CHEMOSPHERE
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2023
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IF 8.8
Jieli Ou,Jiewen Deng,Zhenran Wang,Yongsheng Fu,Yiqing Liu
A Cu(II)/heat coactivated peracetic acid (PAA) system for enhancing diclofenac (DCF) degradation was proposed in this work. The superiority of this synergetic activation strategy for PAA, working reactive species, catalytic mechanism and effects of reaction parameters on DCF elimination in this system were simultaneously investigated. Based on our results, the DCF loss rate in Cu(II)-heat/PAA process at pH 8.0 was about 49.3 and 4.2 times of that in Cu(II)/PAA and heat/PAA processes, respectively. Increasing the reaction temperature to 60 о C not only motivated the conversion of Cu(II) to Cu(I) but also facilitated the one-electron transfer between Cu(I) and PAA, boosting the generation of radicals. Organic radicals (mainly CH 3 C(O)O• and CH 3 C(O)OO•) were evidenced to be the core oxidizing substances dominating in the destruction of DCF while hydroxyl radical (•OH) made a minor contribution in this system by electron paramagnetic resonance (EPR) method together with scavenging experiments. This study broads the eyes into enhanced PAA activation initiated by homogenous Cu(II), providing a simple but efficient tool to degrade micropollutants .
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高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiajun Ruan,Tao Zhong,Yuxi Guo
The key elements that influence the properties and capabilities of particulate photocatalysts are their crystallinity , size, and surface active sites. However, simultaneously controlling these three variables remains a challenge. In this study, we present the first exploration into the use of a simple ethylenediaminetetraacetate (EDTA) etching technique to decrease the particle size and increase the surface active sites of photocatalysts while preserving their high crystallinity. By employing SrTiO 3 as a model photocatalyst, we were able to create an ordered step nanostructure on the surface of sintered SrTiO 3 . As a result of the EDTA treatment, the particle size was reduced while the crystallinity was maintained. The separation of photogenerated electrons and holes is enhanced by the combination of reduced particle size and high crystallinity. To enhance chemical reaction activities, the organized surface nano-step structures serve as high-activity sites. As a result, when subjected to simulated light irradiation , the EDTA-treated SrTiO 3 samples demonstrate improved photocatalytic performance for water splitting into H 2 and O 2 in a stoichiometric amount that is 3.8 times greater than that of untreated SrTiO 3 . Since EDTA interacts with most metals, this simple EDTA etching technique has the potential to be further developed to modify additional photocatalysts with exceptional performance for a variety of applications.
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Theranostics
·
2023
·
IF 12.4
Naihan Huang,Along Qian,Yiming Zou,Miaoli Lin,Weilun Pan,Ming Chen,Wei Meng,Wenhua Zhang,Jinxiang Chen
Background: Due to the immunosuppressive tumor microenvironment (TME), radiation therapy (RT)-mediated immune response is far from satisfactory. How to improve the efficacy of immunogenic RT by priming strong immunogenic cell death (ICD) is an interesting and urgent challenge. Methods: A polyacrylic acid-coated core-shell UiO@Mn 3 O 4 (denoted as UMP) nanocomposite is constructed for immunogenic RT via multiple strategies. Results: Reshaping the TME via Mn 3 O 4 -mediated integration of O 2 production, GSH depletion, ROS generation and cell cycle arrest, accompanied by Hf-based UiO-mediated radiation absorption, eventually amplifies UMP-mediated RT to induce intense ICD. With the potent ICD induction and reprogrammed tumor-associated macrophages, this synergetic strategy can promote dendritic cells maturation and CD8 + T cells infiltration, and potentiate anti-tumor immunity against primary, distant, and metastatic tumors. Conclusion: This work is expected to shed light on the immunosuppressive TME-reshaping via multiple strategies to reinforce the immunogenic RT outcome and facilitate the development of effective cancer nanomedicine.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Heng Li,Xiaoying Jin,Qin Li,Zuliang Chen
