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Removing polybrominated diphenyl ethers in pure water using Fe/Pd bimetallic nanoparticles

Min ZHANG,Jian LU,Zhencheng XU,Yiliang HE,Bo ZHANG,Song JIN,Brian BOMAN

《环境科学与工程前沿(英文)》 2015年 第9卷 第5期   页码 832-839 doi: 10.1007/s11783-015-0778-x

摘要: Polybrominated diphenyl ethers (PBDEs) have been widely used as fire-retardants. Due to their high production volume, widespread usage, and environmental persistence, PBDEs have become ubiquitous contaminants in various environments.Nanoscale zero-valent iron (ZVI) is an effective reductant for many halogenated organic compounds. To enhance the degradation efficiency, ZVI/Palladium bimetallic nanoparticles (nZVI/Pd) were synthesized in this study to degrade decabromodiphenyl ether (BDE209) in water. Approximately 90% of BDE209 was rapidly removed by nZVI/Pd within 80 min, whereas about 25% of BDE209 was removed by nZVI. Degradation of BDE209 by nZVI/Pd fits pseudo-first-order kinetics. An increase in pH led to sharply decrease the rate of BDE209 degradation. The degradation rate constant in the treatment with initial pH at 9.0 was more than 6.8 × higher than that under pH 5.0. The degradation intermediates of BDE209 by nZVI/Pd were identified and the degradation pathways were hypothesized. Results from this study suggest that nZVI/Pd may be an effective tool for treating polybrominated diphenyl ethers (PBDEs) in water.

关键词: degradation     bimetallic nanoparticles     nanoscale zero-valent iron     polybrominated diphenyl ethers    

Photocatalytic degradation of polybrominated diphenyl ethers in pure water system

Min ZHANG,Jian LU,Yiliang HE,P Chris WILSON

《环境科学与工程前沿(英文)》 2016年 第10卷 第2期   页码 229-235 doi: 10.1007/s11783-014-0762-x

摘要: Due to the low water solubility of polybrominated diphenyl ethers, organic solvent is usually added into the oxidation system to enhance the removal efficiency. In this study the photocatalytic degradation of decabromodiphenyl ether (BDE209), a type of polybrominated diphenyl ether used throughout the world, in pure water without the addition of organic solvent was investigated. In the pure water system, BDE209 was not dissolved but dispersed as nano-scale particles with a mean diameter of 166 nm. Most of BDE209 (>98%) were removed within 4 h and the final debromination ratio was greater than 80%. Although the addition of organic solvent (tetrahydrofuran, THF) could lead to a relatively high BDE209 degradation rate, the final debromination ratio (<50%) was much lower than that in pure water system. Major oxidation intermediates of tetrahydrofuran, including tetrahydro-2-furanol and γ-butyrolactone, were detected indicating the engagement of THF in the BDE209 degradation process. The photocatalytic degradation of BDE209 in the pure water system followed first-order kinetics. The BDE209 degradation rate constant increased from 0.0011 to 0.0023 min as the pH increased from 3 to 9.

关键词: polybrominated diphenyl ethers     photocatalytic degradation     solvent    

Legacies and health risks of heavy metals, polybrominated diphenyl ethers, and polychlorinated dibenzo-dioxins

《环境科学与工程前沿(英文)》 2023年 第17卷 第7期 doi: 10.1007/s11783-023-1679-z

摘要:

● Heavy metals and organic toxins may persist in legacy sites for a long time.

