CELLULOSE
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2019
·Vol. 26
·期 11
·6813-6823
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IF 3.917
Li Shusheng,Yang Shanshan,Zhu Xiaoli,Jiang Xubao,Kong Xiang Zheng
Owing to the increasing amount of industrial wastewater and ocean pollution, separation of water and oil from their mixtures and emulsions has been an active area in water treatment industry and in academic research. Using cellulose filter paper as the substrate, a porous superoleophobic membrane (OP) was easily prepared by immersing the paper in an acetonitrile solution of toluene diisocyanate and that of N -(2,4-diaminophenyl) maleimide, alternatively and repeatedly, coating the paper with maleimide-containing polyurea (PU). PU coated paper was then functionalized by 2-[(tris(hydroxymethyl)methyl)amino]-1-ethanesulfonic acid through aza-Michael addition. The formation of PU coating and the subsequent functionalization were confirmed by FTIR, NMR and XPS analyses. The produced OP paper was shown to be superoleophobic and had excellent performance for oil–water separation from their mixtures and emulsions. This study provides therefore a novel protocol for preparation of superoleophobic materials, featuring easy operation, low cost, and in particular, versatile applicability to different natural and synthetic materials.
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SCIENCE OF THE TOTAL ENVIRONMENT
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2019
·
IF 5.589
Cong Lyu,Dan He,Yuming Chang,Qihui Zhang,Fang Wen,Xiansheng Wang
The persulfate/Fe 2+ system has been proposed for the chemical oxidation for soil remediation , however, the homogeneous iron catalyst was hard to reuse which limited the further application. Cobalt oxyhydroxide (CoOOH) existed as a mineral in nature, which was environmentally friendly. Thus, in this study, CoOOH was selected as an efficient heterogeneous catalyst for peroxymonosulfate (PMS) activation to remediate oil contaminated soil by chemical oxidized reaction. 88.3% of oil at the initial concentration of 78–99 mg/kg can be removed within 24 h under the conditions of 1.0 g/L CoOOH and 0.1 M PMS at room temperature. The residual oil content was approximately 11.5 mg/kg which was lower than the standard of petroleum hydrocarbons for residential land (30 mg/kg), published by the Canadian Council of Ministers of the Environment (CCME). Specifically, the PMS/CoOOH system had a relatively high apparent reaction rate constant (0.3078 h −1 ), which was approximately twice that of the PS/Fe 2+ system (0.1601 h −1 ). Furthermore, multiple radicals and reactive oxygen species (ROS), such as SO 4 − , O 2 − and 1 O 2 , were involved in the oil removal oxidation reaction. Moreover, 73% total organic carbon (TOC) had been removed after the reaction. The findings of this study suggested that the oil-contaminated soil and CoOOH could both be recycled after remediation using the PMS/CoOOH system. In summary, the results indicated that CoOOH is a promising heterogeneous catalyst, and the PMS/CoOOH system could be considered as a feasible alternative to the PS/Fe 2+ system for the remediation of oil-contaminated soil.
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Energy Storage Materials
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2019
·
IF 0
Tao Dai,Lie Yang,Xiaohui Ning,Danli Zhang,R. Lakshmi Narayan,Ju Li,Zhiwei Shan
Due to their compactness, storage/supply flexibility, modularity and factory manufacturability, batteries are excellent candidates for large scale energy storage applications . However, the widespread application of most batteries hitherto developed is hindered by their high cost. Here, an intermediate temperature molten salt battery is developed that emphatically resolves this issue by using all earth-abundant and cheap elements. Operated at 170 °C, the cell comprises of an Fe metal anode, NaCl saturated NaAlCl 4 electrolyte and an AlCl 4 − intercalated graphite cathode in the fully charged state. It has a capacity retention of 85% after nearly 10,000 cycles. After characterizing the anode, it was determined that the high reversibility of the Fe to FeCl 2 solid state transformation are responsible for the absence of dendritic growth on such a metal anode. Different electrode capacity matching strategies are discussed in the context of ensuring safe operation during overcharging. Finally, the overall material cost of the Fe/Graphite cell is estimated to be 33.9 $ kWh −1 , which can potentially meet the demands of the commercial energy storage market.
