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超超临界 2

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Ball milling promoted direct liquefaction of lignocellulosic biomass in supercritical ethanol

Chunyan Yang, Xiaoliang Yuan, Xueting Wang, Kejing Wu, Yingying Liu, Changjun Liu, Houfang Lu, Bin Liang

《化学科学与工程前沿（英文）》 2020年 第14卷 第4期   页码 605-613 doi: 10.1007/s11705-019-1841-0

摘要： In the present work, ball milling was applied for the pretreatment of lignocellulose to obtain high conversion and bio-oil yield in supercritical ethanol. Ball milling substantially decreased the crystallinity and particle size of lignocellulose, thereby improving its accessibility in ethanol solvent. An increased bio-oil yield of 59.2% was obtained for the ball milled camphorwood sawdust at 300°C, compared with 39.6% for the original lignocellulose. Decreased crystallinity significantly benefited the conversion of the cellulose component from 60.8% to 91.7%, and decreased particle size was beneficial for the conversion of all components. The obtained bio-oil had a high phenolic content, as analyzed by gas chromatography-mass spectrometry. Methoxylation and retro-aldol condensation were observed during alcoholysis, and the reaction pathways of lignocellulose in supercritical ethanol were attributed to the action of free radicals.

关键词： ball milling     lignocellulose     supercritical ethanol     liquefaction     bio-oil    

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Direct ethanol production from rice straw by coculture with two high-performing fungi

Maki TAKANO, Kazuhiro HOSHINO

《化学科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 139-145 doi: 10.1007/s11705-012-1281-6

摘要： To develop efficient and economical direct ethanol production from fine rice straw crashed mechanically, two high-performing fungi, which can secret hyperactive cellulases and/or ferment effectively various sugars, were selected from some strains belong to preserved in our laboratory. The simultaneous saccharification and fermentation (SSF) by coculture with these fungi was investigated. The screening of high-performing fungi resulted in the selection of NBRC 4572 as an ethanol-producing fungus and NBRC 5398 as a cellulase-secreting fungus. The strain 4572 produced ethanol aerobically from glucose and xylose in high yields of 0.420 g/g at 36 h and 0.478 g/g at 60 h, respectively, but secreted fairly low cellulases. On the other hand, the strain 5398 also produced ethanol from glucose in yield of 0.340 g/g though it had a little growth in xylose culture. However, it secreted hyperactive cellulases that are essential for hydrolysis of rice straw in culture and the maximum activities of endo-β-glucanase and β-glucosidase were 2.11 U/L and 1.47 U/L, respectively. In SSF of rice straw by coculture with two fungi selected, the ethanol production reached 1.28 g/L after 96 h when the inoculation ratio of the strain 5398 to the strain 4572 was 9.

关键词： Mucor circinelloides     ethanol production     cellulase secretion     SSF     coculture     rice straw    

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Thermodynamic analysis of ethanol synthesis from hydration of ethylene coupled with a sequential reaction

Jie Gao, Zhikai Li, Mei Dong, Weibin Fan, Jianguo Wang

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 847-856 doi: 10.1007/s11705-019-1848-6

摘要： Coal-based ethanol production by hydration of ethylene is limited by the low equilibrium ethylene conversion at elevated temperature. To improve ethylene conversion, coupling hydration of ethylene with a potential ethanol consumption reaction was analyzed thermodynamically. Five reactions have been attempted and compared: (1) dehydration of ethanol to ethyl ether ( ), (2) dehydrogenation of ethanol to acetaldehyde ( ), (3) esterification of acetic acid with ethanol ( ), (4) dehydrogenation of ethanol to ethyl acetate ( ), and (5) oxidative dehydrogenation of ethanol to ethyl acetate ( ). The equilibrium constants and equilibrium distributions of the coupled reactions were calculated and the effects of feed composition, temperature and pressure upon the ethylene equilibrium conversion were examined. The results show that dehydrogenation of ethanol to acetaldehyde has little effect on ethylene conversion, whereas for dehydrogenation of ethanol to acetaldehyde and ethyl acetate, ethylene conversion can be improved from 8% to 12.8% and 18.5%, respectively, under conditions of H O/C H = 2, 10 atm and 300°C. The esterification of acetic acid with ethanol can greatly enhance the ethylene conversion to 22.5%; in particular, ethylene can be actually completely converted to ethyl acetate by coupling oxidative dehydrogenation of ethanol.

