Journal of Water Process Engineering
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2024
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IF 6.3
S. Jafari,A.R. Faraji,A. Gil,F. Ashouri
Valorizing single-use plastic waste as an effective activator in environmental protection has gained great interest from policymakers, legislators, and scientific research communities. Herein, low-cost and highly porous alkali Fe/Mn-doped carbon nanomaterials derived from polyethylene terephthalate (PET) waste (MF/ c PET- x ) were fabricated via facile pyrolysis and alkali-metal impregnation methods. Detailed characterizations of MF- c PET- x demonstrated that the ratio of alkaline impregnation and pyrolysis temperature affects the porous characteristics, content, and size of active sites, specific surface area, and yield of carbon residue/nanocomposite. The main aim of this study was to evaluate and optimize the MF/ c PET- x applied for the detoxification of various kinds of pharmaceutical drugs ( tetracycline , naproxen , paracetamol , and levofloxacin ) and various dyestuff in their single, binary, ternary, and quaternary solutions. The magnetic porous MF/ c PET-1 was found to show a most effective PMS activation for single/multiple toxic pollutants removal attaining levels >91.0 % in a wide range of temperatures (5–35 °C) and pH (3.0–9.0), without significant detectable metal leaching (>0.16 mg L −1 ). The outstanding catalytic performance in complex water environments was mainly attributed to the deposition of Mn/Fe nanoparticles with small grain size on a polymeric scaffold, bimetal synergistic effect, high specific surface area, high stability, and excellent anti-interference capability against coexisting substances. Physicochemical properties of the recycled composite, masking, and EPR analyses confirmed that the dominant reactive species in the following order: 1 O 2 > OH > SO 4 − > O 2 − . This work offers a new and straightforward approach for preparing porous alloy composite from plastic waste for pollutant degradation in various water matrices.
研究领域:
环境科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2022
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IF 16.744
Wei Li,Zhilin Liu,Yangbo Dong,Luoqi Wang,Zhi Liu,Ling Zhang,Zhen-An Qiao
The spontaneous recombination of photogenerated carriers greatly limits the improvement of photocatalytic efficiency for bismuth oxychloride-based catalysts. Constructing porous or heterostructure photocatalysts can effectively inhibit their recombination. However, owing to the fast hydrolysis/condensation rates and uncontrollable nucleation/growth kinetics of Bi 3+ species, it is difficult to achieve inorganic–organic co-assembly, and form mesoscopic structure and heterostructure. Herein, a series of mesoporous bismuth oxychloride-based materials (Bi 2 O 3 at a stoichiometric ratio of 0 for Cl, Bi 12 O 17 Cl 2 , heterostructured Bi 12 O 17 Cl 2 /BiOCl and BiOCl) with various stoichiometry, tunable compositions and large surface areas are synthesized by a micellar interface modulation self-assembly strategy. In this strategy, Pluronic P123 and cetyltrimethyl ammonium chloride (CTAC) form P123/CTA + composite micelles, which assemble with Bi 3+ precursors by Coulomb interactions. Moreover, the Cl - ions are induced and modulated through composite micelles to involve in the slow hydrolysis and condensation of Bi 3+ precursors at the hydrophilic-hydrophobic interface of composite micelles to form mesophase, thereby realizing the synthesis of mesoporous bismuth oxychloride with various stoichiometry and compositions by regulating CTAC amount. The prepared mesoporous Bi 12 O 17 Cl 2 /BiOCl-O V shows superior photocatalytic activity (degrade 83% within 30 min for 10 mg/L carbamazepine and 99% within 10 min for 10 mg/L ciprofloxacin), which can be ascribed to the mesoporous architecture, intimate contact heterojunction and abundant surface oxygen vacancies. This work provides a new idea and strategy for design and synthesis of high-efficiency mesoporous bismuth oxychloride-based photocatalysts.
