RSC Advances
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2023
·Vol. 13
·期 12
·8383-8393
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IF 3.9
Yan Wang,Jingyu Xiu,Tao Gan,Haiming Zou,Feiyue Li
In this work, a visible light-driven La/TiO2@g-C3N4 photocatalyst was synthesized for the photodegradation of tetracycline hydrochloride (TCH) in the presence of peroxydisulfate (PDS) in an internal loop-lift reactor. The surface morphology and structure of La/TiO2@g-C3N4 have been characterized by XRD, SEM-EDS, FTIR, XPS, and UV/vis DRS. La/TiO2@g-C3N4 displays outstanding photocatalytic performance and reusability. After four reuse cycles of the vis/La/TiO2@g-C3N4/PDS system, the TCH degradation rate and efficiency still reached 0.083 min−1 and 97.68%, respectively. Reactive species in this system included free radicals SO4˙−, ˙OH, and ˙O2−, as well as non-radicals e−, and h+, as established from the results of chemical quenching experiments. Moreover, a mechanism of action of the vis/La/TiO2@g-C3N4/PDS system for TCH degradation was proposed. The acute toxicity of the reaction solution towards Photobacterium phosphoreum T3 spp. in the vis/La/TiO2@g-C3N4/PDS process increased during the first 60 min and then decreased, illustrating that vis/La/TiO2@g-C3N4/PDS provided an effective and safe method for the removal of TCH.
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JOURNAL OF HAZARDOUS MATERIALS
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2023
·
IF 13.6
Yingpeng Gu,Yue Sun,Weisheng Zheng
Cupric (Cu(II)) complexes in industrial wastewater are responsible for the failure of conventional alkaline precipitation, but the properties of cuprous (Cu(I)) complexes at alkaline circumstance have not been focused. This report proposed a novel strategy for the remediation of Cu(II)-complexed wastewater by coupling alkaline precipitation with green benign reductant, namely, hydroxylamine hydrochloride (HA). This remediation process (HA-OH) exhibits superior Cu removal efficiency that cannot be achieved with the same dosage of oxidants (3 mM). The possibility of Cu(I) activated O 2 catalysis and self-decomplexation precipitation were investigated, and the results identified that 1 O 2 was generated from Cu(II)/Cu(I) cycle, but it was insufficient to annihilate organic ligands. Cu(I) self-decomplexation was the dominate mechanism of Cu removal. For real industrial wastewater, HA-OH process can realize the efficient Cu 2 O precipitation and Cu recovery. This novel strategy utilized intrinsic pollutant in wastewater without introducing other metals, complicated materials, and expensive equipment, broadening the insight for the remediation of Cu(II)-complexed wastewater.
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ULTRASONICS SONOCHEMISTRY
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2023
·
IF 8.4
Ching-Hsiang Fan,Nan Wu,Chih-Kuang Yeh
Sonodynamic therapy involving the non-invasive and local generation of lethal reactive oxygen species (ROS) via ultrasound (US) with sonosensitizers has been proposed as an emerging tumor therapy strategy. However, such therapy is usually associated with inertial cavitation and unnecessary damage to healthy tissue because current sonosensitizers have insufficient sensitivity to US. Here, we report the use of a new proposed sonosensitizer, carbon dots (C-dots), to assemble microbubbles with a gas core (C-dots MBs). As the C-dots were directly integrated into the MB shell, they could effectively absorb the energy of inertial cavitation and transfer it to ROS. Our results revealed the appearance of 1 O 2 , •OH, and H 2 O 2 after US irradiation of C-dots MBs. In in vitro experiments, treatment with C-dots MBs plus US induced lipid peroxidation, elevation of intracellular ROS, and apoptosis in 32.5%, 45.3%, and 50.1% of cells respectively. In an animal solid tumor model, treatment with C-dots MBs plus US resulted in a 3-fold and 2.5-fold increase in the proportion of ROS-damaged cells and apoptotic cells, respectively, compared to C-dots MBs alone. These results will pave the way for the design of novel multifunctional sonosensitizers for SDT tumor therapy.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yinxu Wang,Andac Armutlulu,Wenyuan Hu,Ruzhen Xie
The sluggish kinetics of Fe(II) regeneration and inactive Fe(III) sludge accumulation strongly hampers the scientific progress of Fenton-related reactions toward practical application. Herein, we developed a durable zero-valent iron super dispersed sodalite-graphene oxide hybrid (Z@GO-SOD) via reactive oxidation species (ROSs) route using industrial waste lithium silicon fume (LSF) as raw material, and first applied it as a visible-light-driven photocatalyst to initiate Fenton-like reaction for effective ciprofloxacin (CIP) remediation. The Z@GO-SOD featured a mesoporous structure with iron strongly interaction with GO hybrid zeolite, the GO hybrid zeolite acted as an efficient mediator, facilitating charge separation and transportation to expedite the iron redox cycle. The presence of persulfate could further act as an electron acceptor to boost photogenerated e − /h + separation, resulting in more OH for fast CIP removal. Over 90 % of CIP was removed within 30 min in the Z@GO-SOD/Vis/PS system with the usage of merely 0.4 g/L catalyst, and as high as 71% CIP was completely mineralized, which outperformed most of the state-of-the-art photo-Fenton catalysts. Meanwhile, Z@GO-SOD also demonstrated excellent reusability and stability. This work indicated the feasibility of utilizing solar energy for both preparation of catalyst and remediation of wastewater, paying the way for a sustainable solution for environmental solid waste pollution and water scarcity issue.
