissociation. Further, an electrolysis reactor was constructed for the on-site generation of reactive oxygen species, which can stably and continuously purify various organic wastewaters. The combined use of an electrolysis reactor and magnetic catalyst in the current study provides a direction for the long-term remediation of organic pollutants on an industrial scale.
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Catalysts
·
2023
·Vol. 13
·期 5
·847
·
IF 3.9
Zhen Li,Wenxuan Jiang,Jingwen Huang,Yawen Wang,He Guo
This paper aims to investigate the promotion of persulfate (PS) activation by ZnO in discharge plasma systems for the degradation of ofloxacin (OFX). Scanning electron microscopy and transmission electron microscopy showed that ZnO nanoparticles were successfully prepared by a hydrothermal method. With an increase in the PS dosage, the removal efficiency of OFX first increased and then decreased. With an increase in the ZnO dosage, the removal efficiency of OFX showed a similar trend. Under the optimum 595 mg/L PS dosage and 295 mg/L ZnO dosage, the removal efficiency of OFX by plasma, plasma/ZnO, and plasma/ZnO/PS systems reached 53.6%, 82.8%, and 98.9%, respectively. Increasing the input power was beneficial to the degradation of OFX. ESR results showed that the addition of ZnO could further stimulate PS to produce more ·OH and ·SO4−than that of plasma alone. The capture agent experiment proved that ·OH, ·SO4−, ·O2−, and1O2all participated in the degradation of OFX. A total organic carbon (TOC) removal of 49.6% was obtained in the plasma/ZnO/PS system. Based on liquid chromatography-mass spectrometry (LC-MS) and the Toxicity Estimation Software Tool (TEST), degradation pathways and toxicity were analyzed. Compared to other technologies, it can be concluded that the plasma/ZnO/PS system is a promising technology for pollutant remediation.
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Arabian Journal of Chemistry
·
2023
·
IF 6
Lei Yang,Hong Huang,Ting Wang,Danling Zhou,Qing Chen,Dan Li,Shuzi Chen,Ping Lin
Endoplasmic reticulum, the largest cellular organelle where protein synthesis, folding, transportation, and the maintenance of Ca 2+ homeostasis occurred, is sensitive to the imbalance of its inner environment. Particularly, overproduction of reactive oxygen species in endoplasmic reticulum region can initiate endoplasmic reticulum stress and is tightly related to many metabolic diseases. In this respect, to retain normal function of endoplasmic reticulum, it is highly important to synthesize antioxidants with endoplasmic reticulum-targeting capability for precisely clearing excessively generated reactive oxygen species in endoplasmic reticulum. Herein, we demonstrate the preparation of endoplasmic reticulum-targeting Se-doped carbon nanodots and assays with HeLa cells as well as in vivo tests with mice have shown that the prepared carbon nanodots can significantly eliminate both •OH and O 2 •− . Experimental results declared that the fabricated carbon nanodots with powerful scavenging capabilities toward •OH and O 2 •- , low cytotoxicity and endoplasmic reticulum targetability can be utilized to protect cells against raised levels of reactive oxygen species in endoplasmic reticulum. What’s more, the fabricated carbon nanodots effectively alleviated phorbol 12-myristate 13-acetate induced ear inflammation in live mice.
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Advanced Healthcare Materials
·
2023
·
IF 10
Yi Lu,Xinni Pan,Cheng Cao,Shanshan Fan,Haisong Tan,Shengsheng Cui,Yanlei Liu,Daxiang Cui
As one of the most widely used drugs, acetaminophen, is the leading cause of acute liver injury. In addition, acetaminophen-induced liver injury (AILI) has a strong relationship with the overproduced reactive oxygen species, which can be effectively eliminated by nanozymes. To address these challenges, mesoporous PdPt@MnO 2 nanoprobes (PPM NPs) mimicking peroxide, catalase, and superoxide dismutase-like properties are synthesized. They demonstrate nontoxicity, high colloidal stability, and exceptional reactive oxygen species (ROS)-scavenging ability. By scavenging excessive ROS, decreasing inflammatory cytokines, and inhibiting the recruitment and activation of monocyte/macrophage cells and neutrophils, the pathology mechanism of PPM NPs in AILI is confirmed. Moreover, PPM NPs’ therapeutic effect and good biocompatibility may facilitate the clinical treatment of AILI.