研究领域:
材料科学
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环境科学
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化学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Fuwei Sun,Haibo Liu,Hanlin Wang,Daobing Shu,Tianhu Chen,Xuehua Zou,Fangju Huang,Dong Chen
Natural iron-bearing minerals have been proven to be effective for activating H 2 O 2 to produce OH, which can be used to degrade organic pollutants . In this study, the performance of siderite to degrade sodium sulfadiazine via catalytic H 2 O 2 degradation was investigated at different solution pH values from 3 to 9. An interesting discovery was made: the performance of the siderite-H 2 O 2 system was excellent under acidic, neutral, and even alkaline conditions. The influence of various factors (e.g. initial concentration, anions, natural organic matters, etc.) on the system under different pH conditions was investigated, which confirmed that siderite exhibited an excellent catalytic performance. By combining EPR characterization with scavenger research, it was proposed that dissolved iron (Fe 2+ ) mainly initiated the homogenous Fenton reaction to degrade pollutants under acidic conditions, while structural Fe 2+ species present in siderite triggered Fenton-like reactions under neutral or even alkaline conditions. From the SEM and XPS characterizations, oxidation and dissolution of Fe 2+ on the surface were also observed, confirming our inference concerning the different reaction mechanisms. The experimental findings show that this siderite-H 2 O 2 system can be used in solutions with pH values from 3 to 9 and that siderite plays a positive role in soil and groundwater remediation when H 2 O 2 is used as an oxidant.
研究领域:
环境科学
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化学
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DOI
高影响因子
CHEMOSPHERE
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2015
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IF 3.34
Xiaofeng Wang,Beihai Zhou,Hongwei Yang,Xiaomao Wang,Yuefeng Xie
Nitro-based compounds are the direct precursors of trichloronitromethane during chlorination disinfection. Two nitro-based pharmaceuticals ranitidine and nizatidine were selected as model compounds to assess the effect of oxidation on the removal of nitro-based pharmaceuticals, as well as the reduction of their trichloronitromethane formation potentials (TCNMFPs). The four oxidants were ozone (O 3 ), chlorine (Cl 2 ), chlorine dioxide (ClO 2 ) and potassium permanganate (KMnO 4 ). The changes in pharmaceuticals and their TCNMFPs during oxidation using various oxidants and dosages were quantified. The relationships between oxidation product structures and TCNMFP changes were also analyzed. The results showed that oxidation with Cl 2 and KMnO 4 were more effective than ClO 2 and O 3 in removing the nitro-based pharmaceuticals. Meanwhile, decreased TCNMFPs by KMnO 4 oxidation but increased TCNMFPs by Cl 2 , ClO 2 and O 3 oxidation were observed. The results of product analysis indicated that chlorine transfer products had higher TCNMFPs, while oxygen transfer products made little contribution to TCNMFPs after oxidation. In addition, one possible reaction pathway leading TCNMFP increase was that chloro-nitromethane or nitromethane , which was a better TCNM precursor, formed when double bond was attacked by oxidants.
研究领域:
环境科学
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药学
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产品关联
DOI
PubMed
高影响因子
RAPID COMMUNICATIONS IN MASS SPECTROMETRY
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2021
·Vol. 35
·期 9
·e9062
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IF 2.419
Shaolan Wang,Jinsheng Lin,Dan Li,Tianpei Huang,Wenquan Zhu,Wenbin Chen,Min Li,Weiyang Shen
Rationale The focus of this work was to study glycosylamine and Amadori rearrangement products (ARPs), the two major degradants in the Maillard reactions of pharmaceutical interest, and utilize their MS 2 fingerprints by liquid chromatography/high-resolution tandem mass spectrometry (LC/HRMS 2 ) to quickly distinguish the two isomeric degradants. These two types of degradants are frequently encountered in the compatibility and stability studies of drug products containing primary or secondary amine active pharmaceutical ingredients (APIs), which are formulated with excipients consisting of reducing sugar functionalities. Methods Vortioxetine was employed as the primary model compound to react with lactose to obtain the glycosylamine and ARP degradants of the Maillard reaction, and their MS 2 spectra (MS 2 fingerprints) were obtained by LC/MS 2 . Subsequently, the two degradants were isolated via preparative HPLC and their structures were confirmed by one- and two-dimensional (1D and 2D) nuclear magnetic resonance (NMR) determination. Results The MS 2 fingerprints of the two degradants display significantly different profiles, despite the fact that many common fragments are observed. Specifically, protonated glycosylamine shows a prominent characteristic fragment of [M vort + C 2 H 3 O] + at m/z 341 (M vort is the vortioxetine core), while protonated ARP shows a prominent characteristic fragment of [M vort + CH] + at m/z 311. Further study of the Maillard reactions between several other structurally diverse primary/secondary amines and lactose produced similar patterns. Conclusions The study suggests that the characteristic MS 2 fragment peaks and their ratios may be used to differentiate the glycosylamine and ARP degradants, the two isomeric degradants of the Maillard reaction, which are commonly encountered in finished dosage forms of pharmaceutical products containing primary and secondary amine APIs.
