JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Xiao Li,Jin Chang,Hexin Zhang,Jing Feng,Jun Ma,Chengying Bai,Yueming Ren
Photocatalytic nitrate (NO 3 - ) reduction is considered a promising green and non-polluting technology to solve the nitrate pollution of groundwater and surface water. Herein, a novel Br-substituted Bi 2 WO 6−x ultrathin nanosheets were prepared by a simple hydrothermal method in a strong acid environment containing sixteen alkyl three methyl bromide (CTAB). The catalytic system solves the problems of low carrier separation efficiency, poor performance under alkaline conditions, and a hard-to-activate N = O bond, achieving efficient NO 3 - removal under alkaline conditions along with high N 2 selectivity . It was confirmed that Br-substituted Bi 2 WO 6−x produced the [W (VI) O 6−x ] units with a strong electron-withdrawing property by changing the polarity of the O-W-O bond. As a result, the effective space charge separation caused by the change of the W valence state and the spontaneous fracture behavior of the N = O bond improved the carriers utilization efficiency and distinctly reduced the reaction energy consumption, synergistically achieving excellent performance.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Jiajun Yu,Xiao Wang,Yan Wang,Xiaofeng Xie,Haijiao Xie,Nat Vorayos,Jing Sun
The removal of indoor/outdoor toluene by photocatalysis has drawn much attention due to its low energy consumption and easy availability. However, light inevitably generates heat, and pollutants desorb from catalysts as the temperature rises, which is not beneficial to degradation. Contrast to the frequently occurred phenomena, we firstly found that the adsorption capacity of UiO-66 (Zr) on toluene increased with increasing temperature as adsorption isotherms and in-situ Fourier transform infrared spectra (in-situ FTIR) showed. The optimum temperature was 30 °C. This stage in which adsorption capacity was positively correlated with temperature was called heating-induced adsorption, which achieved a toluene removal efficiency of 69.6 %. By density functional theory (DFT) calculations and changing the metal centers and organic ligands of UiO-66 (Zr) respectively, we disclosed that the heating-induced adsorption was mainly related to the π-π stacking interaction of MOF ligands and toluene. The analysis of samples before and after adsorption showed that the interaction between UiO-66 (Zr) and adsorbed toluene facilitated the charge transfer and prolonged the carrier lifetime, leading to the increase of hydroxyl radicals (•OH) in photocatalysis. Therefore, a synergistic effect between heating-induced adsorption and photocatalysis was proposed by analyzing the adsorption of toluene on UiO-66 (Zr) in detail. This work provided new viewpoint to understand the role of concomitant heat contributed to the adsorption and degradation of toluene during photocatalysis.
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Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Jiangwei Shang,Shuwen Fan,Shihu Cao,Xinrui Gan,Jing Nie,Tianning Zhang,Xiangchen Li,Dan Feng,Xiuwen Cheng
In this study, a CuCo 2 S 4 microporous composite membrane (CCSM) was successfully prepared by loading CuCo 2 S 4 nanoparticles on a membrane substrate, and then used to activate PMS to degrade carbamazepine (CBZ). Meanwhile, the physicochemical properties of the nanomaterial and the effects of various reaction parameters, such as, catalyst film loads, PMS dosage, initial pH value, and co-existing substances on the catalytic degradation performance were investigated. The results showed that CCSM/PMS exhibited admirable catalytic performance, and 90.3% CBZ could be degraded within 3 min under the optimum conditions ([CuCo 2 S 4 ] = 0.05 g L −1 , [PMS]=0.30 g L −1 , [CBZ] 0 =10 g L −1 and Initial pH = 6.95). Furthermore, the CCSM/PMS system could efficiently degrade various antibiotics (sulfamethoxazole, metronidazole, hydrochloride and ciprofloxacin). In addition, the reusable ability of CCSM without significant efficiency loss after 10 cycles. The quenching experiments and electron paramagnetic resonance (EPR) characterization showed that the main active species were SO 4 • - , •OH, O 2 • - and 1 O 2, and SO 4 • - played a dominant role in this system. Finally, based on the data analysis, the study proposed the possible degradation mechanism and four degradation routes of CBZ.
