CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Ruijie Xie,Jian Ji,Kaiheng Guo,Dongxue Lei,Qingjuan Fan,Dennis Y.C. Leung,Haibao Huang
In this study, wet scrubber coupled with UV/peroxymonosulfate (PMS) was used as a semi-batch process for removing gaseous VOCs. Both ethyl acetate and toluene could be removed efficiently using this coupled process due to the generation of SO 4 − and HO . The mass-transfer coefficients in this coupled process were larger than in wet scrubbing only process. The roles of SO 4 − and HO were investigated, in which SO 4 − acted as the predominant radical for toluene degradation while HO was major for ethyl acetate. This could be further confirmed by simultaneous degradation of ethyl and toluene. Moreover, the reaction solution reused at least four times still showed excellent performance for VOCs removal via re-adding PMS. A possible mechanism on toluene degradation was proposed based on the evolutions of intermediates during the process. This study clarified the roles of non-selective radical (i.e. HO ) and selective radical (i.e. SO 4 − and Cl ) in the removal of a continuous-flow gaseous VOCs by this coupled process.
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Journal of Materials Chemistry B
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2018
·Vol. 6
·期 41
·6534-6543
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IF 4.776
Lizhen Zhang,Zhaoxing Lin,Yun-Xiang Yu,Bang-Ping Jiang,Xing-Can Shen
It is of vital importance to engineer the surface structures of carbon dots (CDs) to satisfy their practical biomedical applications, including imaging and treatment. In this work, one type of hyaluronic acid-derived CD (HA-CD) was synthesized via a facile one-step hydrothermal method using cancer cell-targeted HA as a precursor. The as-prepared HA-CDs were targeted actively toward CD44 receptor-overexpressing cancer cells because a partial HA structure remained on the HA-CD surface. Beyond this, HA-CDs can act as a novel photosensitizer, because they can generate O2˙− under 650 nm laser irradiation, and they also exhibit excellent blue photoluminescence emission. The in vitro results revealed that HA-CDs imaged selectively CD44-overexpressing cancer cells and inhibited their growth under 650 nm laser irradiation. Thus, HA-CDs can serve as a promising self-targeted imaging-guided photodynamic therapy (PDT) agent for cancer. The present research provides a promising new method to simply construct multifunctional CD-based targeted phototheranostic systems.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2018
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IF 11.698
Zhi Zhu,Xu Tang,Tianshuai Wang,Wenqian Fan,Zhi Liu,Chunxiang Li,Pengwei Huo,Yongsheng Yan
Developing low-cost and high-efficiency g-C 3 N 4 (CN) semiconductor with modification has been proved to possess the potential advantage for environmental remediation in recent years. Herein, element doping of CN framework was found significantly on controlling its electronic structure. The new two-dimensional photocatalyst of Co-doped CN (Co-CN) applicable in photocatalytic reactions for 2-Mercaptobenzothiazole degradation was designed and synthesized. It was for the first time revealed that the Co-N bonding could lead to enhance significantly photoelectric properties, the rate for electron-hole pairs separation and photocatalytic activity in comparison with bulk CN. The characterization and density functional theory (DFT) results insight into the reason that the 3d electrons of the doped Co has excellent contribution to adjust the band gap of Co-CN. The present work provide a broadening window for Metal-doped CN with outstanding performance.
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ACS Nano
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2018
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IF 13.709
Sufeng An,Guanghui Zhang,Tingwen Wang,Wenna Zhang,Keyan Li,Chunshan Song,Jeffrey T. Miller,Shu Miao,Junhu Wang,Xinwen Guo
Ultra-small metal clusters have attracted great attention owing to their superior catalytic performance and extensive application in heterogeneous catalysis. However, the synthesis of high-density metal clusters is very challenging due to their facile aggregation. Herein, one-step pyrolysis was used to synthesize ultra-small clusters and single-atom Fe sites embedded in graphitic carbon nitride with high density (iron loading up to 18.2 wt %), evidenced by high-angle annular dark field-scanning transmission electron microscopy, X-ray absorption spectroscopy, X-ray photoelectron spectroscopy, and 57Fe Mössbauer spectroscopy. The catalysts exhibit enhanced activity and stability in degrading various organic samples in advanced oxidation processes. The drastically increased metal site density and stability provide useful insights into the design and synthesis of cluster catalysts for practical application in catalytic oxidation reactions.