研究领域:
药学
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分析化学
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药物稳定性研究
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产品关联
DOI
PubMed
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Wei Yang,Yan Zou,Zhihui Pang,Yanrong Zhang,Manabu Fujii
Sulfite [S(IV)] activation processes have aroused increasing attention in the field of wastewater treatment. In this study, a novel humic acid-derived carbon (HAC-10) material was demonstrated as highly active and environmentally friendly S(IV) activator for the efficient elimination of recalcitrant pharmaceutical contaminants. The results suggested that quinone groups and conductivity served as the active site/structure for S(IV) activation, while the rapid adsorption process of contaminant significantly reduced the migration distance of generated SO 4 – , thus facilitating the degradation processes. The carbon–S(IV)* complexes were confirmed to be the primary step to produce SO 4 – . The mineralization process of tetracycline hydrochloride (TC, a model pharmaceutical) could effectively reduce its biological toxicity. In addition, S(IV)/HAC-10 system exhibited excellent adaptability to different pharmaceuticals, natural water matrix and was capable of effectively eliminating contaminants in actual wastewater. Furthermore, a continuous flow reactor consisting of HAC-10 catalyst membrane showed excellent reactivity and durability. Overall, this study provides novel insights into the activation mechanism of S(IV) by carbon materials, and advances the practical application of S(IV) activation processes in the decontamination and detoxification of pharmaceutical wastewater.
研究领域:
环境科学
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废水处理
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污染控制
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Guangjian Xing,Lei Zhang,Yan Zhao,Sai Li,Tian Li,Tiantian Lv,Chunna Yu,Chang Zhao
The visible-light-responsive photocatalysts with high efficiency have been attracting tremendous focus in environmental remediation. Herein, three-dimensional (3D) Sb 2 X 3 ( X = S , Se) nanowires/graphene aerogel (Sb 2 X 3 /GA) monoliths were prepared by a facile hydrothermal route. The as-prepared Sb 2 X 3 /GA monoliths show the shape of a cylinder with a hierarchical porous structure. FESEM and porosimetry analyses revealed that the monoliths have high porosity, large total pore area as well as large pore volume . Sb 2 X 3 /GA demonstrated excellent photodegradation performance for the representative anionic/cationic dyes (methyl orange, rhodamine B , and crystal violet) and antibiotic drug (tetracycline hydrochloride) under 120 min of visible light irradiation. The degradation efficiencies of Sb 2 X 3 /GA were found to be 92.6–99.8% for the above-mentioned dye/drug, which were much larger than that of the pristine Sb 2 X 3 nanowires . The enhanced photodegradation activity could be ascribed to the synergistic effect between the Sb 2 X 3 nanowires and graphene aerogel, which was confirmed by the results of the photoluminescence and electrochemical impedance spectra. These findings provide an innovative strategy for designing 3D visible-light-responsive photocatalysts for water purification .