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CHEMOSPHERE
·
2023
·
IF 8.8
Zhujun Luo,Wantang Huang,Wenyan Yu,Shaoyu Tang,Kun Wei,Yuanyuan Yu,Lei Xu,Hua Yin,Junfeng Niu
Tris (2-butoxyethyl) phosphate (TBOEP) has gained significant attention due to its widespread presence and potential toxicity in the environment. In this study, the degradation of TBOEP in aquatic media was investigated using electrochemical oxidation technology . The anode Ti/SnO 2 –Sb/La–PbO 2 demonstrated effective degradation performance, with a reaction constant ( k ) of 0.6927 min −1 and energy consumption of 1.24 kW h/m 3 at 10 mA/cm 2 . CV tests, EPR tests, and quenching experiments confirmed that indirect degradation is the main degradation mechanism and ·OH radicals were the predominant reactive species, accounting for up to 93.8%. The presence of various factors, including Cl − , NO 3 − , HCO 3 − and humic acid (HA), inhibited the degradation of TBOEP, with the inhibitory effect dependent on the concentrations. A total of 13 intermediates were identified using UPLC-Orbitrap-MS/MS, and subsequent reactions led to their further degradation. Two main degradation pathways involving bond breaking, hydroxylation, and oxidation were proposed. Both Flow cytometry and the ECOSAR predictive model indicated that the intermediates exhibited lower toxic than the parent compound, resulting in a high detoxification rate of 95.9% for TBOEP. Although the impact of TBOEP on the phylum-level microbial community composition was found to be insignificant, substantial alterations in bacterial abundance were noted when examining the genus level. The dominant genus Methylotenera , representing 17.4% in the control group, decreased to 6.9% in the presence of TBOEP and slightly increased to 8.7% in the 4-min exposure group of degradation products . Electrochemical oxidation demonstrated its effectiveness for the degradation and detoxification of TBOEP in aqueous solutions, while it is essential to consider the potential impact of degradation products on sediment microbial communities.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zuming He,Kai Lin,Ngie Hing Wong,Jaka Sunarso,Yongmei Xia,Xiaofei Fu,Jiangbin Su,Zhengyi Huang,Yong Wang,Bin Tang
Semiconductor photocatalysis technology for environmental remediation faces primary challenges, such as charge-carrier recombination and interfacial charge transfer inhibition, which affect its degradation efficiency in removing organic contaminants. In this work, we successfully synthesized a unique Z-scheme KNbO 3 /ZnIn 2 S 4 hollow core–shell microsphere via a combined hard template, thermal treatment, and hydrothermal processes as the photocatalyst for ciprofloxacin (CIP), oxytetracycline hydrochloride (OTCH), and rhodamine B (RhB) remediation under sunlight irradiation. Compared to the pure KNbO 3 and ZnIn 2 S 4 , our optimized 15-KNbO 3 /ZnIn 2 S 4 composite exhibited enhanced photodegradation performance with up to 99.8 %, 96.8 % and 97.5 % for CIP, OTCH, and RhB removal within 110 min, respectively. At the KNbO 3 /ZnIn 2 S 4 heterojunction interface, the composite developed its internal electric field and enhanced its photoabsorption under visible light region, thus boosting its charge separation. Subsequently, we evaluate the removal of total organic carbon (TOC) concentration and the influence of different ions on CIP degradation. In addition, we systematically investigated the Z-scheme charge migration process within the heterojunction with a series of experiments. Our results indicated that the hydroxyl and superoxide radicals were the dominant active species during photocatalysis. The composite also could achieve excellent stability and adaptability. We also managed to identify the CIP-degraded intermediates and deduce their possible degradation pathways. Lastly, our toxicity analysis revealed that CIP toxicity could decrease gradually during photocatalysis. In this work, we presented a unique method for preparing inexpensive and highly efficient Z-scheme hollow core–shell structure photocatalysts with excellent antibiotic remediation in water under simulated sunlight illumination.
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Theranostics
·
2023
·
IF 12.4
Wenjie Feng,Wanrui Shi,Yanqi Cui,Jiajun Xu,Shuwei Liu,Hang Gao,Shoujun Zhu,Yi Liu,Hao Zhang
Immunoadjuvants, as an indispensable component of tumor vaccines, can observably enhance the magnitude, breadth, and durability of antitumor immunity. However, current immunoadjuvants suffer from different issues such as weak immunogenicity, inadequate cellular internalization, poor circulation time, and mono-functional bioactivity. Methods: Herein, we construct Fe 3+ -Shikonin metal-phenolic networks (FeShik) nanomedicines as immunogenic cell death (ICD) stimulants and multifunctional immunoadjuvants for tumor vaccination. The multifunctionality of FeShik nanomedicines is investigated by loading ovalbumin (OVA) as the model antigen to construct OVA@FeShik nanovaccines or 4T1 tumor cell fragment (TF) as homologous antigen to construct TF@FeShik nanovaccines. In vitro examinations including GSH responsive, •OH generation, colloid stability, cellular uptake, cytotoxicity mechanism of ferroptosis and necroptosis, ICD effect, the promotion of DC maturation and antigen cross-presentation were studied. In vivo observations including pharmacokinetics and biodistribution, antitumor effect, abscopal effect, immune memory effect, and biosafety were performed. Results: The presence of FeShik nanomedicines can significantly prolong the blood circulation time of antigens, increasing the bioavailability of antigens. Upon phagocytosis by tumor cells, FeShik nanomedicines can disassemble into Fe 2+ and Shikonin in response to tumor microenvironments, leading to ICD of tumor cells via ferroptosis and necroptosis. Consequently, ICD-released autologous tumor cell lysates and pro-inflammatory cytokines not only stimulate DC maturation and antigen cross-presentation, but also promote macrophage repolarization and cytotoxic T lymphocyte infiltration, resulting in the activation of adaptive immune responses toward solid tumors. Conclusion: In a word, our FeShik supramolecular nanomedicines integrate bioactivities of ICD stimulants and immunoadjuvants, such as eradicating tumor cells, activating antitumor immune responses, modulating immunosuppressive tumor microenvironments, and biodegradation after immunotherapy. Encouraged by the diversity of polyphenols and metal ions, our research may provide a valuable paradigm to establish a large library for tumor vaccination.
