CHEMOSPHERE
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2022
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IF 8.943
Yanzhuo Zhang,Mengqi Xu,Rui He,Jing Zhao,Wei Kang,Jinghua Lv
Because of the increasingly widespread contamination of antibiotics, the preparation of biochar by heteroatom doping to further improve the catalytic degradation efficiency of antibiotics has become a major focus of research. In this study, N-doped (NBC), S-doped (SBC), and NS-doped (NSBC) moso bamboo biochar were obtained at preparation temperatures of 300–700 °C. The concentration of environmentally persistent free radicals (EPFRs) in all biochars peaked when the preparation temperature was 500 °C: 2.45 × 10 19 spins·g −1 (BC), 9.23 × 10 19 spins·g −1 (NBC), 6.10 × 10 19 spins·g −1 (SBC), and 4.36 × 10 19 spins·g −1 (NSBC). After heteroatom doping, EPFR species were more abundant, and the distribution of three types of EPFRs (oxygen-centered (g > 2.0040), carbon-centered (g < 2.0030), and carbon-centered radicals with oxygen atom free radicals (2.0030 < g < 2.0040) varied with the preparation temperature. In the process of antibiotic degradation, both NBC and SBC increased the degradation rate of antibiotics, whereas NSBC reduced the degradation rate. Compared with the degradation rate of antibiotics of biochar (79.86%), the degradation rate of antibiotics by NBC, SBC, and NSBC via PMS activation was 92.23%, 88.86%, and 70.97% on average in 30 min, respectively. The greatest contributors to the catalytic degradation were SO 4 •- , followed by 1 O 2 , •OH, and O 2 •- . EPFRs and 1 O 2 might be the main contributors to the free radical and non-free radical pathways. The enhancement of EPFRs following the N doping or S doping of biochar is the key factor underlying PMS activation. Therefore, changes in the structure of biochar can better activate PMS to produce reactive oxygen species-degrading antibiotics. The mineralization rate of antibiotics by BC, NBC, SBC, and NSBC was 42.12%, 47.06%, 44.99%, and 39.01%, respectively. This means that a small portion of the antibiotics was completely decomposed into CO 2 , H 2 O, and inorganic substances after degradation. Cyclic experiments showed that heteroatom-doped biochar had higher reusability, and the degradation rate decreased less than 15%.
研究领域:
环境科学
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化学工程
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材料科学
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DOI
PubMed
高影响因子
CHEMOSPHERE
·
2022
·
IF 8.943
Jiaxin Xu,Xiuquan Lan,Jianhua Cheng,Xinhui Zhou
Water pollution , deriving from the contamination of pathogenic bacteria, has posed a threat to human's survival and development. Photocatalytic disinfection is being widely studied in decentralized drink water safety, as traditional disinfection technologies are limited by harmful disinfection by-product and excessive energy consumption. Herein, a novel composite membrane (PN/Ag) with plasmonic heterojunction was synthesized for the efficient photocatalytic disinfection through the combination of polyacrylonitrile (PAN), N -doped carbon dots (NCDs)/g-C 3 N 4 and Ag 2 C 2 O 4 by electrospinning technique and successive ionic layer adsorption and reaction (SILAR) process. The surface plasmon resonance (SPR) effect of Ag nanoparticles and Schottky barrier formation between metal and semiconductor contributed to the efficient separation of electron-hole pairs and the generation of reactive species, resulting in outstanding photocatalytic disinfection of PN/Ag composite membranes (7.48 and 7.70 log inactivation of E. coli and S. aureus respectively in 80 min) and good reusability under visible light illumination. Moreover, the potential Z-scheme photocatalytic mechanisms were proposed for PN/Ag system according to the band structure and reactive species analysis. The as-proposed PN/Ag composite membranes may shed light on the design and application of materials in water purification .