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ANALYTICA CHIMICA ACTA
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2019
·
IF 5.256
Zhongtang Wang,Zhaoya Huang,Yun Xie,Zhaoyi Tan
Plutonium has been extensively studied in the environment, for the purpose of radiological assessment, environmental behavior study and nuclear emergency response. To determine Pu isotopes in environmental soil and sediment, a novel analytical method was established in this study using a new type of extraction resin, TK200 resin. Firstly an investigation was performed to study the extraction behaviors of Pu, U, Th, Hg, Tl, Pb, Bi and Hf on TK200 resin. On the basis of the results, a new chromatographic procedure was then proposed to separate Pu from the elements that interfere the accurate determination of Pu isotopes by mass spectrometry. Owing to the excellent separation efficiency between Pu and interfering elements (IEs) of the developed procedure, high decontamination factors (DFs) were obtained for IEs, e.g. the DF(U) (>7.5 × 10 7 ) was the highest reported value. The separation procedure was finally combined with HNO 3 leaching, CaF 2 /LaF 3 coprecipitation and sector field-inductively coupled plasma mass spectrometry (SF-ICPMS) measurement to establish a complete method. The established method was evaluated by analyzing four standard reference materials (soil, sediment), and the results showed that both 239+240 Pu activity and 240 Pu/ 239 Pu isotopic ratio were accurately determined, with stable and high Pu chemical recoveries (81–91%). The whole analytical method only took about 15 h, and the limits of detection were calculated to be 0.13–0.24 fg g −1 for Pu isotopes (for 2 g soil or sediment), guaranteeing the rapid determination of ultra-trace level Pu in soil and sediment samples.
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ELECTROANALYSIS
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2018
·Vol. 30
·期 11
·2768-2773
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IF 2.851
Xin Feng,Xiaomei Dong,Qingcheng Zhang,Cuixia Cui,JingJing Zhang,Zhen Chen,Changmi Wu,Huile Jin,Shun Wang,Jichang Wang
In this study carbon materials with a hierarchical pore structure have been fabricated through a scalable and template free solvothermal method in the presence of metal catalysts, where the presence of metal catalysts was found to be essential for the initial polymerization process. The as-prepared carbon contained trace amounts of metal residues and exhibited highly efficient catalytic activity toward the oxygen reduction reaction (ORR). Among all the metal catalysts studied, cobalt containing porous carbon exhibited the highest ORR electrocatalytic activity with great tolerance to methanol crossover and excellent long-term cycling stability, outperforming the commercial 30 % ( w / w ) Pt/C catalysts. The great performance may be contributed to the unique porous structure, the large specific surface area of cobalt-doped carbon and chemical activity of cobalt. The result provides useful guidance for the development of carbon-based electrocatalysts.
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WATER RESEARCH
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2018
·
IF 7.051
Zisheng Zhao,Yaobin Zhang,Yang Li,Xie Quan,Zhiqiang Zhao
Anaerobic digestion is one of the most promising technologies to stabilize waste-activated sludge (WAS) and recover energy. However, the low efficiency of anaerobic digestion of WAS constrains its application. Supplementing zero valent iron (ZVI) and Fe 3 O 4 in digesters could improve the sludge digestion performance, which has recently been extensively studied. However, the mechanisms behind this improvement remain unclear. In this study, the effects of ZVI and Fe 3 O 4 on the four stages of anaerobic digestion of WAS (solubilization, hydrolysis, acidification and methanogenesis) were investigated. Results showed that ZVI had only a slight effect on the solubilization , hydrolysis and acidification processes, while ZVI significantly promoted the hydrogenotrophic methanogenesis , increasing methane production by 70%. Further investigation indicated that coenzyme F420 activity in the ZVI added reactor was 32.3% higher than in the blank. These results indicate that ZVI promoted anaerobic digestion of WAS through promoting hydrogenotrophic methanogenesis. On the other hand, Fe 3 O 4 obviously promoted the solubilization, hydrolysis and acidification of sludge. Vast Fe 2+ was detected in the aqueous phase of the Fe 3 O 4 digester which was a result of dissimilatory iron reduction that can utilize complicated matter as a substrate. This was in agreement with the acceleration of the solubilization, hydrolysis and acidification of the sludge. However, the acetoclastic and hydrogenotrophic methanogenesis with Fe 3 O 4 decreased by 27% and 22% compared to the Fe 3 O 4 -free digester, respectively. Further study indicated that Fe 3 O 4 competed with CH 3 ▪S▪CoM for electrons and thus inhibited the methanogenesis process.
