Journal of Environmental Sciences
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2020
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IF 4.302
Ting Li,Jianru Liang,Lixiang Zhou
Here we reported an effective method to solve the rate-limiting steps, such as the reduction of Fe 3+ to Fe 2+ and an invalid decomposition of H 2 O 2 in a conventional Fenton-like reaction. A magnetic heterogeneous photocatalyst, Fe 3 O 4 -schwertmannite (Fe 3 O 4 -sch) was successfully developed by adding Fe 3 O 4 in the formation process of schwertmannite . Fe 3 O 4 -sch shows excellent electrons transfer ability and high utilization efficiency of H 2 O 2 (98.5%). The catalytic activity of Fe 3 O 4 -sch was studied through the degradation of phenol in the heterogeneous photo-Fenton process. Phenol degradation at a wide pH (3 - 9) was up to 98% within 6 min under visible light illumination with the Fe 3 O 4 -sch as heterogeneous Fenton catalyst, which was higher than that using pure schwertmannite or Fe 3 O 4 . The excellent photocatalytic performance of Fe 3 O 4 -sch is ascribed to the effective recycling between Fe 3+ and Fe 2+ by the photo-generated electron, and also profit from the formation of the “Z-Scheme” system. According to the relevant data, photocatalytic mechanism of Fe 3 O 4 -sch for degrading phenol was proposed. This study not only provides an efficient way of enhancing heterogeneous Fenton reaction , but also gives potential application for iron oxyhydroxysulfate mineral.
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APPLIED SURFACE SCIENCE
·
2020
·
IF 6.182
Binrong Li,Yanhua Cui,Yonghai Feng,Chundu Wu,Yongsheng Yan,Minjia Meng
The directional design of interfacial defects is a promising way to promote charge separation but simultaneously a great challenge due to their random formation in heterojunction. Herein, an alternative Bi 12 O 17 Cl 2 /Bi 2 WO 6 heterojunction with interfacial defects formed spontaneously is prepared by controlling the growth of Bi 2 WO 6 on the edges of Bi 12 O 17 Cl 2 nanobelts via ion exchange process. These interfacial defects can efficiently increase the carrier density and serve as charge separation centers to extend the lifetime of carriers and activate O 2 to O 2 − and further to OH. The zigzag interfaces and irregular edges facilitate the interaction between active sites and reactants. The heterojunction morphology and the interfacial defect concentration can be controlled by tuning the solvothermal time. Consequently, the optimal Bi 12 O 17 Cl 2 /Bi 2 WO 6 heterojunction exhibits significantly enhanced visible light photocatalytic performance toward the degradation of phenols, antibiotics and dyes as compared to that of mono-Bi Bi 12 O 17 Cl 2 and Bi 2 WO 6 photocatalyst.
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CHEMISTRY-A EUROPEAN JOURNAL
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2020
·Vol. 26
·期 66
·15159-15169
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IF 4.857
Ting Chen,Rongtao Huang,Jiawei Liang,Bo Zhou,Xiao-Lu Guo,Xing-Can Shen,Bang-Ping Jiang
Graphical Anti-cancer nanozymes : Nanozymes comprising natural polyphenol–vanadium oxide nanosheets (TA@VO x NSs) are developed. In this nanosystem, the peroxidase-like activity of VO x provides the possibility to achieve tumor-specific chemodynamic therapy (CDT). As a valid supplement to CDT, NIR absorption enables that TA@VO x NSs can realize NIR light-mediated photothermal therapy (PTT). Such combination of chemodynamic and photothermal activities means that TA@VO x NSs can be applied for effective synergistic CDT/PTT of cancers. The selection of suitable nanozymes with easy synthesis, tumor specificity, multifunction, and high therapeutics is meaningful for tumor therapy. Herein, a facile one-step assembly approach was employed to successfully prepare a novel kind of natural polyphenol tannic acid (TA) hybrid with mixed valence vanadium oxide nanosheets (TA@VO x NSs). In this system, VO x is assembled with TA through metal–phenolic coordination interaction to both introduce superior peroxidase-like activity and high near infrared (NIR) absorption owing to partial reduction of vanadium from V 5+ to V 4+ . The presence of mixed valence vanadium oxide in TA@VO x NSs is proved to be the key for the catalytic reaction of hydrogen peroxide (H 2 O 2 ) to . OH, and the corresponding catalytic mechanism of H 2 O 2 by TA@VO x NSs is proposed. Benefitting from such peroxidase-like activity of TA@VO x NSs, the overproduced H 2 O 2 of the tumor microenvironment allows the realization of tumor-specific chemodynamic therapy (CDT). As a valid supplement to CDT, the NIR absorption enables TA@VO x NSs to have NIR light-mediated conversion ability for photothermal therapy (PTT) of cancers. Furthermore, in vitro and in vivo experiments confirmed that TA@VO x NSs can effectively inhibit the growth of tumors by synergistic CDT/PTT. These results offer a promising way to develop novel vanadium oxide-based nanozymes for enhanced synergistic tumor-specific treatment.
