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Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 329-338 doi: 10.1007/s11705-018-1741-8

摘要：

Copper nanoparticles-decorated polyaniline-derived mesoporous carbon that can serve as noble metal-free electrocatalyst for the hydrazine oxidation reaction (HzOR) is synthesized via a facile synthetic route. The material exhibits excellent electrocatalytic activity toward HzOR with low overpotential and high current density. The material also remains stable during the electrocatalytic reaction for long time. Its good electrocatalytic performance makes this material a promising alternative to conventional noble metal-based catalysts (e.g., Pt) that are commonly used in HzOR-based fuel cells.

关键词： copper nanoparticles     mesoporous carbon     noble metal-free electrocatalyst     hydrazine oxidation reaction     polyaniline    

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Platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

《化学科学与工程前沿（英文）》 2022年 第16卷 第6期   页码 930-938 doi: 10.1007/s11705-021-2130-2

摘要： Ammonia electrooxidation reaction involving multistep electron-proton transfer is a significant reaction for fuel cells, hydrogen production and understanding nitrogen cycle. Platinum has been established as the best electrocatalyst for ammonia oxidation in aqueous alkaline media. In this study, Pt/nitrogen-doped graphene (NDG) and Pt/tungsten monocarbide (WC)/NDG are synthesized by a wet chemistry method and their ammonia oxidation activities are compared to commercial Pt/C. Pt/NDG exhibits a specific activity of 0.472 mA∙cm–2, which is 44% higher than commercial Pt/C, thus establishing NDG as a more effective support than carbon black. Moreover, it is demonstrated that WC as a support also impacts the activity with further 30% increase in comparison to NDG. Surface modification with Ir resulted in the best electrocatalytic activity with Pt-Ir/WC/NDG having almost thrice the current density of commercial Pt/C. This work adds insights regarding the role of NDG and WC as efficient supports along with significant impact of Ir surface modification.

关键词： Ammonia electro-oxidation reaction     electrocatalyst supports     platinum     nitrogen doped graphene     tungsten carbide    

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

Milan Malhotra, Anurag Garg

《环境科学与工程前沿（英文）》 2021年 第15卷 第1期 doi: 10.1007/s11783-020-1305-2

摘要： Abstract • Hydrothermal treatment can greatly improve resource recovery from sewage sludge. • tCOD removal during WO was ~55% compared with ~23% after TH. • TOC solubilization during hydrothermal treatment followed first-order kinetics. • Solids and carbon balance confirmed loss of organics during thermal hydrolysis. • Reaction pathways for thermal hydrolysis and wet oxidation are proposed. We evaluated the effect of hydrothermal pretreatments, i.e., thermal hydrolysis (TH) and wet oxidation (WO) on sewage sludge to promote resource recovery. The hydrothermal processes were performed under mild temperature conditions (140°C–180°C) in a high pressure reactor. The reaction in acidic environment (pH= 3.3) suppressed the formation of the color imparting undesirable Maillard’s compounds. The oxidative conditions resulted in higher volatile suspended solids (VSS) reduction (~90%) and chemical oxygen demand (COD) removal (~55%) whereas TH caused VSS and COD removals of ~65% and ~27%, respectively at a temperature of 180°C. During TH, the concentrations of carbohydrates and proteins in treated sludge were 400–1000 mg/L and 1500–2500 mg/L, respectively. Whereas, WO resulted in solids solubilization followed by oxidative degradation of organics into smaller molecular weight carboxylic acids such as acetic acid (~400–500 mg/L). Based on sludge transformation products generated during the hydrothermal pretreatments, simplified reaction pathways are predicted. Finally, the application of macromolecules (such as proteins), VFAs and nutrients present in the treated sludge are also discussed. The future study should focus on the development of economic recovery methods for various value-added compounds.