关键词: E-waste     Human health risk     Organ risk     Heavy metal toxicity     PBDE     PCDD/F    

Joint effects of Penta-BDE and heavy metals on

Baohua TANG, Lingyan ZHU, Qixing ZHOU

《环境科学与工程前沿(英文)》 2011年 第5卷 第1期   页码 99-110 doi: 10.1007/s11783-010-0260-8

摘要: The joint toxicity of Penta-BDE (Pe-BDE) and heavy metals including cadmium and copper on ( ) was evaluated on the basis of determining the 48 h survival, antioxidative enzyme responses, and lipid peroxidation. The response was classified as additive, greater than additive, or less than additive by comparing the measured “toxic units, TU” with one. Based on the survival of , less-than-additive interactions were found in most of mixtures treatments. This may be attributed to the different toxicity mechanism between Pe-BDE and metals. Cu and Cd played a greater role in toxicity than what Pe-BDE did. As for the superoxide dismutase (SOD) and catalase (CAT) activity, most response was less than additive. For the glutathione -transferases (GST) activity, most of the greater-than-additive responses were found in the Cu plus Pe-BDE treatments, but the additive responses occurred in Cd plus Pe-BDE treatments and binary metal treatments. For lipid peroxide levels, which were measured as malondialdehyde (MDA) levels, less-than-additive response occurred in the 50% Cd plus 50% Cu and ternary mixture treatments. Results suggested that Pe-BDE, Cd, and Cu could induce different patterns of antioxidant enzyme responses, such as antioxidant/prooxidant responses, depending on their capability to produce reactive oxygen species and antioxidant enzymes to detoxify them.

关键词: polybrominated diphenyl ethers (PBDEs)     heavy metal     mixture toxicity     toxic units (TUs)     antioxidant enzyme     lipid peroxidation    

Solvent-resistant porous membranes using poly(etherether ketone): preparation and application

《化学科学与工程前沿(英文)》 2023年 第17卷 第10期   页码 1536-1559 doi: 10.1007/s11705-022-2221-8

摘要: Poly(ether−ether ketone) (PEEK) is a linear aromatic macromolecule, which can form semi-crystalline aggregative status, allowing PEEK materials to have strong environment tolerance and excellent physicochemical properties. PEEK materials have become a promising alternative to fabricate particular membranes used in extreme conditions. In the past few decades, many researches and evolutions have emerged in membrane fabrication with PEEK materials and its applications for treating organic solvents and their mixtures; however, there are little systematic and comprehensive literature to summarize fabrication approaches, compile applications, and elaborate PEEK property-structure relationship. In this review, the main approaches to fabricate PEEK-based membranes are illustrated concretely, including conventional thermal-induced and non-solvent-induced phase separation, and novel chemical-induced crystallization; the representative applications in ultrafiltration, nanofiltration and membrane contactor containing organic solvents are demonstrated systematically. Meanwhile, the mechanism to tune PEEK solubility in solvents, which can be achieved by altering monomers in synthesis processes or changing membrane preparation routes, is deeply analyzed. Moreover, the existing problems and the future prospects are also discussed. This review provides positive guidance for designing and fabricating membranes using PEEK and its derivative materials for task-specific applications in harsh conditions.

关键词: PEEK     phase inversion     solvent-resistant membrane     nanofiltration     membrane contactor    

Sulfonated poly(ether ether ketone)/zirconium tricarboxybutylphosphonate composite proton-exchange membranes

GAO Qijun, HUANG Mianyan, WANG Yuxin, CAI Yuquan, XU Li

《化学科学与工程前沿(英文)》 2008年 第2卷 第1期   页码 95-101 doi: 10.1007/s11705-008-0012-5

摘要: Sulfonated poly(ether ether ketone) (SPEEK) is a very promising alternative membrane material for direct methanol fuel cells. However, with a fairly high degree of sulfonation (DS), SPEEK membranes can swell excessively and even dissolve at high temperature. This restricts membranes from working above a high tolerable temperature to get high proton conductivity. To deal with this contradictory situation, insolvable zirconium tricarboxybutylphosphonate (Zr(PBTC)) powder was employed to make a composite with SPEEK polymer in an attempt to improve temperature tolerance of the membranes. SPEEK/Zr(PBTC) composite membranes were obtained by casting a homogeneous mixture of Zr(PBTC) and SPEEK in N,N-dimethylacetamide on a glass plate and then evaporating the solvent at 60°C. Many characteristics were investigated, including thermal stability, liquid uptake, methanol permeability and proton conductivity. Results showed significant improvement not only in temperature tolerance, but also in methanol resistance of the SPEEK/Zr(PBTC) composite membranes. The membranes containing 30 wt-% ∼ 40 wt-% of Zr(PBTC) had their methanol permeability around 10 cm·s at room temperature to 80°C, which was one order of magnitude lower than that of Nafion115. High proton conductivity of the composite membranes, however, could also be achieved from higher temperature applied. At 100% relative humidity, above 90°C the conductivity of the composite membrane containing 40 wt-% of Zr(PBTC) exceeded that of the Nafion115 membrane and even reached a high value of 0.36 S·cm at 160°C. Improved applicable temperature and high conductivity of the composite membrane indicated its promising application in DMFC operations at high temperature.

