Journal of Water Process Engineering
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2023
·
IF 7
Jingyang Li,Haiyu Cao,Hongying Qi,Yuexiang Li,Sha Zhu,Xue Ye,Jintao Zhang,Zifeng Yu,Jiao Zhu,Xin Zhao
A series of CoFe-LDHs@MoS 2 -x (x = 0.1, 0.2 and 0.5) samples were successfully synthesized to activate peroxymonosulfate (PMS) for tetracycline (TC) removal. With the introduction of MoS 2 could promote the catalytic performance via accelerating the Fe 2+ /Fe 3+ and Co 2+ /Co 3+ cycle. About 98.8 % of TC could be removed over 12 min under a neutral condition in the CoFe-LDHs@MoS 2 -0.2/PMS system, which was 4.4 times higher than that of CoFe-LDHs/PMS system. The main reactive oxygen species (ROS) in CoFe-LDHs@MoS 2 -0.2/PMS system were also explored by using quenching and free radical capture experiments. The singlet oxygen ( 1 O 2 ) played a major role for the TC removal. Besides, the decomposition pathways of TC were deduced by UPLC-QTOF/MS, and the stability of catalysts had also been studied. This work provided theoretical and experimental basis for designing and preparation more effective heterogeneous catalysts for PMS activation .
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MOLECULES
·
2023
·Vol. 28
·期 10
·4237
·
IF 4.6
Zhiyao Zhang,Zhaolin Li,Xue Bai,Juan Shi,Min Hu,Jin Chai,Keqian Li,Pengkang Jin
Commonly used peroxydisulfate (PS) or peroxymonosulfate (PMS) activation methods have been limited in their practical application due to certain drawbacks, such as high cost, high energy consumption and secondary pollution. In this study, a catalyst-free alizarin green (AG) self-activating PMS catalytic system was constructed based on photosensitization properties of dye, which ultimately achieved efficient degradation of the dye activator, also the target pollutant. Here, 52.5% of the 100 mL mixture of 10 mg/L AG decomposed within 60 min with 1 mM PMS under visible-light irradiation, thereby showing a strong pH adaptation. Mechanism of AG self-activating PMS was revealed that the photo-excited AG can effectively transfer photo-induced electrons to PMS for its activation, which generates reactive oxidizing species dominated by singlet oxygen (1O2), and supplemented by hydroxyl radical (•OH), superoxide radical (O2•−) and sulfate radical (SO4•−) to realize the efficient self-degradation of the dye pollutants. Moreover, such self-catalytic system operated well under natural sunlight irradiation, indicating the great application potential in the actual wastewater treatment. Herein, photosensitive dye acted as an ideal PMS activator realizing its efficient self-degradation, which provides a novel idea of “using waste to treat waste” for developing wastewater treatment process in a high-efficiency and low-consumption way.Keywords:alizarin green dye;photosensitization;PMS;catalysis;using waste to treat waste
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Journal of Water Process Engineering
·
2023
·
IF 7
Lu Qin,Dongqi Wang,Cong Liu,Guodong Chai,Mingliang Fang,Jiake Li,Hui Wang,Zhe Wang,Haiyu Meng,Xing Zheng,Mengbo Huang,Yi Xiao,Yishan Lin,Long Chen
Aqueous pathogenic microorganisms pose a significant risk to public health, but conventional disinfection methods present numerous drawbacks. By employing bactericidal tests, radical quenching experiments, and quantitative toxicogenomic assay, this study aimed to evaluate the effectiveness and associated cellular mechanism of a novel disinfection process combining recyclable copper ferrite (CuFe 2 O 4 ) nanoparticles with sulfite. At the optimal CuFe 2 O 4 (800 mg/L) and sulfite (4 mM) concentrations determined, the CuFe 2 O 4 /sulfite system inactivated 4.65-log (>99.99 %) of Escherichia coli cells at an initial concentration of 10 8 colony-forming units (CFU)/mL in 3 h. Meanwhile, the E. coli cells at the initial concentration of 10 4 − 10 6 CFU/mL were 100 % inactivated within 1–2 h. Cuprous ions (Cu(I)) rather than sulfate radicals (SO 4 •− ) played the dominant role in the inactivation process, by breaking the cell membrane, damaging intracellular components (such as adenosine triphosphate and nicotinamide adenine dinucleotide), and stimulating increased reactive oxygen species production. Correspondingly, the toxicogenomics-based toxicity assessment indicated the induction of oxidative damage to exposed cells as a dominant molecular-level disinfection mechanism of the CuFe 2 O 4 /sulfite system. Moreover, the CuFe 2 O 4 /sulfite system exhibited comparable inactivation efficiency against three other bacterial species, while gram-positive strains ( Staphylococcus aureus and Bacillus subtilis ) were more susceptible to this system than gram-negative ones ( Pseudomonas aeruginosa and E. coli ). The magnetic recyclable CuFe 2 O 4 /sulfite system is a promising water disinfection method owing to its efficacy, convenience, and environmental sustainability.
