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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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Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidationreaction

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

《能源前沿（英文）》 2017年 第11卷 第3期   页码 310-317 doi: 10.1007/s11708-017-0491-5

摘要： Pd nanoparticles supported on nitrogen doped carbon black (Vulcan XC-72R) with two different levels of doping were prepared by the microwave-assisted ethylene glycol reduction process and used as catalyst for the formic acid electro-oxidation (FAEO). The results indicate that the different nitrogen doping contents in Pd/N-C catalysts have a significant effect on the performance of FAEO. A higher N content facilitates the uniform dispersion of Pd nanoparticles on carbon black with narrow particle size distribution. Furthermore, the electrochemical results show that the catalyst with a higher N-doping content possesses a higher catalytic activity and a long-term stability for FAEO. The peak current density of the Pd/N-C (high) catalyst is 1.27 and 2.31 times that of the Pd/N-C (low) and homemade Pd/C-H catalyst. The present paper may provide a simple method for preparation of high-performance anode catalyst for direct formic acid fuel cells (DFAFCs).

关键词： formic acid electro-oxidation     nitrogen doped     oxidized carbon     nitrogen content    

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Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

《能源前沿（英文）》 doi: 10.1007/s11708-023-0908-2

摘要： The Haber-Bosch process is the most widely used synthetic ammonia technology at present. Since its invention, it has provided an important guarantee for global food security. However, the traditional Haber-Bosch ammonia synthesis process consumes a lot of energy and causes serious environmental pollution. Under the serious pressure of energy and environment, a green, clean, and sustainable ammonia synthesis route is urgently needed. Electrochemical synthesis of ammonia is a green and mild new method for preparing ammonia, which can directly convert nitrogen or nitrate into ammonia using electricity driven by solar, wind, or water energy, without greenhouse gas and toxic gas emissions. Herein, the basic mechanism of the nitrogen reduction reaction (NRR) to ammonia and nitrate reduction reaction (NO3− RR) to ammonia were discussed. The representative approaches and major technologies, such as lithium mediated electrolysis and solid oxide electrolysis cell (SOEC) electrolysis for NRR, high activity catalyst and advanced electrochemical device fabrication for NO3 − RR and electrochemical ammonia synthesis were summarized. Based on the above discussion and analysis, the main challenges and development directions for electrochemical ammonia synthesis were further proposed.

关键词： electrochemical ammonia synthesis     nitrogen     nitrate     nitrogen reduction reaction (NRR) to ammonia     nitrate reduction reaction (NO–3 RR)    

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A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 388-394 doi: 10.1007/s11783-012-0475-y

摘要： Direct formic acid fuel cells are a promising portable power-generating device, and the development of efficient anodic catalysts is essential for such a fuel cell. In this work Pt-Bi nanoparticles supported on micro-fabricated gold wire array substrate were synthesized using an electrochemical deposition method for formic acid oxidation in fuel cells. The surface morphology and element components of the Pt-Bi/Au nanoparticles were characterized, and the catalytic activities of the three Pt-Bi/Au nanoparticle electrodes with different Pt/Bi ratios for formic acid oxidation were evaluated. It was found that Pt Bi /Au had a much higher catalytic activity than Pt Bi /Au and Pt Bi /Au, and Pt Bi /Au exhibited a current density of 2.7 mA·cm , which was 27-times greater than that of Pt/Au. The electro-catalytic activity of the Pt-Bi/Au electrode for formic acid oxidation increased with the increasing Bi content, suggesting that it would be possible to achieve an efficient formic acid oxidation on the low Pt-loading. Therefore, the Pt-Bi/Au electrode offers a promising catalyst with a high activity for direct oxidation of formic acid in fuel cells.

关键词： catalyst     electrochemical deposition     formic acid oxidation     fuel cell     gold wire array     microfabrication    

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Enhancement on the ammonia oxidation capacity of ammonia-oxidizing archaeon originated from wastewater

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-020-1375-1

摘要：

• AOA’s ammonia oxidizing capacity was enhanced under moderate magnetic field.

关键词： Ammonia-oxidizing archaeon     Ammonia oxidation     Magnetic field     Magnetotaxis     Heredity    

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Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

《环境科学与工程前沿（英文）》 2022年 第16卷 第4期 doi: 10.1007/s11783-021-1476-5

摘要：

• MES was constructed for simultaneous ammonia removal and acetate production.

关键词： Biocathode     Carbon dioxide     Electrochemical oxidation     Graphite anode     Boron-doped diamond    

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The combined effects of biomass and temperature on maximum specific ammonia oxidation rate in domestic

《环境科学与工程前沿（英文）》 2021年 第15卷 第6期 doi: 10.1007/s11783-021-1411-9

摘要：

• Actual SAORs was determined using MLVSS and temperature.