关键词: homogeneous mixture     PBTC     zirconium tricarboxybutylphosphonate     Nafion115     DMFC    

Synthesis and fluorescence behavior of 2,5-diphenyl-1,3,4-oxadiazole-containing bismaleimides and bissuccinimides

Xin ZHANG, Zichen LI

《化学科学与工程前沿(英文)》 2013年 第7卷 第4期   页码 381-387 doi: 10.1007/s11705-013-1359-9

摘要: Bismaleimides bearing 2,5-diphenyl-1,3,4-oxadiazole chromophores at , , position and corresponding saturated bissuccinimides were synthesized. Several synthetic strategies for these bismaleimides were discussed in detail. Almost no or very weak fluorescence was observed for these bismaleimides, however, the bissuccinimides show a strong fluorescence. The effect of molecular geometry on optical behavior and fluorescence quenching mechanism were investigated by UV-vis absorption and fluorescence emission spectroscopy. The electron coupling of ground state of -bismaleimide is stronger than those of - and -bismaleimides. -Bissuccinimide displays increasing fluorescence quantum yields with red shifts of 22–24 nm, compared to -bissuccinimide. Polymerizable C=C bonds play a key role in the intramolecular fluorescence quenching.

关键词: fluorescence     bismaleimide     oxadiazole     succinimide    

Biomass to dimethyl ether by gasification/synthesis technology

Tiejun WANG, Yuping LI, Longlong MA, Chuangzhi WU

《能源前沿(英文)》 2011年 第5卷 第3期   页码 330-339 doi: 10.1007/s11708-010-0121-y

摘要: Technical and economic analysis was done for the biomass to dimethyl ether (DME) technology to promote the gasification/synthesis route for biofuel production and its application as a fossil fuel substitute. The technology of biomass gasification/synthesis has obvious advantages, including production flexibility, environmental friendliness, economic feasibility, and application versatility. Biomass gasification/synthesis technology integrates bio-DME synthesis, fertilizer production, electricity generation, and waste heat utilization to convert waste biomass residues to DME for use as liquid petroleum gas, transportation fuel substitute, and chemical intermediates, which has been proven to be one of the most effective and clean biomass utilization routes. The 1000 t/a-scale demonstration plant has a bio-DME production rate of 6 to 7 / , biomass gasification efficiency of≥82%, once-through CO conversion of ≥70%, DME selectivity (DME/DME+other organic products) of ≥90%, and a total system efficiency of ≥38%. The demonstration plant also has self-sufficient steam and electricity supply. The 10,000tons/a-scale bio-DME production cost with or without feedstock subsidy is estimated to be 1968 Yuan/t and 2868 Yuan/t, respectively in China. Because of the limitation in biomass feedstock collection cost, massive and disperse commercial plants with a capacity of 10000 t/a bio-DME are more suitable for rural areas.

