ACS ES&T Engineering
·
2021
·
IF 0
Cong Wang,Shao-Yi Jia,You Han,Yang Li,Yong Liu,Hai-Tao Ren,Song-Hai Wu,Xu Han
Enzymatic polymerization of phenolic contaminants to polyphenolics by H2O2 is an effective method to turn phenolic wastes to useful polymers. However, the sensitivities and the high costs of enzymes always limit their applications in the long-run treatment of industrial wastewater. In this study, a highly efficient CuO-persulfate (PS) system is reported to be a promising candidate for enzyme–H2O2 and shows high reactivity to polymerize various phenolic contaminants to polymers under alkaline conditions with the ratio of PS/phenolics less than 2.0. Compared with the generally accepted mechanism that the oxidizing species of SO4•– and ·OH generated during PS activation primarily contribute to the oxidation of various organic contaminants, quenching experiments, EPR (electron paramagnetic resonance) analysis and DFT calculations in this study indicate that PS is activated on CuO via a nonradical pathway under alkaline conditions, and the O–O bond in PS is moderately elongated from 1.45 to 1.58 Å. The inversely linear relationship between log kobs and BDEO–H values of various phenolics in the Hammett plot confirms H-abstraction from various phenolics under alkaline conditions. DFT calculations further reveal the formation of phenolic radicals after the activated PS abstracts H from phenolic −OH, followed by subsequent polymerization of phenoxyl radicals to polyphenolics. Characterizations of the oxidation products confirm that more than 80% phenolic contaminants have been transformed to polyphenolics. This study provides a new alternative for recovering various phenolic contaminants from industrial wastewater.
✓ 已验证
产品关联
DOI
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2021
·
IF 4.539
Chunxiang Wan,Yuzhen Pan,Zhen Chen,Jinglu Hu,Zhe Zhang,Yawen Sun,Wei Ma
The application of Zinc oxide has drawn great attention in bacterial inhibition and contaminant degradation field in recent years. The internal structure and the morphology of the material was characterized by XRD , XPS , SEM , TEM. The dopant of 1 wt% graphene oxide（GO） and 30 wt% Al 2 O 3 shows excellent piezocatalytic and antibacterial ability. Application potential of the material is investigated by the degradation of RhB and the inhibition of Bacillus. It is found that the RhB solution can be degraded 92.5% by ZA-GO in 15 min, while ZnO can degrade 64.2%. It shows superior catalytic behavior in successive experiments of degradation of RhB without obvious decrease in efficiency. The quenching experiment combined with ESR spectrum demonstrate that both •O 2 - and •OH radicals were generated, while •OH did the most damage. Bacterial inhibition tests have also proven that the generation of reactive oxygen species cause the bacteria inactivated. In this work, a novel composite ZnO-Al 2 O 3 /GO has been successfully prepared based on mechanical synthesis method. Graphene oxide has higher mechanical strength and higher specific surface area. Zn ions doping carbon materials not only increases its stability, but also promotes its conductivity. The doping of Al atoms effectively reduce the work function of ZnO. Graphene oxide together with alumina coordinate the band gap of piezoelectric materials ZnO and the catalytic reaction efficiency was dramatically enhanced. What’s more, this work provides a facile approach eliminated the use of solvents and organic reagents, ensuring greater environmental safety. The novel zinc oxide matrix composites are depicted as a promising candidate to be used as intelligent antibacterial agent and alleviate environmental pollution.
