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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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Diversity-oriented synthesis of blue emissive nitrogen heterocycles and their conjugation with carbon nano-onions

Viviana Maffeis, Lisa Moni, Daniele Di Stefano, Silvia Giordani, Renata Riva

《化学科学与工程前沿（英文）》 2020年 第14卷 第1期   页码 76-89 doi: 10.1007/s11705-019-1833-0

摘要： The search for new fluorescent molecules for possible applications as functional -electron systems and their conjugation with different nanomaterials is nowadays of paramount importance to broaden the availability of materials with different properties. Herein we present a diversity-oriented approach to heterocyclic luminophores based on a multicomponent Ugi reaction followed by a Pd-mediated cascade sequence. The new molecules are coupled to carbon nano-onions, and hybrid systems represent the first example of blue emitters conjugated with these carbon nanoparticles.

关键词： carbon nano-onions     multicomponent reactions     blue emitters     fluorescence     isoquinolines    

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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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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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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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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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Reactivity of Pyrogenic Carbonaceous Matter (PCM) in mediating environmental reactions: Current knowledge

Wenqing Xu, Mark L. Segall, Zhao Li

《环境科学与工程前沿（英文）》 2020年 第14卷 第5期 doi: 10.1007/s11783-020-1265-6

摘要： Abstract • Pyrogenic Carbonaceous Matter (PCM) promote both chemical and microbial synergies. • Discussion of PCM-enhanced abiotic transformation pathways of organic pollutants. • Conjugated microporous polymers (CMPs) can mimic the performance of PCM. • CMPs offer a platform that allows for systematic variation of individual properties. Pyrogenic Carbonaceous matter (PCM; e.g., black carbon, biochar, and activated carbon) are solid residues from incomplete combustion of fossil fuel or biomass. They are traditionally viewed as inert adsorbents for sequestering contaminants from the aqueous phase or providing surfaces for microbes to grow. In this account, we reviewed the recently discovered reactivity of PCM in promoting both chemical and microbial synergies that are important in pollutant transformation, biogeochemical processes of redox-active elements, and climate change mitigation with respect to the interaction between biochar and nitrous oxide (N2O). Moreover, we focused on our group’s work in the PCM-enhanced abiotic transformation of nitrogenous and halogenated pollutants and conducted in-depth analysis of the reaction pathways. To understand what properties of PCM confer its reactivity, our group pioneered the use of PCM-like polymers, namely conjugated microporous polymers (CMPs), to mimic the performance of PCM. This approach allows for the controlled incorporation of specific surface properties (e.g., quinones) into the polymer network during the polymer synthesis. As a result, the relationship between specific characteristics of PCM and its reactivity in facilitating the decay of a model pollutant was systematically studied in our group’s work. The findings summarized in this account help us to better understand an overlooked environmental process where PCM synergistically interacts with various environmental reagents such as hydrogen sulfide and water. Moreover, the knowledge gained in these studies could inform the design of a new generation of reactive carbonaceous materials with tailored properties that are highly efficient in contaminant removal.

关键词： pyrogenic carbonaceous matter     Conjugated microporous polymer     remediation     Biochar     Hydrolysis     Pollutant degradation    

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Review of plasma-assisted reactions and potential applications for modification of metal–organic frameworks

Tingting Zhao, Niamat Ullah, Yajun Hui, Zhenhua Li

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 444-457 doi: 10.1007/s11705-019-1811-6

摘要： Plasma catalysis is drawing increasing attention worldwide. Plasma is a partially ionized gas comprising electrons, ions, molecules, radicals, and photons. Integration of catalysis and plasma can enhance catalytic activity and stability. Some thermodynamically unfavorable reactions can easily occur with plasma assistance. Compared to traditional thermal catalysis, plasma reactors can save energy because they can be operated at much lower temperatures or even room temperature. Additionally, the low bulk temperature of cold plasma makes it a good alternative for treatment of temperature-sensitive materials. In this review, we summarize the plasma-assisted reactions involved in dry reforming of methane, CO methanation, the methane coupling reaction, and volatile organic compound abatement. Applications of plasma for modification of metal–organic frameworks are discussed.

关键词： plasma catalysis     methane     carbon dioxide     VOCs     metal–organic frameworks    

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Easy access to pharmaceutically relevant heterocycles by catalytic reactions involving

Ximei Zhao, Matthias Rudolph, Abdullah M. Asiri, A. Stephen K. Hashmi

《化学科学与工程前沿（英文）》 2020年 第14卷 第3期   页码 317-349 doi: 10.1007/s11705-019-1874-4

摘要： This review summarizes recent advances in the field of gold-catalyzed synthesis of pharmaceutically relevant aza-heterocycles via generated -imino gold carbene complexes as intermediates.

