ACS Nano
·
2024
·
IF 15.8
Qing Luo,Qian Ma,Taoxia Liu,Yiting Luo,Lianying Wang,Chang Guo,Leyu Wang
We developed an intrinsic hydrophilic single-atom iron nanobowl (Fe-SANB) for magnetic resonance imaging (MRI)-guided tumor microenvironment-triggered cancer therapy. Benefiting from the sufficient exposure of Fe single atoms and the intrinsic hydrophilicity of the bowl-shaped structure, the Fe-SANBs exhibited a superior performance for T1-weighted MRI with an r1 value of 11.48 mM–1 s–1, which is 3-fold higher than that of the commercial Gd-DTPA (r1 = 3.72 mM–1 s–1). After further coembedding Gd single atoms in the nanobowls, the r1 value can be greatly improved to 19.54 mM–1 s–1. In tumor microenvironment (TME), the Fe-SANBs can trigger pH-induced Fenton-like activity to generate highly toxic hydroxyl radicals for high-efficiency chemodynamic therapy (CDT). Both the MRI and CDT efficiency of these nanobowls can be optimized by tuning the ratio of Fe(II)/Fe(III) in the Fe-SANBs via controlling the calcination temperature. Furthermore, the generation of •OH at the tumor site can be accelerated via the photothermal effect of Fe-SANBs, thus promoting CDT efficacy. Both in vitro and in vivo results confirmed that our nanoplatform exhibited high T1-weighted MRI contrast, robust biocompatibility, and satisfactory tumor treatment, providing a potential nanoplatform for MRI-guided TME-triggered precise cancer therapy.
研究领域:
生物医学工程
·
纳米医学
·
肿瘤学
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产品关联
DOI
PubMed
高影响因子
DIAMOND AND RELATED MATERIALS
·
2025
·
IF 5.1
Liu Ouyang,Huihu Wang,Lizhong Duan,Jingle Zhang,Shenghao Jiang,Yu Xiong,Chenhuinan Wei,Xing Xiang,Yun Zhao,Qianyu Wang
Tetracycline (TC), a widely detected aquatic pollutant, poses significant ecological risks, necessitating the development of effective remediation strategies. Photocatalytic degradation, which converts TC into harmless CO 2 and H 2 O, offers a promising eco-friendly solution. This study successfully synthesized a novel 2D/3D g-C 3 N 5 /BiVO 4 (N-CN/BiVO 4 ) S-scheme heterojunction via a hydrothermal method. The optimized 5 % N-CN/BiVO 4 exhibited exceptional performance in activating the Fe 2+ /PMS system under visible light, achieving a 96.8 % TC removal efficiency with an apparent rate constant 4.4 times higher than that of BiVO 4 . Mechanistic studies, including ultraviolet photoelectron spectroscopy (UPS) and valence band X-ray photoelectron spectroscopy (VB-XPS), confirmed the S-scheme interfacial charge transfer pathway. Furthermore, radical quenching experiments revealed that the enhanced photocatalytic activity originated from the synergistic contribution of multiple reactive species ( OH, SO 4 − , O 2 − , h + , and 1 O 2 ), validating both the efficient activation of Fe 2+ /PMS and the proposed S-scheme charge transfer mechanism. This work presents an innovative approach for high-performance pollutant degradation by coupling an S-scheme heterojunction with the Fe 2+ /PMS activation system.
研究领域:
环境科学
·
光催化
·
水污染修复
·
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Chengwu Zhang,Anqi Yang,Bing Qin,Wei Zhao,Chuipeng Kong,Chuanyu Qin
It has been reported that tripolyphosphate (TPP) can effectively enhance the activation of O 2 by Fe(II) to remove organic pollutants in the environment. However, the influence of solution pH on the generation and conversion of reactive oxygen species (ROS) and their degradation of pollutants in the Fe(II)/O 2 /TPP system needs further investigation. In this study, we demonstrated that O 2 •– and •OH were the main ROS responsible for degradation in the system at different pH conditions, and their formation rates were calculated using a steady-state model. Experiments combined with density functional theory (DFT) calculations showed that the p -nitrophenol (PNP) degradation pathway in the Fe(II)/O 2 /TPP system is regulated by solution pH. Specifically, at pH = 3, the existence of Fe(II) in the solution is dominated by [Fe(II)(HTPP) 2 ] 2− , which leads to a rapid conversion from O 2 and HO 2 • to generate •OH, and PNP is primarily oxidatively degraded. However, at pH = 5/7, [Fe(II)(TPP) 2 ] 4− is taking the lead with which O 2 •– is accumulated in the solution due to the slow conversion to •OH in this condition, and the PNP is mainly reductively degraded. This study proposes a new strategy to achieve the targeted oxidative/reductive removal of different types of pollutants by simply varying the solution pH in the Fe(II)/O 2 /TPP system.
