Nanoscale
·
2018
·Vol. 11
·期 3
·1286-1294
·
IF 7.233
Yulian Li,Lingyun Feng,Wei Yan,Irshad Hussain,Li Su,Bien Tan
Copper nanoclusters (CuNCs) exhibit susceptibility to oxidation in the subnanometer size range. In this work, a facile and green protocol is reported for the successful synthesis of water soluble CuNCs, with poly(vinylpyrrolidone) as a template and ascorbic acid as a mild reducing agent. The as-prepared CuNCs exhibit a green fluorescence and high quantum yield (QY = 44.67%) in water, which is the highest among the reported water soluble CuNCs. The origin of their highly luminescent nature was also investigated. In addition, the obtained CuNCs show good tolerability to high ionic strength, superior antioxidation properties, good photostability, time-stability, a large Stokes shift and ultralow cytotoxicity, laying the foundation for living cell imaging in THP-1 macrophages. A bright green fluorescence can be observed from the cells, indicating the potential practicality of CuNCs as a fluorescence marker in bioapplications. Interestingly, the as-prepared CuNCs exhibit a good selective fluorescence quenching response towards trinitrophenol over other nitro compounds. Furthermore, CuNCs were employed for sensing trinitrophenol based on the inner filter effect. A good linear relationship was obtained in the low concentration range of trinitrophenol, with a limit of detection of 3.91 × 10−7 M in aqueous medium. This result suggests the potential application of CuNCs as a probe in sensing and monitoring toxic trinitrophenol in the field of environmental security.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2018
·
IF 5.091
Man Yuan,Renzi Yang,Shuoyun Wei,Xiwei Hu,Dan Xu,Jin Yang,Zhengping Dong
Porous organic polymers (POPs) containing nitrogenous substituents have potential practical applications as heterogeneous catalysts based upon controlled porous structure and surface-anchored noble metal nanoparticles (NMNPs). In this work we prepared a POP material from piperazine and cyanuric chloride starting materials (PC-POP). The PC-POP material contains numerous triazinyl moieties, thus rendering the pores hydrophobic. Subsequently, by means of a novel reverse double-solvent approach (RDSA), microdroplets of Pd(AcO) 2 /CH 2 Cl 2 were introduced into the hydrophobic pores of PC-POP in an aqueous environment; Pd(II) was rapidly reduced by NaBH 4 to form ultra-fine Pd NPs and confined within the pores of PC-POP at high dispersity. The extensive porosity and dispersity of the Pd NPs made the active sites readily accessible, and led to efficient mass transfer. Thus, Pd@PC-POP exhibits superior catalytic performance in catalytic reduction of various nitroarenes. Furthermore, Pd@PC-POP has excellent recyclability, without significant loss of activity nor leaching of Pd active sites during 10 successive reaction cycles. This work points to a practical and cost-effective approach to preparation of POP materials, and also for confining ultra-fine NMNPs in POPs for use as catalysts.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2018
·
IF 5.091
Jin Huang,Jie Cao,Ni Tu,Huaping Dong,Jianfa Li,Jianxin Shou,Yimin Li
Nonionic and anionic surfactants often occur in anaerobic environments, but their roles in the removal of organic contaminants by Fe-bearing mineral/Fe(II) have not been determined. In this study, batch experiments were performed to investigate the effects of a nonionic surfactant (TX-100) and an anionic surfactant (SDBS) on the removal of nitrobenzene (NB) by Fe-bearing montmorillonite (FM)/Fe(II). Mössbauer spectrum and XPS were applied to analyze the edge surface bound Fe(II) and secondary minerals formed on FM. The contribution of surfactant to the enrichment of NB on FM was studied. The results showed that TX-100 and SDBS had opposite effects on the removal of NB by FM/Fe(II) at neutral pH. The presence of TX-100 improved the removal efficiency of NB from 36.4% to 70.0%, and increased the initial removal rate by 1.7 times. This enhancement effect was mainly attributed to the formation of more active edge surface bound Fe(II) that can reduce more NB to aniline. Formation of more magnetite on FM and selective enrichment of NB on the reactive surface also contributed to the removal of NB. In contrast, the presence of SDBS reduced the amount of edge surface bound Fe(II) via formation of SDBS-Fe(II) complex, which decreased the removal efficiency of NB.