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WATER RESEARCH
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2018
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IF 7.051
Da Wang,Haodan Xu,Jun Ma,Stefanos Giannakis,Xiaohui Lu,Huizhong Chi,Shuang Song,Jingyao Qi
A light-weight granular mixed-quartz sand (denoted as L-GQS) combined with stirring-assisted bubble column reactor was firstly applied in catalytic ozonation of atrazine. The L-GQS, with a density of 2.36 g cm −3 and average diameter of ca. of 4 mm, was readily churned up and uniformly distributed within the solution in the reactor. The introduction of L-GQS was found to exhibit enhanced catalytic ozonation of atrazine, with the increase in degradation rate and the dissolved organic carbon (DOC) removal being more than 2-fold for the catalytic process (L-GQS dosage = 5 g L −1 , [atrazine] 0 = 50 μM, [O 3 ] = 25 mg L −1 , gas flow = 0.2 L min −1 , at pH 7.0 and 293 K). The L-GQS settled at the bottom of the reactor after experimentation, allowing its easy separation from the solution. A complete characterization of the material (XRD, XPS, FTIR , FE-SEM/EDS, BET and pH pzc ) revealed that L-GQS consisted of α-quartz, β-cristobalite, anorthoclase and small amount of iron oxy-hydroxides. Hydroxyl groups, Bronsted acid sites and Lewis acid sites on the surface of L-GQS all contributed to the atrazine adsorption, ozone decomposition and ·OH generation. The L-GQS catalyzed ozonation exhibited superior atrazine degradation and mineralization rates in a wide range of pH (3.0–9.0) and reaction temperatures (278 K–293 K). Also, an enhancement of DOC abatement was observed both in presence of natural organic matter isolates and natural water matrices (river water) when L-GQS was used. Finally, the degradation mechanism was proposed, based on the intermediates and by-products formation analyzed by LC-QTOF-MS/MS and ionic chromatography. Our results indicate that the L-GQS combined with stirring-assisted bubble column reactor could be utilized as an enhancement of ozone-based advanced oxidation processes .
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CHEMICAL ENGINEERING JOURNAL
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2018
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IF 6.735
Xiaodong Du,Yongqing Zhang,Fan Si,Chenhui Yao,Meimei Du,Imtyaz Hussain,Hyunook Kim,Shaobin Huang,Zhang Lin,Waseem Hayat
Non-radical activation of persulfate by CuO to degrade chlorinated organic pollutants has been studied. Currently, reduced graphene oxide modified spindle-like CuO (CuO/rGO, no preferential exposed crystal facet) and CuO with preferential exposed crystal facet (0 0 1) (sheet-like CuO) has been prepared to improve the performance of persulfate activation. Results showed that CuO/rGO-persulfate system and sheet-like CuO-persulfate system exhibited much better 2,4,6-trichlorophenol (TCP) removal rate than spindle-like CuO-persulfate system. The formation of Cu–O–C bond between CuO and rGO enhanced the persulfate activation by CuO. On the other hand, CuO showed crystal facet effect on persulfate activation, and the crystal facet (0 0 1) of CuO (all exposed atoms were Cu) were proved to be efficient for persulfate non-radical activation, revealing that Cu atom on surface was active site for persulfate activation. Furthermore, the pollutants selective removal by CuO/rGO-persulfate system has been found. 4-chloroaniline was most easily degraded, followed by 2,4,6-trichlorophenol, 2,4-dichlorophenol and 4-chlorophenol, under acidic, neutral and weak basic condition (pH 3–9). What’s more, pollutants with benzene ring was more reactive than that with double bond of carbon in the system.