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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光催化
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水处理
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DOI
PubMed
高影响因子
Journal of Water Process Engineering
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2022
·
IF 7.34
Yanzhuo Zhang,Shengxu Liang,Rui He,Jing Zhao,Jinghua Lv,Wei Kang,Jian Zhang
Antibiotics in the water environment pose harm to animals, plants, and humans. In this study, biochar doped with sulfur (S), nitrogen (N), and NS was used to adsorb and activate peroxymonosulfate (PMS) to degrade the antibiotics chlortetracycline, ofloxacin, and sulfadiazine in an aqueous solution. The adsorption capacity of the biochar doped with single atoms increased significantly, and the maximum saturated adsorption capacities of undoped, N-doped, S-doped, and NS-doped biochar were 40.7, 85.5, 63.3, and 40.7 mg/g, respectively. The increase in specific surface area and the number of functional groups was the main cause for the increase in the adsorption capacity of heteroatom-doped biochar. The antibiotic degradation process involved the use of biochar to activate PMS and produce reactive oxygen species (ROS) for complete removal. The concentration of environmentally persistent free radicals (EPFRs) increased in response to heteroatom-doped biochar, and the type of EPFRs changed, which enhanced the ability of biochar to degrade antibiotics. At the 500 °C preparation temperature, the degradation rates of antibiotics by the undoped, N-doped, S-doped, and NS-doped biochar were 73.83%, 84.32%, 79.60%, and 74.10%, respectively, whereas the degradation rates at 900 °C were 82.38%, 93.78%, 91.11%, and 81.55%, respectively. The sulfate radical was produced during the activation process and made the largest relative ROS contribution to the increased adsorption capacity, followed by singlet oxygen, hydroxyl radical , and superoxide radical. Recycling experiments confirmed that the heteroatom-doped biochar was highly reusable and that the removal rates of N-doped biochar and S-doped biochar were high (81.94% and 78.06%, respectively).
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
JOURNAL OF MOLECULAR STRUCTURE
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2022
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IF 3.841
Zhixia Wang,Hang Song
s A series of quaternary N-alkyl tropinium cationic surfactants (TILS) were synthesized and characterized. The effect of temperature, hydrophobic chain length and anions on their properties were studied. By changing the structure of anion, the krafft point was significantly reduced (from 313.15 K to below 273.15 K) and wide temperature window was obtained. The critical micelle concentration ( CMC ) value of TILS based on electrical conductivity method was found to be decreased about 4-5 times by increasing hydrophobicity of anions. At lower temperature and longer hydrophobic chain, TILS had lower CMC value and better surface activity. The thermodynamic properties of micellization Gibbs free energy Δ G mic , enthalpy Δ H mic and entropy T Δ S mic of micelles were obtained by Mass action model. The result indicates that the micellization process of the TILS was spontaneous and more stable with the increase of anionic hydrophobicity. In addition, with the increase of hydrophobic side chain length, the driving force of surfactant micellization may be enthalpy driven at higher temperature and entropy driven at lower temperature. The micro-environment of TILS solution with different concentrations was studied by UV spectrophotometry with curcumin as a probe and the change of micro-environment was used to determine the CMC of TILS. The CMC values were similar obtained by two methods.
研究领域:
化学
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材料科学
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界面科学
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产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
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2022
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IF 7.968
Jingzhen Wang,Linlin Zang,Libin Wang,Yutong Tian,Zhiyu Yang,Yumei Yue,Liguo Sun
Photocatalytic degradation is an effective technique for removing antibiotics from contaminated water . The kernel of photocatalytic degradation lies in the design and preparation of high-performance and recyclable catalysts. Herein, magnetic porous cobalt ferrite/reduced graphene oxide (CF/rGO) balls were prepared by calcination of spherical composites obtained via modified microfluidic method for effective photocatalytic degradation of oxytetracycline (OTC). The strong interfacial interaction between rGO and cobalt ferrite nanoparticles in porous balls enhanced electron transfer , charge separation and light absorption . Porous spherical structure was favorable for light harvesting. The catalyst could rapidly and efficiently absorb OTC. These characteristics were beneficial to the enhancement of photocatalytic efficiency. The optimized sample (CF/rGO-0.2) exhibited an excellent apparent rate constant (0.0410 min −1 ) for OTC degradation under visible light irradiation, which was 3.73 times that of CF/rGO-0 (0.0110 min −1 ). CF/rGO-0.2 had excellent stability in cycle experiments and could be quickly recovered by magnets. The trapping experiments showed that hole (h + ) and superoxide radicals (·O 2 - ) acted an extremely important role in degradation of OTC, thus suggesting a possible photocatalytic reaction mechanism. This work provides a potential photocatalyst for antibiotic removal from water.