研究领域:
环境科学
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材料科学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2017
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IF 9.446
Fei Wu,Huawang Huang,Tiefeng Xu,Wangyang Lu,Nan Li,Wenxing Chen
Recently, peroxymonosulfate (PMS)-based advanced oxidation processes (AOPs) have received increasing attention because of their capability and adaptability in decontamination. The couple of solar light and PMS activation is an environmentally friendly and efficient strategy for environmental remediation. Herein, the iron hexadecachlorophthalocyanine (FePcCl 16 ) was used to coordinate with graphitic carbon nitride (g-C 3 N 4 ), which was functionalized by pyridine-based ligand isonicotinic acid (INA) to prepare a distinctive catalyst, g-C 3 N 4 -INA-FePcCl 16 . The experimental results revealed that g-C 3 N 4 -INA-FePcCl 16 can activate PMS efficiently for the elimination of carbamazepine (CBZ) under visible light irradiation over a wide pH range. Upon irradiation with visible light, CBZ was destroyed by the solider g-C 3 N 4 with generated sulfate (SO 4 − ) and hydroxyl ( OH) radicals, on the other hand, high-valent iron (Fe (IV) = O) species accompanied by SO 4 − and OH radicals were produced by excited-state FePcCl 16 (*FePcCl 16 ) during oxidation, which is different from a traditional PMS activation system. The axial pyridine-based ligand was protected under the FePcCl 16 macrocyclic structure shield. Noteworthy, in the absence of visible light, g-C 3 N 4 -INA-FePcCl 16 showed a higher catalytic performance than pure g-C 3 N 4 , FePcCl 16 and a mechanical mixture of the two. This study allows for the construction of an effective and environmental catalytic system, which can be applied to purify water that contains refractory pollutants.
研究领域:
环境科学
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化学工程
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产品关联
DOI
高影响因子
Frontiers in Materials
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2023
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IF 3.2
Ye Chao,Li Chengui
A type II band aligned BaTiO3/CeO2 photocatalysts was constructed by a simple one-step solution synthesis method. The BaTiO3/CeO2 photocatalysts contain only cubic phase BaTiO3 and CeO2, and the particles are approximately spherical with a small amount of adhesion and agglomeration, and the average particle size is about 50 nm. Transmission electron microscopy (TEM) observation and element Mapping characterization confirmed the formation of special heterojunction between BaTiO3 and CeO2 and the presence of a large number of oxygen vacancies, which resulted in high visible optical absorption coefficient. The BaTiO3/CeO2 photocatalysts demonstrated high photocatalytic activity for the degradation of oxytetracycin hydrochloride, and the optimal drug concentration, catalyst content and pH value are 50 mg/L, 1 g/L and 7, respectively. Simultaneously, the BaTiO3/CeO2 photocatalysts were selective for degradation of aureomycin hydrochloride, doxycycline hydrochloride and tetracycline hydrochloride. Other photocatalytic experiments show that the BaTiO3/CeO2 photocatalysts have high chemical and cyclic stability, and the synergistic effect of holes, hydroxyl radicals and superoxide radicals plays an important role in the whole photocatalytic process. This simple synthesis route provides a technical reference for constructing other wide-band gap semiconductors to respond to simulated sunlight.
研究领域:
材料科学
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环境科学
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药物化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMOSPHERE
·
2021
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IF 7.086
Yun Xia,Nan Li,Wangyang Lu,Wentao Wang,Yuyuan Yao,Zhexin Zhu,Tiefeng Xu,Yan Gu,Wenxing Chen
The overuse of antimicrobials has resulted in serious damage to the ecosystem and human health. Therefore, the development of an efficient, stable, and reusable catalyst to eliminate antimicrobials under mild conditions is highly desired. Drawing inspiration from the metabolism of drugs by the enzymes in the human body, such as heme catalase , we developed a simulated enzyme catalyst, perchloride iron phthalocyanine (FePcCl 16 ), immobilized on pyridine-modified multiwalled carbon nanotubes (FePcCl 16 -Py-MWCNTs). In the catalyst, FePcCl 16 worked as the active site, and the axial fifth ligand, 4-aminopyridine, was introduced to cleave H 2 O 2 heterolytically. Inspired by the reaction mechanism of heme catalase and H 2 O 2 , the catalytic system was designed based on FePcCl 16 -Py-MWCNTs for oxidizing 4-chloro-3,5-dimethylphenol (PCMX) by H 2 O 2 activation. The results showed that the catalytic activity of the system was significantly increased under simulated solar light irradiation, which can promote electron transfer for heterolytic cleavage of H 2 O 2 . The enzyme-like catalyst achieved much higher catalytic activity than the Fenton reaction when the pH was close to neutral. It turned out that the main active species was high-valent iron-oxo (Fe(Ⅳ) = O) rather than hydroxyl radial (•OH) or superoxide radical (•O 2 − ), different from most mechanisms. Ultraperformance liquid chromatography-high-definition mass spectrometry showed that the substrate was degraded to small molecule acids by Fe(Ⅳ) = O active species and further mineralization indicated by total organic carbon . The catalytic system exhibited highly efficient, stable, recyclable catalytic performance under mild conditions and did not cause secondary pollution to the environment. This study of a simulated enzyme catalytic system offers important insight into sewage treatment .