关键词： Hydrothermal pretreatment     Reaction kinetics     Reaction pathway     Sewage sludge     Thermal hydrolysis     Wet oxidation    

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Numerical modeling of mass transfer processes coupling with reaction for the design of the ozone oxidation

Hong Li, Fang Yi, Xingang Li, Xin Gao

《化学科学与工程前沿（英文）》 2021年 第15卷 第3期   页码 602-614 doi: 10.1007/s11705-020-1963-4

摘要： A computational model for an ozone oxidation column reactor used in dyeing wastewater treatment is proposed to represent, simulate, and predict the ozone bubble process. Considering the hydrodynamics, mass transfer, and ozone oxidation reaction, coupling modeling can more realistically calculate the ozone oxidation bubble process than the splitting methods proposed in previous research. The modeling is validated and shows great consistency with experimental data. The verified model is used to analyze the effect of operating conditions, such as the initial gas velocity and the ozone concentration, and structural conditions, such as multiple gas inlets. The ozone consumption is influenced by the gas velocity and the initial ozone concentration. The ozone’s utilization decreases with the increasing gas velocity while nearly the same at different initial ozone concentrations. Simulation results can be used in guiding the practical operation of dyeing wastewater treatment and in other ozonation systems with known rate constants in wastewater treatment.

关键词： ozone     wastewater treatment     numerical simulation     mass transfer    

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Kinetics of oxidation of dimethyl trisulfide by potassium permanganate in drinking water

Xiaoyan MA, Shifei HU, Hongyu WANG, Jun LI, Jing HUANG, Yun ZHANG, Weigang LU, Qingsong LI

《环境科学与工程前沿（英文）》 2012年 第6卷 第2期   页码 171-176 doi: 10.1007/s11783-011-0319-1

摘要： Metabolites of algae such as geosmin, 2-methylisoborneol etc. are reported to induce pungent odors into drinking water and attract additional scientific attention. Recently, in China, taste and odor outbreaks in drinking water supply have become increasingly common. In source water affected by eutrophication, dimethyl trisulfide, speculated to be produced by decayed algae, was found to be the source of taste and odor issues and can be removed effectively by usual oxidation agents. In this experimental study, batch scale tests were carried out focusing on the removal of dimethyl trisulfide. Reaction kinetics of dimethyl trisulfide oxidized by potassium permanganate in water had been studied; influence factors such as pH, organic substrate, other existed taste, and odor contaminant in equivalent concentration were also discussed. Results showed that dimethyl trisulfide can be removed by potassium permanganate efficiently; the ratio can reach more than 70% with oxidant dosage of 4 mg·L and contact time prolonged to 120 min. The dimethyl trisulfide decomposition followed a second-order kinetics pattern with a rate constant = 0.00213 L·(min·mg) . Typically, the degradation rate of dimethyl trisulfide was increased with the increasing KMnO dosage, but dramatically dropped with the increasing levels of humic acid (1.8–4.5 mg·L ) and other odor-causing compounds (e.g. -cyclocitral, 0–1886.0 μg·L ). Solution pH (5.2–9.0) and initial dimethyl trisulfide concentration did not significantly affected the degradation. This study demonstrates that KMnO oxidation is an effective option to remove dimethyl trisulfide from water.

关键词： odor and taste     oxidation reaction     reaction kinetics     water treatment    

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Enhancement of extracellular Cr(VI) reduction for anammox recovery using hydrazine: performance, pathways

《环境科学与工程前沿（英文）》 2023年 第17卷 第9期 doi: 10.1007/s11783-023-1715-z

摘要：

● N2H4 addition enhanced and recovered anammox performance under Cr(VI) stress.

