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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    

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Electrocatalytic debromination of BDE-47 at palladized graphene electrode

Hongtao YU, Bin MA, Shuo CHEN, Qian ZHAO, Xie QUAN, Shahzad AFZAL

《环境科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 180-187 doi: 10.1007/s11783-013-0552-x

摘要： Graphene electrodes (Ti/Gr) were prepared by depositing Gr sheets on Ti substrate, followed by an annealing process for enhancing the adhesion strength. Electrochemical impedance spectroscopies and X-ray diffraction patterns displayed that the electrochemical behavior of Ti/Gr electrodes can be improved due to the generation of TiO layer at Ti-Gr interface during the annealing process. The palladized Gr electrodes (Ti/Gr/Pd) were prepared by electrochemical depositing Pd nanoparticles on Gr sheets. The debromination ability of Ti/Gr/Pd electrodes was investigated using BDE-47 as a target pollutant with various bias potentials. The results indicated that the BDE-47 degradation rates on Ti/Gr/Pd electrodes increased with the negative bias potentials from 0 V to -0.5 V (vs. SCE). Almost all of the BDE-47 was removed in the debromination reaction on the Ti/Gr/Pd electrode at -0.5 V for 3 h, and the main product was diphenyl ethers, meaning it is promising to debrominate completely using the Ti/Gr/Pd electrode. Although the debromination rate was slightly slower at -0.3 V than that under -0.5 V, the current efficiency at -0.3 V was higher, because the electrical current acted mostly on BDE-47 rather than on water.

关键词： graphene     palladium     debromination     BDE-47    

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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    

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CD47 blockade improves the therapeutic effect of osimertinib in non-small cell lung cancer

《医学前沿（英文）》 2023年 第17卷 第1期   页码 105-118 doi: 10.1007/s11684-022-0934-1

摘要： The third-generation epidermal growth factor receptor (EGFR) inhibitor osimertinib (OSI) has been approved as the first-line treatment for EGFR-mutant non-small cell lung cancer (NSCLC). This study aims to explore a rational combination strategy for enhancing the OSI efficacy. In this study, OSI induced higher CD47 expression, an important anti-phagocytic immune checkpoint, via the NF-κB pathway in EGFR-mutant NSCLC HCC827 and NCI-H1975 cells. The combination treatment of OSI and the anti-CD47 antibody exhibited dramatically increasing phagocytosis in HCC827 and NCI-H1975 cells, which highly relied on the antibody-dependent cellular phagocytosis effect. Consistently, the enhanced phagocytosis index from combination treatment was reversed in CD47 knockout HCC827 cells. Meanwhile, combining the anti-CD47 antibody significantly augmented the anticancer effect of OSI in HCC827 xenograft mice model. Notably, OSI induced the surface exposure of “eat me” signal calreticulin and reduced the expression of immune-inhibitory receptor PD-L1 in cancer cells, which might contribute to the increased phagocytosis on cancer cells pretreated with OSI. In summary, these findings suggest the multidimensional regulation by OSI and encourage the further exploration of combining anti-CD47 antibody with OSI as a new strategy to enhance the anticancer efficacy in EGFR-mutant NSCLC with CD47 activation induced by OSI.

关键词： osimertinib     anti-CD47 antibody     combination strategy     ADCP     EGFR    

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Solvent-resistant porous membranes using poly(ether−ether 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    

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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    

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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    

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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    

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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    

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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    

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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    

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Crown ether-thiourea conjugates as ion transporters

Zhixing Zhao, Bailing Tang, Xiaosheng Yan, Xin Wu, Zhao Li, Philip A. Gale, Yun-Bao Jiang

《化学科学与工程前沿（英文）》 2022年 第16卷 第1期   页码 81-91 doi: 10.1007/s11705-021-2049-7

摘要： Na , Cl and K are the most abundant electrolytes present in biological fluids that are essential to the regulation of pH homeostasis, membrane potential and cell volume in living organisms. Herein, we report synthetic crown ether-thiourea conjugates as a cation/anion symporter, which can transport both Na and Cl across lipid bilayers with relatively high transport activity. Surprisingly, the ion transport activities were diminished when high concentrations of K ions were present outside the vesicles. This unusual behavior resulted from the strong affinity of the transporters for K ions, which led to predominant partitioning of the transporters as the K complexes in the aqueous phase preventing the transporter incorporation into the membrane. Synthetic membrane transporters with Na , Cl and K transport capabilities may have potential biological and medicinal applications.