关键词： Specific ammonia oxidation rate     Sequencing batch reactor     Biomass     Temperature coefficient     Model simulation    

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ROOT EXUDATES FROM CANOLA EXHIBIT BIOLOGICAL NITRIFICATION INHIBITION AND ARE EFFECTIVE IN INHIBITING AMMONIAOXIDATION IN SOIL

《农业科学与工程前沿（英文）》 2022年 第9卷 第2期   页码 177-186 doi: 10.15302/J-FASE-2021421

摘要：

A range of plant species produce root exudates that inhibit ammonia-oxidizing microorganisms. This biological nitrification inhibition (BNI) capacity can decrease N loss and increase N uptake from the rhizosphere. This study sought evidence for the existence and magnitude of BNI capacity in canola ( Brassica napus). Seedlings of three canola cultivars, Brachiaria humidicola(BNI positive) and wheat ( Triticum aestivum) were grown in a hydroponic system. Root exudates were collected and their inhibition of the ammonia oxidizing bacterium, Nitrosospira multiformis, was tested. Subsequent pot experiments were used to test the inhibition of native nitrifying communities in soil. Root exudates from canola significantly reduced nitrification rates of both N. multiformis cultures and native soil microbial communities. The level of nitrification inhibition across the three cultivars was similar to the well-studied high-BNI species B. humidicola. BNI capacity of canola may have implications for the N dynamics in farming systems and the N uptake efficiency of crops in rotational farming systems. By reducing nitrification rates canola crops may decrease N losses, increase plant N uptake and encourage microbial N immobilization and subsequently increase the pool of organic N that is available for mineralization during the following cereal crops.

关键词： ammonia oxidizing microorganisms / biological nitrification inhibition / farming rotations / nitrogen cycling / nitrogen use efficiency    

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Identification of resistant pharmaceuticals in ozonation using QSAR modeling and their fate in electro-peroxone

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-021-1394-6

摘要：

• Effect of converting ozonation to E-peroxone was studied on pharmaceutical removal.

关键词： Ozone     Electro-peroxone     Wastewater     Quantitative structure activity relationship     Advanced oxidation processes    

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Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1345-7

摘要： Abstract • Electrode fouling is characterized by non-destructive characterization. • Electrode fouling is highly dependent on electrochemical process. • Active chlorine can prevent the formation of polymeric fouling film. Electrode fouling is a problem that commonly occurs during electro-oxidation water purification. This study focused on identifying the fouling behavior of Pt electrode associated with the formation of polymeric layer during electro-oxidation of phenol. The in situ electrochemical measurements and non-destructive observation of the electrode morphology were reported. The results demonstrated that the electrode fouling was highly dependent on thermodynamic process of electrode that was controlled by anode potential. At anode potential lower than 1.0 V vs SHE, the direct electro-oxidation caused the electrode fouling by the formation of polymeric film. The fouling layer decreased the electrochemically active surface area from 8.38 cm2 to 1.57 cm2, indicated by the formation of polymeric film with thickness of 2.3 mm, increase in mass growing at a rate of 3.26 μg/cm2/min. The degree to which the anode was fouled was independent of anion in the electrolyte. In comparison, at anode potential higher than 2.7 V vs SHE, the anions (e.g., chloride) could exert a major influence to the behavior of electrode fouling. The presence of chloride was shown to mitigate the fouling of electrode significantly through preventing the formation of polymeric film by active chlorine (e.g., Cl• and Cl2) produced from anodic oxidation of chloride. Since chloride is the most abundant anionic species existing in both natural and engineered water system, this study not only offers a deep insight into the mechanism of electrode fouling, but also suggests strategies for anti-fouling in the presence of chloride in electro-oxidation process.

关键词： Electro-oxidation     Electrode fouling     Polymeric film     Chloride ions    

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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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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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标题 作者 时间 类型 操作

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

期刊论文

Nitrogen-doped carbon black supported Pd nanoparticles as an effective catalyst for formic acid electro-oxidationreaction

Na SUN, Minglei WANG, Jinfa CHANG, Junjie GE, Wei XING, Guangjie SHAO

期刊论文

Recent advances and challenges of nitrogen/nitrate electro catalytic reduction to ammonia synthesis

期刊论文

A Pt-Bi bimetallic nanoparticle catalyst for direct electro-oxidation of formic acid in fuel cells

Shu-Hong LI, Yue ZHAO, Jian CHU, Wen-Wei LI, Han-Qing YU, Gang LIU, Yang-Chao TIAN

期刊论文

Enhancement on the ammonia oxidation capacity of ammonia-oxidizing archaeon originated from wastewater

期刊论文

Electricity-driven ammonia oxidation and acetate production in microbial electrosynthesis systems

期刊论文

The combined effects of biomass and temperature on maximum specific ammonia oxidation rate in domestic

期刊论文

ROOT EXUDATES FROM CANOLA EXHIBIT BIOLOGICAL NITRIFICATION INHIBITION AND ARE EFFECTIVE IN INHIBITING AMMONIAOXIDATION IN SOIL

期刊论文

Identification of resistant pharmaceuticals in ozonation using QSAR modeling and their fate in electro-peroxone

期刊论文

Characterization of electrode fouling during electrochemical oxidation of phenolic pollutant

Xuefeng Liu, Shijie You, Fang Ma, Hao Zhou

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

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