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CO₂ EOR 1

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二甲醚 1

太阳能，光伏，集中太阳能，生物质，水电解，二甲醚 1

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Ozone kinetics of dimethyl sulfide in the presence of water vapor

Haitao WANG

《环境科学与工程前沿（英文）》 2013年第7卷第6期页码 833-835 doi: 10.1007/s11783-013-0570-8

摘要： The outdoor smog chamber was used to thorough investigate the rate constants of gas-phase reaction between dimethyl sulfide (DMS) and ozone (O ) under conditions of relative humidity 55.0%–67.8% at (296±2)K for the first time. The rate constants were measured, at a total pressure of 1 atm, to be (10.4±0.2) × 10 cm ·molecule ·s at relative humidity of 67.5%±0.3% at 298K, (10.1±0.1) × 10 cm ·molecule ·s at relative humidity of 66.5%±0.5% at 296K, (7.75±0.39) × 10 cm ·molecule ·s at relative humidity of 64.8%±0.1% at 294K and (3.42±0.21) × 10 cm ·molecule ·s at relative humidity of 55.8%±0.8% at 295K. Base on these results, it is possible to see the reaction of O /DMS in the presence of water vapor as an important sink for DMS in the earth atmosphere.

关键词： rate constants ozone (O₃) dimethyl sulfide (DMS) water vapor

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Catalytic activity of cerium-doped Ru/AlO during ozonation of dimethyl phthalate

ZHOU Yunrui, ZHU Wanpeng, CHEN Xun

《环境科学与工程前沿（英文）》 2008年第2卷第3期页码 354-357 doi: 10.1007/s11783-008-0059-z

摘要： In this paper, factors influencing the mineralization of dimethyl phthalate (DMP) during catalytic ozonation with a cerium-doped Ru/AlO catalyst were studied. The catalytic contribution was calculated through the results of a comparison experiment. It showed that doping cerium significantly enhanced catalytic activity. The total organic carbon (TOC) removal over the doped catalyst at 100 min reached 75.1%, 61.3% using Ru/AlO catalyst and only 14.0% using ozone alone. Catalytic activity reached the maximum when 0.2% of ruthenium and 1.0% of cerium were simultaneously loaded onto AlO support. Results of experiments on oxidation by ozone alone, adsorption of the catalyst, Ce ion’s and heterogeneous catalytic ozonation confirmed that the contribution of heterogeneous catalytic ozonation was about 50%, which showed the obvious effect of Ru–Ce/AlO on catalytic activity.

关键词： Ru–Ce/AlO dimethyl phthalate mineralization comparison experiment catalytic ozonation

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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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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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Novel eco-efficient reactive distillation process for dimethyl carbonate production by indirect alcoholysis

Iulian Patraşcu, Costin S. Bîldea, Anton A. Kiss

《化学科学与工程前沿（英文）》 2022年第16卷第2期页码 316-331 doi: 10.1007/s11705-021-2047-9

摘要： Dimethyl carbonate is an eco-friendly essential chemical that can be sustainably produced from CO , which is available from carbon capture activities or can even be captured from the air. The rapid increase in dimethyl carbonate demand is driven by the fast growth of polycarbonates, solvent, pharmaceutical, and lithium-ion battery industries. Dimethyl carbonate can be produced from CO through various chemical pathways, but the most convenient route reported is the indirect alcoholysis of urea. Previous research used techniques such as heat integration and reactive distillation to reduce the energy use and costs, but the use of an excess of methanol in the trans-esterification step led to an energy intensive extractive distillation required to break the dimethyl carbonate-methanol azeotrope. This work shows that the production of dimethyl carbonate by indirect alcoholysis of urea can be improved by using an excess of propylene carbonate (instead of an excess of methanol), a neat feat that we showed it requires only 2.64 kW·h·kg dimethyl carbonate in a reaction-separation-recycle process, and a reactive distillation column that effectively replaces two conventional distillation columns and the reactor for dimethyl carbonate synthesis. Therefore, less equipment is required, the methanol-dimethyl carbonate azeotrope does not need to be recycled, and the overall savings are higher. Moreover, we propose the use of a reactive distillation column in a heat integrated process to obtain high purity dimethyl carbonate (>99.8 wt-%). The energy requirement is reduced by heat integration to just 1.25 kW·h·kg dimethyl carbonate, which is about 52% lower than the reaction-separation-recycle process. To benefit from the energy savings, the dynamics and control of the process are provided for ±10% changes in the nominal rate of 32 ktpy dimethyl carbonate, and for uncertainties in reaction kinetics.