关键词： ethylene     ethanol     thermodynamics     coupling    

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Mechanism of ethanol/water reverse separation through a functional graphene membrane: a molecular simulation

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 347-357 doi: 10.1007/s11705-022-2246-z

摘要： Reverse-selective membranes have attracted considerable interest for bioethanol production. However, to date, the reverse-separation performance of ethanol/water is poor and the separation mechanism is unclear. Graphene-based membranes with tunable apertures and functional groups have shown substantial potential for use in molecular separation. Using molecular dynamics simulations, for the first time, we reveal two-way selectivity in ethanol/water separation through functional graphene membranes. Pristine graphene (PG) exhibits reverse-selective behavior with higher ethanol fluxes than water, resulting from the preferential adsorption for ethanol. Color flow mappings show that this ethanol-permselective process is initiated by the presence of ethanol-enriched and water-barren pores; this has not been reported in previous studies. In contrast, water molecules are preferred for hydroxylated graphene membranes because of the synergistic effects of molecular sieving and functional-group attraction. A simulation of the operando condition shows that the PG membrane with an aperture size of 3.8 Å achieves good separation performance, with an ethanol/water separation factor of 34 and a flux value of 69.3 kg∙m‒2∙h‒1∙bar‒1. This study provides new insights into the reverse-selective mechanism of porous graphene membranes and a new avenue for efficient biofuel production.

关键词： reverse separation     graphene membrane     ethanol/water separation     molecular simulation    

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对用生物质原料生产燃料用乙醇之我见

倪维斗,李政,靳晖

《中国工程科学》 2001年 第3卷 第5期   页码 44-49

摘要：

从资源、成本、能源安全、粮食安全和环境效益等方面对用粮食制取乙醇作为车用燃料作了分析，指出这种措施可以是一种消化陈粮的短期做法，但不能作为我国解决液体燃料短缺的长期战略措施，因为我国的具体情况和美国及巴西有很大的不同。此外，按照美国的经验，掺入乙醇作为车用燃料需要有政府的大量补贴，从长期角度看也是有问题的。对我国用酶水解方法由秸秆制造燃料用酒精也作了初步评估。最后从可持续发展的角度，对缓解我国大量进口石油的压力、提高能源安全的战略措施提出了意见。

关键词： 汽油-乙醇混合物     乙醇     玉米乙醇     酶水解     能源安全    

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Anion-exchange membrane direct ethanol fuel cells: Status and perspective

T.S. Zhao, Y.S. Li, S.Y. Shen

《能源前沿（英文）》 2010年 第4卷 第4期   页码 443-458 doi: 10.1007/s11708-010-0127-5

摘要： Direct ethanol fuel cells (DEFCs) are a promising carbon-neutral and sustainable power source for portable, mobile, and stationary applications. However, conventional DEFCs that use acid proton-exchange membranes (typically Nafion type) and platinum-based catalysts exhibit low performance (i.e., the state-of-the-art peak power density is 79.5 mW/cm at 90°C). Anion-exchange membrane (AEM) DEFCs that use low-cost AEM and non-platinum catalysts have recently been demonstrated to yield a much better performance (i.e., the state-of-the-art peak power density is 160 mW/cm at 80°C). This paper provides a comprehensive review of past research on the development of AEM DEFCs, including the aspects of catalysts, AEMs, and single-cell design and performance. Current and future research challenges are identified along with potential strategies to overcome them.

