APPLIED ORGANOMETALLIC CHEMISTRY
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2019
·Vol. 33
·期 5
·e4850
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IF 3.259
Mingliang Ma,Yuying Yang,Yanyan Liu,Wenting Li,Guopeng Chen,Yong Ma,Ping Lyu,Shunhe Li,Yubao Wang,Guanglei Wu
In this paper, a simple route for palladium (Pd) nanoparticles attached to the surface of hollow magnetic Fe 3 O 4 /P (GMA-DVB)-polyethyleneimine (PEI) microspheres was established. Due to the large amount of imidogen groups and tertiary amine groups presenting in the PEI, Pd 2+ ions could be anchored to the support by complexation with a polyfunctional organic ligand. Thereafter, a magnetic Pd catalyst having a high loading amount and good dispersibility was obtained by reducing Pd 2+ ions. Afterwards, the prepared catalyst was characterized by TEM, SEM, FTIR, XRD, TGA, VSM, and UV–vis in detail. Ultimately, their catalytic activity was evaluated using the reduction of 4-nitrophenol (4-NP). Research showed that the Fe 3 O 4 /P (GMA-DVB)-PEI/Pd catalyst possessed high catalytic performances for the reduction of 4-NP with a conversion rate of 98.43% within 540 s. Furthermore, the catalyst could be easily recovered and reused at least for nine successive cycles.
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Journal of Materials Chemistry A
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2019
·Vol. 7
·期 18
·10980-10987
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IF 10.733
Xiaoqing Cao,Jun Zhou,Hongna Wang,Song Li,Wei Wang,Gaowu Qin
Supported Au nanoparticles have been attracting increasing attention due to their unique catalytic performance. However, their thermal and catalytic stability against sintering and aggregation during preparation and reactions remains a serious issue in practical applications, and what is even more difficult is to solve this mutually exclusive problem by a feasible technique. Here, we propose a simple one-step ultra-low temperature interfacial plasma electrolytic oxidation (ULTPEO) process to successfully prepare sub-10 nm and highly stable Au NPs, supported on a porous MgO layer, with high activity and a long lifespan. The obtained Au NPs, with partially exposed free surfaces, are encapsulated into a porous MgO support film. This unique embedded structure restrains their sintering on the support surface during high temperature treatment even up to 600 °C and shows good thermal stability and excellent recyclability in a model reaction of the hydrogenation of 4-nitrophenol. Moreover, the developed technique allows the facile control of the average size of Au NPs down to ∼3 nm with high monodispersity by liquid nitrogen cooling, and hence a further significant improvement in catalytic activity and the lowest catalytic activation energy of ∼14 kJ mol−1 among the reported literature are obtained. This simple technique is also extended to other metal NP catalysts (e.g. Ru and Pd) that support MgO and exhibit excellent catalytic activity for the hydrolysis of sodium borohydride and oxidation of silanes, respectively.
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JOURNAL OF CHROMATOGRAPHY A
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2019
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IF 3.858
Xiaolan Wang,Xufeng Meng,Qiuhua Wu,Chun Wang,Zhi Wang
A solid phase extraction (SPE) method with a porous organic polymer as adsorbent was established for the extraction of five carbamate pesticides (metolcarb, carbaryl, isoprocarb, bassa and diethofencarb) from milk, white wine and juice samples prior to high performance liquid chromatography-diode array detection. The main factors affecting the SPE were optimized, including sample volume, sample loading rate, sample solution pH, desorption conditions and cartridge reusability. Under the optimal conditions, a good linearity existed in the range from 1.0 to 320.0 ng mL −1 for milk and white wine samples and from 0.5 to 160.0 ng mL −1 for juice sample with the correlation coefficients between 0.9956 and 0.9998. The method recoveries of the carbamates were 82.0%–110.0%. The limits of detection were 0.12-0.40 ng mL -1 for milk and white wine samples, and 0.06-0.20 ng mL −1 for juice sample. The adsorption mechanism of the adsorbent was investigated by the extraction of different types of organic compounds (carbamates, benzoylurea insecticides, endocrine disrupting chemicals and polycyclic aromatic hydrocarbons) with the adsorbent. The results showed that the existence of the hydrogen-bonding between the adsorbent and the analytes is favorable for the adsorption and strong hydrophobicity seems to have an adverse effect.
