APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Fanqing Meng,Wei Ma,Chunying Duan,Xin Liu,Zhen Chen,Moyan Wang,Jian Gao,Zhe Zhang
Two dimensional transition metal dichalcogenides as potential catalysts to solve energy and environmental crises have caused significant research interests in recent years. In this work, edge-selectively Fe@3D-WS 2 nanoflowers with the abundant single-layer were efficiently prepared by dry ball milling for levofloxacin (LEVO) elimination. Together with the advantages of the single-layer active edges and the stretch of W S bond, the as-prepared Fe@3D-WS 2 showed the ultra-high degradation efficiency for LEVO under ball-milling condition. This high degradation activity was demonstrated to be originated from piezo-catalysis, rather than adsorption or thermocatalysis. In addition, the Fe@3D-WS 2 also showed an ultra-high reusability during the cyclic tests, which is due to its special “self-renewing” behavior under ball milling condition. The degradation efficiency of the Fe@3D-WS 2 still reached ˜ 99% after ten cyclic tests. Both oxygen radicals ( 1 O 2 , O 2 ·− ) and ·OH radicals were generated and took part in the LEVO degradation, while oxygen radicals were more contributed to the LEVO degradation. The present work not only provides an important insight for designing efficient catalysts, but also extends the possible application areas of ball milling technique.
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高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2019
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IF 3.834
Qiuyue Men,Tao Wang,Changchang Ma,Lili Yang,Yang Liu,Pengwei Huo,Yongsheng Yan
In this paper, a simple in-suit method was used to load CdSe quantum dots (QDs) onto HTC (abbreviated as Hydrothermal biochar, HTC) to form CdSe/HTC composites. Fourier transform infrared spectrometer and X-ray photoelectron spectroscopy were used to detect and analyze the surface valence and composition of CdSe/HTC composites. The photocatalytic degradation activity was judged by photodegrading tetracycline (TC). Compared with pure CdSe quantum dots, the best photocatalytic degradation efficiency of CdSe/HTC complex containing 15% HTC was 73%, which was attributed to the high carrier transport efficiency of HTC and the inhibition reorganization of photogenerated electron-hole pairs. More importantly, the hydrothermal biochar used in this paper was extracted from waste biomass and had the characteristics of economy, environmental protection and high utilization rate, and was in line with the basic viewpoint of sustainable use of resources.
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ANALYTICAL CHEMISTRY
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2019
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IF 6.35
Muhammad Saqib,Shahida Bashir,Haijuan Li,ShanShan Wang,Yongdong Jin
Development of simple and effective chemiluminescence (CL) systems for multiple sensing applications is significantly important but still a challenge. Until now, the majority of CL systems primarily utilized hydrogen peroxide (H2O2) as coreactant, which is limited in its stability and selectivity due to the easy decomposition of H2O2 in the presence of several ions. In this study, we develop a new and intense CL system by combined use of tris(2-carboxyethyl)phosphine (TCEP), a highly solution stable and pH-tolerant tertiary phosphine, with lucigenin for the first time. The effective pairing leads to a significant ∼23 times CL enhancement over classic the lucigenin–H2O2 system without employing additional catalysts. By virtue of this fascinating platform, a sensitive CL method has been developed for the multiple detection of TCEP (LOD = 70 nM), lucigenin (LOD = 4.0 nM), superoxide dismutase (LOD = 0.8 ng/mL), Hg2+(LOD = 0.3 nM), and dopamine (LOD = 3.0 nM), with a linear range of 0.1–320 μM, 0.01–55 μM, 0.005–0.5 μg/mL, 1.0–600 nM, and 0.01–0.8 μM, respectively. Remarkably, this CL method exhibited superior selectivity over several potential interferents. Moreover, the proposed method achieved excellent recoveries in the range of 94.0–102.3% for both Hg2+ detection in lake water and dopamine detection in human serum real samples. We envision that broad applications of TCEP may lead to construct new CL systems, pushing forward for efficient detection of various analytes.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yanjuan Huang,Yali Jiang,Zhanghong Xiao,Yifeng Shen,Liangfeng Huang,Xiaoyu Xu,Gaofei Wei,Congjun Xu,Chunshun Zhao
Strategies utilizing reactive oxygen species (ROS) to cause cell death are widely practiced for cancer therapy, including photodynamic therapy (PDT) and chemodynamic therapy (CDT). However, the efficiency of PDT alone is greatly hindered by tumor hypoxia, laser penetration depth and the relatively low oxidation performance of 1 O 2 and its subsequent products H 2 O 2 . Meanwhile, CDT is limited by the deficiency of endogenous H 2 O 2 in cancer cells. If the ROS, produced in PDT process, served as the substrate in CDT, the total ROS production would be greatly enhanced. However, the increased ROS could be scavenged by the overexpressed glutathione (GSH) in cancer cells, impairing the effect of PDT and CDT. Thus, in this study, a self-reinforcing ferric pyrophosphate based nanoagent (FeP-ZnPc) for synergetic NIR-triggered photo/chemodynamic therapy with glutathione depletion ability was constructed. The constructed FeP-ZnPc exhibited “triple use”: PDT, CDT and GSH depletion function. Upon internalized into cancer cells, the FeP-ZnPc could release Fe 3+ which underwent a redox reaction with GSH, resulting in GSH depletion and the production of Fe 2+ . Upon laser, Zinc phthalocyanine (ZnPc) in the FeP-ZnPc could generate ROS for PDT directly. Moreover, the elevated ROS particularly H 2 O 2 could serve as the substrate of CDT, accelerating the Fenton reaction process, producing the strongest oxidants, hydroxyl radical ( OH) and leading to ROS burst to expedite cell death. This combination strategy of enhancing ROS production and inhibiting ROS elimination could eventually break down the redox homeostasis and enhance the ROS-mediated cancer therapy.