关键词： fuel cell     direct ethanol fuel cells     anion-exchange membrane     ethanol oxidation reaction     oxygen reduction reaction     cell performance    

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Calculation and analysis of sub/supercritical methanol preheating tube for continuous production of biodieselvia supercritical methanol transesterification

Wen CHEN, Weiyong YING, Cunwen WANG, Weiguo WANG, Yuanxin WU, Junfeng ZHANG,

《能源前沿（英文）》 2009年 第3卷 第4期   页码 423-431 doi: 10.1007/s11708-009-0075-0

摘要： Biodiesel is an important renewable energy. Supercritical methanol transesterification for biodiesel has recently been concerned because of its obvious advantages. The tubular reactor is an ideal reactor for continuous preparation of biodiesel via supercritical methanol transesterification. A methanol preheating tube is necessary for the tubular reaction system because the reaction temperature for supercritical methanol transesterification is usually 520―600K. Therefore, in the range of 298―600K, changes of the density, isobaric capacity, viscosity and thermal conductivity of sub/supercritical methanol with temperature are first discussed. Then on the basis of these thermophysical properties, an integration method is adopted for the design of sub/supercritical methanol preheating tube when methanol is preheated from 298K to 600K at 16MPa and the influencing factors on the length of the preheating tube are also studied. The computational results show that the Reynolds number and the local convection heat-transfer coefficient of sub/supercritical methanol flowing in ф6mm×1.5mm preheating tube change drastically with temperature. For the local overall heat transfer coefficient and the average overall heat transfer coefficient , temperature also has an important influence on them when the inlet velocity of methanol is lower than 0.5m/s. But when the inlet velocity of methanol is higher than 0.5m/s, and almost keep invariable with temperature. Additionally, both the outlet temperature and the inlet velocity of methanol are the key affecting factors for the length of the preheating tube, especially when the outlet temperature is over the critical temperature of methanol. At the same time, the increase of tin bath’s temperature can shorten the required length of the preheating tube. At the inlet flow rate of 0.5m/s, the required length of the preheating tube is 2.0m when methanol is preheated from 298K to 590K at 16MPa with keeping the tin bath’s temperature 620K, which is in good agreement with the experimental results.

关键词： sub/supercritical methanol     preheating tube     integration method     biodiesel    

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A review on catalytic & non-catalytic bio-oil upgrading in supercritical fluids

Sainab Omar, Yang Yang, Jiawei Wang

《化学科学与工程前沿（英文）》 2021年 第15卷 第1期   页码 4-17 doi: 10.1007/s11705-020-1933-x

摘要： This review article summarizes the key published research on the topic of bio-oil upgrading using catalytic and non-catalytic supercritical fluid (SCF) conditions. The precious metal catalysts Pd, Ru and Pt on various supports are frequently chosen for catalytic bio-oil upgrading in SCFs. This is reportedly due to their favourable catalytic activity during the process including hydrotreating, hydrocracking, and esterification, which leads to improvements in liquid yield, heating value, and pH of the upgraded bio-oil. Due to the costs associated with precious metal catalysts, some researchers have opted for non-precious metal catalysts such as acidic HZSM-5 which can promote esterification in supercritical ethanol. On the other hand, SCFs have been effectively used to upgrade crude bio-oil without a catalyst. Supercritical methanol, ethanol, and water are most commonly used and demonstrate catalyst like activities such as facilitating esterification reactions and reducing solid yield by alcoholysis and hydrolysis, respectively.