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
·
2021
·
IF 6.498
Jinhui Wang,Huiyu Duan,Mengxue Wang,Qikai Shentu,Chaoming Xu,Yuchen Yang,Weiyang Lv,Yuyuan Yao
Developing filtering materials with high permeation flux and contaminant removal rate is of great importance for oily wastewater remediation. Herein, a robust three-dimensional (3D) activated carbon fibers (ACFs) based composite with uniformly grown layered double hydroxide (LDH) on the surface was successfully constructed through a feasible hydrothermal strategy. The LDH with a high surface energy and vertically aligned structure could provide superhydrophilicity to ACFs. Systematic investigation confirmed that the 3D material could overcome the size mismatch between the ACFs macropores and tiny emulsified droplets through the combination of size-sieving filtration on the surface and oil droplet coalescence in the fiber network. This process efficiently separated the intractable surfactant-stabilized oil-in-water emulsions with high permeation flux (up to 4.16 × 10 6 L m −2 h −1 bar −1 ). Notably, the LDH also had well-dispersed catalytic active sites, which could initiate advanced oxidation processes (AOPs) to efficiently eliminate various types of water-soluble organic pollutants (e.g., pharmaceuticals, phenolic compounds and organic dyes). The resulting modified ACFs exhibited exceptional removal rates for both oil and organic pollutants in the complex sewage during the continuous filtration process. These versatile abilities integrated with the facile preparation method reported herein provide outstanding prospects for the large-scale treatment of oily wastewater.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2021
·
IF 19.503
Jibo Dou,Jie Cheng,Zhijiang Lu,Ziqi Tian,Jianming Xu,Yan He
In this study, N/B co-doped biochars were employed as metal-free activators of peroxydisulfate (PDS) for tetracycline degradation, more importantly, the roles of dopants and the relative contribution of radical vs nonradical oxidations were comprehensively investigated. Integrating with electron paramagnetic resonance and kinetics calculations, we showed that co-doping N and B into biochars not only boosted the catalytic activity but also switched the radical PDS-activated process into the electron transfer-dominated nonradical process. Compared with pristine biochar/PDS systems (22%), the nonradical contribution of N/B co-doped biochar/PDS systems increased to 59%, exhibiting outstanding stability and selectivity. Galvanic oxidation tests and theoretical simulations unveiled that doped biochars as conductive tunnels accelerate the potential difference-driven electron transfer from the highest occupied molecular orbital of pollutants to the lowest unoccupied molecular orbital of PDS due to the lower energy gap. This study provided new insights into the critical role of heteroatom-doped carbocatalysts in PDS nonradical activation.
✓ 已验证
产品关联
DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
·
2021
·
IF 7.963
Lu Bai,Guanjun Wang,Dongdong Ge,Yanting Dong,Hui Wang,Yuhui Wang,Nanwen Zhu,Haiping Yuan
Dewatering treatment is an essential step to diminish sludge volume, cut down transportation costs, and improve subsequent disposal efficiency. In this study, ozone-peroxymonosulfate (O 3 /PMS) oxidation process was employed to ameliorate sludge dewaterability. Sludge capillary suction time (CST) and water content (Wc) of dewatered sludge cake could reduce from 70.5 s and 81.93% to 26.7 s and 65.65%, respectively, under the optimal dosage of 30 mg/g TS O 3 and 0.4 mmol/g TS PMS. The increased sludge zeta potential , particle size, and fluidity promoted sludge dewatering performance apparently. The decreased hydrophilic, fluorescent EPS components and proteins/peptides-like + Lipids percentage in EPS as well as the ratio of α-helix/(β-sheet + random coil) of treated EPS protein secondary structure was greatly responsible for the enhanced sludge dewaterability. SO 4 − and OH were detected in ozone-peroxymonosulfate process to crack sludge flocs, eliminate hydrophilic substances and liberate bound water. Moreover, the concentrations of both heavy metals and polycyclic aromatic hydrocarbons (PAHs) of sludge after O 3 /PMS conditioning were decreased, and the stability and toxicity of heavy metals were also reduced, except Zn. In conclusion, this work offered a comprehensive insight based on ozone-peroxymonosulfate (O 3 /PMS) advanced oxidation for improving the sludge dewaterability and environmental implication.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 23
·7683-7693
·
IF 6.119
Jialiang Sheng,Chunqiang Wang,Fang Duan,Shengrong Yan,Shuanglong Lu,Han Zhu,Mingliang Du,Xin Chen,Mingqing Chen
The reasonable construction of Z-scheme heterojunctions is an effective pathway to enhance the photocatalytic performance. In this work, a direct Z-scheme cadmium sulfide–nickel phthalocyanine (CdS–NiPc) heterojunction was successfully constructed by a one-step solvothermal method, which exhibited highly efficient photocatalytic activity for hydrogen evolution and good cyclic stability under visible light irradiation. An optimal sample CdS–10%NiPc with 10 wt% NiPc was obtained, and the photocatalytic hydrogen production rate could reach 17.74 mmol h−1 g−1, which was 19.1 times higher than that of the pure CdS sample. The reasons for the improvement and the photocatalytic mechanism were studied in detail. The result indicated that the formation of a direct Z-scheme heterojunction made a close contact between CdS and NiPc, which effectively accelerated the separation and migration of charges. This study enriches the CdS-based composite photocatalysts for hydrogen evolution and provides a simple method for the construction of efficient Z-scheme inorganic–organic heterojunctions.
