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Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1389-1398 doi: 10.1007/s11705-022-2285-5

摘要： Hydrothermal and catalytic stability of UIO-66 MOFs with defective structures are critical aspects to be considered in their catalytic applications, especially under the conditions involving water, moisture and/or heat. Here, we report a facile strategy to introduce the macromolecular acid group to UIO-66 to improve the stability of the resulting UIO-66−PhSO3H MOF in aqueous phase catalysis. In detail, UIO-66−PhSO3H was obtained by grafting benzenesulfonic acid on the surface of the pristine UIO-66 to introduce the hydrophobicity, as well as the Brønsted acidity, then assessed using catalytic hydrolysis of cyclohexyl acetate (to cyclohexanol) in water. The introduction of hydrophobic molecules to UIO-66 could prevent the material from being attacked by hydroxyl polar molecules effectively, explaining its good structural stability during catalysis. UIO-66−PhSO3H promoted the conversion of cyclohexyl acetate at ca. 87%, and its activity and textural properties were basically intact after the cyclic stability tests. The facile modification strategy can improve the hydrothermal stability of UIO-66 significantly, which can expand its catalytic applications in aqueous systems.

关键词： metal−organic frameworks (MOFs)     UIO-66     hydrolysis of cyclohexyl acetate     hydrophobicity     Brønsted acidity    

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Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

《环境科学与工程前沿（英文）》 2022年 第16卷 第4期 doi: 10.1007/s11783-021-1476-5

摘要：

• MES was constructed for simultaneous ammonia removal and acetate production.

关键词： Biocathode     Carbon dioxide     Electrochemical oxidation     Graphite anode     Boron-doped diamond    

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Durable and recyclable BiOBr/silk fibroin-cellulose acetate composite film for efficient photodegradation

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1765-1775 doi: 10.1007/s11705-023-2323-y

摘要： A stable and recyclable of BiOBr/silk fibroin-cellulose acetate composite film was prepared by blending-wet phase transformation and in situ precipitate technology. The cellulose acetate film modified by silk fibroin formed a finger-shaped porous structure, which provided a large space for the uniform growth of BiOBr nanosheets and facilitated the shuttle flow of dyes in film. The morphology, phase structure, and optical properties of the composite films were characterized using various techniques, and their photocatalytic performance for dye wastewater was evaluated under visible light irradiation. Results showed that the BiOBr/SF-CA composite film exhibited efficient photocatalytic activity with 99.9% of rhodamine B degradation rate. Moreover, the composite film maintained high catalytic stability because Bi as the active species deposited on the film showed almost no loss. Finally, the possible photocatalytic mechanisms in the BiOBr/SF-CA composite film were speculated through radical-trapping experiments and electron spin resonance testing.

关键词： BiOBr nanosheet     cellulose acetate     silk fibroin     photocatalytic degradation     dye wastewater    

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Methyl acetate–methanol mixture separation by extractive distillation: Economic aspects