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CHEMICAL ENGINEERING RESEARCH & DESIGN
·
2018
·
IF 2.795
Hao Feng,Biao Zhang,Xun Zhu,Rong Chen,Qiang Liao,Ding-ding Ye,Jian Liu,Ming Liu,Gang Chen
Microreactors are promising for fine chemistry and value-added chemical synthesis, but the small dimension places significant challenges in catalyst layer fabrication. Meanwhile, enhancing catalyst dispersion to obtain smaller particle size are of great interests. We proposed a multilayered Pd nanocatalysts with nano-bulge structure inside a microreactor for multiphase catalytic reaction. The unique bulged nanostructure can provide more accessible sites for precursor (PdCl 4 2− ) adsorption, and extend the available area to reduce the Pd nanoparticle size. Experimental results show rugged Pd catalyst layer with the nano-bulge structure was prepared, and both the precursor utilization rate and Pd nanocatalysts dispersion were enhanced, resulting in 35.4% higher catalyst loading and 4-fold smaller particle size. Benefitting from these advantages, compared with conventional Pd coated polydopamine catalyst layer, the proposed multilayered Pd nanocatalyst can significantly intensify the reaction rate and obtain an order of magnitude longer durability in nitrobenzene hydrogenation. This versatile and convenient fabrication method can be used in fabricating high performance and durable catalyst layers in microreactors.
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CHEMICAL ENGINEERING JOURNAL
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2013
·
IF 3.473
Jinhua Wu,Weizhao Yin,Jingjing Gu,Ping Li,Xiangde Wang,Bo Yang
Batch experiment was conducted to evaluate the capability of a biotic Fe 0 –H 2 O for nitrobenzene (NB) removal from groundwater. In this study, iron dosage was 0.25 g L −1 throughout the whole experiment and the Fe 0 –H 2 O system was amended with 180 mg L −1 VSS of mixed culture. The biotic system was tested at low concentrations (50 mg L −1 as COD) of organic substrates (e.g., ethanol, glucose and sodium acetate) and different concentrations of sulfate, nitrate and dissolved oxygen. The bio-iron system exhibited higher NB removal rate and more AN production. The increasing order of efficiency of tested substrates was: glucose > sodium acetate > ethanol. A complicated enhancement from oxygen was obtained, with 100% of NB removal rate and without any AN accumulation in the solution amended by dissolved oxygen. Sulfate and nitrate functioned as inhibitors since they competed with NB for electron donors (H 2 ), and nitrate showed more significant suppression on NB removal as compared to sulfate. AN elimination occurred during both sulfate-reducing and nitrate-reducing processes and microorganisms got extra reduction capacity from the degradation of AN to reduce nitrate and sulfate, causing the mineralization of NB under anaerobic or anoxic conditions. It suggested that the bio-iron treatment could function as a simplified process for the remediation of groundwater contaminated by combined NB and sulfate, nitrate.
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CHINESE CHEMICAL LETTERS
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2013
·
IF 1.21
Cheng Feng,Hai-Yan Zhang,Ning-Zhao Shang,Shu-Tao Gao,Chun Wang
Graphene-Fe 3 O 4 nanocomposite (G-Fe 3 O 4 ) was synthesized by a chemical co-precipitation method which was used as an efficient catalyst for the reduction of nitroarenes with hydrazine hydrate. The method has been applied to a broad range of compounds with different properties and the yields were in the range of 75%–92%. The G-Fe 3 O 4 catalyst can be readily recovered and reused 5 times without significant loss of the catalytic activity.