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
Biomaterials Science
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2022
·Vol. 10
·期 13
·3637-3646
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IF 7.59
Qingyan Zhang,Ying Huang,Ruoxi Yang,Junmei Mu,Zhanwei Zhou,Minjie Sun
Despite the great progress in the control of primary tumor growth, metastasis remains the major challenge of breast cancer therapy in clinics, which is highly related to the upregulation of reactive oxygen species (ROS) and overexpression of its relevant pro-survival miR-155 gene. Therefore, we fabricated a poly-antioxidant (FTP) to deliver anti-miR-155 for synergistic treatment of metastatic breast cancer by ROS scavenging and miR-155 inhibition. FTP was synthesized by the polymerization of fluorated-polyethyleneimine (FPEI) and antioxidants (TEMPOL), using a glutathione (GSH) responsive linker for controlled drug release. Notably, the poly-drug strategy could not only promote the tumoral accumulation of small molecular antioxidants but also enhance the transfection efficiency of anti-miR-155 owing to the hydrophobic property of TEMPOL. After synergistic treatment, the NF-κB pathway was significantly blocked, thereby generating strong anti-metastatic ability both in vitro and in vivo. The poly-antioxidant could be a new type of nanoplatform for highly efficient and safe miRNA delivery, which also provides a promising strategy for the synergistic treatment of metastatic breast cancer.
研究领域:
肿瘤学
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药学
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分子生物学
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DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
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IF 9.965
Chunchun Wang,Shijie Li,Mingjie Cai,Ruyu Yan,Kexin Dong,Junlei Zhang,Yanping Liu
Constructing novel Z-scheme heterojunctions is an effective strategy for obtaining high-performance photocatalysts. Herein, tetra (4-carboxyphenyl) porphyrin (TCPP) and graphene quantum dots (GQDs) were loaded on the surface of Bi 2 MoO 6 (BMO) to fabricate novel Z-scheme heterojunctions of TCPP/G/BMO. Especially, TCPP/G/BMO-2 showed an exceptional visible-light photoactivity for tetracycline (TC) degradation (81.0%, 40 min) and Cr(VI) reduction (90.7%, 60 min), respectively by 2.38 folds and 2.96 folds enhancement compared to sole Bi 2 MoO 6 . The substantial enhancement of activity is attributed to the synergy effect of the Z-scheme charge transfer mechanism and the improved light absorption. The degradation pathways of TC were inferred by determining the generated intermediates using high performance liquid chromatography-mass spectrometry (HPLC-MS), and the toxicity of the transformation products was assessed by Toxicity Estimation Software Tool (T.E.S.T). Overall, on the basis of trapping experiments and electron spin resonance spectra (ESR) analysis, the photocatalytic mechanisms of Cr(VI) reduction and TC degradation by the TCPP/G/BMO Z-scheme heterojunction was proposed. This work indicates TCPP/G/BMO could be a promising photocatalyst for wastewater treatment.