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INORGANIC CHEMISTRY
·
2023
·
IF 4.6
Xuan Jiang,Zhaodong Nan
Multiple oxidation states of first-row transition-metal cations were always doped in g-C3N4 to enhance the catalytic activity by the synergistic action between the cations in the Fenton-like reaction. It remains a challenge for the synergistic mechanism when the stable electronic centrifugation (3d10) of Zn2+ was used. In this work, Zn2+ was facilely introduced in Fe-doped g-C3N4 (named xFe/yZn-CN). Compared with Fe-CN, the rate constant of the tetracycline hydrochloride (TC) degradation increased from 0.0505 to 0.0662 min–1 for 4Fe/1Zn-CN. The catalytic performance was more outstanding than those of similar catalysts reported. The catalytic mechanism was proposed. With the introduction of Zn2+ in 4Fe/1Zn-CN, the atomic percent of Fe (Fe2+ and Fe3+) and the molar ratio of Fe2+ to Fe3+ at the catalyst’s surface increased, where Fe2+ and Fe3+ were the active sites for adsorption and degradation. In addition, the band gap of 4Fe/1Zn-CN decreased, leading to enhanced electron transfer and conversion from Fe3+ to Fe2+. These changes resulted in the excellent catalytic performance of 4Fe/1Zn-CN. Radicals •OH, •O2–, and 1O2 formed in the reaction and took different actions under various pH values. 4Fe/1Zn-CN exhibited excellent stability after five cycles under the same conditions. These results may give a strategy for synthesizing Fenton-like catalysts.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 10
·2744-2753
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IF 7.3
Jiaxin Lv,Ruixin Chen,Zhen Wu,Yang Bai,Han Song,Chen Tian,Mengye Wang,Zhang Lin
The enrichment of microplastics in polar ice is a typical phenomenon discovered in recent years. Thus, it is worthwhile to explore the degradation behavior of microplastics in frozen environments, which is crucial to evaluate their impact on polar ecosystems. Here, taking polystyrene (PS) as an example, the degradation behaviors of MPs in frozen anoxic Fe(II)-containing solutions were investigated. The results revealed that PS degradation rate in frozen solution was 14.6-fold higher than that in water. Mechanism study showed that freezing-induced aggregation and extrusion of PS enhanced the generation of environmentally persistent free radicals (EPFRs), which in turn contributed to the formation of H2O2. Moreover, freezing-induced enrichment of Fe(II) further interreacted with H2O2 to form Fe(IV) and OH free radicals at a pH of ∼6.5, and thus accelerated the degradation of PS. Such reaction was accompanied by the formation of Fe(III)-containing products, which would further react with aged PS to produce new EPFRs and Fe(II). Such cycles of aged PS/EPFRs and Fe(III)/Fe(II) continued to accelerate the degradation of PS in the frozen solution. This study provides an overlooked pathway for microplastic degradation in frozen Fe(II)-containing solutions, which would be of key importance to understand the degradation behaviors of microplastics in frozen environments.
