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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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Sustainable functionalization and modification of materials via multicomponent reactions in water

《化学科学与工程前沿（英文）》 2022年 第16卷 第9期   页码 1318-1344 doi: 10.1007/s11705-022-2150-6

摘要： In materials chemistry, green chemistry has established firm ground providing essential design criteria to develop advanced tools for efficient functionalization and modification of materials. Particularly, the combination of multicomponent reactions in water and aqueous media with materials chemistry unlocks a new sustainable way for constructing multi-functionalized structures with unique features, playing significant roles in the plethora of applications. Multicomponent reactions have received significant consideration from the community of material chemistry because of their great efficiency, simple operations, intrinsic molecular diversity, and an atom and a pot economy. Also, by rational design of multicomponent reactions in water and aqueous media, the performance of some multicomponent reactions could be enhanced by the contributing “natural” form of water-soluble materials, the exclusive solvating features of water, and simple separating and recovering materials. To date, there is no exclusive review to report the sustainable functionalization and modification of materials in water. This critical review highlights the utility of various kinds of multicomponent reactions in water and aqueous media as green methods for functionalization and modification of siliceous, magnetic, and carbonaceous materials, oligosaccharides, polysaccharides, peptides, proteins, and synthetic polymers. The detailed discussion of synthetic procedures, properties, and related applicability of each functionalized/modified material is fully deliberated in this review.

关键词： materials     multicomponent reactions     modification     functionalization     water    

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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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Redox reactions of iron and manganese oxides in complex systems

Jianzhi Huang, Huichun Zhang

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1255-8

摘要： • Mechanisms of redox reactions of Fe- and Mn-oxides were discussed. • Oxidative reactions of Mn- and Fe-oxides in complex systems were reviewed. • Reductive reaction of Fe(II)/iron oxides in complex systems was examined. • Future research on examining the redox reactivity in complex systems was suggested. Conspectus Redox reactions of Fe- and Mn-oxides play important roles in the fate and transformation of many contaminants in natural environments. Due to experimental and analytical challenges associated with complex environments, there has been a limited understanding of the reaction kinetics and mechanisms in actual environmental systems, and most of the studies so far have only focused on simple model systems. To bridge the gap between simple model systems and complex environmental systems, it is necessary to increase the complexity of model systems and examine both the involved interaction mechanisms and how the interactions affected contaminant transformation. In this Account, we primarily focused on (1) the oxidative reactivity of Mn- and Fe-oxides and (2) the reductive reactivity of Fe(II)/iron oxides in complex model systems toward contaminant degradation. The effects of common metal ions such as Mn2+ , Ca2+, Ni2+, Cr3+ and Cu2+, ligands such as small anionic ligands and natural organic matter (NOM), and second metal oxides such as Al, Si and Ti oxides on the redox reactivity of the systems are briefly summarized.

关键词： Iron oxides     manganese oxides     reduction     oxidation     complex systems     reaction kinetics and mechanisms    

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Kinetic Monte Carlo simulations of plasma-surface reactions on heterogeneous surfaces

Daniil Marinov

《化学科学与工程前沿（英文）》 2019年 第13卷 第4期   页码 815-822 doi: 10.1007/s11705-019-1837-9

摘要： Reactions of atoms and molecules on chamber walls in contact with low temperature plasmas are important in various technological applications. Plasma-surface interactions are complex and relatively poorly understood. Experiments performed over the last decade by several groups prove that interactions of reactive species with relevant plasma-facing materials are characterized by distributions of adsorption energy and reactivity. In this paper, we develop a kinetic Monte Carlo (KMC) model that can effectively handle chemical kinetics on such heterogenous surfaces. Using this model, we analyse published adsorption-desorption kinetics of chlorine molecules and recombination of oxygen atoms on rotating substrates as a test case for the KMC model.