关键词： dimethyl carbonate reactive distillation process design plantwide control

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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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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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Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl

Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA

《化学科学与工程前沿（英文）》 2012年第6卷第4期页码 415-422 doi: 10.1007/s11705-012-1214-4

摘要： The catalysts supported on LiAl O (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H . Li/Al molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-Al-O oxides. Desirable LiAl O (spinel) was formed at 800°C, while LiAl O (primitive cube) formed at 900°C is undesirable for the reaction. A high Li/Al molar ratio, which was related with LiAlO , also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuCl -PdCl /LiAl O (spinel) with better electron transfer ability and low Pd reduction temperature exhibited a better catalytic ability.

关键词： Wacker-type catalyst dimethyl carbonate methyl nitrite spinel

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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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Impact of dimethyl ether on engine seal materials

WU Ning, ZHANG Wugao, HUANG Zhen

《能源前沿（英文）》 2008年第2卷第3期页码 279-284 doi: 10.1007/s11708-008-0042-1

摘要： The resistance of many kinds of rubber materials to dimethyl ether (DME) was studied. Both the mass and volume change of rubber materials, which were put in DME and then exposed to the air for different periods of time were measured. The results show that fluorine rubber (FKM), silicone rubber (SIR), and nitrile rubber (NBR) are unsuitable as seal materials for DME engines. Common polyvinylchloride (PVC) dissolved completely in DME, which has almost no impact on vulcanizing nylon material. The constitution of ethylene propylene terpolymer rubber (EPDM) has a major impact on its resistance to DME. A kind of EPDM with good resistance to DME was found, whose reliability was validated by 100 hours of DME engine operation.

关键词： impact Common polyvinylchloride different constitution ethylene propylene

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Direct synthesis of dimethyl carbonate over rare earth oxide supported catalyst

JIANG Qi, CHENG Jiye, GAO Zhiqin

《化学科学与工程前沿（英文）》 2007年第1卷第3期页码 300-303 doi: 10.1007/s11705-007-0055-z

摘要： Solid base catalysts for the direct synthesis of dimethyl carbonate (DMC) from carbon dioxide, methanol, and propylene oxide were prepared by loading KCl and KCO on the surface of LaO, YO, CeO and NdO. The catalysts were characterized by thermogravimetric analysis (TGA) and X-ray diffraction (XRD) techniques. The catalytic activities were efficiently influenced by the preparation conditions. The optimal loading amount of KCO is 17.6% (mass) for KCl-KCO/YO and 22.2% for other catalysts. Supports affected the activity of catalyst. KCl-KCO/NdO exhibited the highest activity. The activity of KCl-KCO/YO increased with the increase of calcination temperature in the range of 800ºC–900ºC. The formation of KYO, YOCl or YO species probably promoted the catalysts.

关键词： thermogravimetric analysis increase KCl-KCO/NdO catalytic KCl-KCO/YO

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Reconstruction of Cu–ZnO catalyst by organic acid and deactivation mechanism in liquid-phase hydrogenation of dimethyl

《化学科学与工程前沿（英文）》 2023年第17卷第9期页码 1311-1319 doi: 10.1007/s11705-022-2281-9

摘要： A reconstructed Cu–ZnO catalyst with improved stability was fabricated by organic acid treatment method for the liquid-phase hydrogenation of dimethyl succinate to 1,4-butanediol. According to the characterization results of the fresh Cu–ZnO and reconstructed Cu–ZnO, three different forms of ZnO were suggested to be presented on the catalysts: ZnO having strong interaction with Cu species, ZnO that weakly interacted with Cu species and isolated ZnO. The first form of ZnO was believed to be beneficial to the formation of efficient active site Cu⁺, while the latter two forms of ZnO took the main responsibility for the deactivation of Cu–ZnO catalysts in the liquid-phase hydrogenation of diesters. The reconstruction of the Cu–ZnO catalyst by the organic acid treatment method resulted in a new Cu–ZnO catalyst with more Cu⁺ and less ZnO species that leads to deactivation. Furthermore, the deactivation mechanism of Cu–ZnO catalysts in liquid-phase diester hydrogenation in continuous flow system was proposed: the deposition of the polyesters on the catalysts via transesterification catalyzed by weakly interacted ZnO and isolated ZnO leads to the deactivation. These results provided meaningful instructions for designing highly efficient Cu–Zn catalysts for similar ester hydrogenation systems.