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ACS Applied Nano Materials
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2019
·
IF 0
Zhuojun Wei,Yangguang Li,Liguang Dou,Muhammad Ahmad,Hui Zhang
A series of bi-transition-metal hybrids Cu3–xNixAl-LDH/rGO (x = 2.5, 2.0, 1.5) were synthesized via a facile preadjusted pH citric-acid-assisted coprecipitation method. Systematic characterizations suggest that the hybrids show honeycomb-like nanosheets array morphology with ultrathin CuNiAl-LDH nanosheets (∼72.3 × 4.2 nm) staggered vertically grown on both sides of rGO substrate. The Cu3–xNixAl-LDH/rGO hybrids present a remarkably superior reduction performance for 4-nitrophenol (4-NP) than pure LDH samples. Particularly, Cu1Ni2Al-LDH/rGO shows the best activity with kapp = 3.4 × 10–2 s–1, ∼1.7-fold of Cu1Ni2Al-LDH. It is worth noting that the activity of this bitransition metals hybrid Cu1Ni2Al-LDH/rGO is 37% higher than our previously reported monotransition metal hybrid Cu1Mg2Al-LDH/rGO (kapp = 2.5× 10–2 s–1). These findings can be ascribed to (1) highly dispersed ultrasmall Cu2O nanoparticles (∼3.8 nm) instantaneously formed via in situ reduction of atomic-level dispersed Cu2+ ions in LDH layer lattices of the Cu3–xNixAl-LDH hybrids beneficial from clear isolation and stabilization effect of Ni–OH; (2) strong promotion of the doping of atomic-level dispersed Ni2+ ions in LDH and possible Cu2O–Ni–OH(CuNiAl-LDH)–rGO three-phase synergistic effect; and (3) enhanced adsorption capacity for reactants upon π–π stacking and the unique honeycomb-like nanosheet array morphology. The series of hybrids exhibit not only excellent reduction properties for varied aromatic nitro compounds but also good decolorization ability for anionic azo dyes. Further fixed bed experiments reveal that Cu1Ni2Al-LDH/rGO can efficiently decolorize the mixed solution of 4-NP and methyl orange at high flow rate (8 mL/min) with TOF of 1.68 × 10–3 s–1, suggesting great application potential of the as-obtained nanosheet array bi-transition-metal hybrids for water remediation.
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INORGANIC CHEMISTRY COMMUNICATIONS
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2019
·
IF 1.795
Tursunjan Aydan,Chao Yang,Yang Xu,Tongtong Yuan,Min Zhang,Hui Li,Xueming Liu,Xintai Su,Jide Wang
A Hybrid magnetic composite material Fe 3 O 4 @Cu x O y /C (where, x = 1–2; y = 0–1) was prepared via pyrolysis of FeOOH decorated Cu 3 (BTC) 2 (where, BTC = 1, 3, 5-benzenetricarboxylic acid) as a precursor. The obtained products was successfully applied to reduction reaction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP) as a catalyst. Compared with other reported materials, Fe 3 O 4 @Cu x O y /C exhibits high catalytic activity with excellent recyclability.
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
·
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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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
·
IF 5.589
Qilu Cheng,Qifa Zhou,Zhuo Jin,Ying Jiang,Ligen Xu,Hui Jiang,Yuhua Zhao
Algal cultures of Dictyosphaerium sp. were treated with a wide range (0–8 mg/L) of nonylphenol (NP) applications to investigate the species' potential to perform bioremediation of NP-contaminated wastewater and explore the mechanism of NP toxicity in algal cell. The algal species exhibited a high tolerance for NP and efficiently removed even high concentrations of NP. The accumulation of NP in algal cells tended to increase and the percentage of NP adhered to the cell walls tended to decrease as the NP concentration increased. The thylakoid density and the pyrenoid size also tended to decrease as the NP concentration rose. The key genes involved in the antioxidative pathways and photosynthetic pathways were down-regulated in the NP-treated algal cells. Algal ribosome genes were especially sensitive to NP. The results indicated that NP could induce oxidative stress in algal cells and that Dictyosphaerium sp. showed potential as a bioremediation agent.