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Journal of the American Chemical Society
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2018
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IF 14.357
Xuning Li,Xiang Huang,Shibo Xi,Shu Miao,Jie Ding,Weizheng Cai,Song Liu,Xiaoli Yang,Hongbin Yang,Jiajian Gao,Junhu Wang,Yanqiang Huang,Tao Zhang,Bin Liu
The Fenton-like process presents one of the most promising strategies to generate reactive oxygen-containing radicals to deal with the ever-growing environmental pollution. However, developing improved catalysts with adequate activity and stability is still a long-term goal for practical application. Herein, we demonstrate single cobalt atoms anchored on porous N-doped graphene with dual reaction sites as highly reactive and stable Fenton-like catalysts for efficient catalytic oxidation of recalcitrant organics via activation of peroxymonosulfate (PMS). Our experiments and density functional theory (DFT) calculations show that the CoN4 site with a single Co atom serves as the active site with optimal binding energy for PMS activation, while the adjacent pyrrolic N site adsorbs organic molecules. The dual reaction sites greatly reduce the migration distance of the active singlet oxygen produced from PMS activation and thus improve the Fenton-like catalytic performance.
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ACS Applied Materials & Interfaces
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2018
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IF 8.097
Da Wang,Haodan Xu,Jun Ma,Xiaohui Lu,Jingyao Qi,Shuang Song
Novel single-crystal hexagonal MnTiO3 nanosheets with exposed {0001} facets have been synthesized via a simple one-pot hydrothermal method using NaOH as a mineralizer and tetraethylammonium hydroxide (TEAH) as a morphology controller. The intermediate morphologies of MnTiO3 nanostructures such as nanoparticles, nanowires, nanorods, and nanodiscs are trapped kinetically by adjusting the synthesis conditions. This approach enables us to elucidate the growth mechanisms of MnTiO3 nanosheets based on the tetraethylammonium cation adsorption abilities on different MnTiO3 crystal facets combined with density functional theory calculations. Dissolution and recrystallization processes are involved during the MnTiO3 crystallization. The surface-controlled MnTiO3 has been found to be effective as a catalyst for ozonation in the degradation of 4-chlorophenol (4-CP). Within typical experimental conditions (catalyst dosage = 0.3 g L–1, [4-CP]0 = 50 mg L–1, [O3] = 20 mg L–1, gas flow = 0.1 L min–1, pH 6.8, and T = 293 K), the total organic carbon (TOC) removal efficiency of 4-CP in catalytic ozonation with well-structured MnTiO3 (MnTiO3-180-10 sample) was 76.3% after 60 min, compared with only 22.1 and 38.5% TOC removal in the absence of catalyst and with uncontrolled MnTiO3 (MnTiO3-no TEAH sample), respectively. Benefiting from the high exposure percentage of {0001} facet, mixed-valences of manganese, surface hydroxyl groups, and the enrichment Lewis acid sites provided by Mn and Ti, the morphology-controlled MnTiO3 nanosheets can be applied as heterogeneous catalytic ozonation catalysts which exhibit excellent pollutant degradation. We anticipate that MnTiO3 can be a promising candidate material for the application in remediation of organic pollutants in water.
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PHYSICA STATUS SOLIDI A-APPLICATIONS AND MATERIALS SCIENCE
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2018
·Vol. 215
·期 11
·1701061
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IF 1.795
Binrong Li,Jinyu Chu,Yi Li,Minjia Meng,Yanhua Cui,Qidi Li,Yonghai Feng
Photocatalytic degradation is an effective method for fast removal of dye-contaminated water. In the present work, a bismuth oxide/zinc sulfide-cellulose acetate photocatalytic membrane (Bi 2 O 3 /ZnS-CA) is successfully fabricated via the phase-inversion method with a Bi 2 O 3 /ZnS heterojunction as the photocatalyst. The Bi 2 O 3 /ZnS-CA membranes shows high photocatalytic activity in degradation of Rhodamine B (RhB) under visible-light irradiation due to the Bi 2 O 3 /ZnS heterojunction structure contributing to the high efficiency of photogenerated charge separation. The photodegradation efficiency of Bi 2 O 3 /ZnS-CA membrane is significantly enhanced (about 30% improvement) and the photodegradation kinetic is four times faster than that of the Bi 2 O 3 -CA and the ZnS-CA membranes. Moreover, the Bi 2 O 3 /ZnS-CA membrane exhibits excellent permeation flux (649.7 L m −2 h −1 ) and high porosity (69.94%). The Bi 2 O 3 /ZnS-CA membrane also shows good adsorption performance of RhB, which could enhance the interaction between RhB and the catalyst. This work provides a new sight to construct highly effective visible-light-driven photocatalytic membranes for continuous organic dye treatment.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