研究领域:
环境科学
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材料科学
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光催化技术
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产品关联
DOI
PubMed
高影响因子
WATER RESEARCH
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2022
·
IF 13.4
Dehua Xia,Qi Chen,Yimu Jiao,Qiyu Lian,Mingzhe Sun,Chun He,Jin Shang,Tianqi Wang
Solar disinfection (SODIS) is regarded as an affordable and effective point-of-use (POU) water disinfection treatment urgently needed in rural developing world. This work developed an enhanced SODIS scheme that utilized a novel flower pollen-based catalyst (Te-TRP). The bench-scale experiments demonstrated 100% photothermocatalytic inactivation of approximately 7-log E. coli K-12, Spingopyxis sp. BM1-1, or S. aureus bacterium by Te-TRP within 40–60 min. Moving toward practical device design, we constructed a flow-through reactor and demonstrated the outstanding water disinfection performance of Te-TRP. The in-depth mechanistic study revealed the synergetic effect between photocatalysis and photothermal conversion and identified the bacterial inactivation pathway. 1 O 2 and ·O 2 ¯ were verified to be the dominant reactive oxygen species involved in the bacterial inactivation. The damage to bacterial cells caused by photothermocatalytic reactions was systematically investigated, demonstrating the cell membrane destruction, the loss of enzyme activity, the increased cell membrane permeability, and the complete inactivation of bacteria without the viable but nonculturable state cells. This work not only affords a facile approach to preparing biomaterial-based catalysts capable of efficient photothermocatalytic bacterial inactivation, but also proposes a prototype of POU water treatment, opening up an avenue for sustainable environmental remediation.
研究领域:
环境科学
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微生物学
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材料科学
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产品关联
DOI
PubMed
高影响因子
BIOCHEMICAL ENGINEERING JOURNAL
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2021
·
IF 3.978
Xiao Li,Xiaomei Wu,Tao Yuan,Junrun Zhu,Yaling Yang
Nitrogen- and iodine-doped carbon dots (I-CDs) were synthesized as peroxidase mimics for the antifungal disinfection of Candida albicans ( C. albicans ). The prepared I-CDs samples exhibited peroxidase-like activity in the presence of exogenous H 2 O 2 . The peroxidase-like activities and antifungal effects of the I-CDs samples were enhanced by increasing their iodine content from 0.1599 g to 0.4796 g. The antifungal activity of the I-CDs (i.e., 2.72 mg/mL) against C. albicans reached > 90% in the presence of exogenous H 2 O 2 (0.5 mM) under visible light irradiation for 120 min. The in vitro experimental results showed the excellent photocatalytic antifungal activity of the designed system against C. albicans . It was theorized that this system promotes the formation of reactive oxygen species, including hydroxyl radicals (·OH), which can successfully inhibit the growth of C. albicans . The antifungal effect of the synergistic I-CDs/H 2 O 2 system on C. albicans could be attributed to the combined effects of its peroxidase-like and photocatalytic activities; the increased activities appeared to be closely related to the iodine content. The results of the present study are expected to broaden the biological applications of the I-CDs and elucidate the relationship between the iodine content and peroxidase-like enzymatic and antifungal activities of the I-CDs.
研究领域:
纳米技术
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生物催化
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抗菌化学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ALLOYS AND COMPOUNDS
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2021
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IF 5.316
Lifen Wang,Yonggang Liu,Yinjun Lin,Yonghao Yu,Xueying Zhang,Ruiqin Zhang,Yunpu Zhai
In this study, an effective Ni-doped Cu 2 (OH) 3 F was synthesized by a simple one-step hydrothermal method to activate H 2 O 2 for degrading organic pollutants in water. The prepared (Cu 2−x Ni x ) 2 (OH) 3 F showed significant degradation performance for the degradation of RhB and TC. The characterization methods of XRD, XPS , TEM , SEM, FT-IR proved that Ni successfully replaced part of the Cu in Cu 2 (OH) 3 F site and provided more active sites for decomposition of H 2 O 2 through the synergistic effect of the bimetal . Besides, the photochemical properties of the prepared catalysts were analyzed by UV–vis, electrochemical impedance spectroscopy and transient photocurrent, which confirmed that the introduction of Ni narrowed the band gap of (Cu 2−x Ni x ) 2 (OH) 3 F and accelerated the separation of photogenerated electrons and hole pairs. Free radical capture experiments showed that •OH, h + , and •O 2 - all contributed to the reaction, and •OH was the main active substance. This research provides a photo-Fenton-like catalyst with simple synthesis, high performance and stable properties for future sewage treatment.
