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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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Simplistic hydrothermal synthesis approach for fabricating photoluminescent carbon dots and its potential

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 536-547 doi: 10.1007/s11705-022-2239-y

摘要： The past decade has witnessed a variety of members of the carbon family along with exposure of carbon dots due to their magnificent properties in sensing, bioimaging, catalytic applications, biomedical fields, and so on. Herein, we report the simple hydrothermal method to fabricate photoluminescent doped carbon quantum dots for the detection of noxious lead(II) ions. Lead(II) ion is very venomous for both the environment and human health for which its detection is demanded area in the research field. The as-prepared carbon dots show excellent photostability, low toxicity and significant photoluminescence properties along with good water solubility. Along with these properties, carbon dots have a quantum yield of approximately 15%. In the practical field of application, these carbon dots have been used as sensing probes for the detection of lead(II) ions with a detection limit of 60 nmol·L–1. The fluorescence intensity of carbon dots was remarkably quenched in the presence of the lead(II) ion selectively among all the tested metal ions. Furthermore, we have studied the Stern–Volmer relationship for lead(II) quenching along with the explanation of the probable quenching mechanism. Ability of the doped carbon dots in heavy metal ions sensing in an environmental sample was demonstrated.

关键词： carbon dots     fluorescence     heavy metal sensing     practical application     photoluminescence    

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Micro-sized hydrothermal carbon supporting metal oxide nanoparticles as efficient catalyst for mono-dehydration

Cheng PAN, Chao FAN, Wanqin WANG, Teng LONG, Benhua HUANG, Donghua ZHANG, Peigen SU, Aqun ZHENG, Yang SUN

《能源前沿（英文）》 2022年 第16卷 第5期   页码 822-839 doi: 10.1007/s11708-020-0677-0

摘要： Most known catalytic dehydration of sugar alcohols such as D-sorbitol and D-mannitol can only produce di-dehydrated forms as major product, but mono-dehydrated products are also useful chemicals. Moreover, both di- and mono-dehydration demand a high temperature (150°C or higher), which deserves further attentions. To improve the mono-dehydration efficiency, a series of metal-containing hydrothermal carbonaceous materials (HTC) are prepared as catalyst in this work. Characterization reveals that the composition of preparative solution has a key influence on the morphology of HTC. In transformation of D-sorbitol, all HTC catalysts show low conversions in water regardless of temperature, but much better outputs are obtained in ethanol, especially at a higher temperature. When D-mannitol is selected as substrate, moderate to high conversions are obtained in both water and ethanol. On the other hand, high mono-dehydration selectivity is obtained for both sugar alcohols by using all catalysts. The origin of mono-dehydration selectivity and role of carbon component in catalysis are discussed in association with calculations. This study provides an efficient, mild, eco-friendly, and cost-effective system for mono-dehydration of sugar alcohols, which means a lot to development in new detergents or other fine chemicals.

关键词： hydrothermal carbon     morphology     catalyst     mono-dehydration     sugar alcohol    

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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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Synthesis of porous carbon from orange peel waste for effective volatile organic compounds adsorption

《化学科学与工程前沿（英文）》 2023年 第17卷 第7期   页码 942-953 doi: 10.1007/s11705-022-2264-x

摘要： Volatile organic compounds have posed a serious threat to the environment and human health, which require urgent and effective removal. In recent years, the preparation of porous carbon from biomass waste for volatile organic compounds adsorption has attracted increasing attention as a very cost-effective and promising technology. In this study, porous carbon was synthesized from orange peel by urea-assisted hydrothermal carbonization and KOH activation. The role of typical components (cellulose, hemicellulose, and lignin) in pore development and volatile organic compounds adsorption was investigated. Among the three components, hemicellulose was the major contributor to high porosity and abundant micropores in porous carbon. Higher hemicellulose content led to more abundant –COOR, amine-N, and pyrrolic/pyridonic-N in the derived hydrochar, which were favorable for porosity formation during activation. In this case, the toluene adsorption capacity of the porous carbon improved from 382.8 to 485.3 mg·g–1. Unlike hemicellulose, cellulose reduced the >C=O, amine-N, and pyrrolic/pyridonic-N content of the hydrochar, which caused porosity deterioration and worse toluene adsorption performance. Lignin bestowed the hydrochar with slightly increased –COOR, pyrrolic/pyridonic-N, and graphitic-N, and reduced >C=O, resulting in comparatively poor porosity and more abundant micropores. In general, the obtained porous carbon possessed abundant micropores and high specific surface area, with the highest up to 2882 m2·g–1. This study can provide guidance for selecting suitable biomass waste to synthesize porous carbon with better porosity for efficient volatile organic compounds adsorption.