研究领域:
环境科学
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生物化学
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材料科学
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DOI
PubMed
高影响因子
CHEMOSPHERE
·
2024
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IF 8.1
Mingya Yao,Shuofeng Zhang,Meng Xie,Lingxi Zhao,Ru-Song Zhao
Peracetic acid (PAA) has garnered significant attention as a novel disinfectant owing to its remarkable oxidative capacity and minimal potential to generate byproducts. In this study, we prepared a novel catalyst, denoted as cobalt modified nitrogen-doped carbon nanotubes (Co@N-CNTs), and evaluated it for PAA activation . Modification with cobalt nanoparticles (∼4.8 nm) changed the morphology and structure of the carbon nanotubes , and greatly improved their ability to activate PAA. Co@N-CNTs/PAA catalytic system shows outstanding catalytic degradation ability of antiviral drugs . Under neutral conditions, with a dosage of 0.05 g/L [email protected] and 0.25 mM PAA, the removal efficiency of acyclovir (ACV) reached 98.3% within a mere 10 min. The primary reactive species responsible for effective pollutant degradation were identified as acetylperoxyl radicals (CH 3 C(O)OO•) and acetyloxyl radicals (CH 3 C(O)O•). In addition, density functional theory (DFT) proved that Co nanoparticles , as the main catalytic sites, were more likely to adsorb PAA and transfer more electrons than N-doped graphene. This study explored the feasibility of PAA degradation of antiviral drugs in sewage, and provided new insights for the application of heterogeneous catalytic PAA in environmental remediation.
研究领域:
环境科学
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催化化学
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污染控制
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产品关联
DOI
PubMed
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Hangjun Zhang,Yunyi He,Mengfan He,Qiyue Yang,Guoyi Ding,Yuanshuai Mo,Zhiquan Liu,Panpan Gao
Sulfate radical mediated advanced oxidation processes (SR-AOPs) have emerged as a promising alternative for emerging contaminants degradation. However, high activity and great stability are commonly difficult to juggle, and the structure-activity correlations are still ambiguous. This study constructed the cubic CaTiO 3 perovskite modified by highly-dispersed cobalt for peroxymonosulfate (PMS) activation to improve the specific lattice plane exposure and reduce the metal leaching simultaneously. 98% of amitriptyline (AMT) degradation was achieved within 60 min under the condition of 200 mg/L Co0.1-CTO and 100 mg/L PMS . The results indicated that surface Co 2+ /Co 3+ redox couple and lattice oxygen were responsible for PMS activation, and the evolution of · OH, SO 4 ·- and 1 O 2 were revealed. According to density functional theory (DFT) calculations, the highly-dispersed Co on cubic surface effectively captured PMS and promoted electron transfer for the generation of · OH and SO 4 ·- , while more oxygen atoms exposed on Co0.1-CTO(200) surface facilitated the generation of 1 O 2 . Briefly, this study provides a novel strategy of catalyst synthesis in PMS activation for water treatment .
研究领域:
环境科学
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催化材料
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水处理技术
✓ 已验证
产品关联
DOI
PubMed
高影响因子