SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
LiWei Yang,YanYan Jia,YaQi Peng,Peng Zhou,Dian Yu,ChuanLiang Zhao,JiaoJie He,ChuanLang Zhan,Bo Lai
Removal of pharmaceutical and personal care products from wastewater is very important in water treatment process. Combining photocatalysis with persulfate (PS) could be a good solvent for this problem. Novel perylene diimide derivative (EHPDI) was designed and synthesized. Furthermore, self-assembled EHPDI/TiO 2 composite photocatalyst (EPT) was prepared and applied in activating persulfate (PS) under visible light to enhance the photodegradation of pollutants. The presence of the alkyl side chain 2-ethylhexyl optimizes the self-assembly process, enabling the composite material to achieve high performance under low EHPDI loading. Various methods were used to detect the physical and chemical characteristics of EPT. Carbamazepine (CBZ) was chosen to be the model pollutant to study the removal efficiency of EPT/PS system under visible light. Within 30 min, 5.0 mg/L CBZ could be almost completely degraded, and the removal ratio of TOC was 75.2% within 60 min. The SO 4 – , OH, O 2 – , 1 O 2 , and h + were proved to be involved in the removal of CBZ by EPR and quenching experiments. Then, other typical pollutants were degraded by this EPT/PS system, demonstrating this system is suitable for degrading different pollutants. Besides, the degradation paths of CBZ were proposed by HPLC/MS. Finally, the EPT showed excellent recyclability and stability.
研究领域:
环境科学
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水处理
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光催化
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材料科学
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2021
·
IF 13.273
Yuxuan He,Jin Qian,Peifang Wang,Jie Wu,Bianhe Lu,Sijing Tang,Pan Gao
The nanocomposite of MoS 2 embedded manganese ferrite doped perovskite (SrCoO 3 /MnFe 2 O 4 /MoS 2 , abbreviated as SMM) was successfully synthesized for peroxymonosulfate (PMS) activation under visible-light. It was optimized that the SMM-3 (mass ratio of MoS 2 modified nanocomposite was 0.3) exhibited excellent catalytic performance to activate PMS for levofloxacin (LVF) degradation, with the degradation efficiency of 95.1% in 20 min. Besides, SMM-3 was able to efficiently degrade LVF under real water matrix. The quenching experiments and electron paramagnetic resonance (EPR) analysis revealed that SO 4 •- and HO • played a dominant role in reaction. Due to the photocatalytic property of nanocomposites, the visible light could excite electrons to react with oxygen and form O 2 •- , which further reacted with HO • to produce 1 O 2 . In the reaction process, the rapid redox cycle of metal ions (including Co, Mn, Fe and Mo) boosted the activation of PMS and promoted the degradation of LVF in a short time. The Density functional theory (DFT) calculation and LC-MS/MS further revealed that oxidation of piperazine ring, decarboxylation and defluorination processes were the main LVF degradation pathways. Finally, the toxicity analysis based on Toxicity Estimation Software Tool (T.E.S.T) verified the ecological risks of transformation residues.
研究领域:
环境科学
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材料科学
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化学工程
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光化学
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催化
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2025
·
IF 9
Ruoyi Li,Jian Zhang,Dong Liu,Haina Bai,Chuntao Zhu,Xinyan Wang,Jia Li
In conventional Electro-Fenton systems, the oxidation process dominated by the Fe 2+ /Fe 3+ cycle and · OH radicals, although effective in degrading organic pollutants, is still limited by a narrow pH applicability range (2–4). To address this challenge, a coral-like ZnO nanospheres modified Cu(OH) 2 @CF composite electrode was synthesized in this study, which significantly broadened the applicable pH range (2–10). The ZnO/Cu(OH) 2 @CF composite electrode enhanced the selective generation of single-linear oxygen ( 1 O 2 ) and overcame the inherent defects, such as the extremely short lifetime of · OH (<1 μs), while enabling the efficient in situ generation of H 2 O 2 (272.51 mg/L, 30 min). And the complete degradation of tigecycline (TGC) was realized within 30 min with an operating cost of only 0.044 ¥·m −3 (energy consumption 0.076 kWh·m −3 ). and a low Tafel slope of only 24.80 mV·dec -1 is required for an efficient Electro-Fenton reaction. Notably, the ZnO/Cu(OH) 2 @CF composite electrode exhibited high degradation rates for a variety of typical antibiotics and could be adapted to different water quality conditions. After 10 cycles of use, its degradation rate of TGC was still as high as 92.67 %. The continuous flow reactor not only maintained more than 90 % degradation efficiency for TGC after 300 min of operation, but also maintained a high degradation rate of 80 % for mixed antibiotic wastewater. The dominant mechanism of action of 1 O 2 was deeply analyzed by bursting experiments and electron paramagnetic resonance (EPR). The two-dimensional correlation spectroscopy (2DCOS), three-dimensional fluorescence spectroscopy (3DEEMs) and liquid chromatography-mass spectrometry (LC-MS) techniques were used to reveal the degradation pathways of the pollutants and the toxicity evolution of the intermediates.