研究领域:
环境科学
·
化学
·
污染控制
·
活性氧物种
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DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2019
·
IF 8.456
Yuda Zhu,Nini Xin,Zi Qiao,Suping Chen,lingwan Zeng,Yusheng Zhang,Dan Wei,Jing Sun,Hongsong Fan
Traditional tumor treatments suffer from severe side effects on account of their invasive process and inefficient outcomes. Featuring a unique physical microenvironment, the tumor microenvironment (TME) provides a new research direction for designing more efficient and safer treatment paradigms. In this study, we fabricated a polydopamine (PDA)-based TME-responsive nanosystem, which successfully integrates glucose degradation, the Fenton reaction, and photothermal therapy for efficient cancer therapy. Through a convenient hydrothermal method, Fe2+-doped Fe(II)–PDA nanoparticles were successfully fabricated, which show an excellent photothermal effect and interesting reactivity for the Fenton reaction. Instead of introducing toxic anticancer agents, natural glucose oxidase (GOD) was grafted on Fe(II)–PDA, forming a cascade catalytic nanomedicine for a specific response to the glucose in TME. GOD grafted on Fe(II)–PDA–GOD is ought to catalyze abundant glucose in TME into gluconic acid and H2O2. The concomitant generation of H2O2 can enhance the efficiency of the sequential Fenton reaction, producing abundant hydroxyl radicals (•OH) for cancer therapy. Besides, the overconsumption of intratumoral glucose also could inhibit tumor growth by reducing the energy supply. Taken together, the in vitro and in vivo antitumor studies of such TME-based Fe(II)–PDA–GOD nanosystems displayed a favorable synergistic potency of glucose degradation, the Fenton reaction, and photothermal therapy against tumor growth. Our design expands the biological application of multifunctional PDA while providing novel strategies toward effective antitumor treatment with minimal side effects.
研究领域:
癌症研究
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纳米技术
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治疗工程
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生物医学科学
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产品关联
DOI
PubMed
高影响因子
Journal of Materials Chemistry A
·
2025
·
IF 9.5
Hui Wang,Xuefeng Zhang,Xiangfeng Wu,Yewei Kang,Yirui Huang,Zhaoye Zhao,Ziyan Li,Tingting Zhou,Junchuan Wang,Wei Zhu,Chengsi Pan
Bimetallic iron-based metal organic frameworks (MFe-MOFs) exhibit promising photocatalytic properties but face challenges typical of pristine MOFs, including low photoresponsive activity, inadequate band gap regulation, and weak photoconductivity. Here, we designed porphyrin-based COFs (TpPAM-COFs) to serve as a shell grown on NH2-Fe-MIL-101 nanoparticles (NPs) using an in situ solvothermal approach. Subsequently, a ligand-anchoring full-range metallization process was applied to introduce hetero metal ions throughout the core–shell composites, establishing a type-II scheme heterojunction (Fe/Cu-M@PC-Cu) via covalent bonding between NH2-Fe/Cu-MIL-101 and Cu-TpPAM-COFs. The Cu-TpPAM-COF shell, with broad light absorption range, enhanced the generation of photogenerated electrons, facilitating the reduction of Cu2+ and Fe3+ within the Fe/Cu-M@PC-Cu heterojunction and promoting the regeneration of Cu+ and Fe2+ Fenton active sites. Moreover, rapid electron transfer between Fe3+ and Cu+ centers amplified the Fe3+/Fe2+ redox cycle, accelerating the catalytic decomposition of H2O2 and increasing ·OH radical production. Additionally, the optimized bandgap structure of Cu-TpPAM-COFs enhanced the oxidation capacity, as evidenced by the Fe/Cu-M@PC-Cu composite achieving exceptional photo-Fenton catalytic efficiency with 92.7% tetracycline hydrochloride (TCH) degradation in 35 minutes, surpassing that of most reported similar catalysts. Furthermore, the composite showed excellent stability, with only an 11.9% loss in photo-Fenton degradation efficiency after 8 cycles, highlighting its great potential for addressing challenging environmental pollutants.
