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Steam reforming of acetic acid over Ni-Ba/Al2O3 catalysts:Impacts of barium addition on coking behaviors and formation of reaction intermediates

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Journal of Energy Chemistry 2020年第4期29卷 208-219页

作者： Zhanming Zhang Yiran Wang Kai Sun Yuewen Shao Lijun Zhang Shu Zhang Xiao Zhang Qing Liu Zhenhua Chen Xun Hu School of Material Science and Engineering University of JinanJinan 250022ShandongChina College of Materials Science and Engineering Nanjing Forestry UniversityNanjing 210037JiangsuChina Fuels and Energy Technology Institute and Western Australia School of Mines:Minerals Energy and Chemical EngineeringCurtin UniversityPerthWA 6845Australia Key Laboratory of Low Carbon Energy and Chemical Engineering College of Chemical and Environmental EngineeringShandong University of Science and TechnologyQingdao 266590ShandongChina Jinzhou Medical University Jinzhou 121001LiaoningChina

The influence of barium addition to a Ni/Al2O3 catalyst on the reaction intermediates formed,the activity,resistance of the catalyst to coking,and properties of the coke formed after acetic acid steam reforming were investigated in this study.The results showed the drastic effects of barium addition on the physicochemical properties and performances of the catalyst.The solid-phase reaction between alumina and BaO formed BaAl2O4,which re-constructed the alumina structure,resulting in a decrease in the specific surface area and an increase in the resistance of metallic Ni to sintering.The addition of barium was also beneficial for enhancing the catalytic activity,resulting from the changed catalytic reaction network.The in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) study of the acetic acid steam reforming indicated that barium could effectively suppress the accumulation of the reaction intermediates of carbonyl,formate,and C=C functional groups on the catalyst surface,attributed to its relatively high ability to cause the gasification of these species.In addition,coking was considerably more significant over the Ba-Ni/Al2O3 catalyst.Moreover,the Ba-Ni/Al2O3 catalyst was more stable than the Ni/Al2O3catalyst,owing to the distinct forms of coke formed (carbon nanotube form over the Ba-Ni/Al2O3 catalyst,and the amorphous form over the Ni/Al2O3 catalyst).

关键词： Barium addition Nickel-based catalysts Steam reforming of acetic acid Reaction intermediates Coking behaviors

Hydrogen bonding of single acetic acid with water molecules in dilute aqueous solutions

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Science China Chemistry 2009年第12期52卷 2219-2225页

作者： PU Liang SUN YueMing ZHANG ZhiBing School of Chemistry and Chemical Engineering Southeast UniversityNanjing 211189China Separation Engineering Research Center of Nanjing University Key Laboratory in Meso-&Microscopic Chemistry of Ministry of Education of ChinaSchool of Chemistry and Chemical EngineeringNanjing UniversityNanjing 210093China

In separation processes,hydrogen bonding has a very significant effect on the efficiency of isolation of acetic acid (HOAc) from HOAc/H2O mixtures. This intermolecular interaction on aggregates composed of a single HOAc molecule and varying numbers of H2O molecules has been examined by using ab initio molecular dynamics simulations (AIMD) and quantum chemical calculations (QCC). Thermodynamic data in aqueous solution were obtained through the self-consistent reaction field calculations and the polarizable continuum model. The aggregation free energy of the aggregates in gas phase as well as in aqueous system shows that the 6-membered ring is the most favorable structure in both states. The relative stability of the ring structures inferred from the thermodynamic properties of the QCC is consistent with the ring distributions of the AIMD simulation. The study shows that in dilute aqueous solution of HOAc the more favorable molecular interaction is the hydrogen bonding between HOAc and H2O molecules,resulting in the separation of acetic acid from the HOAc/H2O mixtures with more difficulty than usual.