关键词: technical and economic analysis     biomass     dimethyl ether     gasification/synthesis    

Direct synthesis of diphenyl carbonate over heterogeneous catalyst: effects of structure of substituted

WU Guangwen, JIN Fang, WU Yuxin, ZHANG Guangxu, LI Dinghuo, WANG Cunwen, MA Peisheng

《化学科学与工程前沿(英文)》 2007年 第1卷 第1期   页码 59-64 doi: 10.1007/s11705-007-0012-x

摘要: The perovskite-type compound LaMnO was substituted for the part of La in position A and for the part of Mn in position B by citrate method. The phases were detected by X-ray diffraction. Powder morphologies were scanned by scanning electron microscopy. The valence of atoms was determined by X-ray photoelectron spectroscopy. It was found that the perovskite can form crystal defect and increase the proportion of high valence B element by doping. Active component Pd was loaded on various perovskite supports for synthesis of diphenyl carbonate. The results showed that the activities of catalysts in which supports have crystal defect by substitution were higher. It can be concluded that perovskite with defect structure by doping could lead to the formation of oxygen vacancy where the lattice oxygen became exchangeable with the oxygen gas. Also, this improved the redox process of the carrier by transferring electrons and activities of catalysts.

关键词: photoelectron spectroscopy     diphenyl carbonate     proportion     diffraction     perovskite    

Dimethyl ether as alternative fuel for CI engine and vehicle

Zhen HUANG , Xinqi QIAO , Wugao ZHANG , Junhua WU , Junjun ZHANG ,

《能源前沿(英文)》 2009年 第3卷 第1期   页码 99-108 doi: 10.1007/s11708-009-0013-1

摘要: As a developing and the most populous country in the world, China faces major challenges in energy supply and environmental protection. It is of great importance to develop clean and alternative fuels for internal combustion engines. On the basis of researches on DME engine and vehicle at Shanghai Jiaotong University in the last twelve years, fuel injection, combustion, performance and exhaust emissions of DME engine and DME vehicle are introduced in this paper. The results indicate that DME engines can achieve high thermal efficiency and ultra low emissions, and will play a significant role in meeting the energy demand while minimizing environmental impact in China.

关键词: dimethyl ether (DME)     fuel injection     combustion process     emission control     CI engine     vehicle    

Study on direct alcohol/ether fuel synthesis process in bubble column slurry reactor

Zhen CHEN, Haitao ZHANG, Weiyong YING, Dingye FANG

《化学科学与工程前沿(英文)》 2010年 第4卷 第4期   页码 461-471 doi: 10.1007/s11705-010-0517-6

摘要: The recent studies of direct alcohol/ether synthesis process in slurry reactors were reviewed, and the research work in our laboratory was carried out in this paper. a global kinetics model for direct dimethyl ether (DME) synthesis from syngas over a novel Cu-Zn-Al-Zr slurry catalyst was established according to the total of 25 experimental data, and a steady-state one-dimensional mathematical model was further developed in bubble column slurry reactor (BCSR), which was assumed that the bubble phase was plug flow, and the liquid phase was fully mixed flow. The numerical simulations of reactor design of 100000 t/a dimethyl ether pilot plant indicate that higher pressure and lower temperature were favorable to the increase of CO conversion, selectivity of dimethyl ether, product yield and height of slurry bed. The optimal operating conditions for DME synthesis process were obtained: reaction temperature at 240°C, reactor pressure at 5 MPa and reactor diameter of 2.5 m.

关键词: syngas     alcohol/ether fuel     slurry catalyst     bubble column slurry reactor     global kinetics     mathematical model    

85 nmUV降解水中二苯甲酮和孔雀石绿的动力学研究

闻瑞梅,葛伟伟

《中国工程科学》 2007年 第9卷 第9期   页码 40-46

摘要:

研究了185 nmUV降解水中 二苯甲酮和孔雀石绿的动力学,主要 包括185 nmUV降解水中有机物的动力 学分析,反应速率常数的理论分析, 各种因素如温度、浓度、pH值以及流 速等影响反应速率常数的因素分析, 并建立化学反应动力学方程;讨论185 nmUV降解水中的二苯甲酮和孔雀石绿的 动力学规律;从理论和实验讨论185 nmUV 降解水中的二苯甲酮和孔雀石绿是符合准 一级动力学规律。

关键词:     185 nmUV     二苯甲酮     孔雀石绿     动力学    

Enhanced debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) by zero-valent zinc with ascorbic