研究领域:
环境科学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Jingli Ren,Yutong Liu,Weimin Cao,Liyang Zhang,Fen Xu,Juan Liu,Yubo Wen,Jian Xiao,Lei Wang,Xiaoxiong Zhuo,Junfeng Ji,Yuanyuan Liu
Sediment-associated Fe(II) is a critical reductant for immobilizing groundwater contaminants, such as Cr(VI). The reduction reactivity of sediment-associated Fe(II) is dependent on its binding environment and influenced by the biogeochemical transformation of other elements (i.e., C, N and Mn), challenging the description and prediction of the reactivity of Fe(II) in natural sediments. Here, anaerobic batch experiments were conducted to study the variation in sediment-associated Fe(II) reactivity toward Cr(VI) in natural sediments collected from an intensive agricultural area located in Guangxi, China, where nitrate is a common surface water and groundwater contaminant. Then, a process-based model was developed to describe the coupled biogeochemical processes of C, N, Mn, Fe, and Cr. In the process-based model, Cr(VI) reduction by sediment-associated Fe(II) was described using a previously developed multirate model, which categorized the reactive Fe(II) into three fractions based on their extractabilities in sodium acetate and HCl solutions. The experimental results showed that Fe(II) generation was inhibited by NO 3 - and/or NO 2 − . After NO 3 − and NO 2 − were exhausted, the Fe(II) content and its reduction rate toward Cr(VI) increased rapidly. As the Fe(II) content increased, the three reactive Fe(II) fractions exhibited approximately linear correlations with aqueous Fe(II) concentrations ( C F e 2 + ), which was probably driven by sorptive equilibrium and redox equilibrium between aqueous and solid phases. The model results indicated that the reaction rate constants of the three Fe(II) fractions ( k n ) significantly increased with incubation time, and log( k n ) correlated well with C F e 2 + [ log ( k 1 ) = 2.84 C F e 2 + − 0.17 , log ( k 2 ) = 5.90 C F e 2 + − 2.49 and log ( k 3 ) = 3.09 C F e 2 + − 3.37 ]. The numerical model developed in this study provides an applicable method to describe and predict Cr(VI) removal from groundwater under dynamic redox conditions .
研究领域:
环境科学
·
地球化学
·
水文地质学
·
生物地球化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ENVIRONMENTAL MANAGEMENT
·
2024
·
IF 8
Xin Li,Aiyu Niu,Shanshan Yang,Fei Liu
Determining the contaminants reduction rate by dissolved ferrous iron (Fe(II) aq ) bound to iron oxides is curial for evaluating the abiotic attenuation of contaminants in aquifers. However, few studies have assessed the contaminants reduction rate controlled by thermodynamic parameters in heterogeneous systems with different iron oxides. In this study, a linear free energy relationship (LFER) was established between the nitrobenzene reduction rate and the thermodynamic driving force (reduction potential (E H ) and pH) in Fe(II) aq -goethite-hematite co-existing systems. Results showed that the reduction rate of nitrobenzene correlated with the E H of the heterogeneous system. The standard reduction potential (E H 0 mix ) of the mixed iron oxides could be obtained by a proportionate linear combination of the single iron oxide system E H 0 . Based on this, the E H of the heterogeneous systems could be calculated theoretically by combining E H 0 mix and the Nernst equation. Furthermore, a parallel LFER with the slope of 1 was established to associate the nitrobenzene reduction rate with E H and pH. The intercept term was related to the adsorption capacity of different iron oxides towards Fe(II) aq . The Fe(II) aq saturation adsorption capacity of hematite was 1.5 times higher than that of goethite. After normalizing the nitrobenzene reduction rate to the Fe(II) aq saturation adsorption capacity, the maximum difference in intercept terms was reduced from 37% to 15%. These findings would provide an important and feasible methodological support for the quantitative evaluation of abiotic attenuation of contaminants in groundwater.