关键词： acetic acid hydrogen bond ab initio molecular dynamics free energy

Removal of gaseous acetic acid using ionic liquid [EMIM][BF_4]

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Green Energy & Environment 2019年第2期4卷 190-197页

作者： Mingli Mu Jun Cheng Chengna Dai Ning Liu Zhigang Lei Yanzhou Ding Jianjiang Lu College of Environmental and Energy Engineering Beijing University of Technology State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical Technology School of Chemistry and Chemical Engineering Shihezi University

This work proposed to use the ionic liquid [EMIM][BF_4] as absorbent for the absorption of gaseous acetic acid. The feasibility of this technology was investigated from molecular level to industrial scale. The acetic acid absorption experiment was carried out using [EMIM][BF_4],and the removal ratio of acetic acid in the gas product can achieve 88.6% at 20C under atmospheric pressure at the laboratory scale. Based on the experimental results, a reliable strict equilibrium phase model embedding the parameters of the UNIFAC model was established. On this basis, the conceptual process design and optimization of acetic acid removal by [EMIM][BF_4] at an industrial scale was done, and the most suitable design and operation parameters were obtained. For a further step, the binding energy between [EMIM][BF_4] and acetic acid was calculated to give some insights into the separation mechanism, and the results indicate that the interaction between acetic acid and IL is much stronger than that between nitrogen and IL. Moreover, hydrogen bond can be formed between the cation-acetic acid as well as the anion-acetic acid.

关键词： Ionic liquid(IL) Gaseous acetic acid Absorption Process simulation Separation mechanism

A catalyst for the carbonylation of methanol to acetic acid in gaseous phase

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Science China Chemistry 1996年第6期39卷 585-592页

作者：潘平来柳忠阳朱长城袁国卿 Institute of Chemsitry Chinese Academy of Sciences Beijing 100080 China

A novel Rh/Ys catalyst for the carbonylation of methanol to acetic acid in gaseous phase is reported. The porous carbon beads (Ys) prepared from the carbonation of poly(vinylidene chloride) were used as the support. This catalyst has a specific surface area of 1 000 m2/g, high mechanical strength and thermal stability. The average diameter of the pore is in the range of 0.8 - 1.2nm. Experimental evidence showed that this catalyst was of high activity and selectivity, which could compare to those of the homogeneous catalyst from Monsanto. The catalytic rate could get to 900 g AcOH/g Rh·h during the carbonylation of methanol to acetic acid. The fine spreading of Ph over the Ys surface is the key factor for the activity.

关键词： supported catalyst acetic acid carbonylation rhodium.

Short-term effect of Salvia miltiorhiza in treating rat acetic acid chronic gastric ulcer and long-term effect in preventing recurrence

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World Journal of Gastroenterology 1998年第2期4卷 77-78页

作者： Wang, GZ Ru, X Ding, LH Li, HQ First Affiliated Hosp Qiqihaer Med Coll Dept Pathophysiol Qiqihaer 161042 Heilongjiang Peoples R China First Affiliated Hosp Qiqihaer Med Coll Dept Surg Qiqihaer 161042 Heilongjiang Peoples R China China Med Univ Dept Pathophysiol Shenyang 110001 Liaoning Peoples R China

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关键词： Danshen disease models, animal Salvia miltiorrhiza stomach ulcer acetic acid cimitidine gastric mucosa recurrence rats , Wistar chronic diseases

Catalytic Hydrogenation of acetic Acid to Acetaldehyde: Synergistic Effect of Bifunctional Co/Ce-Fe Oxide Solid Solution Catalysts

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Chinese Journal of Chemistry 2019年第7期37卷 709-719页

作者： Naixu Li Qi Zhang Rehana Bibi Quanhao Shen Richard Ngulube Yunyi Liu Jiancheng Zhou School of Chemistry and Chemical Engineering Southeast University Nanjing Jiangsu 211189 China Jiangsu Key Laboratory for Biomass Energy and Material Nanjing Jiangsu 210042 China Jiangsu Province Hi-Tech Key Laboratory for Bio-medical Research Southeast University Nanjing Jiangsu 211189 China

