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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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Plasma-electrochemical synthesis of europium doped cerium oxide nanoparticles

Liangliang Lin, Xintong Ma, Sirui Li, Marly Wouters, Volker Hessel

《化学科学与工程前沿（英文）》 2019年 第13卷 第3期   页码 501-510 doi: 10.1007/s11705-019-1810-7

摘要： In the present study, a plasma-electrochemical method was demonstrated for the synthesis of europium doped ceria nanoparticles. Ce(NO ) ·6H O and Eu(NO ) ·5H O were used as the starting materials and being dissolved in the distilled water as the electrolyte solution. The plasma-liquid interaction process was investigated by an optical emission spectroscopy, and the obtained products were characterized by complementary analytical methods. Results showed that crystalline cubic CeO :Eu nanoparticles were successfully obtained, with a particle size in the range from 30 to 60 nm. The crystal structure didn’t change during the calcination at a temperature from 400°C to 1000°C, with the average crystallite size being estimated to be 52 nm at 1000°C. Eu ions were shown to be effectively and uniformly doped into the CeO lattices. As a result, the obtained nanophosphors emit apparent red color under the UV irradiation, which can be easily observed by naked eye. The photoluminescence spectrum further proves the downshift behavior of the obtained products, where characteristic D → F transitions of Eu ions had been detected. Due to the simple, flexible and environmental friendly process, this plasma-electrochemical method should have great potential for the synthesis of a series of nanophosphors, especially for bio-application purpose.

关键词： plasma-electrochemical method     europium doped ceria     rare earth nanoparticles     photoluminescence    

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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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Synthesis, spectroscopic, and electrochemical properties of two dyads consisted of tetrathiafulvalene

Guoqiao LAI, Yibo LIU, Meijiang LI, Yongjia SHEN

《化学科学与工程前沿（英文）》 2009年 第3卷 第2期   页码 192-195 doi: 10.1007/s11705-009-0015-x

摘要： Two donor-σ-acceptor molecules containing tetrathiafulvalene (TTF) and carbazole moieties were synthesized by the reaction of 9-(4-bromo-butyl)-carbazole ( ) with 2,6-bis(hexylthio)-3-(2-cyanoethylthio)-7-(methylthio)-tetrathiafulvalene ( ) or 2,6-bis(2-cyanoethylthio)-3,7-bis(methylthio)tetrathiafulvalene ( ) in the presence of CsOH·H O, respectively. The structures of the molecules were characterized by H NMR, C NMR, MS, and elemental analyses. They showed negligible intramolecular charge-transfer interaction in their ground states as indicated by their UV-Vis spectroscopics and cyclic voltammetry results. Compared with carbazole, their fluorescence was strongly quenched, which implied that a photo induced electron transfer (PET) interaction between TTF and carbazole moieties occurred.

关键词： donor-σ-acceptor molecule     intramolecular charge transfer interaction     photo induced electron transfer     tetrathiafulvalene     carbazole    

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Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

《环境科学与工程前沿（英文）》 2013年 第7卷 第3期   页码 428-434 doi: 10.1007/s11783-013-0517-0

摘要： This work describes the environmentally friendly technology for oxidation of ammonia (NH ) to form nitrogen at temperatures range from 423K to 673K by selective catalytic oxidation (SCO) over a nanosized Pt-Rh/γ-Al O catalyst prepared by the incipient wetness impregnation method of hexachloroplatinic acid (H PtCl ) and rhodium (III) nitrate (Rh(NO ) ) with γ-Al O in a tubular fixed-bed flow quartz reactor (TFBR). The characterization of catalysts were thoroughly measured using transmission electron microscopy (TEM), three-dimensional excitation-emission fluorescent matrix (EEFM) spectroscopy, UV-Vis absorption, dynamic light-scattering (DLS), zeta potential meter, and cyclic voltammetry (CV). The results demonstrated that at a temperature of 673K and an oxygen content of 4%, approximately 99% of the NH was removed by catalytic oxidation over the nanosized Pt-Rh/γ-Al O catalyst. N was the main product in NH -SCO process. Further, it reveals that the oxidation of NH was proceeds by the over-oxidation of NH into NO, which was conversely reacted with the NH to yield N . Therefore, the application of nanosized Pt-Rh/γ-Al O catalyst can significantly enhance the catalytic activity toward NH oxidation. One fluorescent peak for fresh catalyst was different with that of exhausted catalyst. It indicates that EEFM spectroscopy was proven to be an appropriate and effective method to characterize the Pt clusters in intrinsic emission from nanosized Pt-Rh/γ-Al O catalyst. Results obtained from the CV may explain the significant catalytic activity of the catalysts.