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Jin Zhang,Hanxuan Zeng,Lingjun Bu,Shiqing Zhou,Zhou Shi,Lin Deng
In this study, zero valent copper (Cu 0 ) was incorporated into ZIF-67 to construct Cu 0 and cobalt/nitrogen doped carbonaceous frameworks x -Cu@Co N C y . The obtained Cu@Co N C was employed to activate PMS to degrade naproxen (NPX) in aqueous phase. Influencing factors on NPX degradation were investigated, including mole ratio of Cu/Co, pyrolysis temperature, pH, catalyst dosage, PMS concentration, and coexisting inorganic anions. In the presence of 0.5 mM PMS and 25 mg/L 1:3-Cu@Co N C 900, complete degradation of NPX (50 μM) could be achieved in 20 min within a wide pH range of 3 to 10. The superior catalytic activity of Cu@Co N C 900 for PMS activation was related to the increased surface –OH groups, accelerated electron transfer rate induced by Cu 0 with strong conductivity, formed surface PMS complexes with high oxidation activity, and synergistic effect between Cu and Co. EPR analysis, radical scavenging and probe tests excluded the participation of SO 4 − and OH in NPX degradation. Nonradical pathways of electron transfer from NPX to PMS and 1 O 2 oxidation contributed to the excellent degradation. The 1:3-Cu@Co N C 900 demonstrated a decent degradation performance even after five consecutive recycles with low cobalt and copper ions leaching due to the encapsulation of Co and Cu on N -doped porous carbon. Further, the intermediates of NPX degradation were identified, and three possible degradation pathways were proposed. Overall, this work provides a feasible strategy to improve the stability and catalytic activity of ZIF-67 by the incorporation of Cu 0 .
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Ying Fang,Qianwen Liu,Yang Song,Feiyue Jia,Ying Yang,Haipu Li
Dissolved organic matter (DOM) extensively exists in high-arsenic groundwater with relatively high concentration, which could not only compete with arsenic for adsorption sites, but also depress As(III) oxidation in persulfate-based advanced processes (PS-AOPs) through scavenging free radicals (SO 4 • − and •OH). In order to effectively avoid the negative effect of DOM , an Fe/Co bimetallic metal–organic framework (Fe/Co MOF)-coupled peroxymonosulfate (Fe/Co MOF-PMS) system was rationally constructed for non-radical-dominated As(III) oxidation and chemisorption-driven As(V) adsorption. Results showed that the Fe/Co MOF-PMS system did realize anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater, which was evidenced by no difference in As(III) immobilization efficiencies in the absence and presence of 20 mg/L humic acid (HA). During the oxidation process, 1 O 2 dominated As(III) oxidation while O 2 • − dominated HA oxidation, and the presence of HA significantly promoted the generation of 1 O 2 besides SO 4 • − and •OH. During the adsorption process, chemical adsorption mainly drove As(V) adsorption such as forming M-O-As (M = Fe, Co) bond, while physical adsorption forces played a major role in HA adsorption, such as π-π interaction, hydrogen bonding, and electrostatic attraction. The synergism of oxidation and adsorption processes made the anti-interference As(III) immobilization in DOM-rich high-arsenic groundwater in Fe/Co MOF-PMS system come true. This work is believed to shed light on the highly efficient purification of DOM-rich high-arsenic groundwater.