Elena Graczová, Branislav Šulgan, Samuel Barabas, Pavol Steltenpohl

《化学科学与工程前沿（英文）》 2018年 第12卷 第4期   页码 670-682 doi: 10.1007/s11705-018-1769-9

摘要：

Methyl acetate is considered low toxicity volatile solvent produced either as a by-product during methanol carbonylation or via acetic acid esterification with methanol. In both cases, pure methyl acetate has to be isolated from the reaction mixture. Simulation of methyl acetate separation from its mixture with methanol by extraction distillation was carried out in ASPEN+ software. In total three case studies were assumed using two different extraction solvents and two solvent regeneration strategies. In case A, novel extraction solvent 1-ethyl-3-methylimidazolium trifluoromethanesulfonate ionic liquid, was considered. Raw material separation was achieved in an extraction distillation column while the solvent regeneration was accomplished in a second distillation column in this case. In case study B, the same extraction solvent was used; however, its regeneration was carried out in a single-effect evaporator. Dimethyl sulfoxide was the second extraction solvent selected. Its use in methyl acetate-methanol separation is presented in case study C. As high purity of dimethyl sulfoxide was required for the methyl acetate-methanol azeotrope breaking, its regeneration was carried out in the second distillation column only. To simulate the ternary methyl acetate–methanol–extraction solvent mixtures separation, vapor–liquid equilibrium was predicted based on the NRTL equation. Further, unknown properties of the considered ionic liquid and variation of these properties with temperature were predicted and introduced into the ASPEN+ components properties database. Based on these data, optimum operation parameters of the respective separation equipment were established. In all case studies, the same condition had to be fulfilled, namely minimum methyl acetate content in the distillate from the extraction distillation column of 99.5mol-%. Results of simulations using the respective optimum operation parameters were employed in the economic evaluation of the three separation unit designs studied. It was found that the least energy-demanding design corresponds to the case study B in terms of both capital as well as operation expenses.

关键词： methyl acetate     1-ethyl-3-methylimidazolium trifluoromethanesulfonate     extraction distillation     dimethyl sulfoxide     economic evaluation    

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Kinetic studies of xylan hydrolysis of corn stover in a dilute acid cycle spray flow-through reactor

Hongman ZHANG, Qiang JIN, Rui XU, Lishi YAN, Zengxiang LIN

《化学科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 252-257 doi: 10.1007/s11705-010-1010-y

摘要： Xylan of corn stover was pretreated with 1%, 2% and 3% (w/w) sulfuric acid at relatively low temperatures (90°C, 95°C and 100°C) in a dilute acid cycle spray flow-through reactor (DCF). The hydrolysis of xylan to its monomeric xylose was modeled by a series of first-order reactions. Both biphasic and Saeman hydrolysis models were applied to fit the experimental data. The results confirmed that the kinetic data of xylan hydrolysis fitted a first-order irreversible reaction model and the experimental data. The reaction rates of xylose monomer formation and degradation were sensitive to catalyst concentration and temperature. Higher catalyst concentration and lower reaction temperature result in high xylose yield. The activation energy for xylose formation and degradation were determined to be 112.9 and 101.0 kJ·mol , respectively. Over 90% theoretical xylose obtained from corn stover can be used to produce ethanol, xylitol and fumaric acid by fermentation.

关键词： corn stover     xylan hydrolysis     biphasic model     Saeman model     cycle spray     kinetics    

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Research progress on hydrothermal dissolution and hydrolysis of lignocellulose and lignocellulosic waste

Yan ZHAO, Wenjing LU, Jiajun CHEN, Xiangfeng ZHANG, Hongtao WANG

《环境科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 151-161 doi: 10.1007/s11783-013-0607-z

摘要： Ethanol production from lignocellulosic waste has attracted considerable attention because of its feasibility and the generation of valuable products. Previous studies have shown that pretreatment and hydrolysis are key processes for lignocellulose conversion. Hydrothermal process is a promising technique because of its efficiency to break down the lignocellulosic structures and produce fermentable hexoses. Most studies in this field have therefore focused on understanding these processes or optimizing the parameters, but commonly reported low yields of fermentable hexoses. The inability to produce high yields of fermentable hexoses is mainly attributed to inadequate information on the conversion mechanisms of lignocellulose, particularly the reaction rules of dissolution, which is a limiting step in the entire conversion process. This paper critically reviewed the progress done in the research and development of the hydrothermal dissolution and hydrolysis of lignocellulose. Principles, processes, and related studies on separate dissolution and asynchronous hydrolysis of lignin, hemicellulose, and cellulose are presented. Potential research prospects are also suggested.