Slow electron migration in iron sulfide nanoparticles (C-FeS NPs) synthesized by co-precipitation severely limits the activation performance of hydrogen peroxide (H 2 O 2 ). Herein, a biofunctional FeS NPs (P-FeS NPs) derived from Pinus massoniana Lamb biomass, with interface coupling effect, was used for enhanced H 2 O 2 activation and norfloxacin (NOR) degradation. It was discovered that P-FeS NPs exhibited superior catalytic activity (100%) compared to C-FeS NPs (53.1%). Fe atoms of FeS NPs and hydroxyl groups (–OH) of Pinus massoniana Lamb biomass were mutually coupled to produce Fe-OH interfacial sites, which significantly increased the generation of multi-reactive species by accelerating the transfer of electrons across interfaces. Additionally, radical quenching tests elucidated that singlet oxygen ( 1 O 2 ) (66.6%) played a leading role, while hydroxyl radicals (•OH) (14.5%) and superoxide radicals (•O 2 – ) (18.9%) were secondary oxidants. Finally, P-FeS NPs showed a high tolerance to a wide range of pH conditions and could remove 96.4% NOR from wastewater. Overall, this work generates important insights into understanding how green sustainable interfacial catalysts can accelerate catalytic activity.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Yiqing Li,Manqin Fu,Xiaoxia Zhang,Chun He,Dingsheng Chen,Ya Xiong,Liqing Guo,Shuanghong Tian
Highly reactive nanoclusters of metal oxides are extremely difficult to be synthesized due to their thermodynamic instability. For the first time, CuO x nanoclusters supported on anatase TiO 2 nanotubes (NT) with many defects as anchoring sites were successfully prepared. Although the copper loading reached as high as 2.5 %, the size of CuO x nanoclusters in the sample of 2.5 %CuO x /NT were mainly around 1.0 nm. The aggregation of copper species during the calcination process was undoubtedly hampered by the anchoring effects of the abundant defects in NT support. Due to the highly exposed undercoordinated atoms of CuO x nanoclusters, the mixed valences of copper, and the strong interface interaction between CuO x nanoclusters and NT support, 2.5 %CuO x /NT-catalyzed ozonation showed the highest pseudo-first-order reaction rate constant of 8.5 × 10 −2 min −1 , 2.2 and 4.0 times that of NT-catalyzed ozonation and ozonation alone, respectively. Finally, the catalytic mechanism was revealed by both experiments and density functional theory calculations (DFT). The results demonstrated that the undercoordinated Cu in CuO x /NT could highly promote the adsorption of ozone with a high adsorption energy of −125.16 eV and the adsorbed ozone was activated immediately, tending to dissociate into a O 2 molecule and a surface O atom. Thus, abundant reactive oxygen species , e.g., hydroxyl radical (·OH), superoxide radical (·O 2 – ) and singlet oxygen ( 1 O 2 ), could be generated via chain reactions. Especially, ·OH mainly contributed to the removal of ibuprofen pollutants. This work sheds a light on the design and preparation of highly reactive nanoclusters of metal oxide catalysts for catalytic ozonation of refractory organic pollutants .
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ENVIRONMENTAL TECHNOLOGY
·
2023
·
IF 2.8
Ping Ma,Chao Han,Qiongqiong He,Zhenyong Miao,Mingqiang Gao,Keji Wan,Enle Xu
Dye wastewater is a kind of refractory organic wastewater. Fenton coupled with micro-nano bubbles (MNBs+FT) was used for the degradation of Congo red (CR), aiming at simplifying the organic pollutants degradation process and reducing the cost of the process. The optimum condition of Fenton alone, the outlet pressure of the cavitation process and different combinations on the degradation of CR dye wastewater were discussed in this study. The results showed that the degradation of CR (100 mg/L) could reach 94.4% by using the MNBs+FT at the pH of 7, which was 72% higher than that using Fenton oxidation alone and 79% higher than that using MNBs alone. Based on the same degradation efficiency, the traditional Fenton process alone required 8 times the dose of oxidants of these combination systems, and the synergy coefficient of MNBs+FT was up to 2.44. ESR analysis indicated that ·OH was the predominant active species during the degradation of CR and MNBs+FT improved the utilization efficiency of H2O2 and produced more ·OH. Besides, the MNBs+FT could extend the pH range of the high-efficiency oxidation reaction, and it could also keep a high degradation rate under neutral conditions, which eliminated the process of adjusting the pH and reduced the anti-corrosion requirements of the equipment. According to the economic analysis results, the total cost of treatment for the MNBs/FT was about 13% of the cost of only the Fenton process. This study provides a reference for the application of MNBs+FT systems in full-scale dye wastewater treatment.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Zhongmou Liu,Pan Zhang,Xiangyu Zhao