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CHEMOSPHERE
·
2023
·
IF 8.8
Zilong Zhao,Shuyu Qi,Jianli Zhou,Yatao Ren,Kaiyun Zheng,Jin Zhang,Wenyi Dong,Hongjie Wang
To enhance the polarization distribution of electron cloud density on the catalyst surface, we have introduced a novel bimetallic-substituted dual-reaction center (DRC) catalyst (FeCo-γ-Al 2 O 3 ) comprising iron (Fe) and cobalt (Co) for the decomplexation and mineralization of heavy metal complex Ni-EDTA in this study. Compared to the catalysts doped solely with Fe or Co, the bimetal-doped catalyst offered several advantages, including enhanced electron cloud polarization distribution, additional electron transfer pathway, and improved capacity of free radical generation. Through DFT calculations and EPR tests, we have elucidated the influences of the catalyst's adsorption toward Ni-EDTA and its decomplexation products on the electron transfer between the pollutant and the catalyst. The competition between the pollutants and H 2 O 2 affects the generation of free radicals in both electron-rich Fe and Co centers as well as electron-deficient Al center. Building on these findings, we have proposed a plausible removal mechanism of Ni-EDTA using the heterogeneous Fenton-like catalyst FeCo-γ-Al 2 O 3 . This study sheds light on the potential of FeCo-γ-Al 2 O 3 as a DRC catalyst and emphasizes the significance of pollutant characteristics in determining the catalyst's performance.
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GREEN CHEMISTRY
·
2023
·Vol. 25
·期 23
·9818-9825
·
IF 9.8
Mengmeng Du,Mengyuan Xing,Wenfang Yuan,Liang Zhang,Tao Sun,Tian Sheng,Chunyu Zhou,Bocheng Qiu
The improper disposal of plastic waste raises significant concerns due to its severe threat to ecosystems and public health. Artificial photosynthesis, compared with the conventional strategies (e.g., pyrolysis) operated under harsh conditions, has emerged as a green and sustainable approach to convert plastic waste into commodity chemicals under ambient conditions. In this study, we have developed a partially oxidized CuIn5S8 nanosheet photocatalyst (O-CuIn5S8) to promote the conversion of polyethylene terephthalate (PET) waste into value-added chemicals while producing hydrogen fuel. After oxygen incorporation, the as-obtained O-CuIn5S8 catalyst demonstrates significantly improved activity, with a hydrogen evolution rate of 2.57 ± 0.02 mmol g−1 h−1, which is 7 times higher than that of the pristine CuIn5S8. Furthermore, O-CuIn5S8 allows an effective transformation of pretreated PET into a range of valuable commodity chemicals, including formate, acetate, and glycolate, via a hole-induced oxidation mechanism. This work paves the way for the rational development of photocatalysts to manage plastic pollution and meanwhile reclaim the carbon source within PET plastic waste.