关键词： lignocellulosic waste     hydrothermal conversion     separate dissolution     asynchronous hydrolysis     mechanism    

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Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

《环境科学与工程前沿（英文）》 2016年 第10卷 第6期 doi: 10.1007/s11783-016-0872-8

摘要： ? The Cu–Ni/γ-Al O catalyst was prepared to study HCN hydrolysis ? On catalyst calcined at 400°C, the HCN removal efficiency reaches a maximum. ? HCN removal is the highest at 480 min at a H O/HCN volume ratio of 150 ? The presence of CO facilitates HCN hydrolysis and increases NH production. ? O increases the HCN removal and NO production but decreases NH production GRAPHIC ABSTRACT To decompose efficiently hydrogen cyanide (HCN) in exhaust gas, g-Al O -supported bimetallic-based Cu–Ni catalyst was prepared by incipient-wetness impregnation method. The effects of the calcination temperature, H O/HCN volume ratio, reaction temperature, and the presence of CO or O on the HCN removal efficiency on the Cu–Ni/g-Al O catalyst were investigated. To examine further the efficiency of HCN hydrolysis, degradation products were analyzed. The results indicate that the HCN removal efficiency increases and then decreases with increasing calcination temperature and H O/HCN volume ratio. On catalyst calcined at 400°C, the efficiency reaches a maximum close to 99% at 480 min at a H O/HCN volume ratio of 150. The HCN removal efficiency increases with increasing reaction temperature within the range of 100°C–500°C and reaches a maximum at 500°C. This trend may be attributed to the endothermicity of HCN hydrolysis; increasing the temperature favors HCN hydrolysis. However, the removal efficiencies increases very few at 500°C compared with that at 400°C. To conserve energy in industrial operations, 400°C is deemed as the optimal reaction temperature. The presence of CO facilitates HCN hydrolysis andincreases NH production. O substantially increases the HCN removal efficiency and NO production but decreases NH production.

关键词： Hydrogen cyanide     Cu–Ni/g-Al2O3     Catalytic hydrolysis    

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Establishment and verification of a shrinking core model for dilute acid hydrolysis of lignocellulose

Cunwen WANG, Xiaoling DUAN, Weiguo WANG, Zihao LI, Yuanhang QIN

《能源前沿（英文）》 2012年 第6卷 第4期   页码 413-419 doi: 10.1007/s11708-012-0212-z

摘要： The kinetics of lignocellulose hydrolysis under the conditions of high temperature and dilute acid (mass fraction 0.05%) was investigated in this paper. By studying the reducing sugar concentration versus reaction temperature (170°C–220°C) and reaction time (150–1800 s) during the hydrolysis process of five kinds of crop straw (rice, wheat, cotton, rape and corn), the shrinking core model was established, and the differential equation of the model and its analytical solution were obtained. With a numerical calculation method, the kinetic equation was estimated, and the degradation of reducing sugar obeyed first-order kinetics was obtained. The calculated results from the equations agreed well with the original experimental data. The calculation by the model showed that the reducing sugar concentration increases as the size of the particles decrease, and the uniform particles increase.

关键词： lignocellulose     dilute acid hydrolysis     shrinking core model    

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Characterization of value-added chemicals derived from the thermal hydrolysis and wet oxidation of sewage