关键词： ion transport     thiourea     crown ether     symport    

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A density functional theory study on the mechanism of Dimethyl ether carbonylation over heteropolyacids

Kai Cai, Ying Li, Hongbao Shen, Zaizhe Cheng, Shouying Huang, Yue Wang, Xinbin Ma

《化学科学与工程前沿（英文）》 2021年 第15卷 第2期   页码 319-329 doi: 10.1007/s11705-020-1957-2

摘要： Dimethyl ether (DME) carbonylation is considered as a key step for a promising route to produce ethanol from syngas. Heteropolyacids (HPAs) are proved to be efficient catalysts for DME carbonylation. In this work, the reaction mechanism of DME carbonylation was studied theoretically by using density functional theory calculations on two typical HPA models (HPW, HSiW). The whole process consists of three stages: DME dissociative adsorption, insertion of CO into methoxyl group and formation of product methyl acetate. The activation barriers of all possible elementary steps, especially two possible paths for CO insertion were calculated to obtain the most favorable reaction mechanism and rate-limiting step. Furthermore, the effect of the acid strength of Brønsted acid sites on reactivity was studied by comparing the activation barriers over HPW and HSiW with different acid strength, which was determined by calculating the deprotonation energy, Mulliken population analyses and adsorption energies of pyridine.

关键词： dimethyl ether     carbonylation     mechanism     heteropolyacids     density functional theory    

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Effect of humic acid and metal ions on the debromination of BDE209 by nZVM prepared from steel pickling

Yuling CAI,Bin LIANG,Zhanqiang FANG,Yingying XIE,Eric Pokeung TSANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 879-887 doi: 10.1007/s11783-014-0764-8

摘要： As a promising in situ remediation technology, nanoscale zero-valent iron (nZVI) can remove polybrominated diphenyl ethers such as decabromodiphenyl ether (BDE209) effectively, However its use is limited by its high production cost. Using steel pickling waste liquor as a raw material to prepare nanoscale zero-valent metal (nZVM) can overcome this deficiency. It has been shown that humic acid and metal ions have the greatest influence on remediation. The results showed that nZVM and nZVI both can effectively remove BDE209 with little difference in their removal efficiencies, and humic acid inhibited the removal efficiency, whereas metal ions promoted it. The promoting effects followed the order Ni >Cu >Co and the cumulative effect of the two factors was a combination of the promoting and inhibitory individual effects. The major difference between nZVM and nZVI lies in their crystal form, as nZVI was found to be amorphous while that of nZVM was crystal. However, it was found that both nZVM and nZVI removed BDE209 with similar removal efficiencies. The effects and cumulative effects of humic acid and metal ions on nZVM and nZVI were very similar in terms of the efficiency of the BDE209 removal.

关键词： steel pickling waste liquor     nanoscale zero-valet metal     nanoscale zero-valent iron     humic acid     metal ion    

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Performance and emission characteristics of QHCCI dimethyl ether engine

WANG Ying, LI Wei, ZHOU Longbao, LIU Shenghua, HU Tiegang

《能源前沿（英文）》 2008年 第2卷 第4期   页码 401-405 doi: 10.1007/s11708-008-0075-5

摘要： Experimental investigation into the effects of different pilot amounts of dimethyl ether (DME) on the performance and emission of a single-cylinder direct-injection DME engine is conducted. The results show that a DME engine can operate at a wider range of speeds and loads at quasi-homogenous charge compression ignition (QHCCI) mode. The brake thermal efficiency increases while the exhaust temperature decreases. NO emission decreases by about 30%–50% although there is a slight increase in HC and CO emissions. NO, HC and CO emissions increase with an increase in the amount of DME pilot. QHCCI is a good way to increase thermal efficiency and decrease NO emission.

关键词： Experimental investigation     single-cylinder direct-injection     exhaust temperature     dimethyl     compression ignition    

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标题 作者 时间 类型 操作

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

Electrocatalytic debromination of BDE-47 at palladized graphene electrode

Hongtao YU, Bin MA, Shuo CHEN, Qian ZHAO, Xie QUAN, Shahzad AFZAL

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

CD47 blockade improves the therapeutic effect of osimertinib in non-small cell lung cancer

期刊论文

Solvent-resistant porous membranes using poly(ether−ether 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

Biomass to dimethyl ether by gasification/synthesis technology

Tiejun WANG, Yuping LI, Longlong MA, Chuangzhi WU

期刊论文

Joint effects of Penta-BDE and heavy metals on

Baohua TANG, Lingyan ZHU, Qixing ZHOU

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

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

Crown ether-thiourea conjugates as ion transporters

Zhixing Zhao, Bailing Tang, Xiaosheng Yan, Xin Wu, Zhao Li, Philip A. Gale, Yun-Bao Jiang

期刊论文

A density functional theory study on the mechanism of Dimethyl ether carbonylation over heteropolyacids

Kai Cai, Ying Li, Hongbao Shen, Zaizhe Cheng, Shouying Huang, Yue Wang, Xinbin Ma

期刊论文

Effect of humic acid and metal ions on the debromination of BDE209 by nZVM prepared from steel pickling

Yuling CAI,Bin LIANG,Zhanqiang FANG,Yingying XIE,Eric Pokeung TSANG

期刊论文

Performance and emission characteristics of QHCCI dimethyl ether engine

WANG Ying, LI Wei, ZHOU Longbao, LIU Shenghua, HU Tiegang

期刊论文