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

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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Two-step hydrothermal conversion of biomass waste to humic acid using hydrochar as intermediate

《环境科学与工程前沿（英文）》 2023年 第17卷 第10期 doi: 10.1007/s11783-023-1719-8

摘要： Converting biomass materials to humic acid is a sustainable method for humic acid production and achieve biomass valorization. A two-step hydrothermal treatment method was adopted in this study to produce humic acid from corn stalks. In the first step of the process, hydrochar was prepared at different hydrothermal temperatures and pH values. Their chemical properties were then analyzed, and the hydrochar-derived humic acids were produced under alkaline hydrothermal conditions (denoted as HHAalk). The hydrochar, prepared under high temperature (200 °C) and strong acidic (pH 0) conditions, achieved high HHAalk yields (i.e., 67.9 wt% and 68.8 wt% calculated based on weight of hydrochar). The sources of HHAalk formation were as follows: 1) production in the hydrochar preparation stage, and 2) increment under the alkaline hydrothermal treatment of hydrochar. The degree of hydrochar unsaturation was suggested as an indicator for evaluating the hydrochar humification potential under alkaline hydrothermal conditions. This study provides an important reference for the preparation of suitable hydrochar with high hydrothermal humification potential.

关键词： Biowaste     Hydrochar     Humic acid     Hydrothermal parameter     Unsaturation    

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Nitrogen distribution in the products from the hydrothermal liquefaction of sp. and sp.

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 985-995 doi: 10.1007/s11705-021-2126-y

摘要： The high contents of nitrogen-containing organic compounds in biocrude obtained from hydrothermal liquefaction of microalgae are one of the most concerned issues on the applications and environment. In the project, Chlorella sp. and Spirulina sp. were selected as raw materials to investigate the influence of different reaction conditions (i.e., reaction temperature, residence time, solid loading rate) on the distribution of nitrogen in the oil phase and aqueous phase. Three main forms of nitrogen-containing organic compounds including nitrogen-heterocyclic compounds, amide, and amine were detected in biocrudes. The contents of nitrogen-heterocyclic compounds decreased with temperature while amide kept increasing. The effect of residence time on the components of nitrogen-containing organic compounds was similar with that of temperature. However, the influence of solid loading rate was insignificant. Moreover, it was also found that the differences of amino acids in the protein components in the two microalgae might affect the nitrogen distribution in products. For example, nitrogen in basic amino acids of Spirulina sp. preferred to go into the aqueous phase comparing with the nitrogen in neutral amino acids of Chlorella sp. In summary, a brief reaction map was proposed to describe the nitrogen pathway during microalgae hydrothermal liquefaction.

关键词： microalgae     hydrothermal liquefaction     biocrude     nitrogen distribution    

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ASSESSMENT OF HEAVY METALS IN HYDROCHAR PRODUCED BY HYDROTHERMAL CARBONIZATION OF DAIRY MANURE

《农业科学与工程前沿（英文）》 2023年 第10卷 第3期   页码 437-447 doi: 10.15302/J-FASE-2023507

摘要：

● Content of heavy metals in hydrochar varies considerably, from 50% to 100%.

关键词： heavy metals     dairy manure     hydrochar     hydrothermal carbonization     waste management    

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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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Enhanced dewatering characteristics of waste activated sludge with Fenton pretreatment: effectiveness

Guangyin ZHEN, Xueqin LU, Baoying WANG, Youcai ZHAO, Xiaoli CHAI, Dongjie NIU, Tiantao ZHAO

《环境科学与工程前沿（英文）》 2014年 第8卷 第2期   页码 267-276 doi: 10.1007/s11783-013-0530-3

摘要： In this work, the enhanced dewaterabing characteristics of waste activated sludge using Fenton pretreatment was investigated in terms of effectiveness and statistical optimization. Response surface method (RSM) and central composite design (CCD) were applied to evaluate and optimize the effectiveness of important operational parameters, i.e., H O concentrations, Fe concentrations and initial pH values. A significant quadratic polynomial model was obtained ( 0.9189) with capillary suction time (CST) reduction efficiency as the response. Numerical optimization based on desirability function was carried out. The optimum values for H O , Fe , and initial pH were found to be 178 mg·g VSS (volatile suspended solids), 211 mg·g VSS and 3.8, respectively, at which CST reduction efficiency of 98.25% could be achieved. This complied well with those predicted by the established polynomial model. The results indicate that Fenton pretreatment is an effective technique for advanced waste activated sludge dewatering. The enhancement of sludge dewaterability by Fenton’s reagent lies in the migration of sludge bound water due to the disintegration of sludge flocs and microbial cells lysis.