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MOLECULAR PHARMACEUTICS
·
2023
·
IF 4.9
Zhaomin Tang,Shuting Jiang,Wanlan Tang,Qian He,Huangzhao Wei,Chengyu Jin,Shuai Wang,Hui Zhang
Chemodynamic therapy (CDT) that involves the use of Fenton catalysts to convert endogenous hydrogen peroxide (H2O2) to hydroxyl radicals (·OH) constitutes a promising strategy for cancer therapy; however, insufficient endogenous H2O2 and glutathione (GSH) overexpression render its efficiency unsatisfactory. Herein, we present an intelligent nanocatalyst that comprises copper peroxide nanodots and DOX-loaded mesoporous silica nanoparticles (MSNs) (DOX@MSN@CuO2) and can self-supply exogenous H2O2 and respond to specific tumor microenvironments (TME). Following endocytosis into tumor cells, DOX@MSN@CuO2 initially decomposes into Cu2+ and exogenous H2O2 in the weakly acidic TME. Subsequently, Cu2+ reacts with high GSH concentrations, thereby inducing GSH depletion and reducing Cu2+ to Cu+ Next, the generated Cu+ undergoes Fenton-like reactions with exogenous H2O2 to accelerate toxic ·OH production, which exhibits a rapid reaction rate and is responsible for tumor cell apoptosis, thereby enhancing CDT. Furthermore, the successful delivery of DOX from the MSNs achieves chemotherapy and CDT integration. Thus, this excellent strategy can resolve the problem of insufficient CDT efficacy due to limited H2O2 and GSH overexpression. Integrating H2O2 self-supply and GSH deletion enhances CDT, and DOX-induced chemotherapy endows DOX@MSN@CuO2 with effective tumor growth-inhibiting properties alongside minimal side effects in vivo.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2023
·
IF 8.6
Shijia Pan,Wenxuan Jiang,Lu Tian,Xiang Li,Jiaxin Wang,Yawen Wang,Zhen Li,He Guo
The simultaneous presence of antibiotics and phosphate (P) in wastewater will threaten human health and ecological security. The purpose of this study is to study the simultaneous removal of oxytetracycline (OTC) and P in water by O 3 /CaO 2 advanced oxidation process. With enhancing CaO 2 dosage, the degradation efficiency of OTC first improved and then declined, whereas the removal efficiency of P kept increasing. Increasing the amount of O 3 increased the removal efficiency of OTC, but had little effect on the removal efficiency of P. With 0.80 g/L CaO 2 and 0.50 g/h O 3 , the removal efficiency of OTC and P reached 98.0 % and 90.5 % respectively. The lower OTC concentration was beneficial to OTC degradation and P precipitation. The P concentration has no effect on OTC degradation, but it would affect itself precipitation. Alkaline environment was conducive to OTC degradation and P removal. ·OH, ·O 2 − , 1 O 2 made major contribution to the degradation of OTC, which was verified by ESR technique and free radical capture experiment. During the degradation of OTC and P removal, TOC and COD values decreased, while pH and conductivity showed a downward trend. Based on UV–Vis spectrum, 3D EEMF spectrum and LC-MS analysis, two main degradation pathways of OTC were proposed. Toxicity analysis of intermediates showed that their toxicity was significantly lower than that of OTC. The O 3 /CaO 2 system can be considered as an efficient and prospective method for the simultaneous removal of OTC and P in water.