研究领域:
环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
Environmental Science-Nano
·
2020
·Vol. 7
·期 10
·2982-2994
·
IF 7.683
Weijian Duan,Jinglei He,Ziliang Wei,Zongren Dai,Chunhua Feng
The heteroatom-doped, carbon-activated peroxymonosulfate (PMS) system proceeding via the non-radical oxidation pathway involving singlet oxygen (1O2) represents a promising advanced oxidation process (AOP) due to the resistance of 1O2 to background anions in solution. However, the performance level of pollutant removal is not yet satisfied, and the mechanism of 1O2 generation remains elusive. Herein, we report the development for the first time of a unique Si-engaged heteroatom (i.e., N)-doped carbon (Si/N–C) nanomaterial for PMS activation, which exhibits outstanding performance in the removal of various kinds of pollutants and an appreciably wide working pH range of 2.5 to 11. Taking rhodamine B (RhB) as an example, the Si/N–C@PMS system achieved a much higher reaction rate (0.64 min−1) than the Si–C (0.047 min−1), N–C (0.017 min−1), SiO2 (0.021 min−1), and Co3O4 (0.026 min−1; a standard catalyst) systems. In addition, the results of electron spin resonance (ESR) and scavenging experiments solidly support the conclusion that the mechanism of 1O2 generation in this system is via the recombination of superoxide radicals O2˙−, a pathway seldom reported for metal-free, catalyst-activated PMS systems. More importantly, we observed apparent inhibition effects of the anions (e.g., HCO3−, HPO42−, and PO43−) on the degradation performance, inconsistent with many previous reports suggesting that the 1O2-mediated oxidative system possesses a high selectivity toward pollutant degradation in the presence of these anions. Further studies with the anions, including Cl−, HCO3−, and HxPO4(3−x) (x = 0, 1, 2), suggest that the reaction between O2˙− and these anions is the main reason for the abnormal salt effect. This work will deepen the understanding of 1O2 formation via the intermediate of O2˙− and provide a new insight into its salt resistance capacity.
研究领域:
环境化学
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材料科学
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催化
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水处理
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DOI
高影响因子
BIOMATERIALS
·
2020
·
IF 10.317
Jing Yan,Qinghua Wu,Ziyin Zhao,Jianhua Wu,Huan Ye,Qiujun Liang,Zhuchao Zhou,Mengying Hou,Xudong Li,Yong Liu,Lichen Yin
The anticancer performance of nanomedicine is largely impeded by insufficient intratumoral penetration. Herein, tumor microenvironment (TME)-amendatory and self-adaptive nanoclusters (NCs) capable of cancer-associated fibroblasts (CAFs) depletion and size/charge conversion were engineered to mediate light-assisted, hierarchical intratumoral penetration. Particularly, large-sized NCs (~50 nm) were prepared via self-assembly of FAP-α-targeting peptide-modified, 1 O 2 -sensitive polymers, which were further used to envelope small-sized dendrimer (~5 nm) conjugated with Ce6 and loaded with DOX (DC/D). After systemic administration, the NCs efficiently targeted CAFs and generated lethal levels of 1 O 2 upon light irradiation, which depleted CAFs and concomitantly dissociated the NCs to liberate small-sized, positively charged DC/D. Such stroma attenuation and NCs transformation collectively facilitated the delivery of DC/D into deeper regions of CAF-rich tumors, where DOX and 1 O 2 provoked synergistic anti-cancer efficacies. This study provides an effective approach to facilitate the tumor penetration of nanomedicine by concurrently and spatiotemporally reconfiguring the nano-properties and remodeling the TME.