关键词： bio-oil     upgrading     supercritical     review    

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Polydimethylsiloxane assisted supercritical CO

Weixia Wang, Shuai Zhou, Zhong Xin, Yaoqi Shi, Shicheng Zhao

《化学科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 396-404 doi: 10.1007/s11705-016-1577-z

摘要： Foamable high melt strength polypropylene (HMSPP) was prepared by grafting styrene (St) onto polypropylene (PP) and simultaneously introducing polydimethylsiloxane (PDMS) through?a?one-step?melt extrusion process. The effect of PDMS viscosity on the foaming behavior of HMSPP was systematically investigated using supercritical CO as the foaming agent. The results show that the addition of PDMS has little effect on the grafting reaction of St and HMSPP exhibits enhanced elastic response and obvious strain hardening effect. Though the CO solubility of HMSPP with PDMS (PDMS-HMSPP) is lower than that of HMSPP without PDMS, especially for PDMS with low viscosity, the PDMS-HMSPP foams exhibit narrow cell size distribution and high cell density. The fracture morphology of PDMS-HMSPP shows that PDMS with low viscosity disperses more easily and uniformly in HMSPP matrix, leading to form small domains during the extrusion process. These small domains act as bubble nucleation sites and thus may be responsible for the improved foaming performance of HMSPP.

关键词： high melt strength polypropylene (HMSPP)     polydimethylsiloxane (PDMS)     supercritical CO2     foaming behavior    

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Study of simultaneous saccharification and fermentation for steam exploded wheat straw to ethanol

LUO Peng, YANG Chuanmin, LIU Zhong, WANG Gaosheng

《化学科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 447-451 doi: 10.1007/s11705-008-0069-1

摘要： Although simultaneous saccharification and fermentation (SSF) has been investigated extensively, the optimum condition for SSF of wheat straw has not yet been determined. Dilute sulfuric acid impregnated and steam explosion pretreated wheat straw was used as a substrate for the production of ethanol by SSF through orthogonal experiment design in this study. Cellulase mixture (Celluclast 1.5 l and -glucosidase Novozym 188) were adopted in combination with the yeast AS2.1. The effects of reaction temperature, substrate concentration, initial fermentation liquid pH value and enzyme loading were evaluated and the SSF conditions were optimized. The ranking, from high to low, of influential extent of the SSF affecting factors to ethanol concentration and yield was substrate concentration, enzyme loading, initial fermentation liquid pH value and reaction temperature, respectively. The optimal SSF conditions were: reaction temperature, 35°C; substrate concentration, 100 g·L; initial fermentation liquid pH, 5.0; enzyme loading, 30 FPU·g. Under these conditions, the ethanol concentration increased with reaction time, and after 72 h, ethanol was obtained in 65.8% yield with a concentration of 22.7 g·L.

关键词： optimal SSF     substrate concentration     optimum condition     enzyme loading     ethanol concentration    

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Effects of the SAPO-11 synthetic process on dehydration of ethanol to ethylene

Lina WU, Xiaoxing SHI, Qun CUI, Haiyan WANG, He HUANG

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 60-66 doi: 10.1007/s11705-010-0540-7

摘要： The effects of the synthetic condition of SAPO-11 molecular sieves on ethanol dehydration to ethylene were studied. Product-compositions, ethanol conversion, and selectivity to ethylene of synthesized and commercial SAPO-11 molecular sieves were compared. Results are as follows: the optimal synthetic conditions for SAPO-11 molecular sieves are adding pseudoboehmite before orthophoshporic, using di-n- propylamine as the template, having a mass fraction of 40% colloidal silica as the silica source and the starting gel obtained, and running at 200°C for 48 h. From the patterns of NH -TPD, the amount of acid synthesized by SAPO-11 molecular sieves is less than that by commercial SAPO-11 molecular sieves, and has a stronger weak acid. Also, ethanol conversion and selectivity to ethylene reached 99% at 280°C on synthesized SAPO-11, lower by 20°C compared to commercial SAPO-11. For two SAPO-11 molecular sieves, the by-products in the gas phase are mainly ethane, propane, propene, isobutane, n-butane, propadiene, butylene and some higher hydrocarbons. The by-products in the liquid phase are ethyl ether and acetaldehyde.