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
Nanoscale
·
2021
·Vol. 13
·期 35
·14713-14722
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IF 7.79
Xiaoshan Fan,Lingjie Ke,Hongwei Cheng,Hu Chen,Zhiguo Li,Enyi Ye,Xian-Jun Loh,Yun-Long Wu,Gang Liu,Zibiao Li
Efficient drug delivery, multifunctional combined therapy and real-time diagnosis are the main hallmarks in the exploitation of precision nanomedicine. Herein, an anthracene-functionalized micelle containing a magnetic resonance imaging (MRI) contrast agent, upconversion nanoparticles (UCNPs) and the photosensitizer IR780 is designed to achieve sustained drug release and enhanced photothermal and photodynamic therapy. The polymer-coated hybrid micelle was achieved by crosslinking anthracene-dimer with UV light (λ > 300 nm), which is converted from near-infrared (NIR) irradiation upon UCNPs. Besides, the water-insoluble photosensitizer IR780 is introduced into the system to achieve efficient drug delivery and photothermal and photodynamic synergistic therapy. As a consequence of NIR-induced anthracene-dimer formation, the cross-linked nanocomposite shows sustained drug release, and the enhanced retention effect of IR780 could increase the photothermal conversion efficiency. Importantly, the incorporation of 2,2,6,6-tetramethyl-piperidineoxyl (TEMPO) as a nitroxide MRI contrast agent presents the potential for real-time diagnosis via nanotheranostics, and the fluorescence imaging of IR780 is applied to monitor drug distribution and metabolism. This strategy of sustained drug delivery by anthracene-dimer formation through the better penetration depth of NIR-II fluorescence provides an executable platform to achieve enhanced phototherapy in biomedical applications.
研究领域:
纳米医学
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生物医学工程
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诊疗学
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药物递送系统
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光疗
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产品关联
DOI
PubMed
高影响因子
COMPOSITES SCIENCE AND TECHNOLOGY
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2022
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IF 9.879
Quan Wang,Xueqing Liu,Zhe Qiang,Zhendong Hu,Xin Cui,Huaixiao Wei,Jinjin Hu,Yuming Xia,Shuohan Huang,Jianming Zhang,Kun (Kelvin) Fu,Yuwei Chen
Photocuring-based 3D printing becomes an emerging technology in various applications owing to their advantages of high design flexibility and low cost. Developing 3D printing resins with high dielectric constant is important for enabling on-demand manufacturing of energy storage materials . Herein, we report a scalable and simple approach for preparing ultraviolet (UV) curable resin composite with high dielectric constant, through the introduction of cellulose nanocrystals (CNCs) as bio-fillers into methacrylate malate photocurable resins (MMPR). MMPR resin was synthesized by reacting methacrylic acid (MAA) with malate resin (MR), while CNCs were also grafted to MAA for allowing the uniform dispersion of fillers in the polymer matrix . Subsequently, high dielectric constant composite resin CNCs-MAA/MMPR was prepared by simply mixing CNCs-MAA with MMPR and the dielectric constant of materials can be manipulated by varying the content of CNCs-MAA particles. Specifically, with the addition of 1 wt% CNCs-MAA, the dielectric constant increases from 4.0 (MMPR) to 10.9 at 1 MHz, which can be attributed to the interfacial effect between CNCs-MAA and MMPR matrix and the abundant presence of polar groups (-OH) from CNCs surface. The prepared resin composite can be directly used for conventional 3D printing technologies. Specifically, practical use of CNCs-MAA/MMPR composites for energy storage was demonstrated, which the capacitance of MAA/MMPR resin with 1 wt% CNCs increases more than 132% compared to pristine MMPR. This work provides an industrially feasible method for preparing photocurable resin composites with high dielectric constants for 3D printing.
研究领域:
材料科学
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能源技术
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化学工程
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）