Reduced graphene oxide supported with ferric ion (Fe(III)-rGO) was successfully prepared, and performed as an excellent catalyst to activate hydrogen peroxide (H 2 O 2 ) and peroxymonosulfate (PMS) for isoprothiolane (IPT) degradation. IPT removal efficiency was proven to be better in the Fe(III)-rGO/H 2 O 2 /PMS system (96.2%) than in the Fenton-like reaction (72.6%) and PMS-AOP (80.0%) individually. X-ray photoelectron spectroscopy showed that Fe(III) was reduced in Fenton-like reaction, and the reduced Fe(II) played a crucial role in the subsequent PMS-AOP. The combination of the Fenton-like reaction and PMS-AOP involved the valence state conversion of Fe, which consequently improved Fe(III)-rGO utilization rate and IPT removal efficiency. Fe(III)-rGO remarkably boosted the Fe(III)/Fe(II) cycle and generated superoxide radical (O 2 − •) and singlet oxygen ( 1 O 2 ) in the Fe(III)-rGO/H 2 O 2 /PMS system. Fe(III)-rGO acts as the electron transfer mediator; thus, promoting electron transfer from IPT to H 2 O 2 and PMS and accelerating the generation of active species. Fe(IV) with high oxidation performance was formed in PMS-AOP and efficiently removed some of the IPT. IPT removal efficiency was more than 90% at a pH range of 3–11; this efficiency could be maintained above 50% even after five consecutive degradation experiments, exhibiting excellent stability and reusability of Fe(III)-rGO. Additionally, iron sludge formation was greatly reduced because of the stable chemical bonding of iron ions to the rGO surface. Therefore, this study provides a new multisystem and synergistic approach for the efficient removal of organic micro-pollutants from water.
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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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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 34
·15951-15962
·
IF 3.3
Qingmei Tan,Wensheng Zhang,Tianren Liu,Ying He,Yuangong Ma,Yingxin Yang,Dongxue Han,Dongdong Qin,Li Niu
Owing to the advantages of easy separation and recovery, the development of magnetic photocatalysts is essential to create a viable photocatalytic technology for the degradation of antibiotic contaminants in water. Herein, magnetic Fe3O4@TiO2–Co nanocomposites as a highly recyclable and effective photocatalyst with various Co loading percentages were successfully prepared via a facile route and evaluated for the photodegradation of model tetracycline (TC) antibiotics. As a result, the optimal Fe3O4@TiO2–Co-2.7 sample possesses a removal rate of 92.4% for TC degradation, which is 3.2 fold and 1.6 fold higher than those of single Fe3O4 (28.8%) and Fe3O4@TiO2 (58.7%), respectively. The enhanced photocatalytic activity is mainly attributed to the advantages of integrating magnetic Fe3O4 nanospheres and metal Co nanoparticles, resulting in the overall magnetic composites of Fe3O4@TiO2–Co having an ameliorative light collection ability, energy-saving recycling process, excellent photocatalytic activity, and high chemical and environmental stability. Satisfactorily, the Fe3O4@TiO2–Co photocatalyst could be easily recovered from the reaction solution by an applied magnetic field, and its photocatalytic activity shows almost no loss after five cycles of repetitive use. Moreover, the intermediates in the degradation pathway were identified via high-performance liquid chromatography–mass spectrometry (HPLC-MS) and the TC degradation pathway in the photocatalytic reaction of the as-designed system was proposed. The present work was successfully applied for the purification of tetracycline antibiotics in water pollutants, demonstrating a promising prospect for application to other pollutant degradation systems.