关键词： ammonia (NH3)     nanosized Pt-Rh/γ-Al2O3 catalyst     excitation-emission fluorescent matrix (EEFM)     selective catalytic oxidation (SCO)     tubular fixed-bed reactor (TFBR)    

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Optimization of electrochemically synthesized Cu

Kasra Pirzadeh, Ali Asghar Ghoreyshi, Mostafa Rahimnejad, Maedeh Mohammadi

《化学科学与工程前沿（英文）》 2020年 第14卷 第2期   页码 233-247 doi: 10.1007/s11705-019-1893-1

摘要： Cu (BTC) , a common type of metal organic framework (MOF), was synthesized through electrochemical route for CO capture and its separation from N . Taguchi method was employed for optimization of key parameters affecting the synthesis of Cu (BTC) . The results indicated that the optimum synthesis conditions with the highest CO selectivity can be obtained using 1 g of ligand, applied voltage of 25 V, synthesis time of 2 h, and electrode length of 3 cm. The single gas sorption capacity of the synthetized microstructure Cu (BTC) for CO (at 298 K and 1 bar) was a considerable value of 4.40 mmol·g . The isosteric heat of adsorption of both gases was calculated by inserting temperature-dependent form of Langmuir isotherm model in the Clausius-Clapeyron equation. The adsorption of CO /N binary mixture with a concentration ratio of 15/85 vol-% was also studied experimentally and the result was in a good agreement with the predicted value of IAST method. Moreover, Cu (BTC) showed no considerable loss in CO adsorption after six sequential cycles. In addition, artificial neural networks (ANNs) were also applied to predict the separation behavior of CO /N mixture by MOFs and the results revealed that ANNs could serve as an appropriate tool to predict the adsorptive selectivity of the binary gas mixture in the absence of experimental data.

关键词： Cu3(BTC)2 electrochemical synthesis     CO2 adsorption     Taguchi optimization     ANN modeling    

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Abundance and distribution of ammonia-oxidizing archaea in Tibetan and Yunnan plateau agricultural soils

Kun DING,Xianghua WEN,Liang CHEN,Daishi HUANG,Fan FEI,Yuyang LI

《环境科学与工程前沿（英文）》 2014年 第8卷 第5期   页码 693-702 doi: 10.1007/s11783-014-0635-3

摘要： As low oxygen and high ultraviolet (UV) exposure might significantly affect the microbial existence in plateau, it could lead to a specialized microbial community. To determine the abundance and distribution of ammonia-oxidizing archaea (AOA) in agricultural soil of plateau, seven soil samples were collected respectively from farmlands in Tibet and Yunnan cultivating the wheat, highland-barley, and colza, which are located at altitudes of 3200–3800 m above sea level. Quantitative PCR (q-PCR) and clone library targeting on gene were used to quantify the abundances of AOA and ammonia-oxidizing bacteria (AOB), and characterize the community structures of AOA in the samples. The number of AOA cells (9.34 × 10 –2.32 × 10 g soil) was 3.86–21.84 times greater than that of AOB cells (6.91 × 10 –1.24 × 10 g soil) in most of the samples, except a soil sample cultivating highland-barley with an AOA/AOB ratio of 0.90. Based Kendall’s correlation coefficient, no remarkable correlation between AOA abundance and the environmental factor was observed. Additionally, the diversities of AOA community were affected by total nitrogen and organic matter concentration in soils, suggesting that AOA was probably sensitive to several environmental factors, and could adjust its community structure to adapt to the environmental variation while maintaining its abundance.

关键词： ammonia-oxidizing archaea     ammonia-oxidizing bacteria     quantitative PCR     clone library     plateau    

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Heat and mass transfer of ammonia-water in falling film evaporator

Xianbiao BU, Weibin MA, Huashan LI

《能源前沿（英文）》 2011年 第5卷 第4期   页码 358-366 doi: 10.1007/s11708-011-0161-y

摘要： To investigate the performance of heat and mass transfer of ammonia-water during the process of falling film evaporation in vertical tube evaporator, a mathematical model of evaporation process was presented, the solution of which that needed a coordinate transformation was based on stream function. The computational results from the mathematical model were validated with experimental data. Subsequently, a series of parameters, such as velocity, film thickness and concentration, etc., were obtained from the mathematical model. Calculated results show that the average velocity and the film thickness change dramatically at the entrance region when <100 mm, while they vary slightly with the tube length in the fully developed region when >100 mm. The average concentration of the solution reduces along the tube length because of evaporation, but the reducing tendency becomes slow. It can be concluded that there is an optimalβrelationship between the tube length and the electricity generated. The reason for the bigger concentration gradient in the direction is that the smooth tube is chosen in the calculation. It is suggested that the roll-worked enhanced tube or other enhanced tube can reduce the concentration gradient in the film thickness direction and enhance the heat and mass transfer rate.