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WATER AIR AND SOIL POLLUTION
·
2023
·Vol. 234
·期 11
·1-12
·
IF 2.9
Wang Xilin,Sun Xiaojing,Dai Ping,Xu Dongyan
This study focuses on preparation of a novel Fe 3 O 4 @C/RM composite by carbothermal reduction of red mud (RM) with scrap tire-derived carbon black and its application for the degradation of orange II in water by activating PMS. X-ray diffraction (XRD) measurements revealed that hematite (Fe 2 O 3 ) was reduced to Fe 3 O 4 in the pyrolysis process above 600 o C. The reduction pathway of Fe 2 O 3 was inferred by detecting the gas emissions during carbothermal reduction. Morphology analysis indicates that Fe 3 O 4 nanoparticles were encapsulated in a carbon matrix, forming a composite with the residual components of RM. The as-prepared Fe 3 O 4 @C/RM composite exhibited high performance toward orange II degradation with 95.9% removal of orange II within 90 min. Electron paramagnetic resonance (EPR) and quenching tests were applied to illustrate the activation processes of peroxymonosulfate. Both radical and non-radical oxygen species are responsible for the efficient degradation of orange II in the Fe 3 O 4 @C/RM/PMS system.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2023
·
IF 9.9
Li Wang,Kun Ge,Jiaqi Duan,Xiaomeng Du,Guoqiang Zhou,Lili Ma,Shutao Gao,Jinchao Zhang
Chemodynamic therapy (CDT) based on hydroxyl radicals (•OH) to suppress tumor cells is a promising strategy due to its efficacy and safety. Nevertheless, in tumor cells, CDT still faces challenges such as insufficient •OH and weak killing effect of tumor cells under physiological conditions due to inadequate amounts of endogenous hydrogen peroxide (H 2 O 2 ) and heightened glutathione expression. These challenges limit the therapeutic potential of CDT. To improve the effects of CDT, combination treatment strategies have been developed. Here, we report a rationally designed nanocomposite (CaO 2 @Cu-LA) with self-supplying H 2 O 2 ability from calcium peroxide, and nitric oxide (NO) generation ability from l -arginine. NO molecules not only exhibit a strong killing effect, but also have the potential to transfer into the more cytotoxic substance peroxynitrite anion by reacting with reactive oxygen species. The results showed that CaO 2 @Cu-LA could significantly suppress tumor growth by increasing •OH radicals and NO molecules. Taken together, the strategy developed here provides a good application foreground to yield a remarkable synergistic antitumor effect of CDT and NO gas therapy.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
·
2023
·
IF 5.2
Changwang Yan,Jing Zou,Li He,Wanhui Jin,Qian Yu,Jing Yu,Zhong Zhao,Guangming Cai,Deshan Cheng,Xin Wang
Inorganic photocatalysts with excellent photocatalytic reactivity have significant potential for wastewater treatment . In this study, using sodium copper chlorophyllin (SCC) as a copper source, Cu atoms were incorporated into the center cavities of g-C 3 N 4 nanosheets by hydrothermal-calcination combined processes. Cu atoms doping led to a narrower optic band gap and the dramatic improvement in photocurrent response as well as corresponding declines in the intensity of electrochemical impedance spectroscopy (EIS) and photoluminescence (PL) spectra. Consequently, the photocatalytic property the Cu/g-C 3 N 4 was enhanced dramatically as evidenced by a 53.4% increase in the photocatalytic degradation rate of tetracycline . Superoxide ions and hydroxyl radicals were found to be the main reactive oxygen species (ROS) causing the degradation. The increased photocatalytic capability of Cu/g-C 3 N 4 might be attributed to the increased chance of intersystem crossing in photosensitizing process of Cu/g-C 3 N 4 as well as the lowered adsorption energy required for the adsorption of O 2 to the catalyst. Minor decline in the photocatalytic efficiency of Cu/g-C 3 N 4 was observed while the crystal structure of the Cu/g-C 3 N 4 remained stable after three cycles of tetracycline degradation. These results indicated the good stability of Cu/g-C 3 N 4 and the possibility of recycling the catalyst during the photocatalytic applications.
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JOURNAL OF HAZARDOUS MATERIALS
·
2023
·
IF 13.6
Afang Wang,Yang Shi,Yang Liu,Wei Li,Heng Zhang,Xiaoqiang Dai,Li Luo,Gang Yao,Bo Lai
Traditional Fenton and Fenton-like processes are affected by the sluggish kinetics of Fe(II) regeneration and Fe(III) accumulation. This research revealed that the degradation efficiency of pollutants was significantly increased by adding Fe(III) to the Vis/PS system. A mechanism is proposed in which photosensitivity pollutants can boost Fe(III) to produce Fe(II) under visible light irradiation. Intriguingly, Fe(III) rapidly combines with LVF in aqueous environments to form Fe(III)-LVF complexes. This research confirms that Fe(III)-pollutant complexes are generated. The proportion of complexes are calculated using mathematical models. Furthermore, the production of Fe(IV) is verified in the Vis/PS/Fe(III) system, which also plays a vital role in boosting LVF degradation. Overall, this study provides comprehensive insights into the degradation mechanism of micropollutants, involving hydroxyl radical ( OH ∙ ), Fe(IV), and Fe(III)-LVF complexes, providing an efficient and green strategy for contaminant removal during wastewater treatment .
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