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ADVANCED FUNCTIONAL MATERIALS
·
2023
·Vol. 33
·期 40
·2302816
·
IF 19
Hui Zhang,Yinkun Sun,Junjie Yang,Zhiyu Sun,Yanxin Zhao,Xin Li,Wei Wang,Dongwei Lu,Jun Ma
Precise adjustment of the pore size, damage repair, and efficient cleaning is all challenges for the wider application of inorganic membranes. This study reports a simple strategy of combining dry-wet spinning and electrosynthesis to fabricate stainless-steel metal–organic framework composite membranes characterized by customizable pore sizes, targeted reparability, and high catalytic activity for membrane cleaning. The membrane pore size can be precisely customized in the range of 14–212 nm at nanoscale, and damaged membranes can be repaired by targeted treatment in 120 s. In addition, advanced oxidation processes can be used to quickly clean the membrane and achieve 98% flux recovery. The synergistic actions of the membrane matrix and the selective layer increase the adsorption energy of active sites to oxidant, shorten the electron transfer cycle, and enhance the overall catalytic performance. This study can provide a new direction for the development of advanced membranes for water purification and high-efficiency membrane cleaning methods.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Kaiyuan Luo,Yang Shi,Rongfu Huang,Xipeng Wei,Zelin Wu,Peng Zhou,Heng Zhang,Yin Wang,Zhaokun Xiong,Bo Lai
Periodate (PI) has recently been studied as an excellent oxidant in advanced oxidation processes , and its reported mechanism is mainly the formation of reactive oxygen species (ROS). This work presents an efficient approach using N-doped iron-based porous carbon (Fe@N-C) to activate periodate for the degradation of sulfisoxazole (SIZ). Characterization results indicated the catalyst has high catalytic activity , stable structure, and high electron transfer activity. In terms of degradation mechanism, it is pointed out that the non-radical pathway is the dominant mechanism. In order to prove this mechanism, we have carried out scavenging experiments, electron paramagnetic resonance (EPR) analysis, salt bridge experiments and electrochemical experiments, which demonstrate the occurrence of mediated electron transfer mechanism. Fe@N-C could mediate the electron transfer from organic contaminant molecules to PI, thus improving the efficiency of PI utilization, rather than simply inducing the activation of PI through Fe@N-C. The overall results of this study provided a new understanding into the application of Fe@N-C activated PI in wastewater treatment .
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ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Fu He,Dan Zhong,Wencheng Ma,Yixing Yuan,Kefei Li,Changlei Dai
The main compositions of pipe deposits from water distribution networks are potential iron resources, which can be used as catalysts to activate the combined hydrogen peroxide (HP) and peroxymonosulphate (PMS) system to produce reactive oxidative species (ROSs) to degrade pollutants. As a result, the degradation efficiency of chloramphenicol (CAP) in the HP/PMS dual-oxidant system could reach as high as 75.21% within 100 min with hydroxylamine (HA) assistance, and the dual-oxidant method had a wide pH applied range. To explore the mechanism of the dual-oxidant system in detail, several main affecting factors were investigated. In addition, the hydroxyl radical(•OH) was identified as the predominant radicals by Electron paramagnetic resonance (EPR) and the Radical scavenger test (RST). According to the competition kinetics experiment, the reaction rate of CAP with •OH was 1.933(± 0.052) × 1010 M−1s−1 in the HP/PMS dual-oxidant system, which was higher than the HP single oxidant system (6.10(± 0.036) × 109 M−1s−1). And the role of HA was explored , including reduction and competition. Six degradation products were detected by the liquid chromatography-mass spectrometry (LC-MS) and their toxicity was analyzed by the ecological structure-activity relationship (ECOSAR) predictive model. These findings further provide a theoretical basis for the practical application of pipe deposits and advance the development of in-situ removal of pollutants in water distribution networks in the future promisingly.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Jiewen Deng,Jieli Ou,Zhenran Wang,Yongsheng Fu,Yiqing Liu