关键词： Fenton pretreatment     response surface methodology (RSM)     capillary suction time (CST)     dewaterabilty     molecular weight distribution    

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Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 95-103 doi: 10.1007/s11705-014-1405-2

摘要： Titanium-containing mesoporous materials (Ti-MCM-41) were obtained by hydrothermal synthesis. Such materials are active catalysts for the transesterification of dimethyl oxalate and phenol to produce diphenyl oxalate. To understand the role of the Ti in the catalytic process, Ti-MCM-41 samples with different Si/Ti ratios (from 5 to 100) were prepared and the samples were analyzed by Fourier transform infrared spectroscopy, UV-visible spectroscopy, and ammonia temperature programmed desorption. It was concluded that the Ti is incorporated into the framework of the MCM-41 and formed weak Lewis acid sites. In addition, the number of Ti(IV) sites increased as the amount of titanium increased. X-ray powder diffraction, N adsorption-desorption and transmission electron microscopy results showed that the Ti-MCM-41 samples have a hexagonal arrangement of mono-dimensional pores. A large number of Ti(IV) sites coupled with the mesoporous structure and large pore diameters are favorable for the transesterification catalytic properties of Ti-MCM-41.

关键词： Ti-MCM-41     mesoporous molecular sieve     acid sites     transesterification     hydrothermal synthesis    

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Underlying mechanism of the hydrothermal instability of Cu

Nadeen Al-Janabi,Abdullatif Alfutimie,Flor R. Siperstein,Xiaolei Fan

《化学科学与工程前沿（英文）》 2016年 第10卷 第1期   页码 103-107 doi: 10.1007/s11705-015-1552-0

摘要： Water induced decomposition of Cu (BTC) (BTC= benzene-1,3,5-tricarboxylate) metal-organic framework (MOF) was studied using dynamic water vapour adsorption. Small-angle X-ray scattering, Fourier transform infrared spectroscopy and differential scanning calorimetry analyses revealed that the underlying mechanism of Cu (BTC) MOF decomposition under humid streams is the interpenetration of water molecules into Cu-BTC coordination to displace organic linkers (BTC) from Cu centres.

关键词： hydrothermal stability     metal-organic framework (MOF)     open metal sites (OMSs)     dynamic water vapour adsorption    

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Effects of metal ions on the morphology of calcium sulfate hemihydrate whiskers by hydrothermal method

Tianjie Liu, Hao Fan, Yanxia Xu, Xingfu Song, Jianguo Yu

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 545-553 doi: 10.1007/s11705-017-1665-8

摘要： The effects of Na , Mg , Al and Fe ion concentrations on the crystal morphology of calcium sulfate hemihydrate whiskers formed via a hydrothermal method have been studied. In the presence of Al concentrations higher than 1×10 mol/L the whiskers were significantly shorter and thicker and the presence of Mg and Fe resulted in shorter whiskers. The presence of Na did not affect the morphology of the whiskers. Through elemental analysis, it was determined that Mg and Al were selectively adsorbed on the surfaces of the crystals, whereas Fe underwent a hydrolysis reaction to form a brown precipitate which decreased the ion concentration in the solution. These results indicate that in raw materials used for the industrial preparation of calcium sulfate whiskers, Al and Fe should be removed and the Mg concentration should be less than 8 × 10 mol/L in order to obtain pure whiskers with high aspect ratios.