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CHEMOSPHERE
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2019
·
IF 5.108
Liping Lou,Qian Huang,Yiling Lou,Jingrang Lu,Baolan Hu,Qi Lin
To investigate the role of adsorption by biochar and biodegradation by bacteria in the wastewater treatment system of microorganisms immobilized on biochar, Nonylphenol (NP) removal (adsorption + degradation) rates and degradation rates from water by NP degrading bacteria immobilized on bamboo charcoal (BC) and wood charcoal (WC) were examined in a short-term and long-term. Results showed that cells immobilized on different biochar had different NP removal effects, and cells immobilized on bamboo charcoal (I-BC) was better. After eight rounds of long-term reuse, the cumulative removal rate and the degradation rate of NP in water by I-BC were 93.95% and 41.86%, respectively, significantly higher than those of cells immobilized on wood charcoal (69.60%, 22.78%) and free cells (64.79%, 19.49%) (P < 0.01). The rise in the ratio of the degradation rate to the removal rate indicated that the long-term NP removal effect is more dependent on biodegradation. The amount of residual NP in I-BC still accounted for about 50%, indicating that the secondary pollution in the disposal of carrier could not be ignored. In addition, promotion effect of biochar on microorganisms were observed by SEM , quantitative PCR and 16S rRNA. Pseudomonas , Achromobacter , Ochrobactrum and Stenotrophomonas were predominant bacteria for NP degradation. The addition of biochar (especially bamboo charcoal) also effectively delayed the transformation of their community structure.
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CHEMICAL ENGINEERING JOURNAL
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2019
·
IF 8.355
Aitang Zhang,Bingping Liu,Shijie Liu,Meixiu Li,Wen Zheng,Li Deng,Jingquan Liu
To achieve high catalytic activity and stability with low noble-metal loadings on green and natural supports has attracted tremendous attention in the past few years. Herein, a facile strategy is exploited to synthesize Au nanoclusters (with size of ∼1.4 nm) which are homogeneously distributed on carbonized natural lotus leaf sheets with less mass. Compared to the pure AuNCs, the AuNCs@carbonized lotus leaf (AuNCs@C-lotus leaf) micro/nanohybrid with the unique papillae structures and large surface area not only exhibits better catalytic activity for the reduction of 4-nitrophenol (4-NP), but also prevent the aggregation of AuNCs. In addition, the catalytic performance of AuNCs@C-lotus leaf catalyst increased with the temperature increasing of the reaction temperature. Moreover, the AuNCs@C-lotus leaf catalyst can be packed into a filtering platform to fabricate a fixed-bed system, with which the catalytic conversion could reach 71.7% for 0.2 mM 4-NP solution that pass through at flow rate of 1 mL/min. Furthermore, the AuNCs@C-lotus leaf catalyst shows excellent recyclability and only slight loss of catalytical activity is observed after recycling for five successive times. This mild and environmental friendly methodology could be generalized to the synthesis of other metallic nanoparticles@carbonized botanical leaf micro/nanohybrids as promising heterogeneous catalysts for varied catalytic reactions.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2019
·
IF 6.361
Yaowen Bai,Qinzhi Wang,Chunbao Du,Tong Bu,Yingnan Liu,Xinyu Sun,Weifang Luo,Rui Li,Yijian Zhao,Xiaohan Zheng,Li Wang
Developing a facile method to fabricate new heterogeneous Metal-Organic Framework (MOFs) based catalysts with high catalytic activity and stability has drawn significant attention. Herein, we demonstrate a simple in-situ pyrolysis reduction strategy to fabricate a novel three-dimensional (3D) Cu-based catalyst, which displays an outstanding performance for the decomposition of 4-nitrophenol (4-NP). Detailed characterization including SEM , FTIR, XPS , ICP-OES, HRTEM , SAED , XRD and BET confirmed the formation of the Cu/C porous composites (Cu/C-PC). Taking advantage of enormous Cu particles in the composite as well as ultrahigh surface area (196.7 m 2 /g) of carbon support, Cu/C-PC presents prominent catalytic activity for the hydrogenation reduction 4-NP to 4-aminophenol (4-AP) with apparent rate constant ( K app ) of 0.0267 s −1 (the ratio of K app to the catalyst amount is 119 s −1 g −1 ), which is dramatically higher than that previous reports. On the contrary, after being washed successively (Cu/C-PC-AW) by FeCl 3 , HCl aqueous solution and deionized water , the Cu/C porous composite materials exhibit fairly weak catalytic activity. The catalytic performance of Cu/C-PC is better than Cu, Cu 2 O and CuO nanoparticles as well as other catalysts in previous reports. Furthermore, Cu/C-PC shows excellent reusability, indicating its potential applications in treatment of water pollution.