关键词： Extracellular Cr(VI) reduction     Electron transfer     Anammox     Hydrazine     Cr(VI) inhibition    

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Modeling the aqueous reaction kinetics of estriol with ferrate

Cong LI, Naiyun GAO

《化学科学与工程前沿（英文）》 2009年 第3卷 第1期   页码 39-45 doi: 10.1007/s11705-009-0098-4

摘要： In this study the aqueous oxidation kinetics of estriol (E3) by potassium ferrate (K FeO ), a chemical for its strong oxidizing power and for producing a coagulant from its reduced state (i.e. Fe(III)), was evaluated in the range of pH 8-12 with different molar ratios of the reactants. As the degree of Fe(VI) protonation varies with the solution pH, it was found that a first order model was not suitable to describe the oxidation reaction. This paper describes a theoretical representation that closely models the reaction kinetics of E3 and ferrate. From this modeling, the reaction rates of HFe and Fe with E3 have been determined. The results show that the reactivity of HFe with dissociated and undissociated E3 is greater than that of Fe , and that E3 is more reactive in its dissociated state.

关键词： ferrate     estriol     endocrine disruptor     kinetics     oxidation    

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Product identification and toxicity change during oxidation of methotrexate by ferrate and permanganate

《环境科学与工程前沿（英文）》 2022年 第16卷 第7期 doi: 10.1007/s11783-021-1501-8

摘要：

• Oxidation of methotrexate by high-valent metal-oxo species was first explored.

关键词： Anticancer drugs     High-valent metal-oxo species     Oxidation kinetics     Reaction mechanisms     Multi-endpoint toxicity    

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Ozonation of the 5-fluorouracil anticancer drug and its prodrug capecitabine: Reaction kinetics, oxidation

Siyu Chen, Lee Blaney, Ping Chen, Shanshan Deng, Mamatha Hopanna, Yixiang Bao, Gang Yu

《环境科学与工程前沿（英文）》 2019年 第13卷 第4期 doi: 10.1007/s11783-019-1143-2

摘要：

Specific second-order rate constants were determined for 5-FU and CAP with ozone.

Reaction sites were confirmed by kinetics, Fukui analysis, and products.

The olefin moiety was the main ozone reaction site for 5-FU and CAP.

Carboxylic acids comprised most of the residual TOC for 5-FU.

Ozonation removed the toxicity associated with 5-FU and products but not CAP.

关键词： Ozone     5-fluorouracil     Capecitabine     Hydroxyl radicals     Chemotherapy agents     Toxicity    

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A novel flavonol-based colorimetric and turn-on fluorescent probe for rapid determination of hydrazine

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 24-33 doi: 10.1007/s11705-022-2171-1

摘要： Hydrazine is extremely toxic and causes severe harm to human body. Herein, a novel fluorescent probe 4-oxo-2-styryl-4H-chromen-3-yl thiophene-2-carboxylate (FHT) was synthesized for detecting hydrazine by using natural cinnamaldehyde as starting material. This probe exhibited significantly enhanced fluorescence response towards hydrazine over various common metal ions, anions, and amine compounds. The detection limit of probe FHT for hydrazine was as low as 0.14 μmol·L–1, significantly lower than that of the threshold value of 0.312 μmol·L–1, imposed by the Environmental Protection Agency. Moreover, the proposed probe was able to detect hydrazine within wide pH (5–10) and linear detection ranges (0–110 μmol·L–1). This probe was employed for determining trace hydrazine in different environmental water samples. The probe FHT-loaded filter paper strips were able to conveniently detect hydrazine of low concentration through distinct naked-eye and fluorescent color changes. Importantly, the probe FHT with low cytotoxicity was successfully applied to visualize hydrazine in living Hela cells and zebrafish.

