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Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

《化学科学与工程前沿（英文）》 2018年第12卷第1期页码 24-31 doi: 10.1007/s11705-017-1669-4

摘要： We have successfully prepared a series of Pd-Ni/TiO catalysts by a one-step impregnation-reduction method. Among these catalysts with different compositions of Ni and Pd, the one with the Ni:Pd ratio of 2.95 showed the best activity. Small monodispersed Pd-Ni bimetallic nanoparticles were loaded on the surface of titanium oxide nanopowder as confirmed with TEM and EDS mapping. The XPS analysis demonstrated that Pd exists as 31% Pd(II) species and 69% Pd(0) species and all nickel is Ni(II). The prepared Pd-Ni/TiO exhibited enhanced catalytic activity compared to an equal amount of Pd/TiO for Suzuki-Miyaura reactions together with excellent applicability and reusability.

关键词： Pd-Ni bimetallic nanoparticles nanocatalysis Suzuki-Miyaura reaction titanium oxide

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Aminopyridine functionalized cellulose based Pd nanoparticles: An efficient and ecofriendly catalyst for the Suzukicross-coupling reaction

Peibo Hu,Yahao Dong,Xiaotian Wu,Yuping Wei

《化学科学与工程前沿（英文）》 2016年第10卷第3期页码 389-395 doi: 10.1007/s11705-016-1575-1

摘要： A palladium catalyst supported on 2-aminopyridine functionalized cellulose was synthesized and fully characterized by inductively coupled plasma atomic emission spectroscopy, transmission electron microscope, Fourier transform infrared spectroscopy, thermogravimetric analysis and X-ray photoelectron spectrometry. This catalyst can be applied in the Suzuki cross-coupling reaction of aryl halides with arylboronic acids in 50% ethanol to afford biaryls in?good yields, and easily recycled by simple filtration after reaction without the loss of metal Pd.

关键词： cellulose-supported 2-aminopyridine palladium nanoparticles ecofriendly catalyst Suzuki cross-coupling reaction

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Simultaneous removal of trihalomethanes by bimetallic Ag/Zn: kinetics study

Ahmed H A DABWAN, Satoshi KANECO, Hideyuki KATSUMATA, Kiyoyuki EGUSA, Tohru SUZUKI, Kiyohisa OHTA,

《化学科学与工程前沿（英文）》 2010年第4卷第3期页码 322-327 doi: 10.1007/s11705-009-0261-y

摘要： In the present work, bimetallic silver/zinc was applied into the degradation of trihalomethanes, THMs: CHCl, CHBrCl, CHBrCl, and CHBr. The kinetics reaction rates and removal efficiencies of the THM compound mixtures, in the aqueous solutions, were investigated. Batch experiments were conducted under mild conditions, ambient temperature, and pressure. The primary degradation reaction followed a pseudo-first-order kinetic law. The first-order rate constants and the degradation efficiencies followed the decreasing order of CHBr>CHBrCl>CHBrCl>CHCl. The bond dissociation energy and hydrophilic/hydrophobic characteristics of the THM compounds may become the most important parameters affecting the degradation kinetics and efficiency by bimetallic Ag/Zn.

关键词： reaction first-order dissociation degradation reaction aqueous

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Development of highly active coated monolith SCR catalyst with strong abrasion resistance for low-temperature application

Lina GAN,Shan LEI,Jian YU,Hongtao MA,Yo YAMAMOTO,Yoshizo SUZUKI,Guangwen XU,Zhanguo ZHANG

《环境科学与工程前沿（英文）》 2015年第9卷第6期页码 979-987 doi: 10.1007/s11783-015-0824-8

摘要： Monolith SCR catalysts coated with V O -WO /TiO were prepared by varying binder and coating thickness. Comparing with a monolith extruded with 100% V O -WO /TiO powder, a coated monolith with a catalyst-coating layer of 260 μm in thickness exhibited the similar initial NO reduction activity at 250°C. After 4 h abrasion (attrition) in an air stream containing 300 g·m fine sands (50–100 μm) at a superficial gas velocity of 10 m·s , the catalyst still has the activity as a 100% molded monolith does in a 24-h activity test and it retains about 92% of its initial activity at 250°C. Estimation of the equivalent durable hours at a fly ash concentration of 1.0 g·m in flue gas and a gas velocity of 5 m·s demonstrated that this coated monolith catalyst is capable of resisting abrasion for 13 months without losing more than 8% of its initial activity. The result suggests the great potential of the coated monolith for application to de-NO of flue gases with low fly ash concentrations from, such as glass and ceramics manufacturing processes.