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Environmental Science-Nano
·
2023
·Vol. 10
·期 4
·1109-1125
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IF 7.3
Xiao Huang,Wen Yan,Jingxiang Sun,Tao Hu,Jinxi Feng,Zhen Huang,Shuanghong Tian,Ya Xiong
The achievement of highly active and stable piezocatalysts is still challenging for the efficient transformation of mechanical energy to chemical energy. Herein various SnOxHy species were prepared by a simple precipitation–thermal treatment method and applied for the piezocatalytic degradation of tricyclazole. It is found that the catalytic activity depended on the thermal treatment and follows the order SnO(OH)2 (80 °C) > SnO2.55H1.1 (200 °C) > SnO2.3H0.6 (300 °C) > SnO2.22H0.24 (400 °C) > SnO2 (500 °C) > rutile SnO2 (800 °C). SnO(OH)2 (80 °C) boosted the degradation of tricyclazole and the reaction constant reached as high as 0.0354 min−1, 7.1 fold that of SnO2 (800 °C). The differences among these SnOxOHy piezocatalysts mainly stemmed from the dissimilarity of the relative content of SnO(OH)2. In addition to the Sn–O piezoelectric motif, SnO(OH)2 had rich hydrogen bond networks, which work like molecular springs under external pressure. Due to such a special structure, SnO(OH)2 had not only a super high piezoelectric constant (d33) of 409.1 pm V−1 among the currently reported piezomaterials, but also a 0.49 eV-higher valence band than SnO2, being beneficial to the generation of stronger oxidative ˙OH. This is the first example of inorganic hydrogen-bonded piezomaterials, which opens a new window to develop advanced piezocatalysts for highly efficient degradation of refractory pollutants by piezocatalysis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Zi-Jie Xiao,Bai-Qin Zhou,Xiao-Chi Feng,Hong-Tao Shi,Yi-Ning Zhu,Cai-Peng Wang,Bart Van der Bruggen,Nan-Qi Ren
How single-atom (SA) materials trigger highly efficient catalysis in peroxymonosulfate (PMS) treatment is not fully understood. In this study, cobalt SA sites were fabricated as a PMS activator for antibiotic degradation and compared with cobalt nanoparticles (NPs). Co-SA/PMS showed superior degradation efficiency, adaptability, and stability to Co-NP/PMS in antibiotic treatment. Identification of the reactive species suggested that Co-SA/PMS were privileged from generating anchored high-valent Co–oxo (Co=O) species for triggering interface oxidation, while Co-NP/PMS generated aqueous radical and non-radical species with less reliability. Theoretical calculations and extended experiments of the oxidation effects showed that Co=O is more stable for Co-SAs than for Co-NPs, providing better accessibility to accomplish interface oxygen transfer. Furthermore, oxidation of different antibiotic contaminants and various typical sulfadoxin degradation pathways were investigated to distinguish the effects of the different pathways. Overall, this study shows the activation improvement caused by different existential forms of cobalt in PMS treatment.
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Nanoscale
·
2023
·Vol. 15
·期 12
·5909-5918
·
IF 6.7
Wenjie Wu,Saiyu Bu,Liang Bai,Yuanting Su,Yenan Song,Haitao Sun,Guangyin Zhen,Ke Dong,Lunhua Deng,Qinghong Yuan,Chengbin Jing,Zhuo Sun
Non-thermal plasma (NTP) degradation of volatile organic compounds (VOCs) into CO2 and H2O is a promising strategy for addressing ever-growing environment pollution. However, its practical implementation is hindered by low conversion efficiency and emissions of noxious by-products. Herein, an advanced low-oxygen-pressure calcination process is developed to fine-tune the oxygen vacancy concentration of MOF-derived TiO2 nanocrystals. Vo-poor and Vo-rich TiO2 catalysts were placed in the back of an NTP reactor to convert harmful ozone molecules into ROS that decompose VOCs via heterogeneous catalytic ozonation processes. The results indicate that Vo-TiO2-5/NTP with the highest Vo concentration exhibited superior catalytic activity in the degradation of toluene compared to NTP-only and TiO2/NTP, achieving a maximum 96% elimination efficiency and 76% COx selectivity at an SIE of 540 J L−1. Mechanistic analysis reveals that the 1O2, ˙O2− and ˙OH species derived from the activation of O3 molecules on Vo sites contribute to the decomposition of toluene over the Vo-rich TiO2 surface. With the aid of advanced characterization and density functional theory calculations, the roles of oxygen vacancies in manipulating the synergistic capability of post-NTP systems were explored, and were attributed to increased O3 adsorption ability and enhanced charge transfer dynamics. This work presents novel insights into the design of high-efficiency NTP catalysts structured with active Vo sites.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Hexiang Wang,Chenliu Tang,Luwei Wang,Zhirong Sun,Xiang Hu