Milan Malhotra, Anurag Garg

《环境科学与工程前沿（英文）》 2021年 第15卷 第1期 doi: 10.1007/s11783-020-1305-2

摘要： Abstract • Hydrothermal treatment can greatly improve resource recovery from sewage sludge. • tCOD removal during WO was ~55% compared with ~23% after TH. • TOC solubilization during hydrothermal treatment followed first-order kinetics. • Solids and carbon balance confirmed loss of organics during thermal hydrolysis. • Reaction pathways for thermal hydrolysis and wet oxidation are proposed. We evaluated the effect of hydrothermal pretreatments, i.e., thermal hydrolysis (TH) and wet oxidation (WO) on sewage sludge to promote resource recovery. The hydrothermal processes were performed under mild temperature conditions (140°C–180°C) in a high pressure reactor. The reaction in acidic environment (pH= 3.3) suppressed the formation of the color imparting undesirable Maillard’s compounds. The oxidative conditions resulted in higher volatile suspended solids (VSS) reduction (~90%) and chemical oxygen demand (COD) removal (~55%) whereas TH caused VSS and COD removals of ~65% and ~27%, respectively at a temperature of 180°C. During TH, the concentrations of carbohydrates and proteins in treated sludge were 400–1000 mg/L and 1500–2500 mg/L, respectively. Whereas, WO resulted in solids solubilization followed by oxidative degradation of organics into smaller molecular weight carboxylic acids such as acetic acid (~400–500 mg/L). Based on sludge transformation products generated during the hydrothermal pretreatments, simplified reaction pathways are predicted. Finally, the application of macromolecules (such as proteins), VFAs and nutrients present in the treated sludge are also discussed. The future study should focus on the development of economic recovery methods for various value-added compounds.

关键词： Hydrothermal pretreatment     Reaction kinetics     Reaction pathway     Sewage sludge     Thermal hydrolysis     Wet oxidation    

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Catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over the

Zhidan Fu, Lisha Liu, Yong Song, Qing Ye, Shuiyuan Cheng, Tianfang Kang, Hongxing Dai

《化学科学与工程前沿（英文）》 2017年 第11卷 第2期   页码 185-196 doi: 10.1007/s11705-017-1631-5

摘要： The Pd catalyst supported on cryptomelane-type manganese oxide octahedral molecular sieve (OMS-2) were prepared. The effect of Pd loading on the catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over Pd/OMS-2 has been investigated. The results show that the Pd loading plays an important role on the physicochemical properties of the Pd/OMS-2 catalysts which outperform the Pd-free counterpart with the 0.5Pd/OMS-2 catalyst being the best. The temperature for 50% conversion was 25, 240 and 160 °C, and the temperature for 90% conversion was 55, 285 and 200 °C for oxidation of CO, toluene, and ethyl acetate, respectively. The low-temperature reducibility and high oxygen mobility of Pd/OMS-2 are the factors contributable to the excellent catalytic performance of 0.5Pd/OMS-2.

关键词： cryptomelane-type manganese oxide octahedral molecular sieve     oxygen mobility     reducibility     carbon monoxide oxidation     volatile organic compound combustion    

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Microwave-assisted catalyst-free hydrolysis of fibrous cellulose for deriving sugars and biochemicals

Songshan Jiang, Helen Daly, Huan Xiang, Ying Yan, Huiping Zhang, Christopher Hardacre, Xiaolei Fan

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 718-726 doi: 10.1007/s11705-019-1804-5

摘要： Microwave (MW) assisted catalyst-free hydrolysis of fibrous cellulose (FC, cellulolysis) at 200°C promoted a cellulose conversion of ca 37.2% and quantitative production of valuable C5/C6 sugars (e.g , glucose) and the according platform biochemicals (e.g , 5-hydroxymethylfurfural), corresponding to an overall selectivity of 96.5%. Conversely, conventional hydrothermal cellulolysis under similar conditions was not effective, even after 24 h, carbonising the FC. Based on the systematic study of MW-assisted cellulolysis, the specific interaction between water molecules and macroscopic FC under the MW irradiation was proposed, accounting for the interpretation of the experimental observation. The kinetic energy of water molecules under the MW irradiation facilitated the C C (in the non-hindered surface CH OH groups) and C O C bond breaking (inside the cellulose cavities) in FC, producing primary cellulolysis products of xylose, glucose and cellobiose.