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CATALYSIS COMMUNICATIONS
·
2014
·
IF 3.32
Haiyan Zhang,Ying Zhao,Weihua Liu,Shutao Gao,Ningzhao Shang,Chun Wang,Zhi Wang
A magnetically separable and highly active Co–Cu mixed spinel catalyst, Cu 6/7 Co 1/7 Fe 2 O 4 –graphene (Cu 6/7 Co 1/7 Fe 2 O 4 –G), was fabricated by a hydrothermal method. The results demonstrated that the Cu 6/7 Co 1/7 Fe 2 O 4 –G possessed excellent catalytic activity for the reduction of a broad range of nitroarenes in the presence of NaBH 4 . The composite catalyst was efficient, stable, low-cost and could be easily recovered due to its magnetic separability.
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TALANTA
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2013
·
IF 3.498
Yingxin Ma,Leyu Wang
This paper reports a rapid, sensitive, and selective nanosensor for the detection of 2,4,6-trinitrotoluene (TNT) in the mixture aqueous solution of nitroaromatics independent of immunoassay or molecularly imprinted technology and complicated instruments. Despite many strategies including immunoassay and molecularly imprinted technologies been successfully developed for the detection of TNT, it is not easy to differentiate TNT from 2,4,6-trinitrophenol (TNP) due to their very similar chemical structures and properties. In this work, the amine functionalized NaYF 4 :Yb 3+ /Er 3+ upconversion luminescence nanoparticles (UCNPs) whose excitation (980 nm) and emission (543 nm) wavelength were far from the absorbance bands of other usual interference nitroaromatics including 2,4-dinitrotoluene (DNT), nitrobenzene (NB), and especially TNP, were utilized as the luminescent nanosensors for TNT luminescence detection. To make these UCNPs highly water stable and render the charge transfer from UCNPs to TNT easier, amino groups were introduced onto the surface of the UCNPs by coating a polymer layer of ethylene glycol dimethacrylate (EGDMA) hybridized with 3-aminopropyltriethoxysilane (APTS). After binding with TNT through amino groups on the UCNPs, the naked eye visible green upconversion luminescence of the UCNPs was dramatically quenched and thus a sensitive UC luminescence nanosensor was developed for TNT detection. However, other nitroaromatics including TNP, DNT, and NB have no influence on the green UC luminescence and thus no influence on the TNT detection. The luminescence intensity is negatively proportional to the concentration of TNT in the range of 0.01−9.0 µg/mL with the 3 σ limit of detection (LOD) of 9.7 ng/mL. The present studies provide a novel and facile strategy to fabricate the upconversion luminescence sensors with highly selective recognition ability in aqueous media and are desirable for label free analysis of TNT in mixed solution independent of immunoassay and molecularly imprinted technology and complicated instruments.
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CHINESE JOURNAL OF CATALYSIS
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2015
·
IF 1.964
Junrui Li,Xiaohong Li,Yue Ding,Peng Wu
Pt nanoparticles entrapped in ordered mesoporous CMK-3 carbons with p6mm symmetry were prepared using a facile impregnation method, and the resulting materials were characterized using X-ray diffraction spectroscopy, N 2 adsorption-desorption, scanning electron microscopy, transmission electron microscopy, energy dispersive X-ray spectroscopy, and X-ray photoelectron spectroscopy. The Pt nanoparticles were highly dispersed in the CMK-3 with 43.7% dispersion. The Pt/CMK-3 catalyst was an effective catalyst for the liquid-phase hydrogenation of nitrobenzene and its derivatives under the experimental conditions studied here. The Pt/CMK-3 catalyst was more active than commercial Pt/C catalyst in most cases. A highest turnover frequency of 43.8 s −1 was measured when the Pt/CMK-3 catalyst was applied for the hydrogenation of 2-methyl-nitrobenzene in ethanol under optimal conditions. It is worthy of note that the Pt/CMK-3 catalyst could be recycled easily, and could be reused at least fourteen times without any loss in activity or selectivity for the hydrogenation of nitrobenzene in ethanol.