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Small
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2019
·Vol. 15
·期 17
·1805478
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IF 10.856
Kai Jia,Jiahua Ye,Guoxin Zhuang,Zanyong Zhuang,Yan Yu
Fabrication of low-dimensional nano-MOFs as well as nanoparticles/metal-organic frameworks (MOFs) hybrids has sparked new scientific interests but remains a challenging task. Taking Cu 3 (BTC) 2 as a proof of concept, it is demonstrated thats NH 3 ⋅H 2 O solution of a confined pH value can readily shape the bulk Cu 3 (BTC) 2 into nanoscale Cu 3 (BTC) 2 , beyond the need to control the crystal growth kinetics of MOFs. Adjusting the pH of NH 3 ⋅H 2 O within a much small range (10–11) allows fine tuning over the size and shape of nanoscale Cu 3 (BTC) 2 . Particularly at pH = 11, NH 3 ⋅H 2 O exhibits weak reducibility that triggers a reduction of part of Cu 3 (BTC) 2 into Cu 2 O, while shaping the other into Cu 3 (BTC) 2 nanowires. Benefiting from the coincidence of reduction and etching effects, the newly generated Cu 2 O dots can in situ anchor onto adjacent Cu 3 (BTC) 2 nanowires at highly dispersive state, forming a well-defined sponge-like architecture built of Cu 2 O dots and nano-Cu 3 (BTC) 2 . The CuO x derived from annealing of the Cu 2 O dots/nano-Cu 3 (BTC) 2 hybrid preserves the sophisticated sponge architecture and high porosity, and exhibits promising applications in phenol scavenging, with efficiency outperforming its counterparts and many other Cu-based catalysts reported in literature. It is anticipated that the findings here pave the way for the rational design of intricate nano-MOFs in a more efficient way.
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高影响因子
WATER RESEARCH
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2019
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IF 7.913
Wanjun Wang,Hanna Wang,Guiying Li,Taicheng An,Huijun Zhao,Po Keung Wong
The development of cost-effective water disinfection methods is highly desired to address the problems caused by outbreak of harmful microorganisms . Sulfate radical (•SO 4 − )-based advanced oxidation technology has attracted increasing attention. However, various catalysts or UV irradiation are usually used to activate persulfate (PS), which is high-cost and the recovery of nano-sized catalysts is also challenging. This work demonstrates a new method of catalyst-free activation of persulfate by visible light (VL) for bacterial inactivation. The 6-log of E. coli cells can be inactivated within 40 min and 7-log of E. coli cells could be inactivated within 120 min by the VL/PS system. The major responsive wavelength is 420 nm, and no heat activation of PS is found during VL irradiation. A synergistic effect with synergy factor of 51.2% is found when combining the VL irradiation with heating at 50 °C. The acidic pH is benefit for the VL/PS-triggered bacterial inactivation, while bicarbonate inhibits the E. coli inactivation at the range of 0.1–20 mg/L. Mechanism study indicates the main reactive species are •SO 4 − , •O 2 − and •OH, in which •SO 4 − plays the most important role. The bacterial inactivation process shows to begin from outer membrane to intracellular components. Subsequently, the antioxidant enzyme (i.e. SOD, CAT) is induced, followed by damaging to the genomic DNA leading to fatal death of the cells. In addition, the VL/PS system is also applicable for the inactivation of other pathogenic bacteria, including Staphylococcus aureus and Pseudomonas aeruginosa , showing universality for water disinfection applications. This work not only provides a new cost-effective disinfection method without a catalyst, but also sheds light on understanding the bacterial inactivation mechanism by •SO 4 − -based AOPs .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Deyou Yu,Lubiao Li,Minghua Wu,John C. Crittenden