关键词： metal ions     morphology     calcium sulfate hemihydrate whiskers     hydrothermal method     selective adsorption    

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Biological pretreatment of corn stover by solid state fermentation of

Jian ZHANG, Xin REN, Wenqun CHEN, Jie BAO

《化学科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 146-151 doi: 10.1007/s11705-012-1220-6

摘要： Biological pretreatment is a promising way to overcome the biorecalcitrance of cleaving the supermolecular structure of lignocellulose by lignin degrading enzymes from microorganisms. Solid state fermentation of corn stover with the white-rot fungus was carried out and the efficiency of this pretreatment was evaluated. The enzymatic hydrolysis yield reached a maximum when the corn stover was biologically pretreated for nine days, and the hydrolysis yield decreased sharply if the solid state fermentation was carried out for more than nine days. A possible explanation for this sharp decrease is that not only the lignin degrading enzymes (LiP and MnP) were secreted, but also other metabolites, which were toxic or fatal to the hydrolysis enzymes resulting in the lower hydrolysis yield were generated during the prolonged period of biopretreatment. These results are useful to help determine the optimal timing and to understand the lignin structure and degradation mechanism in biological pretreatment processes.

关键词： biological pretreatment     Phanerochaete chrysosporium     solid state fermentation     biorecalcitrance     hydrolysis yield    

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木质纤维原料制乙醇原料预处理技术

靳胜英,张福琴,张礼安

《中国工程科学》 2008年 第10卷 第11期   页码 82-88

摘要：

从预处理的必要性出发，论述了木质纤维原料的预处理技术，分析了主要预处理技术的特点和处理纤维质原料的效果，并对未来预处理技术的发展方向提出了建议，供从事木质纤维素制乙醇的研究人员参考。

关键词： 木质纤维原料     乙醇     预处理技术    

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Hydrothermal treatment of MSWI fly ash for simultaneous dioxins decomposition and heavy metal stabilization

Jinlong XIE, Yuyan HU, Dezhen CHEN, Bin ZHOU,

《环境科学与工程前沿（英文）》 2010年 第4卷 第1期   页码 108-115 doi: 10.1007/s11783-010-0013-8

摘要： Researches on the hydrothermal treatment of municipal solid waste incineration (MSWI) fly ash were conducted to eliminate dioxins and stabilize heavy metals. In order to enhance decomposing polychlorinated dibenzo-dioxins (PCDDs) and polychlorinated dibenzo-furans (PCDFs) during hydrothermal process, a strong reductant carbohydrazide (CHZ) is introduced. A hydrothermal reactor was set up by mixing raw MSWI fly ash or the pre-treated fly ash with water and then heated to a pre-set temperature; CHZ was spiked into solution according to specially defined dosage. Experimental results showed that under the temperatures of 518K and 533K, the decomposition rates of PCDDs/PCDFs were over 80% and 90%, respectively, by total concentration. However, their toxic equivalent (TEQ) decreased only slightly or even increased due to the rising in concentration of congeners 2, 3, 7, 8-TCDD/TCDF, which might be resulted from the highly chlorinated congeners losing their chlorine atoms and being degraded during the hydrothermal process. Better results of TEQ reduction were also obtained under the higher tested temperature of 533K and reactor with addition of 0.1%wt CHZ was corresponded to the best results. Good stabilization of heavy metals was also obtained in the same hydrothermal process especially when ferrous sulphate was added as auxiliary agent.

关键词： municipal solid wastes incineration (MSWI)     fly ashes     polychlorinated dibenzo-dioxins (PCDDs)     polychlorinated dibenzo-furans (PCDFs)     hydrothermal     heavy metal stabilization    

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Thermochemical pretreatment of meat and bone meal and its effect on methane production

Guangxue WU , Zhenhu HU , Mark G. HEALY , Xinmin ZHAN ,

《环境科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 300-306 doi: 10.1007/s11783-009-0031-6

摘要： Since the solubilization of meat and bone meal (MBM) is a prerequisite in many MBM disposal approaches, enhancement of the solubilization by means of thermochemical pretreatment was investigated in this study at two temperatures (55°C and 131°C) and six sodium hydroxide (NaOH) concentrations (0, 1.25, 2.5, 5, 10 and 20g/L). The MBM volatile solid (VS) reduction ratio was up to 66% and 70% at 55°C and 131°C, respectively. At the same temperature, the VS reduction ratio increased with the increase in the dosage of NaOH. The study on the methane (CH) production potential of pretreated MBM shows that the addition of NaOH at 55°C did not cause the inhibition of the succeeding CH production process. However, CH production was inhibited by the addition of NaOH at 131°C. The CH production potential was in the range of 389 to 503mL CH/g VS MBM and 464 to 555mL CH/g VS MBM at 55°C and 131°C, respectively.