关键词： coated monolith low-temperature denitration abrasion resistance attrition

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Evaluation method of dam behavior during construction and reservoir filling and application to real dams

Yuji KOHGO, Akira TAKAHASHI, Tomokazu SUZUKI,

《结构与土木工程前沿（英文）》 2010年第4卷第1期页码 92-101 doi: 10.1007/s11709-010-0009-2

摘要： In this paper we analyzed a real fill-type dam, named the Minami-Aiki Dam, to verify a numerical consolidation method with an elastoplastic model for unsaturated soils. The validities were conducted by comparing the analyzed and measured values during construction and impounding. The settlements calculated showed good agreement to those observed. Though the changing patterns of the measured and calculated pore water pressures were similar, the amounts of pore water pressures induced by the self-weights of embankment and the dissipation speeds were different. The earth pressures measured at the bottom of the core zone showed good agreement with those calculated. This method is valid for estimating behavior of fill-type dams during construction and impounding.

关键词： fill dam consolidation analysis unsaturated geo-materials impounding construction

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Enhanced hydrogen production from aqueous methanol solution using TiO

Paramasivan GOMATHISANKAR,Tomoko NODA,Hideyuki KATSUMATA,Tohru SUZUKI,Satoshi KANECO

《化学科学与工程前沿（英文）》 2014年第8卷第2期页码 197-202 doi: 10.1007/s11705-014-1417-y

摘要： The photocatalytic hydrogen production from aqueous methanol solution using titanium dioxide (TiO ) was investigated in the addition of metal particles including copper, lead, tin, and zinc. The results show that only the addition of copper particles enhances the hydrogen production. The copper usage and reaction temperature were further optimized for TiO /Cu photocatalyts. Under the optimal conditions, the hydrogen production using TiO /Cu as photocatalysts is approximately 68 times higher than that obtained with only TiO .

关键词： photocatalytic hydrogen generation methanol copper particles TiO₂ metal-semiconductor interface

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Determination of aniline derivatives in water samples after preconcentration with oxidized multiwalled carbon nanotubes as solid-phase extraction disk

Hideyuki KATSUMATA, Yuta ODA, Satoshi KANECO, Tohru SUZUKI, Kiyohisa OHTA

《化学科学与工程前沿（英文）》 2012年第6卷第3期页码 270-275 doi: 10.1007/s11705-012-1298-x

摘要： A sensitive and selective preconcentration method using solid-phase extraction (SPE) disk made from oxidized multiwalled carbon nanotubes (OMWCNTs), has been developed for the determination of aniline derivatives, such as 2-nitroaniline (2-NA), 4-nitroaniline (4-NA), and 2,4-dichloroaniline (2,4-DCA) in water samples. Anilines were extracted onto OMWCNT disk and then determined by high performance liquid chromatography (HPLC) with UV detector. Several parameters on the recovery of the analytes were investigated. The experimental results showed that it was possible to obtain quantitative analysis when the solution pH was 8 using 200 mL of validation solution containing 2 μg of anilines and 10 mL of acetonitrile/ethanol (8/2, v/v) as an eluent. Relative standard deviations for five determinations were 7.5% (2-NA), 6.5% (4-NA) and 3.8% (2,4-DCA) under optimum conditions. The linear range of calibration curves were 0.5 ng·mL to 15 ng·mL for each analyte with good correlation coefficients. The detection limits (3S/N) of 2-NA, 4-NA and 2,4-DCA were 30 pg·mL , 31 pg·mL and 26 pg·mL , respectively. Our method was successfully applied to the determination of aniline compounds in river water sample with high precision and accuracy.