The photocatalytic activity of metal-organic frameworks (MOFs) is drawing great attention in the field of environmental remediation. However, the efficiency of MOFs still remains low because of the rapid recombination of valence band holes and conduction band electrons (a.k.a., charge carriers). The combination of photocatalysis and electron acceptors such as ozone are believed to be an efficient strategy to reduce the charge carrier recombination. Herein, we report that photocatalytic ozonation (PCO) using an Fe-based MOF (MIL-88A(Fe)) has greater destruction than photocatalysis and/or catalytic ozonation in terms of 4-nitrophenol (4-NP) degradation and mineralization. It is worth noting that our Fe-based MOF has a large number of Lewis acid sites (LAS). The pseudo-first order kinetic rate constants ( k ) of 4-NP degradation using PCO, photocatalysis and catalytic ozonation systems are 0.1632, 0.0143 and 0.0840 min −1 , respectively. The TOC removal of 4-NP in the PCO system is approximately 75.4% ([4-NP] = 100 ppm, ozone input dosage = 1.5 mg/min-L, UV light intensity = 3.46 × 10 -6 Einstiens/L-s, treatment time = 30 min) and this is much greater than those of photocatalysis (17.6%) and catalytic ozonation (38.7%). Most importantly, both the k value and TOC removal in the PCO system are much higher than the sum of those in other two processes, implying a strong synergistic effect in the PCO process. Mechanistic studies were conducted using electrochemical impedance spectroscopy (EIS) and photoluminescence (PL) measurements and demonstrate that the synergistic effect may originate from the enhanced photoinduced carrier separation using ozone as an electron acceptor. Furthermore, OH, O 2 − , and 1 O 2 are found to be the principal reactive oxygen species (ROS) for 4-NP degradation and mineralization. Integrating the analysis of band structure, EPR and scavenging experiment results, ozone is not only able to reduce charge carrier recombination but also can be catalytically decomposed to generate more ROS on the LAS of MIL-88A(Fe). This study provides deep insights into the use of MOFs as effective advanced oxidation processes (AOPs).
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Nuanqin Zhang,Junyi Chen,Zhanqiang Fang,Eric Pokeung Tsang
The development of an ultra-efficient heterogeneous Fenton catalyst that has practical application and can be easily separated is of great importance. In this study, a novel nanocomposite, Fe 0 /CeO 2 , was successfully synthesised and applied for Fenton oxidation of tetracycline. The results show that Fe 0 /CeO 2 significantly enhanced the removal of pollutants, which suggests a synergistic effect between nanoscale zero-valent iron and CeO 2 . Furthermore, the composite catalyst exhibited ideal reusability and wide pH adaptation. A radical identification experiment revealed that surface-bounded OH ( OH ads) played a critical role in Fenton reaction, and compared with bare nanoscale zero-valent iron, Fe 0 /CeO 2 remarkably promoted the generation of OH in the Fenton system, mostly because CeO 2 not only increased the adsorption properties of the catalyst, it also accelerated electron transfer to promote the decomposition of H 2 O 2 due to the abundance of surface oxygen vacancies. A reasonable degradation pathway was also proposed for tetracycline on the basis of the detected intermediates. Our findings help to understand the mechanism of tetracycline degradation by heterogeneous Fenton-like, and also provide an efficient system for organic wastewater treatment.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
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IF 5.589
Lu Gan,Qiang Zhong,Aobo Geng,Linjie Wang,Chi Song,Shuguang Han,Juqing Cui,Lijie Xu
We prepared carbon nanofiber (CCNF) using cellulose as the carbon source in this study and utilized for the first time as the support to enhance the catalytic performance of the cobalt ferrite (CoFe 2 O 4 ) for peroxymonosulfate (PMS) activation. The catalytic capability of the CoFe 2 O 4 /CCNF nanocomposites activated PMS was investigated through degrading dimethyl phthalate (DMP), a classical organic pesticide pollutant, in water media. The influence factors like CCNF content, nanocomposite and PMS dosage, DMP content, and pH value on the degradation speed were systematically investigated and analyzed. Since CoFe 2 O 4 is a spinel structured molecule which is magnetically separable, the reusability of the prepared CoFe 2 O 4 /CCNF nanocomposites under multiple cycles was also tested. Besides, the degradation intermediates during the catalytic process were also analyzed and identified by liquid chromatography-mass spectrometry (LC-MS) with a possible degradation mechanism. The results indicated that the prepared nanocomposite had promising catalytic capability in degrading DMP, in which the SO 4 − radicals played the main role as the active oxidation agent. Furthermore, the CoFe 2 O 4 /CCNF nanocomposites exhibited very good stability and reusability. The present study provides a clean biochar supported catalyst which could readily enhance the PMS activation efficiency for recycled decontamination of refractory organic pollutants in water media.