Chaojin Jiang, Xiaoqian Jiang, Lixun Zhang, Yuntao Guan

《环境科学与工程前沿(英文)》 2020年 第14卷 第3期 doi: 10.1007/s11783-020-1224-2

摘要: Highly efficient debromination of BDE-47 was achieved in the ZVZ/AA system. BDE-47 debromination by the ZVZ/AA can be applied to a wide range of pH. AA inhibits the formation of (hydr)oxide and accelerates the corrosion of ZVZ. Reduction mechanism of BDE-47 debromination by the ZVZ/AA system was proposed. A new technique of zero-valent zinc coupled with ascorbic acid (ZVZ/AA) was developed and applied to debrominate the 2,2′,4,4′-Tetrabromodiphenyl ether (BDE-47), which achieved high conversion and rapid debromination of BDE-47 to less- or non-toxic forms. The reaction conditions were optimized by the addition of 100 mg/L ZVZ particles and 3 mmol/L AA at original solution pH= 4.00 using the solvent of methanol/H2O (v:v= 4:6), which could convert approximately 94% of 5 mg/L BDE-47 into lower-brominated diphenyl ethers within a 90 min at the ZVZ/AA system. The high debromination of BDE-47 was mainly attributed to the effect of AA that inhibits the formation of Zn(II)(hydr)oxide passivation layers and promotes the corrosion of ZVZ, which leads to increase the reactivity of ZVZ. Additionally, ion chromatography and gas chromatography mass spectrometry analyses revealed that bromine ion and lower-debromination diphenyl ethers formed during the reduction of BDE-47. Furthermore, based on the generation of the intermediates products, and its concentration changes over time, it was proposed that the dominant pathway for conversion of BDE-47 was sequential debromination and the final products were diphenyl ethers. These results suggested that the ZVZ/AA system has the potential for highly efficient debromination of BDE-47 from wastewater.

关键词: 2     2′     4     4′-tetrabromodiphenyl ether (BDE-47)     Ascorbic acid     Reductive debromination     Zero-valent zinc    

Exergy losses in premixed flames of dimethyl ether and hydrogen blends

Tongbin ZHAO, Jiabo ZHANG, Dehao JU, Zhen HUANG, Dong HAN

《能源前沿(英文)》 2019年 第13卷 第4期   页码 658-666 doi: 10.1007/s11708-019-0645-8

摘要: A second-law thermodynamic analysis was conducted for stoichiometric premixed dimethyl ether (DME)/hydrogen (H )/air flames at atmospheric pressure. The exergy losses from the irreversibility sources, i.e., chemical reaction, heat conduction and species diffusion, and those from partial combustion products were analyzed in the flames with changed fuel blends. It is observed that, regardless of the fuel blends, chemical reaction contributes most to the exergy losses, followed by incomplete combustion, and heat conduction, while mass diffusion has the least contribution to exergy loss. The results also indicate that increased H substitution decreases the exergy losses from reactions, conduction, and diffusion, primarily because of the flame thickness reduction at elevated H substitution. The decreases in exergy losses by chemical reactions and heat conduction are higher, but the exergy loss reduction by diffusion is slight. However, the exergy losses from incomplete combustion increase with H substitution, because the fractions of the unburned fuels and combustion intermediates, e.g., H and OH radical, increase. The overall exergy losses in the DME/H flames decrease by about 5% with increased H substitution from 0% to 100%.

关键词: second law analysis     flame     dimethyl ether (DME)     hydrogen     binary fuels    

Removal of decabromodiphenyl ether (BDE-209) by sepiolite-supported nanoscale zerovalent iron