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CHEMICAL ENGINEERING JOURNAL
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2023
·
IF 15.1
Yun-fei Zhang,Jia-le Gao,Shen-gui Chen,Lei Li,Jian-hui Xu,Dan Li,Yu-feng Liu,Xin Quan,Xin Fu,Ya-zi Xie,Jing-nan Wu,Dan-ying Lin,Ting-ting Zheng
In this study, a novel 3D printed (3DP) Nb 2 O 5 /Ti electrode with a three-dimensional pore structure was prepared using selective laser melting (SLM) 3DP technology. The electrode exhibited high degradation efficiency, low energy consumption (16.02 Wh/L for 90% removal of 5 mg/L of Florfenicol (FLO)), and promising lifetime. Specifically, the 3DP 3% Nb 2 O 5 /Ti electrode maintained a 97.0% degradation efficiency for FLO within 120 min when consecutively used for 20 cycles. It was proposed that the Nb 2 O 5 served as an n-type dopant for Ti (IV), creating an electronegative surface environment that leads to stronger binding of electrons from H 2 O or FLO to the electrode surface. Consequently, the 3D-printed Nb 2 O 5 /Ti electrode exhibits higher OER potential and a greater yield of reactive oxygen species (ROSs) compared to the undoped Ti electrode. The electrode also achieved an 82.5% defluorination ratio for FLO, which is the best dehalogenation yield reported so far. Additionally, the toxicity of intermediates was significantly reduced after electrooxidation treatment, and 11 degradation products were identified by UPLC-MS/MS for potential degradation pathways identification. This study suggests that the 3D printed Nb 2 O 5 /Ti electrode holds great promise in remediating pharmaceuticals and personal care products (PPCPs)-contaminated water, and that SLM 3D printing technology is a beneficial method for producing Ti-stabilized anodes.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Jun Wang,Hao Lv,Xiandong Tong,Wei Ren,Yi Shen,Lun Lu,Yang Zhang
In order to minimize the knowledge gap between single and binary pollutants degradation by persulfate-based advanced oxidation processes (PS-AOPs), iron-loaded N-doped carbon nanotubes (Fe-NCNT) and its acid-washing sample (Fe-NCNT-W) were synthesized as peroxymonosulfate (PMS) activator for simultaneous oxidation of acid orange 7 (AO7) and electron-rich (phenol/ibuprofen) or electron-deficient pollutants (nitrobenzene/benzoic acid). Mechanistic studies revealed that both radical (HO•, SO 4 •− ) and nonradical (electron-transfer, high-valent iron) pathways involved for organic oxidation in Fe-NCNT/PMS system, while electron-transfer pathway (ETP) and high-valent iron-oxo species accounted for pollutant degradation at the surface and inner space of Fe-NCNT-W, respectively. The oxidation performances in single or binary systems were systematically investigated. In comparison to benchmark radical-based (Fe 2+ /PMS), nonradical ETP (NCNT/PMS) and mixed (Fe-NCNT/PMS) systems, Fe-NCNT-W/PMS outperformed superior performance toward oxidation of binary pollutants with little inference from solution pH or background substances, which could also be fabricated into membrane reactor for actual dyeing sewage treatment . Such superiorities should be mainly ascribed to the particular selectivity and intensive treatment of nonradical pathways in Fe-NCNT-W/PMS system with nanoconfinement effect. This work affords novel insights into the treatment of combined pollution via PMS activation by engineered nanomaterials .