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CHEMICAL ENGINEERING JOURNAL
·
2014
·
IF 4.058
Weizhao Yin,Jinhua Wu,Weilin Huang,Chaohai Wei
Nitrobenzene (NB) infiltrated in groundwater has caused serious threats to the safety of drinking water due to its persistence and high toxicity. In this study, abiotic zero-valent iron (ZVI) column and biotic ZVI column were employed to investigate abiotic and biotic effects between iron and microorganisms on NB removal and column longevity. Physical removal and kinetics analysis revealed that NB was largely removed through adsorption and/or co-precipitation and the reduction of NB to aniline (AN) via abiotic reaction in the abiotic column and via both abiotic and biotic reactions in the biotic column. Due to the interactive effect of ZVI and microorganisms, more effective iron consumption and more reactive minerals such as green rust and iron sulfide were found in the biotic column. This led to approximately 50% higher total NB removal and 6 times higher AN production in the biotic column as compared to the abiotic column during the entire operation. According to the NB breakthrough curves, longer stability and longer life-span of the column system could be maintained in regard of microbial activity. It indicated that additional microorganisms might improve the performance of iron-based permeable reactive barrier (PRB) for groundwater remediation.
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CHEMICAL ENGINEERING JOURNAL
·
2015
·
IF 4.321
Xiaori Fu,Xiaogang Gu,Shuguang Lu,Minhui Xu,Zhouwei Miao,Xiang Zhang,Yacong Zhang,Yunfei Xue,Zhaofu Qiu,Qian Sui
In this study, the application of sodium percarbonate (SPC) catalyzed by various chelated-Fe(II) to stimulate the degradation of benzene in groundwater remediation was investigated. Effective oxidation of benzene was achieved in CIT/SPC/Fe(II) and OA/SPC/Fe(II) systems. The reaction mechanism for benzene degradation in CIT/SPC/Fe(II) and OA/SPC/Fe(II) systems was elucidated by free radical probe compound tests, free radical scavenger tests and electron paramagnetic resonance (EPR) analysis. And hydroxyl radical (HO ) and superoxide anion radical ( O 2 - ) were confirmed as the predominant species responsible for benzene degradation. Besides, the effects of various factors, such as the solution characteristics including the presence of anions (Cl − , HCO 3 − , SO 4 2− and NO 3 − ), natural organic materials (NOM), and the initial solution pH on benzene degradation were also evaluated. The influences caused by SO 4 2− , NO 3 − , Cl − and NOM were negligible, but HCO 3 − anion had a slightly inhibitive effect in low concentration (1 mM) and an apparently inhibitive effect in high concentration (10–100 mM). However, the additions of CIT and OA eliminated the adverse influence of HCO 3 − and ensured a high benzene degradation efficiency at wider pH range. Finally, results obtained in actual groundwater test strongly demonstrated that Fe(II)-CIT and Fe(II)-OA catalyzed SPC systems are applicable for the remediation of benzene-contaminated groundwater in practice.
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ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2015
·Vol. 23
·期 7
·6758-6766
·
IF 2.828
Fu Xiaori,Gu Xiaogang,Lu Shuguang,Miao Zhouwei,Xu Minhui,Zhang Xiang,Danish Muhammad,Cui Hang,Farooq Usman,Qiu Zhaofu,Sui Qian
Effective degradation of benzene was achieved in sodium percarbonate (SPC)/Fe(II)-Glu system. The presence of glutamate (Glu) could enhance the regeneration of Fe(III) to Fe(II), which ensures the benzene degradation efficiency at wider pH range and eliminate the influence of HCO 3
− in low concentration. Meanwhile, the significant scavenging effects of high HCO 3
− concentration could also be overcome by increasing the Glu/SPC/Fe(II)/benzene molar ratio. Free radical probe compound tests, free radical scavenger tests, and electron paramagnetic resonance (EPR) analysis were conducted to explore the reaction mechanism for benzene degradation, in which hydroxyl radical (HO•) and superoxide anion radical (O 2
•− ) were confirmed as the predominant species responsible for benzene degradation. In addition, the results obtained in actual groundwater test strongly indicated that SPC/Fe(II)-Glu system is applicable for the remediation of benzene-contaminated groundwater in practice.
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