关键词： microwave     fibrous cellulose     hydrolysis     sugars     mechanism    

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Dissolution and enzymatic hydrolysis of casein micelles studied by dynamic light scattering

LIU Rui, QI Wei, SU Rongxin, ZHANG Yubin, JIN Fengmin, HE Zhimin

《化学科学与工程前沿（英文）》 2007年 第1卷 第2期   页码 123-127 doi: 10.1007/s11705-007-0023-7

摘要： The effects of temperature, ionic strength, and enzymatic hydrolysis on the average hydrodynamic radius () of casein micelles in phosphate buffer were studied by using dynamic light scattering. The results showed that the average value of casein micelles decreased irreversibly during the heating, decreased with the increase of ionic strength in lower ionic strength solution (less than 0.05 mol/L), but opposite in higher ionic strength solution (above 0.1 mol/L). The value of casein increased rapidly during the process of enzymatic hydrolysis, and the structural model of casein micelles in the enzymatic hydrolysis process was also proposed, i.e. the casein micelle changed from compact sphere into unfolded and regularly flocky peptides.

关键词： compact     strength     temperature     regularly flocky     heating    

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Development of combined coagulation-hydrolysis acidification-dynamic membrane bioreactor system for treatment

Xue Shen, Lei Lu, Baoyu Gao, Xing Xu, Qinyan Yue

《环境科学与工程前沿（英文）》 2019年 第13卷 第1期 doi: 10.1007/s11783-019-1093-8

摘要：

• We created a combined system for treating oilfield polymer-flooding wastewater.

• The system was composed of coagulation, hydrolysis acidification and DMBR.

• Coagulant integrated with demulsifier dominated the removal of crude oil.

• The DMBR proceed efficiently without serious membrane fouling.

关键词： Coagulation     Hydrolysis acidification     Dynamic membrane bioreactor     Polymer flooding    

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Energy-efficient recovery of tetrahydrofuran and ethyl acetate by triple-column extractive distillation

Ao Yang, Yang Su, Tao Shi, Jingzheng Ren, Weifeng Shen, Teng Zhou

《化学科学与工程前沿（英文）》 2022年 第16卷 第2期   页码 303-315 doi: 10.1007/s11705-021-2044-z

摘要： An energy-efficient triple-column extractive distillation process is developed for recovering tetrahydrofuran and ethyl acetate from industrial effluent. The process development follows a rigorous hierarchical design procedure that involves entrainer design, thermodynamic analysis, process design and optimization, and heat integration. The computer-aided molecular design method is firstly used to find promising entrainer candidates and the best one is determined via rigorous thermodynamic analysis. Subsequently, the direct and indirect triple-column extractive distillation processes are proposed in the conceptual design step. These two extractive distillation processes are then optimized by employing an improved genetic algorithm. Finally, heat integration is performed to further reduce the process energy consumption. The results indicate that the indirect extractive distillation process with heat integration shows the highest performance in terms of the process economics.

关键词： extractive distillation     solvent selection     conceptual design     process optimization     heat integration    

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Acceleration of the particulate organic matter hydrolysis by start-up stage recovery and its original

Yanqing Duan, Aijuan Zhou, Xiuping Yue, Zhichun Zhang, Yanjuan Gao, Yanhong Luo, Xiao Zhang

《环境科学与工程前沿（英文）》 2021年 第15卷 第1期 doi: 10.1007/s11783-020-1304-3

摘要： Abstract • Carbon availability was partially solved by POM recovery and fermentation. • 12% carbon sources were regenerated by fermentation of the entrapped 35% TCOD. • The unique microbial communities facilitated the efficient hydrolysis of the POM. • Considerable economic benefits in aeration power and ECS dosage were anticipated. To address the availability of carbon sources for denitrification, the accelerated hydrolysis of the most abundant but low-availability fraction of particulate organic matter (POM) was investigated. Mesh sieves with different pore sizes were used as primary pretreatment at the start-up-stage of the biological process to separate some POM from the liquid system. The changes in soluble carbohydrates and proteins were monitored to investigate the hydrolysis performance of the sieved POM, with waste activated sludge (WAS) as the control test. The results showed that an average of 35% POM could be entrapped before filtrate mat development. In addition, benefiting from the high polysaccharides concentration, as well as the high availability due to the relatively loose physical structure, a 23% hydrolysis efficiency of POM was obtained, in contrast to that of WAS (3.4%), with a hydrolysis constant of 0.39 h−1. The prominent performance was also attributed to the unique microbial communities having been domesticated at a lower temperature, especially the cellulose-degrading bacteria Paraclostridium and psychrophile Psychrobacter, making up 6.94% and 2.56%, respectively. Furthermore, the potential benefits and application of improved POM hydrolysis by start-up stage recovery via mesh sieves combined with anaerobic fermentation were evaluated, including selective POM entrapment, alleviation of blockage and wear, and a reduction in aeration energy. By the proposed strategy, carbon availability for biological nutrient removal (BNR) processes is anticipated to be improved more economically than that can be achieved by primary clarifier elimination.