关键词： biomass waste     porous carbon     feedstock composition     urea-assisted hydrothermal carbonization     toluene adsorption     N-doped hydrochar    

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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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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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Revealing the GHG reduction potential of emerging biomass-based CO utilization with an iron cycle system

《环境科学与工程前沿（英文）》 2023年 第17卷 第10期 doi: 10.1007/s11783-023-1727-8

摘要：

● Greenhouse gas mitigation by biomass-based CO2 utilization with a Fe cycle system.

关键词： Carbon dioxide utilization     Hydrothermal reactions     Biomass-based CO2 reduction     Simulation     Ex-ante LCA    

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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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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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Promotional effect of ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2021年 第15卷 第2期 doi: 10.1007/s11783-020-1322-1

摘要： Abstract • K+ hinder the structural degradation of Cu/SAPO-34 under humid condition<100°C. • K+ on Cu/SAPO-34 brings lower acidity and inferior SCR activity at high temperature. • Fe/Beta was used to compensate the low activity of Cu/SAPO-34 at high temperature. • The hybrid catalysts with KCu/SAPO-34 and Fe/Beta show a great potential for using. K ions were introduced onto Cu/SAPO-34 catalysts via the ion-exchange process in order to improve their stability under low-temperature hydrothermal aging. The changes in structure and copper-species contents of these catalysts upon hydrothermal aging were probed in order to investigate their effects on selective catalytic reduction (SCR) activity. For the fresh Cu/SAPO-34 catalysts, K ions had little influence on the chabazite framework but effected their acidities by exchanging with acid sites. After hydrothermal aging, the structural integrity and amount of active sites decreased on pure Cu/SAPO-34. While the K-loaded catalysts showed improved chabazite structure, acidity, and active site conservation with increasing K loading. However, although the 0.7 wt% K catalyst maintained the same crystallinity, active site abundance, and low-temperature SCR activity as the fresh catalyst upon aging, an apparent decrease in SCR activity at high temperature was observed because of the inevitable decrease in the number of Brönsted acid sites. To compensate for the activity disadvantage of K-loaded Cu/SAPO-34 at high temperature, Fe/Beta catalysts were co-employed with K-loaded Cu/SAPO-34, and a wide active temperature window of SCR activity was obtained. Thus, our study reveals that a combined system comprising Fe/Beta and K-loaded Cu/SAPO-34 catalysts shows promise for the elimination of NOx in real-world applications.

关键词： Selective catalytic reduction     Cu/SAPO-34 catalyst     Ion-exchanged K     Low-temperature hydrothermal stability     Fe/Beta catalyst    

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标题 作者 时间 类型 操作

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

期刊论文

Simplistic hydrothermal synthesis approach for fabricating photoluminescent carbon dots and its potential

期刊论文

Micro-sized hydrothermal carbon supporting metal oxide nanoparticles as efficient catalyst for mono-dehydration

Cheng PAN, Chao FAN, Wanqin WANG, Teng LONG, Benhua HUANG, Donghua ZHANG, Peigen SU, Aqun ZHENG, Yang SUN

期刊论文

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

期刊论文

Synthesis of porous carbon from orange peel waste for effective volatile organic compounds adsorption

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

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

Revealing the GHG reduction potential of emerging biomass-based CO utilization with an iron cycle system

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

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

ZHAO Jinglian, WANG Xinping, ZHAO Liang

期刊论文

Promotional effect of ion-exchanged K on the low-temperature hydrothermal stability of Cu/SAPO-34 and

Chen Wang, Jun Wang, Jianqiang Wang, Meiqing Shen

期刊论文