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JOURNAL OF HAZARDOUS MATERIALS
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2018
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IF 6.434
Ailin Li,Zihao Wu,Tingting Wang,Shaodong Hou,Bangjie Huang,Xiujuan Kong,Xuchun Li,Yinghong Guan,Rongliang Qiu,Jingyun Fang
The abatement of pharmaceuticals and personal care products (PPCPs), including carbamazepine (CBZ), acetaminophen (ACP) and sulfamethoxazole (SMX), by zero-valent iron (Fe°) activated peroxydisulfate (PDS) system (Fe°/PDS) in pure water and groundwater was investigated. The removal rates of CBZ, ACP and SMX were 85.4%, 100% and 73.1%, respectively, within 10 min by Fe°/PDS in pure water. SO 4 •− , • OH and O 2 •− were identified in the Fe°/PDS system, and O 2 •− was indicated to play an important role in the ACP degradation. The degradation of PPCPs increased with increasing dosages of Fe° and PDS or with decreasing pH and initial PPCP concentrations. Interestingly, the degradation of PPCPs by Fe°/PDS was significantly enhanced in groundwater compared with that in pure water, which was partially attributed to SO 4 2− and Cl − . The first-order constants of CBZ, ACP and SMX increased from 0.021, 0.242 and 0.013 min− 1 to 0.239, 2.536 and 0.259 min −1 , and to 0.172, 1.516 and 0.197 min −1 , respectively, with increasing the concentrations of SO 4 2− and Cl − to 100 mg/L and 10 mg/L, respectively. This study firstly reports the unexpected enhancement of groundwater matrix on the degradation of micropollutants by Fe°/PDS, demonstrating that Fe°/PDS can be an efficient technology for groundwater remediation.
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APPLIED ENERGY
·
2018
·
IF 7.9
Xiaowen Zhang,Rui Zhang,Helei Liu,Hongxia Gao,Zhiwu Liang
To enhance the energy efficiency of the CO 2 desorption process, the regeneration behaviors of the CO 2 -loaded 6 M MEA-AMP-PZ (monoethanolamine, 2-amino-2-methyl-1-propanol and piperazine) tri-solvent blends with different AMP/PZ molar ratios with four different solid acid catalysts (H-ZSM-5, γ-Al 2 O 3 , SAPO-34 and SO 4 2− /TiO 2 ) and a blank at 96 °C were investigated in terms of CO 2 desorption rate, cyclic capacity and relative heat duty. For the no-catalytic runs, the results showed that all the tri-solvent blended amines greatly increased CO 2 desorption rate, cyclic capacity and decreased the relative heat duty in comparison with 5 M MEA. The 13 C NMR analysis indicated that the 3 M MEA-2.5 M AMP-0.5 M PZ blend with the highest AMP/PZ ratio produced the largest amount of bicarbonate and less carbamate, which resulted in the best desorption performance. With regard to catalyst, when the solid acid catalysts were introduced, the regeneration performance of the blend was further improved. The best of the blends along with H-ZSM-5 provided the combination with the best performance in CO 2 desorption, and reduced the relative heat duty by 61.6% as compared to 5 M MEA without catalyst (100%). Five relevant physicochemical properties of the catalyst were obtained and used to better understand the catalytic regeneration process. A possible catalytic CO 2 desorption mechanism was analyzed. The results revealed that the mesopore surface area coupled with total acid sites of the catalyst had the most positive influence on improving the CO 2 desorption performance. Findings from this work imply that the combination of solid acid catalyst with tri-solvent blended amines is a promising alternative method for further reduction of solvent regeneration energy requirement.
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
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2018
·
IF 6.653
Juntao Tang,Jianlong Wang
A novel Fenton-like catalyst, metal organic framework MIL-100(Fe) with FeII/FeIII mixed-valence coordinatively unsaturated iron center (CUS-MIL-100(Fe)), was synthesized, characterized, and used for the degradation of sulfamethazine (SMT). The catalytic performance of CUS-MIL-100(Fe) was investigated on the basis of various parameters, including initial pH, H2O2 concentration, catalyst dosage, and initial SMT concentration. The results showed that CUS-MIL-100(Fe) could effectively degrade SMT, with almost 100% removal efficiency within 180 min (52.4% mineralization efficiency), under the reaction conditions of pH 4.0, 20 mg L–1 SMT, 6 mM H2O2, and 0.5 g L–1 catalyst. Moreover, CUS-MIL-100(Fe) displayed a higher catalytic activity than that of MIL-100(Fe) for SMT degradation. Combined with the physical–chemical characterization, the enhanced catalytic activity can be ascribed to the incorporation of FeII and FeIII CUSs (coordinatively unsaturated metal sites), the large specific surface area, as well as the formation of mesopores. Furthermore, CUS-MIL-100(Fe) exhibited a good stability and reusability. The possible catalytic mechanism of CUS-MIL-100(Fe) was tentatively proposed.