关键词： falling film evaporation     ammonia-water     heat and mass transfer    

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Facile synthesis of hierarchical flower-like Ag/Cu

Mengyun Wang, Shengbo Zhang, Mei Li, Aiguo Han, Xinli Zhu, Qingfeng Ge, Jinyu Han, Hua Wang

《化学科学与工程前沿（英文）》 2020年 第14卷 第5期   页码 813-823 doi: 10.1007/s11705-019-1854-8

摘要： Novel, hierarchical, flower-like Ag/Cu O and Au/Cu O nanostructures were successfully fabricated and applied as efficient electrocatalysts for the electrochemical reduction of CO . Cu O nanospheres with a uniform size of ~180 nm were initially synthesized. Thereafter, Cu O was used as a sacrificial template to prepare a series of Ag/Cu O composites through galvanic replacement. By varying the Ag/Cu atomic ratio, Ag /Cu O, having a hierarchical, flower-like nanostructure with intersecting Ag nanoflakes encompassing an inner Cu O sphere, was prepared. The as-prepared Ag /Cu O samples presented higher Faradaic efficiencies (FE) for CO and relatively suppressed H evolution than the parent Cu O nanospheres due to the combination of Ag with Cu O in the former. Notably, the highest CO evolution rate was achieved with Ag /Cu O due to the larger electroactive surface area furnished by the hierarchical structure. The same hierarchical flower-like structure was also obtained for the Au /Cu O composite, where the FE (10%) was even higher than that of Ag /Cu O. Importantly, the results reveal that Ag /Cu O and Au /Cu O both exhibit remarkably improved stability relative to Cu O. This study presents a facile method of developing hierarchical metal-oxide composites as efficient and stable electrocatalysts for the electrochemical reduction of CO .

关键词： bimetallic nanostructure     hierarchical metal/oxide nanomaterial     galvanic replacement     electrochemical reduction of CO2    

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Simulation on thermodynamic state of ammonia carbonation at low temperature and low pressure

Jingcai ZHAO, Xingfu SONG, Ze SUN, Jianguo YU

《化学科学与工程前沿（英文）》 2013年 第7卷 第4期   页码 447-455 doi: 10.1007/s11705-013-1370-1

摘要： This study on thermodynamic property of NH -CO -H O system provided the basic data for ammonia carbonation. Simulations on vapor-liquid equilibrium (VLE) of ammonia carbonation with different physical properties were discussed in NH -H O and NH -CO -H O systems, respectively. The results indicated that at low temperature (303.15 K–363.15 K) and pressure (0.1–0.4 MPa), the PR (Peng-Robinson) equation was suitable for the description of the thermodynamic state in NH -H O system. NRTL (Non-Random-Two-Liquid) series models were selected for NH -CO -H O mixed electrolyte solution system. VLE data regression results showed that NRTL series models were suitable for describing thermodynamic properties of NH -CO -H O system, because average relative error fitting with each model was about 1%. As an asymmetric electrolytes model in NRTL model, E–NRTLRK (Electrolyte NRTL Redlich Kwong) could most accurately fit VLE data of NH -CO -H O system, with fitting error less than 1%. In the extent temperature range of 273.15 K–363.15 K, the prediction of product component using E-NRTLRK model for ammonia carbonation agreed well with the data reported in literature.