研究领域:
纳米技术
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癌症治疗
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药学
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生物医学工程
✓ 已验证
DOI
PubMed
高影响因子
CHEMOSPHERE
·
2021
·
IF 7.086
Likun Chen,Kewen Xing,Qikai Shentu,Yifei Huang,Weiyang Lv,Yuyuan Yao
Developing single-atom Fenton-like catalysts with the maximum utilization of active sites present an attractive potential in environmental remediation. Herein, the single-atom Fe and N co-doped hollow carbon microsphere loaded g-C 3 N 4 catalyst (HFeNC-g-C 3 N 4 ) was prepared by an innovative cascade anchoring strategy using polystyrene as the hard template, iron phthalocyanine, polydopamine and urea as the Fe, N and C precursor, in which the in-situ generated g-C 3 N 4 could not only effectively anchor Fe atom to create the well-dispersed Fe-N x active sites, but also accelerate the electron transfer in peroxymonosulfate (PMS) activation. Taking advantages of such sequential protecting strategy, the as-synthesized HFeNC-g-C 3 N 4 catalyst with single-atom Fe-N x active sites, verified by XRD , XPS and HAADF-STEM, could work as an efficient Fenton-like catalyst for PMS activation, which achieved almost 100% removal of 4-chlorophenol (4-CP) in 5 min with the turnover frequency calculated to be 34.6 times higher than that of the homogeneous Fe 2+ catalyst. The mechanism of O 2 •- dominated radical combined with nonradical 1 O 2 pathway was confirmed by quenching experiments and ESR analysis, which might be interrelated to the improvement of pH adaptability and interference immunity of HFeNC-g-C 3 N 4 /PMS system. Overall, the present findings provided an innovation strategy for the synthesis of excellent single-atom Fe based catalyst in wastewater purification.
研究领域:
环境科学
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催化
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Caiyun Xu,Junqin Li,Chunlei Ou,Jing Yang,Shuting Fu,Weiqing Hu,Li Wang,Zefeng Wang,Luo Hai,Le Deng,Dinggeng He
Chemodynamic therapy (CDT) involving highly toxic hydroxyl radical (•OH) with no drug resistance has gained widespread attention for antibacterial applications. However, the CDT effect is seriously confined by overexpressed glutathione (GSH) and limited hydrogen peroxide (H 2 O 2 ) in the infection sites. Here, we have constructed a cascade enzyme/nanozyme assembly (MCS/GOx) composing of a bimetallic sulfide MoCuS x (MCS) nanozyme loaded with natural glucose oxidase (GOx) for synergistic photothermal/photodynamic enhanced chemodynamic antimicrobial therapy with high performance. The loaded GOx can promote the peroxidase (POD)-like activity of MCS by providing an acidic microenvironment and self-supplying H 2 O 2 , achieving cascade generation of •OH for efficient CDT. The CDT effect can be further promoted by a co-catalysis mediated by the Mo 4+ /Mo 6+ redox couple. Upon exposure to an 808 nm near-infrared laser, MCS/GOx provides hyperpyrexia for photothermal antibacterial therapy (PTT), and produce singlet oxygen ( 1 O 2 ) for photodynamic therapy (PDT). Moreover, MCS/GOx can significantly consume antioxidant glutathione via the Cu + /Cu 2+ redox couple and PDT-mediated 1 O 2 production, thereby enhancing CDT antibacterial effect. In vitro experiments exhibit that MCS/GOx has combined antimicrobial effect against Staphylococcus aureus and Escherichia coli . Further in vivo studies demonstrate that MCS/GOx can efficiently eliminate bacterial cells in wound tissues and accelerate wound healing with low inflammatory response and good biosafety. Consequently, the proposed MCS/GOx with multiple bactericidal modalities shows a great potential in fighting wound infections.