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Polymer Chemistry
·
2019
·Vol. 10
·期 33
·4537-4550
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IF 4.76
Yu Yang,Haixun Ji,Haichao Duan,Yuqin Fu,Siwen Xia,Changli Lü
In this work, catechol-formaldehyde resin (CFR) microspheres were successfully prepared by a solvothermal method under alkaline conditions. Furthermore, the impacts of the concentration, solvent ratio and temperature on the size and morphology of the as-synthesized CFR microspheres were studied in detail. The results showed that the size of the CFR microspheres could be controlled between 50 and 800 nm by changing the reaction conditions, and the morphology of the CFR microspheres was significantly different under different conditions. The as-prepared CFR microsphere as a support was also used to construct a CFR-stabilized Ag nanoparticle (CFR@Ag) nanohybrid via an in situ reduction and growth process on mussel-inspired CFR layers. Upon alkaline solution treatment on the CFR microspheres, silver nanoparticles could be deposited onto the surface or inside of the CFR microspheres. Additionally, the abundant hydroxyl groups on the CFR spheres could act as reducing agents for both the Ag+ precursor and ligands to stabilize Ag NPs without additional reducing agents. The as-prepared CFR@Ag and alkali-treated CFR microsphere stabilized Ag NP (TCFR@Ag) nanohybrids could serve as highly efficient nanocatalysts for the reduction of 4-nitrophenol and methylene blue (MB) dye with good cycling stability. In addition, the nanohybrids as outstanding antibacterial agents also showed long-term inhibition of microbial growth against bacteria Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus).
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CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Zhiqiang Sun,Lei Zhao,Caihong Liu,Yufei Zhen,Jun Ma
In this study, a high capacity ( q m = 1351 mg g −1 ) with fast adsorption process (t < 5 min) towards bisphenol A (BPA) from water was achieved by an in-situ sp 2 C dominant N-doped carbon (polydopamine-carbon, PDA-C). The adsorption mechanism facilitating to the superior removal performance of PDA-C was systematically investigated by relationship study (adsorption capacity VS physiochemical property) and theoretical calculation. It could be concluded that the dominant sp 2 C ( I D /I G = 0.92–1.02) and N-heteroatom (2.26–5.09 at. %) in PDA-C contributed to enhancing the adsorptive interactions of π-π electron donor-acceptor and hydrophobic effect between the PDA-C and BPA, thus realized a ~1.8 times enhancement of q m in comparison with the conventional carbon (PRF-C). Calculated adsorption energy from the density functional theory (DFT) further demonstrated that the adsorption potential of N-doped carbon towards BPA increased linearly with increasing doping of N-heteroatom, especially for the pyridinic N which determined the hydrophobic effect of carbon. This finding firstly points out the dominant strengthening mechanism of N-heteroatom for carbonaceous adsorbent. The synthesized PDA-C showed a promising environmental application potential as revealed from the stable BPA adsorption efficiency in the interferences (H + /OH − , NaCl and HA), dynamic adsorption operation and multiple cycling test.
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