关键词： aniline determination solid-phase extraction oxidized multiwalled carbon nanotubes water sample HPLC-UV

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Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

《化学科学与工程前沿（英文）》 2022年第16卷第12期页码 1700-1712 doi: 10.1007/s11705-022-2207-6

摘要： The chain length and hydrocarbon type significantly affect the production of light olefins during the catalytic pyrolysis of naphtha. Herein, for a better catalyst design and operation parameters optimization, the reaction pathways and equilibrium yields for the catalytic pyrolysis of C_5–8 n/iso/cyclo-paraffins were analyzed thermodynamically. The results revealed that the thermodynamically favorable reaction pathways for n/iso-paraffins and cyclo-paraffins were the protolytic and hydrogen transfer cracking pathways, respectively. However, the formation of light paraffin severely limits the maximum selectivity toward light olefins. The dehydrogenation cracking pathway of n/iso-paraffins and the protolytic cracking pathway of cyclo-paraffins demonstrated significantly improved selectivity for light olefins. The results are thus useful as a direction for future catalyst improvements, facilitating superior reaction pathways to enhance light olefins. In addition, the equilibrium yield of light olefins increased with increasing the chain length, and the introduction of cyclo-paraffin inhibits the formation of light olefins. High temperatures and low pressures favor the formation of ethylene, and moderate temperatures and low pressures favor the formation of propylene. n-Hexane and cyclohexane mixtures gave maximum ethylene and propylene yield of approximately 49.90% and 55.77%, respectively. This work provides theoretical guidance for the development of superior catalysts and the selection of proper operation parameters for the catalytic pyrolysis of C_5–8 n/iso/cyclo-paraffins from a thermodynamic point of view.

关键词： naphtha catalytic pyrolysis reaction pathway equilibrium yield

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催化裂化过程反应化学的进展

许友好,汪燮卿

《中国工程科学》 2007年第9卷第8期页码 6-14

摘要：

面对催化裂化工艺所遇到的挑战，提出了催化裂化过程反应化学的多维反应结构模式。多维反应结构模式的建立是基于对烃类在酸性催化剂上反应化学认识而进行的知识创新，但多维反应结构不同于烃类在酸性催化剂上反应化学。具有多维反应结构的催化裂化工艺更具有多样性和灵活性，基于此已成功地开发了多产异构烷烃的催化裂化工艺和生产清洁汽油和多产丙烯的催化裂化工艺。

关键词：催化裂化反应化学催化剂多维反应结构两个反应区

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Heterogeneous reaction mechanism of gaseous HNO

Nan ZHAO,Qingzhu ZHANG,Wenxing WANG

《环境科学与工程前沿（英文）》 2016年第10卷第5期 doi: 10.1007/s11783-016-0836-z

摘要： We studied the heterogeneous reaction mechanism of gaseous HNO with solid NaCl. HCl is released from heterogeneous reactions between gaseous HNO and solid NaCl. Water molecules induce surface reconstruction of NaCl to facilitate the reaction. Sea salt particles containing NaCl are among the most abundant particulate masses in coastal atmosphere. Reactions involving sea salt particles potentially generate Cl radicals, which are released into coastal atmosphere. Cl radicals play an important role in the nitrogen and O cycles, sulfur chemistry and particle formation in the troposphere of the polluted coastal regions. This paper aimed at the heterogeneous reaction between gaseous HNO and solid NaCl. The mechanism was investigated by density functional theory (DFT). The results imply that water molecules induce the surface reconstruction, which is essential for the heterogeneous reaction. The surface reconstruction on the defective (710) surface has a barrier of 10.24 kcal·mol and is endothermic by 9.69 kcal·mol , whereas the reconstruction on the clean (100) surface has a barrier of 18.46 kcal·mol and is endothermic by 12.96 kcal·mol . The surface reconstruction involved in water-adsorbed (710) surface is more energetically favorable. In comparison, water molecules adsorbed on NaCl (100) surface likely undergo water diffusion or desorption. Further, it reveals that the coordination number of the Cl is reduced after the surface reconstruction, which assists Cl to accept the proton from HNO . HCl is released from heterogeneous reactions between gaseous HNO and solid NaCl and can react with OH free radicals to produce atomic Cl radicals. The results will offer further insights into the impact of gaseous HNO on the air quality of the coastal areas.

关键词： Seasalt particles NaCl HNO₃ Heterogeneous reaction Reaction mechanism Density functional theory

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Dual-reaction-center catalytic process continues Fenton’s story