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Journal of Materials Chemistry A
·
2020
·Vol. 8
·期 34
·17657-17669
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IF 11.301
Xiaoli Li,Ting Wang,Xueqin Tao,Ganhua Qiu,Can Li,Benxia Li
Metal-modified semiconductors are being deemed as one of the most promising photocatalysts for various applications. Although great efforts have been devoted to developing a variety of metal-modified semiconductor photocatalysts, the exact functions of their interfaces in governing photocatalytic processes still remain elusive. Herein, the interfacial synergy of metal sites and defective semiconductor with oxygen vacancies (VOs) was investigated toward the photocatalytic selective oxidation of toluene, by taking the Pd/BiOBr photocatalyst as an example. The presence of Pd induces the generation of more VOs on the BiOBr surface due to the electronic interaction at the Pd–BiOBr interface. The coexistence of the Pd and VO sites on BiOBr enables the favorable adsorption of O2 and toluene molecules. The Pd–BiOBr interface governs the charge separation and prompts the activation of O2 and toluene, leading to 1.5 times the activity of BiOBr–VO for the photocatalytic selective oxidation of toluene to benzaldehyde with a high selectivity (>99%). Moreover, the typical influencing factors, such as the illumination intensity and toluene concentration, were optimized to improve the photocatalytic efficiency. The active species and intermediates in the photocatalytic reaction were identified by a series of controlled experiments, as well as in situ ESR measurements. Therefore, both experimental and theoretical results provide the direct evidence to understand the key roles of the interfacial Pd and VO sites in enhancing photocatalysis toward the selective oxidation of toluene.
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ACS Applied Materials & Interfaces
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2020
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IF 8.758
Wenjing Ma,Yuansheng Li,Mengjie Zhang,Shuting Gao,Jiaxin Cui,Chaobo Huang,Guodong Fu
Wastewater pollution has always been one of the most severe worldwide environmental problems. In addition, in light of the frequent oil spills that have occurred in recent years, the treatment of oily wastewater is particularly important. In this work, a novel zeolitic imidazolate framework-8@thiolated graphene (ZIF-8@GSH) composites-based polyimide (PI) nanofibrous membrane was developed via a facile electrospinning and in situ hydrothermal synthesis approaches for effective purification of oily wastewater. The membrane showed superhydrophobicity/superoleophilicity and high separation efficiency (>99.9%) for a wide range of oil/water mixtures and water-in-oil emulsions. Besides, the membrane demonstrated excellent photocatalytic dye degradation, antibacterial, self-cleaning, and mechanochemical durable abilities, showing high potential in oily wastewater treatment and water remediation.