研究领域:
纳米技术
·
生物医学工程
·
材料科学
·
药学
·
细菌学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Qiansheng Li,Hong Lu,Xiaolei Wang,Zhongqiang Hong,Ze Fu,Xinxin Liu,Jiti Zhou
Low solar energy utilization, instability of Fe ions and Fe(III)/Fe(II) cycle difficulty are three main factors, limiting the photocatalytic activity of the Fe/peroxymonosulfate (PMS) system. Herein, based on the N and Fe co-doped carbon dots (N, Fe-CDs) synthesized by a facile one-pot hydrothermal method, a new Fe(III)/Fe(II) cycle system for PMS activation under visible light irradiation was proposed. The characterization experiments showed that Fe has been successfully doped to the sp 2 graphitic structure and mainly existed as Fe-N and Fe-OH complexes, which played an important role in harvesting visible light, enhancing the stability of Fe ions and acting as active sites to accelerate electron transfer. Under visible light irradiation, the photogenerated electrons of N, Fe-CDs could be directly transferred to Fe (III) for Fe (II) formation via the ligand-to-mental charge transfer process, thus accelerating the Fe(III)/Fe(II) cycle. When N, Fe-CDs were used for activating PMS under visible light irradiation, aminopyrine could be efficiently degraded and mineralized to CO 2 via the cleavage of pyrazole ring, demethylation, hydroxylation, decarbonylation and the cleavage of benzene ring. The produced O 2 − and 1 O 2 played the main roles in the whole photocatalytic reaction. The above results revealed that the novel N, Fe-CDs could effectively activate PMS under visible light irradiation for the degradation of pharmaceuticals in the polluted water.
研究领域:
环境科学
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光催化
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水处理
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 42
·16119-16125
·
IF 4.569
Shengnan Liu,Jiahong Han,Weijin Wang,Yulei Chang,Runlin Wang,Ziwei Wang,Guangzhe Li,Dongxia Zhu,Martin R. Bryce
Photodynamic therapy (PDT) is a promising cancer treatment method. Traditional small-molecule photosensitizers (PSs) suffer from low intersystem crossing (ISC) ability and aggregation-caused quenching (ACQ), which adversely affects the luminous efficiency and singlet oxygen (1O2) yield of PSs in the aggregated state. Ir(III) complexes are promising PSs with long excited-state lifetime, good photophysical and photochemical properties and large Stokes shifts. Aggregation-induced emission (AIE) characteristics could reduce the nonradiative recombination and improve the ISC ability of excited states through the restriction of the intramolecular motions in aggregated states. Accordingly, two AIE-active Ir(III) complexes Ir-1-N+ and Ir-2-N+ were successfully designed and obtained based on Schiff base ligands. Experimental results showed that Ir-1-N+ and Ir-2-N+ have good photophysical properties and the corresponding nanoparticles (NPs) have good water solubility and 1O2 generation ability. Notably, Ir-2-N+ NPs can be efficiently taken up by mouse breast cancer cells (4T1 cells) with good biocompatibility, low dark toxicity and excellent phototoxicity. This work demonstrates a versatile strategy for exploiting efficient transition metal PSs with a cationic ligand in PDT.
研究领域:
化学
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材料科学
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生物医学工程
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癌症研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
·
2022
·
IF 14.224
Wensong Zou,Jing Li,Ranhao Wang,Jingyi Ma,Zhijie Chen,Lele Duan,Hongwei Mi,Hong Chen
Herein, we converted spent LiFePO 4 battery to the sea urchin-like material (SULM) with a highly efficient and environment-friendly method, which can contribute to building a zero-waste city. With SULM as a Fenton-like catalyst, a highly-efficient degradation process was realized for organic pollutants with interface and solution synergistic effect. In our SULM+NH 2 OH+H 2 O 2 Fenton-like system, NH 2 OH can effectively promote the interface iron ( Fe(Ⅲ)/ Fe(Ⅱ)) and solution iron (Fe(Ⅲ)/Fe(Ⅱ)) redox cycle, thus promoting the generation of reactive oxygen species (ROS). However, the ROS generation process and organic pollutants degradation pathway with the presence of NH 2 OH remains a puzzle. Here the detailed ROS generation mechanism and pollutants degradation pathway have been illustrated carefully based on experimental exploration and characterization. Therein, hydroxyl radicals (·OH) and singlet oxygen ( 1 O 2 ) are the main ROS for oxidizing and degrading organic pollutants. Notably, 1 O 2 can be converted from superoxide radicals (·O 2 ) in SULM+NH 2 OH+H 2 O 2 system. This study not only demonstrates the strategy of "trash-to-treasure" and "waste-to-control-waste" to simultaneously reduce the hazardous release from industrial solid waste and organic wastewater, it also provides new mechanistic insights for NH 2 OH mediated Fenton-like redox system.
研究领域:
环境科学
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材料科学
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化学工程
·
废物管理
✓ 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）