关键词： cinnamaldehyde     3-hydroxychromone derivative     hydrazine     fluorescent probe    

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Room temperature preparation of hydrazine-linked covalent organic frameworks coated capillaries for

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 548-556 doi: 10.1007/s11705-022-2252-1

摘要： Covalent organic frameworks (COFs) have been increasingly used in capillary electrochromatography due to their excellent characteristics. In this work, hydrazine-linked TFPB-DHzDS (TFPB: 1,3,5-tris(4-formylphenyl)benzene; DHzDS: 2,5-bis(3-(ethylthio)propoxy)terephthalohydrazide) was first synthesized by a simpler and easier method at room temperature and introduced into capillary electrochromatography as coating material. The TFPB-DHzDS coated capillaries were prepared by an in-situ growth process at room temperature. After optimizing the coating concentration and experimental conditions of capillary electrochromatography, baseline separation of two groups of polycyclic aromatic hydrocarbons was achieved based on the TFPB-DHzDS coated capillary. And the established method was used successfully to determine PAHs in natural water and soil samples. The spiked recoveries of polycyclic aromatic hydrocarbons in these samples ranged from 90.01% to 111.0%, indicating that the method is reliable and could detect polycyclic aromatic hydrocarbons in natural samples. Finally, molecular simulation was applied to study and visualize the interaction between the analytes and coating COF materials to investigate the molecular level separation mechanism further.

关键词： hydrazine-linked TFPB-DHzDS     in-situ growth method     open-tubular capillary electrochromatography     molecular simulations    

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A perspective on the promoting effect of Ir and Au on Pd toward the ethanol oxidation reaction in alkaline

S. Y. SHEN, Y. G. GUO, G. H. WEI, L. X. LUO, F. LI, J. L. ZHANG

《能源前沿（英文）》 2018年 第12卷 第4期   页码 501-508 doi: 10.1007/s11708-018-0586-7

摘要： There remain great challenges in developing highly efficient electrocatalysts with both high activity and good stability for the ethanol oxidation reaction in alkaline media. Herein, two architectures of tri-metallic PdIrAu/C electrocatalysts are designed and the promoting effect of Au and Ir on Pd toward the ethanol oxidation reaction (EOR) in alkaline media is investigated in detail. On the one hand, the tri-metallic Pd Au Ir/C electrocatalyst with a solid solution alloy architecture is less active relative to Pd Ir/C and Pd/C while the stabilizing effect of Au leads to both a higher activity and a lower degradation percentage after 3000 cycles of the accelerated degradation test (ADT) on Pd Au Ir/C than those on Pd Ir/C. On the other hand, the tri-metallic Pd Ir@(1/3Au)/C electrocatalyst with a near surface alloy architecture delivers a much higher activity with an improvement up to 50.4% compared to Pd Ir/C. It is speculated that for the tri-metallic Pd Ir@(1/3Au)/C electrocatalyst, certain Au atoms are well designed on surfaces to introduce an electronic modification, thus leading to an anti-poisoning effect and improving the EOR activity.

关键词： fuel cells     catalysts     ethanol oxidation     alkaline media     solid solution alloy     near surface alloy    

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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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Anion-exchange membrane direct ethanol fuel cells: Status and perspective

T.S. Zhao, Y.S. Li, S.Y. Shen

《能源前沿（英文）》 2010年 第4卷 第4期   页码 443-458 doi: 10.1007/s11708-010-0127-5

摘要： Direct ethanol fuel cells (DEFCs) are a promising carbon-neutral and sustainable power source for portable, mobile, and stationary applications. However, conventional DEFCs that use acid proton-exchange membranes (typically Nafion type) and platinum-based catalysts exhibit low performance (i.e., the state-of-the-art peak power density is 79.5 mW/cm at 90°C). Anion-exchange membrane (AEM) DEFCs that use low-cost AEM and non-platinum catalysts have recently been demonstrated to yield a much better performance (i.e., the state-of-the-art peak power density is 160 mW/cm at 80°C). This paper provides a comprehensive review of past research on the development of AEM DEFCs, including the aspects of catalysts, AEMs, and single-cell design and performance. Current and future research challenges are identified along with potential strategies to overcome them.