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2021
·Vol. 11
·期 23
·7727-7739
·
IF 6.119
Biao Zhu,Qianxin Xu,Xiaoyan Bao,Dawei Lu,Hao Yin,Yumei Qin,Xing-Can Shen
The development of efficient and stable photocatalysts to solve environmental issues is essential and remains a big challenge. In this work, flower-like CoNiFe-LDH is deposited in situ on g-C3N4 nanosheets, successfully constructing a Z-scheme heterojunction CoNiFe-LDH/g-C3N4 photocatalyst for the photoreduction of CO2 and photodegradation of MB dye. The synthesized nanohybrid shows superior photocatalytic CO2 performance (42.04 μmol g−1 h−1) and fast photodegradation MB performance (0.1057 min−1). The improved photocatalytic performance was attributed to the formation of the Z-scheme heterojunction with matched energy bands, and the intimate heterojunction contact interface, which significantly enhanced the interfacial charge transfer rate and improved the separation efficiency of electron–hole pairs. Moreover, the photocatalytic mechanism was proposed based on PL, photocurrent responses, EIS, and EPR experiments. This work can shed light on further application for environmental problems of Z-scheme heterojunction photocatalysts.
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 52
·33149-33159
·
IF 3.361
Yu-qiong Gao,Yan-yan Rao,Han Ning,Da-qiang Yin,Nai-yun Gao
In this study, molybdenum disulfide (MoS2) was chosen as a co-catalyst to enhance the removal efficiency of phenacetin (PNT) in water by a ferrous ion-activated peroxymonosulfate (Fe2+/PMS) process. Operating parameters, such as the initial solution pH and chemical dose on PNT degradation efficiency were investigated and optimized. Under an initial pH of 3, an Fe2+ dose of 25 μM, a PMS dose of 125 μM and a MoS2 dose of 0.1 g L−1, the degradation efficiency of PNT reached 94.3%, within 15 min. The presence of common water constituents including Cl−, HCO3−, SO42− and natural organic matter (NOM) will inhibit degradation of PNT in the MoS2/Fe2+/PMS system. Radical quenching tests combined with electron paramagnetic resonance (EPR) results indicated that in addition to free radical species (˙OH, SO4˙− and O2˙−), nonradical reactive species (1O2) were also crucial for PNT degradation. The variations in the composition and crystalline structure of the MoS2 before and after the reaction were characterized by XPS and XRD. Further, the degradation pathways of PNT were proposed according to the combined results of LC/TOF/MS and DFT calculations, and primarily included hydroxylation of the aromatic ring, cleavage of the C–N bond of the acetyl-amino group, and cleavage of the C–O bond of the ethoxy group. Finally, toxicity assessment of PNT and its products was predicted using the ECOSAR program.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Nature Communications
·
2021
·Vol. 12
·期 1
·1-11
·
IF 14.919
Long Yanping,Li Ling,Xu Tao,Wu Xizheng,Gao Yun,Huang Jianbo,He Chao,Ma Tian,Ma Lang,Cheng Chong,Zhao Changsheng
Pathogenic drug-resistant bacteria represent a threat to human health, for instance, the methicillin-resistant Staphylococcus aureus (MRSA). There is an ever-growing need to develop non-antibiotic strategies to fight bacteria without triggering drug resistance. Here, we design a hedgehog artificial macrophage with atomic-catalytic centers to combat MRSA by mimicking the “capture and killing” process of macrophages. The experimental studies and theoretical calculations reveal that the synthesized materials can efficiently capture and kill MRSA by the hedgehog topography and substantial generation of •O 2 − and HClO with its Fe 2 N 6 O catalytic centers. The synthesized artificial macrophage exhibits a low minimal inhibition concentration (8 μg/mL Fe-Art M with H 2 O 2 (100 μM)) to combat MRSA and rapidly promote the healing of bacteria-infected wounds on rabbit skin. We suggest that the application of this hedgehog artificial macrophage with “capture and killing” capability and high ROS-catalytic activity will open up a promising pathway to develop antibacterial materials for bionic and non-antibiotic disinfection strategies.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Wenting Li,Xinglu Zhou,Shikai Liu,Jialing Zhou,He Ding,Shili Gai,Rumin Li,Lei Zhong,Huijie Jiang,Piaoping Yang
Therapeutic nanosystems triggered by a specific tumor microenvironment (TME) offer excellent safety and selectivity in the treatment of cancer by in situ conversion of a less toxic substance into effective anticarcinogens. However, the inherent antioxidant systems, hypoxic environment, and insufficient hydrogen peroxide (H2O2) in tumor cells severely limit their efficacy. Herein, a new strategy has been developed by loading the chemotherapy prodrug disulfiram (DSF) and coating glucose oxidase (GOD) on the surface of Cu/ZIF-8 nanospheres and finally encapsulating manganese dioxide (MnO2) nanoshells to achieve efficient DSF-based cancer chemotherapy and dual-enhanced chemodynamic therapy (CDT). In an acidic TME, the nanocatalyst can biodegrade rapidly and accelerate the release of internal active substances. The outer layer of MnO2 depletes glutathione (GSH) to destroy the reactive oxygen defensive mechanisms and achieves continuous oxygen generation, thus enhancing the catalytic efficiency of GOD to burst H2O2. Benefiting from the chelation reaction between the released Cu2+ and DSF, a large amount of cytotoxic CuET products is generated, and the Cu+ are concurrently released, thereby achieving efficient chemotherapy and satisfactory CDT efficacy. Furthermore, the release of Mn2+ can initiate magnetic resonance imaging signals for the tracking of the nanocatalyst.