关键词： SAPO-11 molecular sieves     synthesis     ethanol     ethylene     dehydration    

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Corrosion mechanisms of candidate structural materials for supercritical water-cooled reactor

Lefu ZHANG, Fawen ZHU, Rui TANG

《能源前沿（英文）》 2009年 第3卷 第2期   页码 233-240 doi: 10.1007/s11708-009-0024-y

摘要： Nickel-based alloys, austenitic stainless steel, ferritic/martensitic heat-resistant steels, and oxide dispersion strengthened steel are presently considered to be the candidate structural or fuel-cladding materials for supercritical water-cooled reactor (SCWR), one of the promising generation IV reactor for large-scale electric power production. However, corrosion and stress corrosion cracking of these candidate alloys still remain to be a major problem in the selection of nuclear fuel cladding and other structural materials, such as water rod. Survey of literature and experimental results reveal that the general corrosion mechanism of those candidate materials exhibits quite complicated mechanism in high-temperature and high-pressure supercritical water. Formation of a stable protective oxide film is the key to the best corrosion-resistant alloys. This paper focuses on the mechanism of corrosion oxide film breakdown for SCWR candidate materials.

关键词： supercritical water-cooled reactor     general corrosion     oxide film     corrosion mechanism    

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Detoxification and concentration of corn stover hydrolysate and its fermentation for ethanol production

Qing Li, Yingjie Qin, Yunfei Liu, Jianjun Liu, Qing Liu, Pingli Li, Liqiang Liu

《化学科学与工程前沿（英文）》 2019年 第13卷 第1期   页码 140-151 doi: 10.1007/s11705-018-1714-y

摘要： Environmental and energy concerns have increased interest in renewable energy sources, particularly biofuels. Thus the fermentation of glucose from sulfuric acid-hydrolyzed corn stover for the production of bioethanol has been explored using a combined acid retardation and continuous-effect membrane distillation treatment process. This process resulted in the separation of the sugars and acids from the acid-catalyzed hydrolysate, the removal of most of the fermentation inhibitors from the hydrolysate and the concentration of the detoxified hydrolysate. The recovery rate of glucose from the sugar-acid mixture using acid retardation was greater than 99.12% and the sulfuric acid was completely recovered from the hydrolysate. When the treated corn stover hydrolysate, containing 100 g/L glucose, was used as a carbon source, 43.06 g/L of ethanol was produced with a productivity of 1.79 g/(L?h) and a yield of 86.31%. In the control experiment, where glucose was used as the carbon source these values were 1.97 g/(L?h) and 93.10% respectively. Thus the integration of acid retardation and a continuous-effect membrane distillation process are effective for the production of fuel ethanol from corn stover.

关键词： corn stover     hydrolysate     acid retardation     continuous-effect membrane distillation     ethanol fermentation    

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Development of a supercritical and an ultra-supercritical circulating fluidized bed boiler

Junfu LYU, Hairui YANG, Wen LING, Li NIE, Guangxi YUE, Ruixin LI, Ying CHEN, Shilong WANG

《能源前沿（英文）》 2019年 第13卷 第1期   页码 114-119 doi: 10.1007/s11708-017-0512-4

摘要： The supercritical circulating fluidized bed (CFB) boiler, which combines the advantages of CFB combustion with low cost emission control and supercritical steam cycle with high efficiency of coal energy, is believed to be the future of CFB combustion technology. It is also of greatest importance for low rank coal utilization in China. Different from the supercritical pulverized coal boiler that has been developed more than 50 years, the supercritical CFB boiler is still a new one which requires further investigation. Without any precedentor engineering reference, Chinese researchers have conducted fundamental research, development, design of the supercritical CFB boilers independently. The design theory and key technology for supercritical CFB boiler were proposed. Key components and novel structures were invented. The first 600 MWe supercritical CFB boiler and its auxiliaries were successfully developed and demonstrated in Baima Power Plant, Shenhua Group as well as the simulator, control technology, installation technology, commissioning technology, system integration and operation technology. Compared with the 460 MWe supercritical CFB in Poland, developed in the same period and the only other supercritical one of commercial running in the word beside Baima, the 600 MWe one in Baima has a better performance. Besides, supercritical CFB boilers of 350 MWe have been developed and widely commercialized in China. In this paper, the updated progress of 660 MWe ultra-supercritical CFB boilers under development is introduced.