Chao Lu, Kanglan Deng, Chun Hu, Lai Lyu

《环境科学与工程前沿（英文）》 2020年第14卷第5期 doi: 10.1007/s11783-020-1261-x

摘要： Abstract • Dual-reaction-center (DRC) system breaks through bottleneck of Fenton reaction. • Utilization of intrinsic electrons of pollutants is realized in DRC system. • DRC catalytic process well continues Fenton’s story. Triggered by global water quality safety issues, the research on wastewater treatment and water purification technology has been greatly developed in recent years. The Fenton technology is particularly powerful due to the rapid attack on pollutants by the generated hydroxyl radicals (•OH). However, both heterogeneous and homogeneous Fenton/Fenton-like technologies follow the classical reaction mechanism, which depends on the oxidation and reduction of the transition metal ions at single sites. So even after a century of development, this reaction still suffers from its inherent bottlenecks in practical application. In recent years, our group has been focusing on studying a novel heterogeneous Fenton catalytic process, and we developed the dual-reaction-center (DRC) system for the first time. In the DRC system, H2O2 and O2 can be efficiently reduced to reactive oxygen species (ROS) in electron-rich centers, while pollutants are captured and oxidized by the electron-deficient centers. The obtained electrons from pollutants are diverted to the electron-rich centers through bonding bridges. This process breaks through the classic Fenton mechanism, and improves the performance and efficiency of pollutant removal in a wide pH range. Here, we provide a brief overview of Fenton’s story and focus on combing the discovery and development of the DRC technology and mechanism in recent years. The construction of the DRC and its performance in the pollutant degradation and interfacial reaction process are described in detail. We look forward to bringing a new perspective to continue Fenton’s story through research and development of DRC technology.

关键词： Dual reaction centers Fenton Pollutant utilization Electron transfer

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Graphene-reinforced metal-organic frameworks derived cobalt sulfide/carbon nanocomposites as efficient multifunctional electrocatalysts

《化学科学与工程前沿（英文）》 2021年第15卷第6期页码 1487-1499 doi: 10.1007/s11705-021-2085-3

摘要： Developing cost-effective electrocatalysts for oxygen reduction reaction (ORR), oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) is vital in energy conversion and storage applications. Herein, we report a simple method for the synthesis of graphene-reinforced CoS/C nanocomposites and the evaluation of their electrocatalytic performance for typical electrocatalytic reactions. Nanocomposites of CoS embedded in N, S co-doped porous carbon and graphene (CoS@C/Graphene) were generated via simultaneous sulfurization and carbonization of one-pot synthesized graphite oxide-ZIF-67 precursors. The obtained CoS@C/Graphene nanocomposites were characterized by X-ray diffraction, Raman spectroscopy, thermogravimetric analysis-mass spectroscopy, scanning electronic microscopy, transmission electronic microscopy, X-ray photoelectron spectroscopy and gas sorption. It is found that CoS nanoparticles homogenously dispersed in the in situ formed N, S co-doped porous carbon/graphene matrix. The CoS@C/10Graphene composite not only shows excellent electrocatalytic activity toward ORR with high onset potential of 0.89 V, four-electron pathway and superior durability of maintaining 98% of current after continuously running for around 5 h, but also exhibits good performance for OER and HER, due to the improved electrical conductivity, increased catalytic active sites and connectivity between the electrocatalytic active CoS and the carbon matrix. This work offers a new approach for the development of novel multifunctional nanocomposites for the next generation of energy conversion and storage applications.

关键词： MOF derivative graphene electrocatalyst oxygen reduction reaction oxygen evolution reaction hydrogen evolution reaction

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Impact and inhibitory mechanism of phenolic compounds on the formation of toxic Maillard reaction products

Jing TENG, Xiaoqian HU, Ningping TAO, Mingfu WANG

《农业科学与工程前沿（英文）》 2018年第5卷第3期页码 321-329 doi: 10.15302/J-FASE-2017182

摘要：

As one of the dominant reactions occurring during thermal treatment of food, the Maillard reaction not only leads to the formation of aroma, browning color and taste compounds, but also contributes to the formation of some unpleasant toxic substances including acrylamide, heterocyclic amines and advanced glycation end products. Polyphenols, one of the most abundant antioxidants in the human diet, are contained in different kinds of foods. In this review, some recent studies on the impact of dietary polyphenols on the formation of acrylamide, heterocyclic amines and advanced glycation end products formed during the Maillard reaction are summarized, including the research work conducted with both chemical model systems and real food model systems; the possible inhibitory mechanisms of different polyphenols are also summarized and discussed in this review. Basically we found that some dietary polyphenols not only scavenge free radicals, but also react with reactive carbonyl species, thus lowering the formation of toxic Maillard reaction products. This review provides a useful theoretical foundation for the application of polyphenols in food safety, and suggests some directions for further study of natural products as inhibitors against the formation of toxic substances in thermally processed food.