关键词： Particulate organic matter (POM)     Hydrolysis     Microbial community     Mass balance    

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标题 作者 时间 类型 操作

Benzenesulfonic acid-grafted UIO-66 with improved hydrophobicity as a stable Brønsted acid catalyst

期刊论文

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

期刊论文

Durable and recyclable BiOBr/silk fibroin-cellulose acetate composite film for efficient photodegradation

期刊论文

Methyl acetate–methanol mixture separation by extractive distillation: Economic aspects

Elena Graczová, Branislav Šulgan, Samuel Barabas, Pavol Steltenpohl

期刊论文

Kinetic studies of xylan hydrolysis of corn stover in a dilute acid cycle spray flow-through reactor

Hongman ZHANG, Qiang JIN, Rui XU, Lishi YAN, Zengxiang LIN

期刊论文

Research progress on hydrothermal dissolution and hydrolysis of lignocellulose and lignocellulosic waste

Yan ZHAO, Wenjing LU, Jiajun CHEN, Xiangfeng ZHANG, Hongtao WANG

期刊论文

Catalytic hydrolysis of gaseous HCN over Cu–Ni/γ-Al

Linxia Yan, Senlin Tian, Jian Zhou, Xin Yuan

期刊论文

Establishment and verification of a shrinking core model for dilute acid hydrolysis of lignocellulose

Cunwen WANG, Xiaoling DUAN, Weiguo WANG, Zihao LI, Yuanhang QIN

期刊论文

Characterization of value-added chemicals derived from the thermal hydrolysis and wet oxidation of sewage

Milan Malhotra, Anurag Garg

期刊论文

Catalytic oxidation of carbon monoxide, toluene, and ethyl acetate over the

Zhidan Fu, Lisha Liu, Yong Song, Qing Ye, Shuiyuan Cheng, Tianfang Kang, Hongxing Dai

期刊论文

Microwave-assisted catalyst-free hydrolysis of fibrous cellulose for deriving sugars and biochemicals

Songshan Jiang, Helen Daly, Huan Xiang, Ying Yan, Huiping Zhang, Christopher Hardacre, Xiaolei Fan

期刊论文

Dissolution and enzymatic hydrolysis of casein micelles studied by dynamic light scattering

LIU Rui, QI Wei, SU Rongxin, ZHANG Yubin, JIN Fengmin, HE Zhimin

期刊论文

Development of combined coagulation-hydrolysis acidification-dynamic membrane bioreactor system for treatment

Xue Shen, Lei Lu, Baoyu Gao, Xing Xu, Qinyan Yue

期刊论文

Energy-efficient recovery of tetrahydrofuran and ethyl acetate by triple-column extractive distillation

Ao Yang, Yang Su, Tao Shi, Jingzheng Ren, Weifeng Shen, Teng Zhou

期刊论文

Acceleration of the particulate organic matter hydrolysis by start-up stage recovery and its original

Yanqing Duan, Aijuan Zhou, Xiuping Yue, Zhichun Zhang, Yanjuan Gao, Yanhong Luo, Xiao Zhang

期刊论文