Rongbing FU,Na MU,Xiaopin GUO,Zhen XU,Dongsu BI

《环境科学与工程前沿(英文)》 2015年 第9卷 第5期   页码 867-878 doi: 10.1007/s11783-015-0800-3

摘要: Nanoscale zerovalent iron (nZVI) synthesized using sepiolite as a supporter was used to investigate the removal kinetics and mechanisms of decabromodiphenyl ether (BDE-209). BDE-209 was rapidly removed by the prepared sepiolite-supported nZVI with a reaction rate that was 5 times greater than that of the conventionally prepared nZVI because of its high surface area and reactivity. The degradation of BDE-209 occurred in a stepwise debromination manner, which followed pseudo-first-order kinetics. The removal efficiency of BDE-209 increased with increasing dosage of sepiolite-supported nZVI particles and decreasing pH, and the efficiency decreased with increasing initial BDE-209 concentrations. The presence of tetrahydrofuran (THF) as a cosolvent at certain volume fractions in water influenced the degradation rate of sepiolite-supported nZVI. Debromination pathways of BDE-209 with sepiolite-supported nZVI were proposed based on the identified reaction intermediates, which ranged from nona- to mono-brominated diphenylethers (BDEs) under acidic conditions and nona- to penta-BDEs under alkaline conditions. Adsorption on sepiolite-supported nZVI particles also played a role in the removal of BDE-209. Our findings indicate that the particles have potential applications in removing environmental pollutants, such as halogenated organic contaminants.

关键词: sepiolite-supported nanoscale zerovalent iron     decabromodiphenyl ether     debromination     adsorption     mechanism    

标题 作者 时间 类型 操作

Removing polybrominated diphenyl ethers in pure water using Fe/Pd bimetallic nanoparticles

Min ZHANG,Jian LU,Zhencheng XU,Yiliang HE,Bo ZHANG,Song JIN,Brian BOMAN

期刊论文

Photocatalytic degradation of polybrominated diphenyl ethers in pure water system

Min ZHANG,Jian LU,Yiliang HE,P Chris WILSON

期刊论文

Legacies and health risks of heavy metals, polybrominated diphenyl ethers, and polychlorinated dibenzo-dioxins

期刊论文

Joint effects of Penta-BDE and heavy metals on

Baohua TANG, Lingyan ZHU, Qixing ZHOU

期刊论文

Solvent-resistant porous membranes using poly(etherether ketone): preparation and application

期刊论文

Sulfonated poly(ether ether ketone)/zirconium tricarboxybutylphosphonate composite proton-exchange membranes

GAO Qijun, HUANG Mianyan, WANG Yuxin, CAI Yuquan, XU Li

期刊论文

Synthesis and fluorescence behavior of 2,5-diphenyl-1,3,4-oxadiazole-containing bismaleimides and bissuccinimides

Xin ZHANG, Zichen LI

期刊论文

Biomass to dimethyl ether by gasification/synthesis technology

Tiejun WANG, Yuping LI, Longlong MA, Chuangzhi WU

期刊论文

Direct synthesis of diphenyl carbonate over heterogeneous catalyst: effects of structure of substituted

WU Guangwen, JIN Fang, WU Yuxin, ZHANG Guangxu, LI Dinghuo, WANG Cunwen, MA Peisheng

期刊论文

Dimethyl ether as alternative fuel for CI engine and vehicle

Zhen HUANG , Xinqi QIAO , Wugao ZHANG , Junhua WU , Junjun ZHANG ,

期刊论文

Study on direct alcohol/ether fuel synthesis process in bubble column slurry reactor

Zhen CHEN, Haitao ZHANG, Weiyong YING, Dingye FANG

期刊论文

85 nmUV降解水中二苯甲酮和孔雀石绿的动力学研究

闻瑞梅,葛伟伟

期刊论文

Enhanced debromination of 2,2′,4,4′-tetrabromodiphenyl ether (BDE-47) by zero-valent zinc with ascorbic

Chaojin Jiang, Xiaoqian Jiang, Lixun Zhang, Yuntao Guan

期刊论文

Exergy losses in premixed flames of dimethyl ether and hydrogen blends

Tongbin ZHAO, Jiabo ZHANG, Dehao JU, Zhen HUANG, Dong HAN

期刊论文

Removal of decabromodiphenyl ether (BDE-209) by sepiolite-supported nanoscale zerovalent iron

Rongbing FU,Na MU,Xiaopin GUO,Zhen XU,Dongsu BI

期刊论文