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Journal of Materials Chemistry B
·
2023
·Vol. 11
·期 33
·8046-8055
·
IF 7
Yujie Gao,Wenxiang Pei,Yang Yang,Mengmeng Li,Hengqiu Sun,Mingchao Chen,Xiaoman Ma,Hui Zhang,Dongming Qi,Jindan Wu
In most circumstances, wounds face the challenges of bacterial invasions and inappropriate inflammatory responses when they lack proper wound management. Endowing dressings with both antibacterial and anti-inflammatory functions is a compelling strategy for resolving the above issues. However, seizing the right moment to change the dressings and providing satisfactory management of wounds are still urgently required. Herein, an antibacterial and anti-inflammatory nanofibrous mat is proposed by encapsulating antibiotic gentamicin sulfate (GS) and anti-inflammatory drug ibuprofen (IB) into nanofibers via a coaxial electrospinning technique and is further decorated with Prussian blue nanocrystals (PBNCs) to enhance anti-inflammatory activity and, more importantly, to monitor bacterial infections and guide dressing changes in a timely manner. Such a nanofibrous mat releases most of the therapeutic drugs within 120 min and reveals excellent antibacterial activity and anti-inflammatory ability. Specifically, it can destroy both Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli), as well as conspicuously reduce the production of reactive oxygen species (ROS) and the expression of pro-inflammatory cytokines in macrophages. In addition, the nanofibrous mat can be used for point-of-use diagnosis of living bacteria relying on the naked eye or color analysis, which exhibits the potential of monitoring wound infection and guiding dressing changes promptly. This finding demonstrates the theranostic applications of multifunctional nanofibrous mats in wound healing.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xin Lv,Chenying Zhou,Zhichao Shen,Yuchen Zhang,Chuanshu He,Ye Du,Zhaokun Xiong,Rongfu Huang,Peng Zhou,Bo Lai
The acceleration of Fe(III)/Fe(II) conversion in Fenton systems is the critical route to achieve the long-lasting generation of reactive oxygen species towards the oxidation of refractory contaminants. Here, we found that waste leather derived porous carbon materials (LPC), as a simple and readily available metal-free biochar material, can promote the Fe(III)/H 2 O 2 system to generate hydroxyl radicals ( • OH) for oxidizing a broad spectrum of contaminants. Results of characterizations, theoretical calculations, and electrochemical tests show that the surface carbonyl groups of LPC can provide electron for direct Fe(III) reduction. More importantly, the graphitic-N on surface of LPC can enhance the reactivity of Fe(III) for accelerating H 2 O 2 induced Fe(III) reduction. The presence of LPC accelerates the Fe(III)/Fe(II) redox cycle in the Fe(III)/H 2 O 2 system, sustainable Fenton chain reactions is thus initiated for long-lasting generation of hydroxyl radicals without adding Fe(II). The continuous flow mode that couples in-situ Fenton-like oxidation and LPC with excellent adsorption catalytic properties, anti-coexisting substances interference and reusability performance enables efficient, green and sustainable degradation of trace organic pollutants . Therefore, the application of metal-free carbon materials in Fenton-like system can solve its rate-limiting problem, reduce the production of iron sludge , achieve green Fenton chemistry , and facilitate the actual engineering application of economic and ecological methods to efficiently remove trace organic contaminants from actual water sources.
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ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Xiaolu Li,Xutao Chen,Yuanyuan Yan,Feng Wang,Leiyu Feng,Yinguang Chen
Nitrogen-doped graphene (NG) was synthesized via direct thermal annealing treatment. The obtained NG showed outstanding removal ability for tetracycline (TC) ascribed to enhanced adsorption and persulfate activation. The maximum TC adsorption capacity calculated from the Langmuir model of NG was 227.3 mg/g, which was 1.66 times larger than nitrogen-free graphene. The coexistence of NG and persulfate (PS) exhibited complete degradation of TC within 120 min attributed to the successful modification of nitrogen. Further analysis demonstrated that non-radical electron transfer was the dominant degradation pathway, which was different from the widely acknowledgeable radical mechanism. An electron donor-mediator-acceptor system was introduced, in which TC, NG, and PS performed as electron donor, mediator, and acceptor, respectively. The potential intermediates in the TC degradation process were detected and toxicity assessment was also performed. In addition, more than 75.8% of total organic carbon was removed, and excellent reusability was manifested in multiple adsorption and degradation experiments.
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