关键词： thermochemical pretreatment     meat and bone meal     solid reduction     solid solubilization     methane production potential    

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Preparation and characterization of ZnO/ZnS hybrid photocatalysts via microwave-hydrothermal method

ZHAO Jinglian, WANG Xinping, ZHAO Liang

《环境科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 415-420 doi: 10.1007/s11783-008-0056-2

摘要： The photocatalytic performance of ZnO/ZnS hybrid nanocomposite was largely higher than that of the mere ZnO or ZnS nanoparticles, but the complicated procedure and misdistribution of final products limited its large-scale productions. The exploration of a novel synthesis route of ZnO/ZnS hybrid photocatalysts with high catalytic performance is becoming a crucial step for the large-scale application of ZnO/ZnS hybrid photocatalytic technique. Preparation and characterization of nanosized ZnO/ZnS hybrid photocatalysts were studied in this paper. The photocatalysts were obtained via microwave-hydrothermal crystallization with the help of sodium citrate. The products were characterized by X-ray diffraction (XRD), transmission electron microscopy (TEM), particle size distribution (PSD), and Fourier transformed infrared spectroscopy (FT-IR). The results indicated that so-synthesized ZnO/ZnS samples consisted of the high pure cubic (sphalerite) ZnS and hexagonal ZnO nanocrystallines with a narrow particle size distribution. The possible formation mechanisms of ZnO/ZnS nanocrystallines were mainly attributed to the superficially protective effect of citrate. The photocatalytic experiments demonstrated that the ZnO/ZnS photocatalysts exhibited a higher catalytic activity for the degradation of acid fuchsine than other monocomponents.

关键词： large-scale     hexagonal     misdistribution     characterization     nanocomposite    

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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要： Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词： extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

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标题 作者 时间 类型 操作

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

Milan Malhotra, Anurag Garg

期刊论文

Two-step hydrothermal conversion of biomass waste to humic acid using hydrochar as intermediate

期刊论文

Nitrogen distribution in the products from the hydrothermal liquefaction of sp. and sp.

期刊论文

ASSESSMENT OF HEAVY METALS IN HYDROCHAR PRODUCED BY HYDROTHERMAL CARBONIZATION OF DAIRY MANURE

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

Enhanced dewatering characteristics of waste activated sludge with Fenton pretreatment: effectiveness

Guangyin ZHEN, Xueqin LU, Baoying WANG, Youcai ZHAO, Xiaoli CHAI, Dongjie NIU, Tiantao ZHAO

期刊论文

Ti incorporation in MCM-41 mesoporous molecular sieves using hydrothermal synthesis

Shengping WANG, Changqing MA, Yun SHI, Xinbin MA

期刊论文

Underlying mechanism of the hydrothermal instability of Cu

Nadeen Al-Janabi,Abdullatif Alfutimie,Flor R. Siperstein,Xiaolei Fan

期刊论文

Effects of metal ions on the morphology of calcium sulfate hemihydrate whiskers by hydrothermal method

Tianjie Liu, Hao Fan, Yanxia Xu, Xingfu Song, Jianguo Yu

期刊论文

Biological pretreatment of corn stover by solid state fermentation of

Jian ZHANG, Xin REN, Wenqun CHEN, Jie BAO

期刊论文

木质纤维原料制乙醇原料预处理技术

靳胜英,张福琴,张礼安

期刊论文

Hydrothermal treatment of MSWI fly ash for simultaneous dioxins decomposition and heavy metal stabilization

Jinlong XIE, Yuyan HU, Dezhen CHEN, Bin ZHOU,

期刊论文

Thermochemical pretreatment of meat and bone meal and its effect on methane production

Guangxue WU , Zhenhu HU , Mark G. HEALY , Xinmin ZHAN ,

期刊论文

Preparation and characterization of ZnO/ZnS hybrid photocatalysts via microwave-hydrothermal method

ZHAO Jinglian, WANG Xinping, ZHAO Liang

期刊论文

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

期刊论文