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CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Yingjie Gao,Qi Zhao,Yunhe Li,Yuanqing Li,Jianfeng Gou,Xiuwen Cheng
Advanced Oxidation Processes (AOPs) play a critical role in the elimination of antibiotics, in which it is essential to explore an environmentally friendly, cheap and effective catalyst. In this study, Ag 2 O-g/eggshell catalyst had been synthesized in a simple strategy, combining with peroxymonosulfate (PMS) to simultaneous remove sulfamethoxazole (SMX). Then, physicochemical properties of catalyst were investigated by series of techniques. Results indicated the Ag species was featured with a spherical-like structure and homogeneously distributed on the surface of eggshell. In addition, Ag 2 O-Ag/eggshell exhibited high degradation efficiency of SMX by activation of PMS (94.6%) under the optimized conditions of 0.1 g•L −1 Ag 2 O-Ag/eggshell, 0.16 mM PMS, 10 mg•L −1 SMX and initial pH 6.42. Moreover, several parameters such as the dosage of catalyst, PMS and the effect of pH, co-existing anions, humic acid (HA) and water matrices on SMX degradation were systematically studied. Besides, scavenging experiments were conducted to distinguish the active radicals. Furthermore, to improve the reusability of powder Ag 2 O-Ag/eggshell, corresponding Microporous Filter Membrane had been synthesized. Subsequently, possible reaction mechanism was proposed. Consequently, these results revealed that the waste eggshell was considered as a promising supporting material for the metal catalyst for the catalytic degradation of antibiotics in water.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2020
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IF 7.489
Zhuoqian Li,Kai Li,Shuanglong Ma,Bingjun Dang,Yi Li,Haichao Fu,Jinge Du,Qingxiang Meng
A convenient and efficient method to fabricate isolated Fe single-atom catalysts deposited on Myriophyllum aquaticum -based biochar (ISA-Fe/MC) is reported for peroxymonosulfate-based organics degradation. Firstly, the Fe nanoparticles anchored on the hierarchical porous biochar (nano-Fe/MC) can be obtained by utilizing K 2 FeO 4 as a synchronous activation and graphitization agent. Subsequently, ISA-Fe/MC was achieved by HCl etching of nano-Fe/MC to remove the excess Fe nanoparticles. Compared with nano-Fe/MC, ISA-Fe/MC demonstrated outperformed catalytic capacity towards PMS activation for phenol degradation. The combination of super high surface area, hierarchical porous structure, graphitization structure and atomically dispersed Fe species should be responsible for prominent catalytic oxidation ability and outstanding resistance to common anions and humic acid. Based on the chemical scavengers, EPR experiments and electrochemistry tests, the SO 4 •– dominated radical degradation pathway for nano-Fe/MC and electron transfer reigned non-radical degradation pathway for ISA-Fe/MC was revealed. In contrast to nano-Fe/MC, density functional theory calculations demonstrated the enhanced density of states around Fermi level in ISA-Fe/MC meaning the increased catalytic performance and more electron transfer between single-atom Fe to adjacent graphitic C and N which could serve as electron transfer channel for PMS activation.
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ADVANCED FUNCTIONAL MATERIALS
·
2020
·Vol. 30
·期 42
·2004108
·
IF 16.836
Jingyu Sun,Jinghong Wen,Guizhu Wu,Ze Zhang,Xue Chen,Guichang Wang,Mingyang Liu
Due to the unique surface atomic arrangement, exposed facets and defects of nanomaterials play critical roles in their physicochemical properties. Herein, BiOI nanosheets with the same type of defects on different exposed facets such as {001} (BI-001) and {110} (BI-110) are engineered to harmonize the electronic structures for antibacterial applications. Results demonstrate that BI-110 exhibits higher activity in killing Escherichia coli under 808 nm light irradiation than that of BI-001 due to its superior electronic structures. The density functional theory calculations show that BI-110 with its excellent geometric effect exhibits stronger adsorption to O 2, leading to the formation of highly concentrated single oxygen species, which causes excellent antibacterial performance. This work with the combination of facets engineering and vacancy engineering will inspire future studies on antibacterial photodynamic therapy.
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APPLIED SURFACE SCIENCE
·
2020
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IF 6.182
Yifei Wang,Jing Niu,Xin Gao,Yanlin Zhang
In this study, Y-doped Ag 3 PO 4 , carbon quantum dots (CQDs), BiVO 4 were used to synthesize Z-scheme Y-Ag 3 PO 4 /CQDs/BiVO 4 . X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS), Fourier transform infrared (FT-IR) and UV–vis diffuse reflectance spectra (DRS) were employed to probe into the crystalline structure, morphology, optical property and chemical composition of Y-Ag 3 PO 4 /CQDs/BiVO 4 . The kinetic constant of the prepared Y-Ag 3 PO 4 /CQDs/BiVO 4 was approximately 2.8 times that of pristine Ag 3 PO 4 for atenolol degradation. The degradation of atenolol mainly depended on the excited holes, •OH and •O 2 − . The photocatalysis mechanism of Y-Ag 3 PO 4 /CQDs/BiVO 4 conforms to the Z-scheme mechanism deduced by reactive species trapping experiment, electron spin resonance (ESR) and photoelectrochemical measurement (photocurrent response and EIS). The introduction of yttrium, CQDs and BiVO 4 significantly promoted the photogenerated carriers separation of Ag 3 PO 4 and inhibited the photogenerated electron-holes pairs recombination of Ag 3 PO 4 during the degradation of atenolol. Oxygen defects caused by the doping of Y 3+ into Ag 3 PO 4 were the centers of capture of photogenerated electrons to generate •O 2 − , inhibiting the recombination of photogenerated electron-holes pairs and the photocorrosion of Ag 3 PO 4 .