关键词： supercritical     circulating fluidized bed boiler     development     demonstration    

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发展“燃料酒精”的建议

章克昌

《中国工程科学》 2000年 第2卷 第6期   页码 89-93

摘要：

文章从缓解能源短缺、缓解地球大气污染及国民经济新的增长点三个方面阐述了采用燃料酒精作汽车燃料的重要意义。介绍了我国实施燃料酒精计划需要解决的如原料供应、降低能耗、酒糟处理及投资效益等主要技术、经济问题及对策。最后提出了21世纪前10年研究课题的建议。

关键词： 燃料酒精     发酵     温室效应     能源    

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标题 作者 时间 类型 操作

Ball milling promoted direct liquefaction of lignocellulosic biomass in supercritical ethanol

Chunyan Yang, Xiaoliang Yuan, Xueting Wang, Kejing Wu, Yingying Liu, Changjun Liu, Houfang Lu, Bin Liang

期刊论文

Direct ethanol production from rice straw by coculture with two high-performing fungi

Maki TAKANO, Kazuhiro HOSHINO

期刊论文

Thermodynamic analysis of ethanol synthesis from hydration of ethylene coupled with a sequential reaction

Jie Gao, Zhikai Li, Mei Dong, Weibin Fan, Jianguo Wang

期刊论文

Mechanism of ethanol/water reverse separation through a functional graphene membrane: a molecular simulation

期刊论文

对用生物质原料生产燃料用乙醇之我见

倪维斗,李政,靳晖

期刊论文

Anion-exchange membrane direct ethanol fuel cells: Status and perspective

T.S. Zhao, Y.S. Li, S.Y. Shen

期刊论文

Calculation and analysis of sub/supercritical methanol preheating tube for continuous production of biodieselvia supercritical methanol transesterification

Wen CHEN, Weiyong YING, Cunwen WANG, Weiguo WANG, Yuanxin WU, Junfeng ZHANG,

期刊论文

A review on catalytic & non-catalytic bio-oil upgrading in supercritical fluids

Sainab Omar, Yang Yang, Jiawei Wang

期刊论文

Polydimethylsiloxane assisted supercritical CO

Weixia Wang, Shuai Zhou, Zhong Xin, Yaoqi Shi, Shicheng Zhao

期刊论文

Study of simultaneous saccharification and fermentation for steam exploded wheat straw to ethanol

LUO Peng, YANG Chuanmin, LIU Zhong, WANG Gaosheng

期刊论文

Effects of the SAPO-11 synthetic process on dehydration of ethanol to ethylene

Lina WU, Xiaoxing SHI, Qun CUI, Haiyan WANG, He HUANG

期刊论文

Corrosion mechanisms of candidate structural materials for supercritical water-cooled reactor

Lefu ZHANG, Fawen ZHU, Rui TANG

期刊论文

Detoxification and concentration of corn stover hydrolysate and its fermentation for ethanol production

Qing Li, Yingjie Qin, Yunfei Liu, Jianjun Liu, Qing Liu, Pingli Li, Liqiang Liu

期刊论文

Development of a supercritical and an ultra-supercritical circulating fluidized bed boiler

Junfu LYU, Hairui YANG, Wen LING, Li NIE, Guangxi YUE, Ruixin LI, Ying CHEN, Shilong WANG

期刊论文

发展“燃料酒精”的建议

章克昌

期刊论文