关键词： advanced glycation end products acrylamide food safety heterocyclic amine Maillard reaction polyphenols

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An overview and recent advances in electrocatalysts for direct seawater splitting

《化学科学与工程前沿（英文）》 2021年第15卷第6期页码 1408-1426 doi: 10.1007/s11705-021-2102-6

摘要： In comparison to pure water, seawater is widely accepted as an unlimited resource. The direct seawater splitting is economical and eco-friendly, but the key challenges in seawater, especially the chlorine-related competing reactions at the anode, seriously hamper its practical application. The development of earth-abundant electrocatalysts toward direct seawater splitting has emerged as a promising strategy. Highly efficient electrocatalysts with improved selectivity and stability are of significance in preventing the interference of side reactions and resisting various impurities. This review first discusses the macroscopic understanding of direct seawater electrolysis and then focuses on the strategies for rational design of electrocatalysts toward direct seawater splitting. The perspectives of improved electrocatalysts to solve emerging challenges and further development of direct seawater splitting are also provided.

关键词： seawater splitting electrocatalysts oxygen evolution reaction hydrogen evolution reaction chlorine chemistry

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Interface engineering for enhancing electrocatalytic oxygen evolution reaction of CoS/CeO heterostructures

《化学科学与工程前沿（英文）》 2022年第16卷第3期页码 376-383 doi: 10.1007/s11705-021-2062-x

摘要： To realize renewable energy conversion, it is important to develop low-cost and high-efficiency electrocatalyst for oxygen evolution reaction. In this communication, a novel bijunction CoS/CeO₂ electrocatalyst grown on carbon cloth is prepared by the interface engineering. The interface engineering of CoS and CeO₂ facilitates a rapid charge transfer from CeO₂ to CoS. Such an electrocatalyst exhibits outstanding electrocatalytic activity with a low overpotential of 311 mV at 10 mA∙cm⁻² and low Tafel slope of 76.2 mV∙dec^–1, and is superior to that of CoS (372 mV) and CeO₂ (530 mV) counterparts. And it has long-term durability under alkaline media.

关键词： interface engineering CoS/CeO₂ electrodeposition electrocatalyst oxygen evolution reaction

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标题作者时间类型操作

Pd-Ni nanoparticles supported on titanium oxide as effective catalysts for Suzuki-Miyaura coupling reactions

Dongxu Han, Zhiguo Zhang, Zongbi Bao, Huabin Xing, Qilong Ren

期刊论文

Aminopyridine functionalized cellulose based Pd nanoparticles: An efficient and ecofriendly catalyst for the Suzukicross-coupling reaction

Peibo Hu,Yahao Dong,Xiaotian Wu,Yuping Wei

期刊论文

Simultaneous removal of trihalomethanes by bimetallic Ag/Zn: kinetics study

Ahmed H A DABWAN, Satoshi KANECO, Hideyuki KATSUMATA, Kiyoyuki EGUSA, Tohru SUZUKI, Kiyohisa OHTA,

期刊论文

Development of highly active coated monolith SCR catalyst with strong abrasion resistance for low-temperature application

Lina GAN,Shan LEI,Jian YU,Hongtao MA,Yo YAMAMOTO,Yoshizo SUZUKI,Guangwen XU,Zhanguo ZHANG

期刊论文

Evaluation method of dam behavior during construction and reservoir filling and application to real dams

Yuji KOHGO, Akira TAKAHASHI, Tomokazu SUZUKI,

期刊论文

Enhanced hydrogen production from aqueous methanol solution using TiO

Paramasivan GOMATHISANKAR,Tomoko NODA,Hideyuki KATSUMATA,Tohru SUZUKI,Satoshi KANECO

期刊论文

Determination of aniline derivatives in water samples after preconcentration with oxidized multiwalled carbon nanotubes as solid-phase extraction disk

Hideyuki KATSUMATA, Yuta ODA, Satoshi KANECO, Tohru SUZUKI, Kiyohisa OHTA

期刊论文

Thermodynamic analysis of reaction pathways and equilibrium yields for catalytic pyrolysis of naphtha

期刊论文

催化裂化过程反应化学的进展

许友好,汪燮卿

期刊论文

Heterogeneous reaction mechanism of gaseous HNO

Nan ZHAO,Qingzhu ZHANG,Wenxing WANG

期刊论文

Dual-reaction-center catalytic process continues Fenton’s story

Chao Lu, Kanglan Deng, Chun Hu, Lai Lyu