研究领域:
环境科学
·
化学工程
·
地球化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL RESEARCH
·
2023
·
IF 8.3
Wen Qin,Jianshan Peng,Jingru Yang,Yang Song,Jun Ma
In this study, the relative residual UV absorbance (UV 254 ) and/or electron donating capacity (EDC) was investigated as a surrogate parameter to evaluate the abatement of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes. In the Fe(II)/PMS process, due to the generation of SO 4 •- and •OH at acidic pH, UV 254 and EDC abatement was greater at pH 5. In the Mn(II)/NTA/PMS process, UV 254 abatement was greater at pH 7 and 9, while EDC abatement was greater at pH 5 and 7. This was attributed to the fact that MnO 2 was formed at alkaline pH to remove UV 254 by coagulation, and manganese intermediates (Mn(V)) were formed at acidic pH to remove EDC via electron transfer . Due to the strong oxidation capacity of SO 4 •- , •OH and Mn(V), the abatement of micropollutants increased with increasing dosages of oxidant in different waters in both processes. In the Fe(II)/PMS and Mn(II)/NTA/PMS processes, except for nitrobenzene (∼23% and 40%, respectively), the removal of other micropollutants was greater than 70% when the oxidant dosages were greater in different waters. The linear relationship between the relative residual UV 254 , EDC and the removal of micropollutants was established in different waters, showing a one-phase or two-phase linear relationship. The differences of the slopes for one-phase linear correlation in the Fe(II)/PMS process (micropollutant-UV 254 : 0.36–2.89, micropollutant-EDC: 0.26–1.75) were less than that in the Mn(II)/NTA/PMS process (micropollutant-UV 254 : 0.40–13.16, micropollutant-EDC: 0.51–8.39). Overall, these results suggest that the relative residual UV 254 and EDC could truly reflect the removal of micropollutants during the Fe(II)/PMS and Mn(II)/NTA/PMS processes.
研究领域:
环境科学
·
化学工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
·
2022
·
IF 13.4
Wenkai Liu,Changrong Zhao,Shiqing Zhou,Bin Liu,Xiaoxiang Cheng,Zhihao Xue,Tingting Zhu
This study was aimed to evaluate the effects of a pre-treatment involving sulfite (S(IV)) synergistically activated by ultraviolet (UV)/Fe(II) on natural organic matter (NOM)-enhanced Ca 2+ scaling during nanofiltration treatment. Based on the variations in the physicochemical properties and correlation analyses of irreversible resistance, the intrinsic fouling mechanisms were revealed from two aspects: bulk crystallization (interaction between NOM and inorganic ions) and surface crystallization (morphology of surface crystallization and a change in the Ca 2+ concentration in the scaling layer). Furthermore, the degradation contribution rates of different free radicals during the UV/Fe(II)/S(IV) (UFS) treatment process were evaluated. During the reactions in the UFS, three free radicals (SO·–4, OH ·– and e- aq) were generated, and in-situ Fe(III) was formed in-situ . The carboxyl groups of the NOM were attacked by the free radicals, resulting in decreased of carboxyl concentration and density. In addition, the bond between Ca 2+ and NOM weakened, and hydrophobic (HPO) substances were mineralized. However, the Fe(III) formed in-situ was active and electropositive, competing with Ca 2+ for the complexation active sites on the NOM. The synergy effect of bulk crystallization and surface crystallization led to a significant decrease in the particle size of feed solution. The crystal size and roughness of membrane surface also decreased, which was conducive to reducing the membrane irreversible resistance. Correlation analysis revealed that the HPO ratio, carboxyl density and particle size (> 100 nm) ratio were effective characterization parameters for predicting irreversible resistance. This study not only provides guidance for alleviating membrane fouling caused by NOM-enhanced Ca 2+ scaling during the nanofiltration process, but also presents the rationality of irreversible resistance during nanofiltration process and various indicators with strong linear correlation.
研究领域:
环境科学
·
水处理工程
✓ 已验证
DOI
PubMed
高影响因子
Small
·
2024
·Vol. 20
·期 27
·2309541
·
IF 13
Tingting Liu,Kaiyue Hu,Yansheng Li,Yanhong Wang,Dongmei Han,Zhihua Wang,Fubo Gu
The Z-scheme MIL-88B/BiOBr (referred to as M x B y , whereas x and y are the mass of MIL-88B(Fe) and BiOBr) heterojunction photocatalysts are successfully prepared by a facile ball milling method. By adding low concentration H 2 O 2 under visible light irradiation, the Z-scheme heterojunction and photocatalytic-Fenton-like reaction synergistically enhance the degradation and mineralization of ciprofloxacin (CIP). Among them, M50B150 showed efficient photodegradation efficiency and excellent cycling stability, with 94.6% removal of CIP (10 mg L −1 ) by M50B150 (0.2 g L −1 ) under 90 min of visible light. In the M x B y heterojunctions, the rapid transfer of photo-generated electrons not only directly decomposed H 2 O 2 to generate · OH, but also improved the cycle of Fe 3+ /Fe 2+ pairs, which facilitated the reaction with H 2 O 2 to generate · OH and · O 2 − radicals. In addition, the effects of photocatalyst dosages, pH of CIP solution, and coexisting substances on CIP removal are systematically investigated. It is found that the photocatalytic- Fenton-like reaction can be carried out at a pH close to neutral conditions. Finally, the charge transfer mechanism of the Z-scheme is verified by electron spin resonance (ESR) signals. The ecotoxicity of CIP degradation products is estimated by the T.E.S.T tool, indicating that the constructed photocatalysis-Fenton-like system is a green wastewater treatment technology.