关键词： gold     heterocycles     alkynes    

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Removal of multicomponent VOCs in off-gases from an oil refining wastewater treatment plant by a compost-based

Dan WU, Chunyan ZHANG, Li HAO, Changjun GENG, Xie QUAN,

《环境科学与工程前沿（英文）》 2009年 第3卷 第4期   页码 483-491 doi: 10.1007/s11783-009-0144-y

摘要： Waste gases from oil refining wastewater treatment plants are often characterized by the presence of multicomponent and various concentrations of compounds. An evaluation of the performance and feasibility of removing multicomponent volatile organic compounds (VOCs) in off-gases from oil refining wastewater treatment plants was conducted in a pilot-scale compost-based biofilter system. This system consists of two identical biofilters packed with compost and polyethylene (PE). This paper investigates the effects of various concentrations of nonmethane hydrocarbon (NMHC) and empty bed residence time (EBRT) on the removal efficiency of NMHC. Based on the experimental results and practical applications, an EBRT of 66 s was applied to the biofilter system. The removal efficiencies of NMHC were within the range of 47%―100%. At an EBRT of 66 s, the average removal efficiency of benzene, toluene, and xylene were more than 99%, 99%, and 100%, respectively. The results demonstrated that multicomponent VOCs in off-gases from the oil refining wastewater treatment plant could be successfully removed in the biofilter system, which may provide useful information concerning the design criteria and operation of full-scale biofilters.

关键词： biodegradation     volatile organic compounds (VOCs)     biofiltration     biofilter    

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A novel method for generating distillation configurations

Hongzhe Hou, Yiqing Luo

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 834-846 doi: 10.1007/s11705-019-1855-7

摘要： An improved matrix method for generating distillation configurations with ( −1) and less than ( −1) columns was proposed for the separation of an -component mixture into essentially pure product streams based on the concepts of streams matrix and 0–1 matrixes proposed by Agrawal. In contrast with the matrix method developed by Agrawal, the present method removes the intermediate process centered on the splits, and complex column configurations, allowing the direct generation of multi-feeds and multi-product streams. Furthermore, certain configurations that cannot be generated directly and that are missing in the matrix method are obtained. Through rigorous simulations and optimization, we have demonstrated that these configurations have the potential to outperform certain existing configurations.

关键词： non-sharp separation     multicomponent distillation     distillation configurations    

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Catalyst particle shapes and pore structure engineering for hydrodesulfurization and hydrodenitrogenation reactions

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 897-908 doi: 10.1007/s11705-021-2127-x

摘要： Catalyst particle shapes and pore structure engineering are crucial for alleviating internal diffusion limitations in the hydrodesulfurization (HDS)/hydrodenitrogenation (HDN) of gas oil. The effects of catalyst particle shapes (sphere, cylinder, trilobe, and tetralobe) and pore structures (pore diameter and porosity) on HDS/HDN performance at the particle scale are investigated via mathematical modeling. The relationship between particle shape and effectiveness factor is first established, and the specific surface areas of different catalyst particles show a positive correlation with the average HDS/HDN reaction rates. The catalyst particle shapes primarily alter the average HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor. An optimal average HDS/HDN reaction rate exists as the catalyst pore diameter and porosity increase, and this optimum value indicates a tradeoff between diffusion and reaction. In contrast to catalyst particle shapes, the catalyst pore diameter and the porosity of catalyst particles primarily alter the surface HDS/HDN reaction rate to adjust the HDS/HDN effectiveness factor. This study provides insights into the engineering of catalyst particle shapes and pore structures for improving HDS/HDN catalyst particle efficiency.

关键词： hydrodesulfurization     hydrodenitrogenation     particle shape     pore structure    

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Kinetics and mechanisms of reactions for hydrated electron with chlorinated benzenes in aqueous solution