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IF 5.091
Jinsuo Gao,Shouchun Wu,Yanling Han,Feng Tan,Yong Shi,Mengyao Liu,Xinyong Li
Increasing the amount of surface active sites of the material may be a feasible way to improve the efficiency of the generation of Fe 2+ in the photo-Fenton process. In this work, a simple synthesis method was adopted to synthesize 3D ordered mesoporous CuFe 2 O 4 with large specific surface area by using ferric nitrate and copper nitrate as the precursor and KIT-6 as the template. The synthesized materials were characterized by nitrogen adsorption-desorption, XRD , TEM , FT-IR and UV–vis DRS . The catalytic properties of the mesoporous material were thoroughly evaluated by activating hydrogen peroxide to remove sulfonamides in near neutral water. Some of the reaction factors, such as the dose of hydrogen peroxide, catalyst usage and pollute concentration, were cautiously tested and discussed. When the catalyst dose is 0.2 g/L, the substrate concentration is 10 mg/L and the concentration of hydrogen peroxide is 10 mM, sulfamethoxazole is almost completely transformed within two hours and its mineralization level reached 31.42%. In the further study of mechanism, hydroxyl radical is proved to be the main active free radical based on EPR . Moreover, mesoporous copper ferric has good circulation, which indicates that it may have excellent application in the field of photo-Fenton.
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CHEMOSPHERE
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2018
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IF 4.427
Bin Deng,Yating Li,Weihua Tan,Zhaoxi Wang,Ziwei Yu,Shuya Xing,Heng Lin,Hui Zhang
Mn-Zn ferrite (Mn 0.6 Zn 0.4 Fe 2 O 4 ) was prepared by a gel method using spent alkaline Zn-Mn batteries as raw materials and employed as catalyst to degrade bisphenol A (BPA) by electro-enhanced heterogeneous activation of peroxydisulfate (PDS). The effects of initial pH, current density, PDS concentration, and Mn-Zn ferrite dosage on BPA removal were investigated. The formation of reactive radicals was verified by electron paramagnetic resonance (EPR) spectroscopy. The results of radical quenching experiments indicate that surface-bound sulfate and hydroxyl radicals played an important role in BPA removal. The stability of Mn 0.6 Zn 0.4 Fe 2 O 4 catalyst was investigated by cycling experiments, which indicates Mn 0.6 Zn 0.4 Fe 2 O 4 is stable and can be reused. This work also provides an alternative way for the reutilization of spent alkaline Zn-Mn batteries.
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ACS Sustainable Chemistry & Engineering
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2018
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IF 6.14
Jinxi Feng,Yao Fu,Xiaosheng Liu,Shuanghong Tian,Shenyu Lan,Ya Xiong
Piezoelectric effect was first used for disinfection. In this process, hydrothermally synthesized nano/micrometer tetragonal-BaTiO3 was selected as the piezo-catalyst which was stressed by ultrasound to generate piezoelectric potential. It was found that the inactivation number of the nano/micrometer tetragonal BaTiO3 exposure or sonication alone within 180 min was 0.30 log and 0.70 log for E. coli in deionized water, respectively, while addition of 2 g tetragonal-BaTiO3 with piezo-activity in the ultrasound system resulted in a 2.72 log inactivation without the input of any additional energy, only by original ultrasound. The latter was 2.72 folds as great as the sum of the two former inactivation numbers. However, addition of cubic-BaTiO3 without piezo-activity only led to a 1.02 log inactivation. And moreover, in the process of serious physical damage and chemical oxidation of cells, substantial leakages of intracellular materials were observed. These great differences not only clearly indicated that the combination of sonication and piezocatalysis possessed a great inactivation potential but also suggested that there was a significant synergistic inactivation effect between piezocatalytic oxidation and sono-mechanical destruction.
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