研究领域:
环境科学
·
材料科学
✓ 已验证
DOI
高影响因子
WATER RESEARCH
·
2024
·
IF 11.4
Zhaobin Liu,Shiliang Heng,Qicai Dai,Yijing Gao,Yule Han,Lingtian Hu,Yisheng Liu,Xueqin Lu,Guangyin Zhen
Waste activated sludge properties vary widely with different regions due to the difference in living standards and geographical distribution, making a big challenge to developing a universally effective sludge dewatering technique. The Fe(II)-activated persulfate (S 2 O 8 2− ) oxidation process shows excellent ability to disrupt sludge cells and extracellular polymeric substances (EPS), and release bound water from sludge flocs. In this study, the discrepancies in the physicochemical characteristics of sludge samples from seven representative cities in China (e.g., dewaterability, EPS composition, surface charge, microbial community, relative abundance of antibiotic resistance genes (ARGs), etc.) were investigated, and the role of Fe(II)-S 2 O 8 2− oxidation in enhancing removal of antibiotic resistance genes and dewatering ability were explored. The results showed significant differences between the EPS distribution and chemical composition of sludge samples due to different treatment processes, effluent sources, and regions. The Fe(II)-S 2 O 8 2− oxidation pretreatment had a good enhancement of sludge dewatering capacity (up to 76 %). Microbial analysis showed that the microbial community in each sludge varied significantly depending on the types of wastewater, the wastewater treatment processes, and the regions, but Fe(II)-S 2 O 8 2− oxidation was able to attack and rupture the sludge zoogloea indiscriminately. Genetic analysis further showed that a considerable number of ARGs were detected in all of these sludge samples and that Fe(II)-S 2 O 8 2− oxidation was effective in removing ARGs by higher than 90 %. The highly active radicals (e.g., SO 4 − ·, ·OH) produced in this process caused drastic damage to sludge microbial cells and DNA stability while liberating the EPS/cell-bound water. Co-occurrence network analysis highlighted a positive correlation between population distribution and ARGs abundance, while variations in microbial communities were linked to regional differences in living standards and level of economic development. Despite these variations, the Fe(II)-S 2 O 8 2− oxidation consistently achieved excellent performance in both ARGs removal and sludge dewatering. The significant modularity of associations between different microbial communities also confirms its ability to reduce horizontal gene transfer (HGT) by scavenging microbes.
研究领域:
环境工程
·
微生物学
·
污水处理
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Tong Zhang,Yuan Chen,Tao Wang,Chang Liu,Dan He,Bin Liu,Yuanyuan Liu
Advanced oxidation processes are widely used to remove petroleum hydrocarbons from soil, but usually consume large quantities of ferrous and acidify the soil. This study tested an advanced oxidation approach based on percarbonate in laboratory experiments. It removed 88% petroleum hydrocarbons in soil with a pH increase from 8.2 to 10.2. ·OH and ·CO 3 - were the main reactive species, and degraded 41% and 37% PHCs from soil respectively. The o-dihydroxybenzene structure in catechin was found to reduce ferric to ferrous, and prolong the generation of ·OH from 120 s to over 1800 s. The petroleum hydrocarbons were degraded to intermediates including alkanes and olefins through hydrogen-abstraction by ·OH and ·CO 3 - , and by dimerization and β-scission of alkyl radicals. These intermediates were then oxidized to CO 2 and H 2 O by ·OH and ·CO 3 - . The main residual intermediates in the soil were low-molecular-weight n-alkanes and branched alkanes, and they were found to inhibit the growth of oats ( Avena sativa L. ) much less than the original petroleum hydrocarbons. These findings provide a fundamental basis for designing effective technologies which use percarbonate to remove organic pollutants .
研究领域:
环境科学
·
土壤修复
✓ 已验证
产品关联
DOI
PubMed
高影响因子
危险品化学品经营许可证（带存储）