The large-scale industrial production of acetic acid (HAc) from carbonylation of methanol has enabled intense research interest from direct hydrogenation of HAc to acetaldehyde (AA).Herein,a series of cerium-iron oxide solid solution supported metallic cobalt catalysts were prepared by modified sol-gel method and were applied in gas-phase hydrogenation of HAc to AA.A synergistic effect between the hydrogenation metal cobalt and Ce-Fe oxide solid solution is revealed.Specifically,oxygen vacancies provide the active sites for adsorption of HAc,while highly uniformly dispersed metallic Co adsorbs H2 and activates the reduction of HAc into AA.Moreover,the metallic Co can also assist the cyclical conversion between Fe3+/Fe2+ and Ce3+/Ce4+ on the surface of Ce1.xFexO2-δ supports.The unique effect substantially enhances the ability of the support material to rapidly capture oxygen atoms from HAc.It is found that the catalyst of 5% Co/Ce0.8Fe0.2O2-δ with the highest concentration of oxygen vacancy presents the best catalytic performance (i.***.acetaldehyde yield reaches 49.9%) under the optimal reaction conditions (i.e.623 K and H2 flow rate =10 mL/min).This work indicates that the Co/Ce-Fe oxide solid solution catalyst can be potentially used for the selective hydrogenation from HAc to AA.The synergy between the metallic Co and Ce1-xFexO2-δ revealed can be extended to the design of other composite catalysts.

关键词： acetic Acid Acetaldehyde Oxide Solid Solution Catalysts

A Computational Study on Iridium-Catalyzed Production of acetic Acid from Ethanol and Water Solution

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Chinese Journal of Chemistry 2019年第9期37卷 883-886,I0002页

作者： Xin Yue Longfei Li Pengjie Li Chenguang Luo Min Pu Zuoyin Yang Ming Lei State Key Laboratory of Chemical Resource Engineering Institute of Computational ChemistryCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029China College of Pharmaceutical Science Hebei UniversityBaodingHebei 071002China

The mechanism for the production of acetic acid from ethanol and water mixture catalyzed by iridium catalyst has been theoretically investigated.The cooperation of the iridium center and bpyO ligand is highlighted,which plays an important role in the catalytic activity.The hydrogen release from the iridium center is the rate-determining step,with an energy barrier of 22.5 kcal/mol.The electronic structure analysis suggests electron-donating substituents could decrease the energy barrier.

关键词： Iridium-Catalyzed Production acetic Acid Ethanol Water Solution

Kinetic studies on vapor phase carbonylation of methanol to acetic acid over Rh/Ys catalyst

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Science China Chemistry 1997年第1期40卷 45-52页

作者：柳忠阳潘平来朱长城袁国卿 Institute of Chemistry Chinese Academy of SciencesBeijing 100080China

A novel catalyst Rh/Ys for the carbonylation of methanol to acetic acid with CH3I as the promoter shows excellent activity and selectivity.The reaction is kinetically controlled.The reaction rate is in proportion to the concentration of Rh and CH3I but has nothing to do with those of CH3OHH and CO.The surface active energy is Ea ~51.02 kJ/mol.A mechanism is also proposed.

关键词： methanol carbonyiation acetic acid kinetics

Photosynthetic conversion of CO_2 to acetic acid by an inorganic-biological hybrid system

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Science China Materials 2016年第2期59卷 93-94页

作者： Yadong Li Department of Chemistry and Collaborative Innovation Center for Nanomaterial Science and Engineering Tsinghua University

Since 7000 BCE,humans have fermented sugars into ethanol,and since work by Louis Pasteur in the 1850s,we have known that microorganisms are responsible for this miraculous feat of chemical synthesis[1].Since then,the ability of biological organisms to cheaply and selectively transform chemicals into useful products has been exploited on a global scale from agriculture to biotechnological synthesis of pharmaceutical compounds.Recently,pho-

关键词： Pasteur pharmaceutical chemicals acetic inorganic agriculture ethanol hazardous permission itself