Since limitedly existing researches suggested Cu(II) had deficiently catalytic ability to PAA, in this work, we tested the oxidation performance of Cu(II)/PAA system on diclofenac (DCF) degradation under neutral conditions. It was found that overwhelming DCF removal could be obtained in Cu(II)/PAA system at pH 7.4 using phosphate buffer solution (PBS) compared to poor loss of DCF without PBS, and the apparent rate constant of DCF removal in PBS/Cu(II)/PAA system was 0.0359 min − 1 , 6.53 times of that in Cu(II)/PAA system. Organic radicals (i.e., CH 3 C(O)O• and CH 3 C(O)OO•) were evidenced as the dominant contributors to DCF destruction in PBS/Cu(II)/PAA system. PBS motivated the reduction of Cu(II) to Cu(I) through chelation effect, and then the activation of PAA by Cu(I) was facilitated. Besides, due to the steric hindrance of Cu(II)-PBS complex (CuHPO 4 ), PAA activation was mediated from non-radical-generating pathway to radical-generating pathway, leading to desirably effective DCF removal by radicals. The transformation of DCF mainly experienced hydroxylation, decarboxylation , formylation and dehydrogenation in PBS/Cu(II)/PAA system. This work proposes the potential of coupling of phosphate and Cu(II) in optimizing PAA activation for organic pollutants elimination .
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wei Chen,Xinning Dai,Zhujun Liu,Bin Du,Xinyu Zheng,Dandan Ma,Xianbin Huang
Periodate-based advanced oxidation processes (PI-AOPs) exhibited a promising future for the reduction of emerging refractory organic pollutants . However, the underlying mechanism and the sulfuretted effect of sulfide-modified metal silicate materials for PI activation were still unclear. In this study, sulfide-modified metal silicates (S-CoSi) were first synthesized and applied in the PI-AOPs system. Different from traditional metal silicate materials, sulfurization improved the catalytic performance. The enhanced degradation performance was from the increase in specific surface area and charge transfer efficiency, which derived from the sulfurization in metal silicate. DFT calculations revealed that the enhanced charge densities of Co-S bonds promoted the existence of Co (Ⅱ), which was more conducive to PI activation. Experimental and calculation results further demonstrated that Co was the active site in S-CoSi, and sulfur species strengthened the radical pathway by assisting Co (Ⅱ) regeneration (electron transfer from S to Co) rather than participating in the PI activation. Moreover, sulfurization promoted the generation of 1 O 2 (non-radical pathway) by increasing oxygen vacancy in the metal silicate. This study provided new insights into the effect of sulfurization on the radical and non-radical pathways in the metal silicates PI system.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Xin Liu,Peng Xu,Zhuoyu Yang,Pengfei Zhu,Baolin Hou
Zero-valent copper/air process was studied in degrading contaminants owing to in-site generation of hydrogen peroxide and reactive oxygen species, while its oxidation efficacy was restrained by the dismutation of cuprous ion. In this study, when the dosages of paracetamol, ferric ion, chloride ion and zero-valent copper were respectively 10 μM, 40 μM, 2 mM and 0.2 g/L at pH 3.0, the paracetamol elimination was greatly enhanced and increased from 9.2% to 76.5% within 30 min with adding both ferric ion and chloride ion in the zero-valent copper/air process. Hydroxyl radical and reactive chlorine species were identified as the dominant reactive oxygen species, and the contribution rates of hydroxyl radical and reactive chlorine species to eliminating paracetamol were respectively 68.2% and 28.9%. In the proposed system, zero-valent copper and cuprous ion expedited the ferric/ferrous circulation, conducing to the production of reactive oxygen species. Moreover, chloride ion coupled with cuprous ion producing the cuprous chloride complexes, and chloride ion contributed to the comproportionation between zero-valent copper with cupric ion to form cuprous chloride, receding the dismutation of cuprous ion and contributing to the formation of hydrogen peroxide and reactive oxygen species. When zero-valent copper reused for three times in the proposed system, the degradation of paracetamol reached 62%. After we increased the end pH to > 7.0 and leaching, the total copper of reaction solution was under 0.85 mg/L and the acute toxicity had no insignificant increase for discharge water. The study provided a new idea to enhance zero-valent copper/air system for the purification of pollutants.
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