关键词： liquid phase hydrogenation Cu–ZnO deactivation mechanism 1 4-butanediol diester

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Kinetics of oxidation of dimethyl trisulfide by potassium permanganate in drinking water

Xiaoyan MA, Shifei HU, Hongyu WANG, Jun LI, Jing HUANG, Yun ZHANG, Weigang LU, Qingsong LI

《环境科学与工程前沿（英文）》 2012年第6卷第2期页码 171-176 doi: 10.1007/s11783-011-0319-1

摘要： Metabolites of algae such as geosmin, 2-methylisoborneol etc. are reported to induce pungent odors into drinking water and attract additional scientific attention. Recently, in China, taste and odor outbreaks in drinking water supply have become increasingly common. In source water affected by eutrophication, dimethyl trisulfide, speculated to be produced by decayed algae, was found to be the source of taste and odor issues and can be removed effectively by usual oxidation agents. In this experimental study, batch scale tests were carried out focusing on the removal of dimethyl trisulfide. Reaction kinetics of dimethyl trisulfide oxidized by potassium permanganate in water had been studied; influence factors such as pH, organic substrate, other existed taste, and odor contaminant in equivalent concentration were also discussed. Results showed that dimethyl trisulfide can be removed by potassium permanganate efficiently; the ratio can reach more than 70% with oxidant dosage of 4 mg·L and contact time prolonged to 120 min. The dimethyl trisulfide decomposition followed a second-order kinetics pattern with a rate constant = 0.00213 L·(min·mg) . Typically, the degradation rate of dimethyl trisulfide was increased with the increasing KMnO dosage, but dramatically dropped with the increasing levels of humic acid (1.8–4.5 mg·L ) and other odor-causing compounds (e.g. -cyclocitral, 0–1886.0 μg·L ). Solution pH (5.2–9.0) and initial dimethyl trisulfide concentration did not significantly affected the degradation. This study demonstrates that KMnO oxidation is an effective option to remove dimethyl trisulfide from water.

关键词： odor and taste oxidation reaction reaction kinetics water treatment

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Pd-Fe/α-Al

Shengping WANG, Xin ZHANG, Yujun ZHAO, Yadong GE, Jing LV, Baowei WANG, Xinbin MA

《化学科学与工程前沿（英文）》 2012年第6卷第3期页码 259-269 doi: 10.1007/s11705-012-1212-6

摘要： Cordierite monoliths coated with Pd-Fe/α-Al O catalysts were prepared at various calcination temperatures and characterized by thermogravimetry, temperature-programmed reduction, transmission electron microscopy, diffuse reflectance infrared Fourier transformation spectroscopy and X-ray diffraction. The performance of the catalytic monoliths for the synthesis of dimethyl oxalate (DMO) through a CO coupling reaction was evaluated. Monolithic catalysts with calcination temperatures ranging from 473 K to 673 K exhibited excellent dispersion of Pd, good CO adsorption properties, and excellent performance for the coupling reaction. The optimized monolithic catalyst exhibited a much higher Pd efficiency (denoted as DMO (g)·Pd (g) ·h ) (733 h ) than that of the granular catalyst (60.2 h ), which can be attributed to its honeycomb structure and the large pore sizes in the α-Al O washcoat which was accompanied with an even distribution of the active component in the coating layer along the monoliths channels.

关键词： dimethyl oxalate coupling Pd cordierite monolith calcination structure

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Catalytic ozonation of organic compounds in water over the catalyst of RuO

Jianbing WANG,Guoqing WANG,Chunli YANG,Shaoxia YANG,Qing HUANG

《环境科学与工程前沿（英文）》 2015年第9卷第4期页码 615-624 doi: 10.1007/s11783-014-0706-5

摘要： This research investigates the performances of RuO /ZrO -CeO in catalytic ozonation for water treatment. The results show that RuO /ZrO -CeO was active for the catalytic ozonation of oxalic acid and possessed higher stability than RuO /Al O and Ru/AC. In the catalytic ozonation of dimethyl phthalate (DMP), RuO /ZrO -CeO did not enhance the DMP degradation rate but significantly improved the total organic carbon (TOC) removal rate. The TOC removal in catalytic ozonation was 56% more than that in noncatalytic ozonation. However this does not mean the catalyst was very active because the contribution of catalysis to the overall TOC removal was only 30%. The adsorption of the intermediates on RuO /ZrO -CeO played an important role on the overall TOC removal while the adsorption of DMP on it was negligible. This adsorption difference was due to their different ozonation rates. In the catalytic ozonation of disinfection byproduct precursors with RuO /ZrO -CeO , the reductions of the haloacetic acid and trihalomethane formation potentials (HAAFPs and THMFPs) for the natural water samples were 38%–57% and 50%–64%, respectively. The catalyst significantly promoted the reduction of HAAFPs but insignificantly improved the reduction of THMFPs as ozone reacts fast with the THMs precursors. These results illustrate the good promise of RuO /ZrO -CeO in catalytic ozonation for water treatment.

关键词： ozonation ruthenium oxalic acid dimethyl phthalate disinfection byproduct