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yuxuan Yang,Yanxiao Chi,Kunlun Yang,Zengshuai Zhang,Peng Gu,Xueli Ren,Xiaorui Wang,Hengfeng Miao,Xinhua Xu
A green, low-cost, high-performance Fe/N co-doped biochar material (Fe-N@C) was synthesized using salvaged cyanobacteria without other extra precursors for peroxymonosulfate (PMS) activation and ofloxacin (OFX) degradation. With the increased pyrolysis temperature, the graphitization degree, the specific surface area and the corresponding groups like OH, COO etc. for Fe-N@C tended to increase, resulting in a greater OFX adsorption. However, the total amount of Fe-N X and graphitic nitrogen groups in the Fe-N@C composites was firstly increased and then decreased, which reached the highest at 800 °C (Fe-N@C-800). All these changes of functional species ascribed to the strong interaction between Fe, N and C led to the highest defect degree of Fe-N@C-800, resulting the highest OFX removal efficiency of 95.0 %. OFX removal experiments indicated the adsorption process promoted the total OFX degradation for different functional groups on Fe-N@C composites separately dominated the process of OFX adsorption and PMS catalysis. Radical quenching and electron paramagnetic resonance (EPR) measurements proved free radical and non-free radical pathways participated in Fe-N@C/PMS system. The non-free radicals based on 1 O 2 and high-valent iron-oxo species played a more important role in OFX degradation, leading to the minimal effect of co-existing anions and the high universality for other antibiotic pollutants. Fe-N X was utilized as the main catalytic sites and graphitic nitrogen contributed more to the electron transfer for PMS activation, whose synergistic effect efficiently facilitated OFX degradation. Finally, the possible degradation route of OFX in the Fe-N@C-800/PMS system was proposed. All these results will provide the new insights into the intrinsic mechanism of Fe/N species in carbon-based materials for PMS activation.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Lulu Chen,Xiaona Dong,Ruonan Feng,Wanying Li,Dahu Ding,Tianming Cai,Canlan Jiang
Triclosan (TCS) is a compound in pharmaceutical and personal care products (PPCPs) that preferentially accumulates in soil and may threaten human health. Iron-based persulfate activation processes (Fe-PAPs) are a promising technique in soil remediation but are limited by their narrow pH application range and resultant iron precipitation. In this study, oxalic acid (OA) was specifically introduced to improve the efficiency of Fe 2+ -activated persulfate (PS) processes for TCS degradation in soil. The complexation of OA and Fe 2+ improved the total iron concentration in the Fe 2+ /OA/PS system and prevented iron precipitation. Fe-minerals in soil were also dissolved by OA, which participated in PS activation. The most appropriate proportion of Fe 2+ /OA/PS is 1:1:1, and approximately 85% of the TCS was degraded within 240 min compared with 45% in the Fe 2+ /PS system. SO 4 • - and 1 O 2 played important roles on TCS oxidation, while O 2 • - and CO 2 • - mainly participated in the iron cycle. The weak stretch of Fe-O in OA containing treatments in ATR-FTIR measurements provided evidence that OA dissolved the Fe-minerals. The introduction of OA in the Fe 2+ /PS system in four different soils reduced the negative effect of soil organic matter on TCS degradation. Three types of intermediates including hydroxylation, cleavage of ether bonds and cyclization products, were identified by LC-Q-TOF-MS. Column experiments were used to study the feasibility of in situ chemical oxidation (ISCO) remediation of TCS in the Fe 2+ /OA/PS system. Our findings indicated the ability of OA to be used as a cheating agent in Fe-PAPs for TCS soil remediation.
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ACS Nano
·
2023
·
IF 17.1
Wanrui Shi,Wenjie Feng,Siyuan Li,Yanqi Cui,Shuwei Liu,Huan Jiang,Yi Liu,Hao Zhang
Nanovaccine-based immunotherapy has been considered as a major pillar to stimulate the host immune system to recognize and eradicate tumor cells as well as establish a long-term immune memory to prevent tumor relapse and metastasis. However, the weak specificity and low cross-presentation of antigens, as well as the immunosuppressive microenvironments of tumor tissues, are still the major obstacles on exerting the therapeutic performance of tumor nanovaccines sufficiently. Herein, we design and construct cytosine guanine dinucleotide (CpG) oligodeoxynucleotide (ODN)-loaded aluminum hydroxyphosphate nanoparticles covered by Fe-Shikonin metal-phenolic networks (MPNs) (Alum-CpG@Fe-Shikonin NPs) as personalized in situ nanovaccines for antitumor immunity. Upon internalization