A MOF-derived carbon material containing CoFe alloy (Co/Fe@NPC-500) by calcining N-doped Co/Fe bimetallic MOF at a lower temperature was successfully synthesized as a cathode in electro-Fenton process for ceftazidime (CAZ) degradation. The presence of Co could accelerate the transfer of electrons from C atoms of carbon material to Fe, thus increasing the content of low-valent metals in the material, which had been demonstrated by characterizations and density functional theory (DFT) calculations. Thanks to the integrity of the MOF structure, the synergistic effect between Fe and Co, Co/Fe@NPC-500 cathode showed efficient removal efficiency for CAZ completely removed within 60 min and obtained a total organic carbon (TOC) removal rate of 52.1% at 90 min. Besides, based on the results of HPLC-MS and DFT calculations, the degradation pathway of CAZ was proposed. This study provides some useful information for the preparation of MOF-derived carbon materials containing low-valent metals for electro-Fenton process.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2023
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IF 5.2
Yifang Mi,Sen Zhang,Yufeng Zhao,Guojin Sun,Zhihai Cao
Fe-based activated biochar composites are promising catalysts for environmental remediation. However, the limited efficiency of Fe(III)/Fe(II) cycling reaction of commercial Fe 2 O 3 at neutral conditions still impeded the catalytic performance of the heterogeneous Fenton-like catalysts. In this work, high-performance Fe 2 O 3 /activated biochar Fenton-like catalysts with Taihu blue algae (hazardous algae to aquatic ecosystems) as carbon precursors were synthesized and used for the degradation of methylene blue (MB). The physicochemical properties of Fe 2 O 3 /activated biochar composites including pore structure , the generated N species, and persistent free radicals (PFRs) were effectively tailored by activation temperatures. ACK-7-Fe (prepared under the activation temperature, 700 °C) showed a stronger adsorption ability while ACK-8-Fe (800 °C) exhibited superior MB degradation performance (∼99.97% in 30 min at neutral pH). The former was ascribed to the formation of more mesopores with suitable size which was beneficial for MB adsorption. The latter is due to the promoting effect of pyrrolic N and PFRs on the Fe(III)/Fe(II) cycle, responsible for the high catalytic efficiency of ACK-8-Fe. The hydroxyl radicals were the dominant active radicals evidenced by scavenging experiments and electron spin resonance. Moreover, the. The ACK-8-Fe exhibited superior reusability, which was crucial for its practical applications.
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JOURNAL OF ALLOYS AND COMPOUNDS
·
2023
·
IF 6.2
Xiaoxi Yu,Xiaocui Wu,Fang Guo,Jingping Liu,Qingshan Zhao
As a promising advanced oxidation process , photo-assisted peroxymonosulfate (PMS) activation for wastewater treatment has attracted widespread attentions. However, rational design of synergetic and recyclable catalysts for PMS photo-activation remains a big challenge. In this study, a carbon layer-coated amorphous CoO x supported on graphitic carbon nitride (CoO x @C/g-C 3 N 4 ) composite was fabricated to drive visible-light-assisted activation of PMS for efficient organic pollutant degradation. Amorphous CoO x nanoparticles were in-situ grown on two-dimensional g-C 3 N 4 substrate, among which a carbon layer serves as a high-speed electron transmission channel, facilitating the separation of photogenerated electron-hole pairs and accelerating the Co 3+ /Co 2+ redox cycle. Simultaneously, the carbon layer provides a protective film to suppress Co leaching, thereby improving the catalytic activity and reusability. Owing to the unique heterostructure and synergetic effect, the optimized 6% CoO x @C/g-C 3 N 4 composite exhibits superior catalytic efficiency and excellent cycling stability towards the degradation of various organic pollutants, which displays nearly 100% elimination of tetracycline (TC) within 80 mins. The h + , SO 4 •- and •OH are determined as the main contributors in the visible light-assisted PMS activation system, and the possible catalytic mechanism is also proposed. This work demonstrates a feasible strategy for constructing synergetic and effective photo-activation PMS catalysts for water remediation.
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