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高影响因子
FUEL PROCESSING TECHNOLOGY
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2019
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IF 4.507
Haotian Li,Feng Liu,Shuhui Wang,Fengjia Wang,Xin Qian,Caiduan Zhang,Yongliang Ma,Lidong Wang
Based on advanced oxidation technology, a new method for the simultaneous removal of SO 2 and NO x from industrial flue gas using Na 2 S 2 O 8 /MgO was proposed. The method does not require the body structure of the wet desulfurization device is changed but adds Na 2 S 2 O 8 to the original equipment to realize simultaneous desulfurization and denitrification. After determining Cl − was additive, the effects of various reaction factors on the simultaneous removal of SO 2 and NO x were investigated, including the Cl − concentration, the initial concentration of the oxidant, the initial pH value of the solution, and the reaction temperature. According to the characterization of removal products and the types of free radicals involved in the reaction by XRD , XPS , and EPR , the reaction mechanism was elucidated. The experimental results indicated that the removal products were mainly sulfates and nitrates. The free radicals involved in the reaction were SO 4 ·− , ·OH, and Cl·, and the key free radical was Cl·.
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2019
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IF 8.355
Yanan Shang,Cheng Chen,Ping Zhang,Qinyan Yue,Yanwei Li,Baoyu Gao,Xing Xu
In this work, the nitrogen-doped carbon nanotubes with encapsulated Fe 3 C nanoparticles (Fe 3 C@NCNTs) were prepared through a simple process by pyrolyzing the precursor of ferric trichloride hexahydrate and melamine composite. It was studied systematically that multiple Fe 3 C@NCNTs synthesized under 600–1000 °C activated persulfate (PS) for the degradation of sulfamethoxazole (SMX), a widely used antibiotic of sulfonamides. Raman spectrum , X-Ray Diffraction (XRD), X-ray photoelectron spectroscopy (XPS) were used to characterize the transformation of catalyst with the increase of annulling temperature. The Fe 3 C@NCNTs synthesized under 800, 900 and 1000 °C showed similar degradation ability to SMX with degradation rates of 0.650–0.893 min −1 . During catalytic process, the specific structure of Fe 3 C encapsulated NCNTs could both benefit the electron transfer and prevent the Fe 3 C dissolving in the solution. The results of quenching experiments coupling with electron paramagnetic resonance (EPR) spectra suggested the OH, SO 4 − and 1 O 2 contributed to the degradation of SMX and the singlet oxygen took effect for longer time. The degradation intermediates were mainly derived from the reactions of hydroxylation, oxidation , aniline ring opening, deamination, desulfonation, as well as bond cleavage. In terms of the density functional theory (DFT) calculations, the graphitic N exhibited the highest ΔE ads (−0.437 eV) for the PS molecule, and it was followed by the pyrrolic N (−0.304 eV), pristine graphene (−0.146 eV) and pyridine N (−0.072 eV), which means that the graphitic N is more favorable for the binding affinity with PS, forming the reactive complexes on the surface of the NCNTs catalysts to promote the nonradical oxidation.
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高影响因子
APPLIED SURFACE SCIENCE
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2019
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IF 5.155
Qiao Wang,Peng Xu,Guangshan Zhang,Limin Hu,Peng Wang
Visible-light responsive g-C 3 N 4 catalysts were successfully prepared by the calcination of urea, i.e., the thermal polycondensation method, and a series of ZnS/g-C 3 N 4 composite photocatalysts were then synthesized using a rapid microwave hydrothermal method . The physicochemical properties of the resulting g-C 3 N 4 and ZnS/g-C 3 N 4 catalysts were characterized via several microscopy and spectroscopy techniques . The reduction of Cr(VI) was used to evaluate the photocatalytic performance of the as-synthesized catalysts under visible light irradiation. The results showed that the calcination temperature substantially affected the crystallinity , specific surface area and photocatalytic performance of g-C 3 N 4 . The optimal temperature for thermal polycondensation in the g-C 3 N 4 synthesis was 600 °C. The bulk g-C 3 N 4 catalyst exhibited no Cr(VI) reduction ability, while a certain amount of ZnS nanoparticles coupling with g-C 3 N 4 significantly improved the Cr(VI) reduction efficiency, creating a synergistic effect between g-C 3 N 4 and ZnS. The simultaneous Cr(VI) reduction and rhodamine B decolorization by the ZnS/g-C 3 N 4 composite catalyst were also accomplished. In addition, a Cr(VI) reduction mechanism under visible light irradiation was proposed.
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