✓ 已验证
产品关联
DOI
PubMed
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Jie Wang,Haibao Liu,Yan Wang,Defang Ma,Guangping Yao,Qinyan Yue,Baoyu Gao,Xing Xu
The newly emerged ultraviolet light-emitting diode (UV-LED) as a new UV source may replace the conventional UV lamps for water treatment in the foreseeable future. In this study, UV-LED with four wavelengths (i.e., 255, 265, 280, and 310 nm) was used to investigate the wavelength-dependency of UV-LED/O 3 process on the radical/non-radical formation and hexazinone degradation. The degradation of hexazinone in UV-LED/O 3 process with different wavelengths (31.1–97.4%) was higher than that of O 3 oxidation process alone (20.0%), and the hexazinone removal rate at 280 nm was the highest (97.4%). The fluence-based rate constant of hexazinone degradation in UV-LED/O 3 process (0.19–2.97 × 10 −5 m 2 ·J −1 ) was higher than that in low-pressure UV/O 3 (LPUV/O 3 ) process (0.15 × 10 −5 m 2 ·J −1 ). Hydroxyl radical (·OH) and superoxide radicals (O 2 − ) were the dominant active species in UV-LED/O 3 process, and the single oxygen ( 1 O 2 ) was also beneficial to the degradation of hexazinone. The possible degradation pathways were proposed based on high resolution mass spectrum (MS). The reaction sites of free radicals were further predicted by density functional theory (DFT) calculations. Besides, the Toxicity Estimation Software Tool (T.E.S.T.) and Vibrio fischeri were used to estimate the potential toxicity of hexazinone and intermediates and it was suggested that alkaline environment and sufficient oxidation time were conductive to reducing the toxicity of wastewater.
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Chuankun Yin,Qianna Xia,Jiao Zhou,Bowen Li,Yu Guo,Aimal Khan,Xiaoxia Li,Aihua Xu
The development of efficient and eco-friendly Mn-based catalysts for peroxymonosulfate (PMS) activation and revealing the mechanism are highly desired for pollutants removal in wastewater. In this study, a ternary mullite oxide YMn 2 O 5 (YMO) was synthesized for bisphenol A (BPA) degradation in the presence of PMS for the first time. Combined with XPS, EPR and TG, abundant surface labile oxygen species (O lab ) with a ratio of 39.7% were identified in the mullite materials, which was higher than that for α-, β-, γ- and δ-MnO 2 . YMO also exhibited higher interfacial conductivity and stronger interactions among the catalyst, PMS and BPA than other MnO 2 . Superior performance in BPA degradation was observed with YMO, and O lab was suggested as the main active sites, for the normalized first-order rate constant was linearly dependent on the ratio of the oxygen species. Chemical quenching experiments, EPR and open circuit potential suggested that the degradation of BPA was mainly caused by the direct electron transfer process through the reactive O lab -PMS complexes. The influence of YMO concentration, PMS concentration, solution pH, different anions and reaction temperature was thoroughly studied. Moreover, the intermediates were identified and the possible degradation pathways were proposed. This work demonstrated that mullite oxide YMO with enriched O lab species can be used as eco-friendly catalysts for efficient PMS activation to remove recalcitrant organic compounds in wastewater.
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）