Haixia YUAN,Huxiang PAN,Jin SHI,Hongjing LI,Wenbo DONG

《环境科学与工程前沿（英文）》 2015年 第9卷 第4期   页码 583-590 doi: 10.1007/s11783-014-0691-8

摘要： The reactions between chlorinated benzenes (CBzs) and hydrated electron ( ) were investigated by the electron beam (EB) and laser flash photolysis (LFP) experiments. Under the EB irradiation, the effects of irradiation dose, initial concentration and the number of Cl atoms on the removal efficiencies were further examined. At 10 kGy, the removal efficiencies of mono-CB, 1,3-diCB, 1,2-diCB and 1,4-diCB were 41.2%, 87.2%, 84.0%, and 84.1%, respectively. While irradiation dose was 50 kGy, the removal efficiencies increased to 47.4%, 95.8%, 95.0%, and 95.2%, respectively. Irradiation of CBzs solutions has shown that the higher the initial concentration, the lower the percentage of CBzs removal. In addition to this, the dechlorination efficiencies of 1,2-dichlorobenzene (1,2-diCB), 1,3-dichlorobenzene (1,3-diCB) and 1,4-dichlorobenzene (1,4-diCB) were much higher than that of chlorobenzene (mono-CB). The kinetics of the reactions was achieved with nanosecond LFP. The rate constants of second-order reaction between with mono-CB, 1,2-diCB, 1,3-diCB and 1,4-diCB were (5.3±0.4) × 10 , (4.76±0.1) × 10 , (1.01±0.1) × 10 and (3.29±0.2) × 10 L·mol ·s , respectively. Density functional theory (DFT) calculations were performed to determine the optical properties of unstable CBzs anion radicals, and the main absorption peaks lied in the range of 300–550 nm. The primary reaction pathway of CBzs with was gradual dechlorination, and the major products were Cl and benzene (CBzs(-Cl )). Furthermore, biphenyl (or chlorobiphenyl) was observed during the LFP, which was probably formed by recombination of benzene radicals.

关键词： chlorinated benzenes     hydrated electron     electron beam     laser flash photolysis    

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A microextraction approach for rapid extraction and separation of Mn(II) and Co(II) using saponified D2EHPA system

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 963-972 doi: 10.1007/s11705-021-2081-7

摘要： In this paper, we proposed a microextraction approach for the extraction and separation of Mn(II) and Co(II) from sulfate solution simulating leachate of spent lithium-ion battery cathode materials using saponified di-(2-ethylhexyl)phosphoric acid system. The effects of the following operational variables were investigated: equilibrium pH, tri-n-butyl phosphate concentration, saponification rate, two-phase ratio and residence time. The results showcased that the microextractor can reach the extraction equilibrium within 20 s, thereby greatly reducing necessary extraction time comparing to that of conventional processes. The volumetric mass transfer coefficient showed 8–21 times larger than that of batch device. With the help of microextractor, 95% of Mn(II) was extracted with a single theoretical stage at a chosen two-phase ratio of 3:1, and the separation factor βMn/Co was as large as 65.5. In the subsequent stripping step, more than 99% of manganese from loaded phase was easily stripped under optimal conditions. The microextraction approach greatly enhances the mass transfer while enabling a continuous and controllable extraction process within a simple structure design. When extracting spent electrode material with microextractors, the comprehensive recovery of mangenese can reach 96%. The microextraction approach has a good applicability in the spent lithium-ion battery cathode materials recycling at both bench and industrial scales.

关键词： extraction equilibrium     mass transfer coefficient     microextraction     multicomponent extraction     di-(2-ethylhexyl)phosphoric acid    

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标题 作者 时间 类型 操作

Sustainable functionalization and modification of materials via multicomponent reactions in water

期刊论文

Diversity-oriented synthesis of blue emissive nitrogen heterocycles and their conjugation with carbon nano-onions

Viviana Maffeis, Lisa Moni, Daniele Di Stefano, Silvia Giordani, Renata Riva

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

Numerical simulation and experimental verification of chemical reactions for SCR DeNO

Qiang ZHANG, Yonglin FAN, Wenyan LI

期刊论文

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

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

Reactivity of Pyrogenic Carbonaceous Matter (PCM) in mediating environmental reactions: Current knowledge

Wenqing Xu, Mark L. Segall, Zhao Li

期刊论文

Review of plasma-assisted reactions and potential applications for modification of metal–organic frameworks

Tingting Zhao, Niamat Ullah, Yajun Hui, Zhenhua Li

期刊论文

Easy access to pharmaceutically relevant heterocycles by catalytic reactions involving

Ximei Zhao, Matthias Rudolph, Abdullah M. Asiri, A. Stephen K. Hashmi

期刊论文

Removal of multicomponent VOCs in off-gases from an oil refining wastewater treatment plant by a compost-based

Dan WU, Chunyan ZHANG, Li HAO, Changjun GENG, Xie QUAN,

期刊论文

A novel method for generating distillation configurations

Hongzhe Hou, Yiqing Luo

期刊论文

Catalyst particle shapes and pore structure engineering for hydrodesulfurization and hydrodenitrogenation reactions

期刊论文

Kinetics and mechanisms of reactions for hydrated electron with chlorinated benzenes in aqueous solution

Haixia YUAN,Huxiang PAN,Jin SHI,Hongjing LI,Wenbo DONG

期刊论文

A microextraction approach for rapid extraction and separation of Mn(II) and Co(II) using saponified D2EHPA system

期刊论文