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CELLULOSE
·
2020
·Vol. 27
·期 14
·8405-8427
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IF 4.21
Zhao Zhong,Zhang Mingwen,Hurren Chris,Zhou Liming,Wu Jihong,Sun Lu
Abstract The light fastness of fabrics dyed with natural dyes is not satisfactory, which limits their applications in the textile industry. So far, the detailed photofading mechanism of natural dyes remains unclear. To improve the light fastness of cotton fabrics dyed with two natural dyes (sodium copper chlorophyllin and gardenia yellow), two additives ethylenediaminetetraacetic acid disodium salt (EDTA-2Na) and sodium citrate were used to treat the dyed cotton fabrics via the dipping-padding method. The performance results showed that both the two additives had good effects on inhibiting the photofading of the dyed fabrics. The photofading mechanism of the two natural dyes was also investigated. The results from 1,1-Diphenyl-2-picrylhydrazyl free radical (DPPH) scavenging assay and cyclic voltammetry tests demonstrated very limited antioxidant properties of the two dyes. Singlet oxygen and hydroxyl radical were detected in the photosensitizing process of the two dyes by electron paramagnetic resonance method. The photo-induced chemiluminescence (PICL) tests confirmed that the color changes of the dyed cotton fabrics were reduced because the reactivities of the two dyes to react with reactive oxygen species were dramatically reduced in the presence of EDTA-2Na and sodium citrate. End products generated in the photofading of the two dyes were detected by high-performance liquid chromatography-mass spectrometry (HPLC–MS). Based on the comprehensive analysis of above results, possible degradation pathways of the two dyes were proposed. The mechanism study in this research may help shed light on proposing universal solutions to the poor light fastness of most natural dyes on cotton. Graphic abstract
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CHINESE JOURNAL OF CATALYSIS
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2020
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IF 6.146
Jiaqi Wang,Qingrong Qian,Qinghua Chen,Xin-Ping Liu,Yongjin Luo,Hun Xue,Zhaohui Li
TiO 2 -seashell composites prepared via a sol-gel method were used to generate carbonate radicals (•CO 3 − ) under solar light irradiation. •CO 3 − , a selective radical, was employed to degrade the target tetracycline hydrochloride contaminant. A series of characterizations was carried out to study the structure and composition of the synthesized TiO 2 -seashell composite. This material exhibits excellent solar light-driven photochemical activity in the decomposition of tetracycline hydrochloride. The possible pathway and mechanism for the photodegradation process were proposed on the basis of high-resolution electrospray ionization time-of-flight mass spectrometry experiments. Finally, we investigated the reusability of the TiO 2 -seashell composite. This study is expected to provide a new facile pathway for the application of •CO 3 − radicals to degrade special organic pollutants in water.
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Science Bulletin
·
2020
·
IF 9.511
Daixing Wei,Yubo Tan,Yiqing Wang,Tingting Kong,Shaohua Shen,Samuel S. Mao
A novel metal/semiconductor photocatalyst , Cu nanoparticles (NPs) modified TiO 2 hollow spheres (Cu/TiO 2 ), was designed for efficient photocatalytic overall water splitting (POWS) under both ultraviolet (UV) and visible (Vis) light. This Cu/TiO 2 photocatalyst possesses excellent POWS performance under Vis light at the highest level among the reported TiO 2 -based photocatalysts. Interestingly, the metal/semiconductor junction formed between Cu and TiO 2 enables controlled water-oxidation product selectivity (H 2 O 2 or O 2 ) via different reaction pathways regulated by irradiation wavelengths. Under UV light , the electrons excited in TiO 2 are captured by Cu NPs through the Cu/TiO 2 Schottky interface for H 2 production, with the photoholes in TiO 2 producing H 2 O 2 through a two-electron process; whilst under Vis light, Cu NPs act as plasmon to inject hot electrons to TiO 2 for H 2 production, while O 2 is produced by hot holes on Cu NPs via a four-electron process. This rational design of function-switchable metal/semiconductor junction may be helpful to understand the mechanisms for POWS with desired gas/liquid water-oxidation products.
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