关键词： plasma-surface interaction     kinetic Monte Carlo     plasma nano technology    

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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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Numerical simulation and experimental verification of chemical reactions for SCR DeNO

Qiang ZHANG, Yonglin FAN, Wenyan LI

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 523-528 doi: 10.1007/s11705-010-0520-y

摘要： Selective catalytic reduction (SCR) is a major commercial technology for NO removal in power plants. There are a lot of complex chemical reactions in SCR reactors, and it is of great significance to understand the internal process of chemical reactions for SCR DeNO and study the impact of various factors on NO removal efficiency. In this paper, the impact of reaction temperature, ammonia-nitrogen molar ratio and resident time in the catalyst bed layer on NO removal efficiency were studied by simulation of chemical reactions. Then calculated results were compared with catalyst activity test data in a power plant, which proved that the simulated results were accurate. As a result, the reaction conditions were optimized in order to get the best removal efficiency of NO, so that we can provide a reference for optimal running of SCR in power plants.

关键词： SCR     NOx     removal efficiency     chemical reactions     simulation    

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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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Chemical reactions of oily sludge catalyzed by iron oxide under supercritical water gasification condition

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 886-896 doi: 10.1007/s11705-021-2125-z

摘要： Supercritical water gasification is a promising technology in dealing with the degradation of hazardous waste, such as oily sludge, accompanied by the production of fuel gases. To evaluate the mechanism of Fe2O3 catalyst and the migration pathways of heteroatoms and to investigate the systems during the process, reactive force field molecular dynamics simulations are adopted. In terms of the catalytic mechanisms of Fe2O3, the surface lattice oxygen is consumed by small carbon fragments to produce CO and CO2, improving the catalytic performance of the cluster due to more unsaturated coordination Fe sites exposed. Lattice oxygen combines with •H radicals to form water molecules, improving the catalytic performance. Furthermore, the pathway of asphaltene degradation was revealed at an atomic level, as well as products. Moreover, the adsorption of hydroxyl radical on the S atom caused breakage of the two C–S bonds in turn, forming •HSO intermediate, so that the organic S element was fixed into the inorganic liquid phase. The heteroatom O was removed under the effects of supercritical water. Heavy metal particles presented in the oily sludge, such as iron in association with Fe2O3 catalyst, helped accelerate the degradation of asphaltenes.

关键词： oily sludge     SCWG     ReaxFF     Fe2O3     heteroatoms    

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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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Solar fuel from photo-thermal catalytic reactions with spectrum-selectivity: a review

Sanli TANG, Jie SUN, Hui HONG, Qibin LIU

《能源前沿（英文）》 2017年 第11卷 第4期   页码 437-451 doi: 10.1007/s11708-017-0509-z

摘要： Solar fuel is one of the ideal energy sources in the future. The synergy of photo and thermal effects leads to a new approach to higher solar fuel production under relatively mild conditions. This paper reviews different approaches for solar fuel production from spectrum-selective photo-thermal synergetic catalysis. The review begins with the meaning of synergetic effects, and the mechanisms of spectrum-selectivity and photo-thermal catalysis. Then, from a technical perspective, a number of experimental or theoretical works are sorted by the chemical reactions and the sacrificial reagents applied. In addition, these works are summarized and tabulated based on the operating conditions, spectrum-selectivity, materials, and productivity. A discussion is finally presented concerning future development of photo-thermal catalytic reactions with spectrum-selectivity.

关键词： photo-thermal catalysis     spectrum-selectivity     solar fuel     full-spectrum    

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标题 作者 时间 类型 操作

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

期刊论文

Sustainable functionalization and modification of materials via multicomponent reactions in water

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

Redox reactions of iron and manganese oxides in complex systems

Jianzhi Huang, Huichun Zhang

期刊论文

Kinetic Monte Carlo simulations of plasma-surface reactions on heterogeneous surfaces

Daniil Marinov

期刊论文

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

期刊论文

Numerical simulation and experimental verification of chemical reactions for SCR DeNO

Qiang ZHANG, Yonglin FAN, Wenyan LI

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

Chemical reactions of oily sludge catalyzed by iron oxide under supercritical water gasification condition

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

Solar fuel from photo-thermal catalytic reactions with spectrum-selectivity: a review

Sanli TANG, Jie SUN, Hui HONG, Qibin LIU

期刊论文