by tumor cells, the shell of Fe-Shikonin MPNs will disassemble into Fe2+ and Shikonin to elicit the immunogenic cell death of tumor cells through ferroptosis and necroptosis. Then, dying tumor cell-released autologous tumor cell lysates will be absorbed by Alum NPs and codelivered with CpG ODN to professional antigen-presenting cells temporally and spatially to activate multistep cascade antitumor immune responses, including dendritic cell maturation, antigen cross-presentation, natural killer cell and cytotoxic T lymphocyte infiltrations, and tumor-associated macrophage repolarization. Benefiting from the synergistic effects of Alum NPs, CpG ODN, and Fe-Shikonin MPNs, our Alum-CpG@Fe-Shikonin NPs exhibit drastic cytotoxicity and accurate selectivity on eradicating primary tumor, strong abscopal effect on inhibiting distant tumor, and a long-term immune memory effect on preventing tumor metastasis and recurrence. Because our report provides a feasible strategy to in situ make full use of autologous tumor cell lysates, which present an entire spectrum of the patient’s personal epitopes without complicated ex vivo processes, such as extraction, purification, and sequencing, it may promote the development of personalized nanovaccines for antitumor immunity.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Wenjing Huang,Hongbo Ming,Xiaoqiong Bian,Can Yang,Yidong Hou,Kaining Ding,Jinshui Zhang
The activation of peroxymonosulfate (PMS) over carbon nitride-based photocatalysts towards refractory organic removal has received growing attention in wastewater treatment. In this study, we successfully synthesized copper single atoms incorporated into crystalline carbon nitride (Cu-CCN) and applied it to activate PMS towards bisphenol A (BPA) removal. The characterization and theoretical calculation results indicated that Cu-CCN had good crystallinity, outstanding charge separation and transfer ability, and numerous PMS adsorption and activation sites provided by Cu single atoms. Consequently, Cu-CCN demonstrated an enhanced ability to activate PMS for BPA degradation. The activity performance of Cu-CCN was affected by the experimental conditions at different levels, and the catalyst had good stability in structure and activity during cyclic runs. A plausible reaction mechanism was also proposed according to free radical trapping and quenching experiments. This oxidation process can efficiently degrade organic pollutants as well as reduce the toxicity. The findings of this work elucidated an efficient photocatalyst for activating PMS towards organic removal and might guide the design of other metal single-atom modified photocatalysts.
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MOLECULES
·
2023
·Vol. 28
·期 16
·6064
·
IF 4.6
Shuai Xu,Shiyue Zhang,Yutong Li,Jiyang Liu
Visual detection based on nanozymes has great potential for the rapid detection of metabolites in clinical analysis or home-based health management. In this work, iron and nitrogen co-doped carbon dots (Fe,N-CDs) were conveniently synthesized as a nanozyme for the visual detection of glucose (Glu) or cholesterol (Chol). Using inexpensive and readily available precursors, Fe,N-CDs with peroxidase-like activity were conveniently prepared through a simple hydrothermal method. Co-doping of Fe and N atoms enhanced the catalytic activity of the nanozyme. The nanozyme had a low Michaelis constant (Km) of 0.23 mM when hydrogen peroxide (H2O2) was used as the substrate. Free radical trapping experiments revealed that the reactive oxygen species (ROS) generated in the nanozyme-catalyzed process were superoxide anion radicals (•O2−), which can oxidize colorless 3,3′,5,5′-tetramethylbenzidine (TMB) to generate blue oxidation product (ox-TMB) with characteristics absorbance at 652 nm. Based on this mechanism, a colorimetric sensor was constructed to detect H2O2ranging from 0.1 μM to 200 μM with a detection limit (DL) of 75 nM. In the presence of glucose oxidase (Gox) or Chol oxidase (Chox), Glu or Chol was oxidized, respectively, and generated H2O2. Based on this, indirect detection of Glu and Chol was realized with linear detection ranges of 5–160 μM and 2–200 μM and DLs of 2.8 μM and 0.8 μM, respectively. A paper-based visual detection platform was fabricated using Fe,N-CDs as nanozyme ink to prepare testing paper by inkjet printing. Using a smartphone to record the RGB values of the testing paper after the reaction, visual detection of Glu and Chol can be achieved with linear detection ranges of 5–160 μM (DL of 3.3 μM) and 2–200 μM (DL of 1.0 μM), respectively.Keywords:visual detection;colorimetric sensor;nanozyme;carbon dots;metabolite detection
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