关键词： fuel cell     direct ethanol fuel cells     anion-exchange membrane     ethanol oxidation reaction     oxygen reduction reaction     cell performance    

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Interaction and independence on methane oxidation of landfill cover soil among three impact factors:

Pinjing HE, Na YANG, Wenjuan FANG, Fan Lü, Liming SHAO

《环境科学与工程前沿（英文）》 2011年 第5卷 第2期   页码 175-185 doi: 10.1007/s11783-011-0320-8

摘要： To understand the influence patterns and interactions of three important environmental factors, i.e. soil water content, oxygen concentration, and ammonium addition, on methane oxidation, the soils from landfill cover layers were incubated under full factorial parameter settings. In addition to the methane oxidation rate, the quantities and community structures of methanotrophs were analyzed to determine the methane oxidation capacity of the soils. Canonical correspondence analysis was utilized to distinguish the important impact factors. Water content was found to be the most important factor influencing the methane oxidation rate and Type II methanotrophs, and the optimum value was 15% (w/w), which induced methane oxidation rates 10- and 6- times greater than those observed at 5% (w/w) and 20% (w/w), respectively. Ambient oxygen conditions were more suitable for methane oxidation than 3% oxygen. The addition of of ammonium induced different effects on methane oxidation capacity when conducted at low or high water content. With regard to the methanotrophs, Type II was sensitive to the changes of water content, while Type I was influenced by oxygen content. Furthermore, the methanotrophic acidophile, , was detected in soils with a pH of 4.9, which extended their known living environments.

关键词： quantitative polymerase chain reaction (PCR)     denaturing gradient gel electrophoresis (DGGE)     principal component analysis (PCA)     canonical correspondence analysis (CCA)    

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标题 作者 时间 类型 操作

Copper nanoparticles/polyaniline-derived mesoporous carbon electrocatalysts for hydrazine oxidation

Tao Zhang, Tewodros Asefa

期刊论文

Platinum on nitrogen doped graphene and tungsten carbide supports for ammonia electro-oxidation reaction

期刊论文

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

Milan Malhotra, Anurag Garg

期刊论文

Numerical modeling of mass transfer processes coupling with reaction for the design of the ozone oxidation

Hong Li, Fang Yi, Xingang Li, Xin Gao

期刊论文

Kinetics of oxidation of dimethyl trisulfide by potassium permanganate in drinking water

Xiaoyan MA, Shifei HU, Hongyu WANG, Jun LI, Jing HUANG, Yun ZHANG, Weigang LU, Qingsong LI

期刊论文

Enhancement of extracellular Cr(VI) reduction for anammox recovery using hydrazine: performance, pathways

期刊论文

Modeling the aqueous reaction kinetics of estriol with ferrate

Cong LI, Naiyun GAO

期刊论文

Product identification and toxicity change during oxidation of methotrexate by ferrate and permanganate

期刊论文

Ozonation of the 5-fluorouracil anticancer drug and its prodrug capecitabine: Reaction kinetics, oxidation

Siyu Chen, Lee Blaney, Ping Chen, Shanshan Deng, Mamatha Hopanna, Yixiang Bao, Gang Yu

期刊论文

A novel flavonol-based colorimetric and turn-on fluorescent probe for rapid determination of hydrazine

期刊论文

Room temperature preparation of hydrazine-linked covalent organic frameworks coated capillaries for

期刊论文

A perspective on the promoting effect of Ir and Au on Pd toward the ethanol oxidation reaction in alkaline

S. Y. SHEN, Y. G. GUO, G. H. WEI, L. X. LUO, F. LI, J. L. ZHANG

期刊论文

Redox reactions of iron and manganese oxides in complex systems

Jianzhi Huang, Huichun Zhang

期刊论文

Anion-exchange membrane direct ethanol fuel cells: Status and perspective

T.S. Zhao, Y.S. Li, S.Y. Shen

期刊论文

Interaction and independence on methane oxidation of landfill cover soil among three impact factors:

Pinjing HE, Na YANG, Wenjuan FANG, Fan Lü, Liming SHAO

期刊论文