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CHEMICAL ENGINEERING JOURNAL
·
2018
·
IF 6.735
Yang Wu,Lifeng Lin,Fidèle Suanon,Anyi Hu,Ya-Nan Sun,Zhi-Min Yu,Chang-Ping Yu,Qian Sun
The aim of this study was to quantify the removal of halogenated pollutants (using triclosan as a model pollutant) from aqueous solution by zero-valent iron coupled with a weak magnetic field. We determined the removal efficiency of triclosan from a sodium sulfate solution at different pH values under both aerobic and anaerobic conditions. The removal of triclosan followed pseudo-first-order kinetics in both the presence and absence of a weak magnetic field. The calculated rate constants indicated higher removal efficiencies of triclosan under the aerobic condition compared to the anaerobic condition. In addition, increase of triclosan removal from acidic solutions was achieved with the assistance of weak magnetic field. X-ray diffraction and X-ray photoelectron spectroscopy analysis indicated that FeO(OH) and Fe 3 O 4 were the main aerobic transformation products, suggesting that the zero-valent iron surfaces were completely oxidized. The aerobic and anaerobic transformation products of triclosan were analyzed by liquid chromatography tandem mass spectrometry. The results indicated that the application of a weak magnetic field could be an efficient and cheap treatment process to improve the removal of halogenated pollutants by zero-valent iron, which may be developed for future use.
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RSC Advances
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2018
·Vol. 8
·期 48
·27181-27190
·
IF 2.936
Yayi Wang,Duanli Wang,Huiying Fang
The feasibility of adding nano-zero valent iron (NZVI: 0.6, 1.0, 4.0, 10.0 g L−1) to enhance anaerobic digestion of waste activated sludge (WAS) was examined by comparison with ZVI, and the mechanisms of NZVI enhancement of the hydrolysis and methanogenesis processes were elucidated. NZVI could enhance hydrolysis–acidification of WAS by destroying the integrity of microbial cells. Both volatile fatty acids production and the acetic acid portion were greatly improved by NZVI additions, peaking at 4.0 g L−1 NZVI. In anaerobic digestion, CH4 production was promoted at a NZVI dosage ≤1.0 g L−1. The optimum dosage of NZVI for methanogenesis was 1.0 g L−1, and further addition of NZVI could cause inhibition of methanogenesis because of long-term accumulation of H2. ZVI could also improve hydrolysis–acidification and the CH4 yield, but its efficiency was relatively low compared with NZVI, and it could not induce cell wall rupture. 16S rDNA high-throughput sequencing results showed that NZVI addition at appropriate dosage facilitated increasing the proportion of microorganisms involved in WAS hydrolysis–acidification and methanogenesis.
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APPLIED CATALYSIS B-ENVIRONMENTAL
·
2018
·
IF 11.698
Ying Lü,Jianfa Li,Yimin Li,Liping Liang,Huaping Dong,Kun Chen,Chunxia Yao,Zhanfeng Li,Jinxiang Li,Xiaohong Guan
Zero-valent iron (ZVI) is a popular reductant that has been successfully applied for remediation of groundwater contaminated with various pollutants, but it still suffers from surface passivation and pH increase in the reaction media. In this study, pyrite, a ubiquitous sulfide mineral in anaerobic environment, was adopted to enhance the reactivity of ZVI for removal of nitrobenzene. The synergetic effect between pyrite and ZVI was observed for nitrobenzene reduction, and the rate constant k obs at the initial pH (pH 0 ) 6.0 was enhanced by 8.55–23.1 folds due to the presence of pyrite with pyrite/ZVI mass ratio ranging from 1.0 to 6.0. Moreover, nitrobenzene could be removed effectively at pH 0 ranging from 5.0 to 10.0 in the presence of pyrite, while negligible removal of nitrobenzene by ZVI (0.5 g/L) alone was observed at pH 0 ≥7.0. ZVI sample recovered from the reacted ZVI/pyrite mixture was also more effective for nitrobenzene degradation than pristine ZVI. The mechanism study revealed that pyrite could suppress the pH increase in reaction media, boost the production of reactive Fe 2+ , and activate the ZVI surface through replacing partially the passive oxide film with iron sulfide (FeS). In particular, the formation of highly reactive FeS@Fe in the reaction system of ZVI/pyrite mixture was proved by XRD, Mössbauer, XANES, XPS and SEM-EDS analyses, which provides a facile way for in-situ sulfidation of ZVI and for enhancing the removal of contaminants with ZVI technology.
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