关键词： vapor-liquid equilibrium     activity coefficient     carbon dioxide     ammonia     NRTL    

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Design guidelines for urea hydrolysers for ammonia demand of the SCR DENOX project in coal-fired power

Peng ZHENG, Xuan YAO, Wei ZHENG

《能源前沿（英文）》 2013年 第7卷 第1期   页码 127-132 doi: 10.1007/s11708-012-0225-7

摘要： Ammonia is highly volatile and will present substantial environmental and operation hazards when leaking into the air. However, ammonia is the most common reactant in the DENOX project to eliminate NO in the flue gas. The storage and transportation of liquid ammonia has always been a dilemma of the power plant. Urea is a perfect substitute source for ammonia in the plant. Urea hydrolysis technology can easily convert urea into ammonia with low expense. Presently, there is still no self-depended mature urea hydrolysis technology for the DENOX project in China; therefore, this paper proposes several guidelines to design the urea hydrolyser by theoretical analysis. Based on theoretical analysis, a simulation model is built to simulate the chemical reaction in the urea hydrolyser and is validated by the operational data of the commercial hydrolyser revealed in the literature. This paper endeavors to propose suggestions and guidelines to develop domestically urea hydrolysers in China.

关键词： urea     hydrolyser     ammonia     selective catalytic reduction (SCR)    

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Recent advances in electrochemical decontamination of perfluorinated compounds from water: a review

《环境科学与工程前沿（英文）》 2023年 第17卷 第2期 doi: 10.1007/s11783-023-1618-z

摘要：

● Recent advances in the electrochemical decontamination of PFAS are reviewed.

关键词： Perfluorinated compounds     Electrochemical approach     Working mechanisms     Impacting factor     Coupled process    

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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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Research progress in tribo-electrochemistry and tribo-electrochemical polishing

ZHAI Wenjie

《机械工程前沿（英文）》 2007年 第2卷 第4期   页码 463-467 doi: 10.1007/s11465-007-0080-0

摘要： In this paper, the status quo and recent progress in the research on tribo-electrochemistry in aqueous and non-aqueous media, respectively, are reviewed. Much more attention has been paid to the tribo-electrochemical mechanisms for the control of friction and wear. Based on a summary of the conventional polishing principles of hard and brittle materials, the tribo-electrochemical polishing method is proposed. The results of the preliminary test show that tribo-electrochemical polishing is promising to become a critical technology in the high efficient polishing and planarization of microelectronic materials.

关键词： tribo-electrochemical mechanisms     planarization     non-aqueous     tribo-electrochemistry     summary    

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Enhanced electrochemical performance of CoNiS@TiCT electrode material through doping of cobalt element

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1440-1449 doi: 10.1007/s11705-023-2333-9

摘要： The composite electrode of CoNiSx and Ti3C2Tx MXene was successfully prepared using a one-step hydrothermal method under the in-situ doping of the cobalt element. The effects of in-situ doping of the cobalt element on the micromorphology and electrochemical performance of the electrodes were investigated. After in-situ doping of the cobalt element, NiS with a needle-like structure was converted into a CoNiSx with petal-like structure. The petal-like CoNiSx with a rough surface was very dense and evenly wrapped on the surface and interlamination of Ti3C2Tx, which helped increase the specific surface area and pore volume of the electrode. Under the identical test conditions, CoNiSx@Ti3C2Tx had a higher specific capacitance and capacitance retention than NiS@Ti3C2Tx. This result indicated that the in-situ doping of the cobalt element promoted the electrochemical performance of the electrode. The energy density of the CoNiSx@Ti3C2Tx/nickel foam (NF)//activated carbon (AC)/NF asymmetric supercapacitor device was 59.20 Wh·kg–1 at a power density of 826.73 W·kg–1, which was much higher than that of NiS@Ti3C2Tx/NF//AC/NF. Three CoNiSx@Ti3C2Tx/NF//AC/NF in series were able to illuminate the light emitting diode lamp for about 10 min, which was higher than the 5 min of three NiS@Ti3C2Tx/NF//AC/NF in series under the same condition. The CoNiSx@Ti3C2Tx/NF//AC/NF with high energy density had better application potential in energy storage than the NiS@Ti3C2Tx/NF//AC/NF.

关键词： MXene     supercapacitor     cobalt doping     structure characterization     electrochemical performance    

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标题 作者 时间 类型 操作

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

期刊论文

Plasma-electrochemical synthesis of europium doped cerium oxide nanoparticles

Liangliang Lin, Xintong Ma, Sirui Li, Marly Wouters, Volker Hessel

期刊论文

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

期刊论文

Synthesis, spectroscopic, and electrochemical properties of two dyads consisted of tetrathiafulvalene

Guoqiao LAI, Yibo LIU, Meijiang LI, Yongjia SHEN

期刊论文

Investigation of fluorescence characterization and electrochemical behavior on the catalysts of nanosized

Chang-Mao HUNG, Wen-Liang LAI, Jane-Li LIN

期刊论文

Optimization of electrochemically synthesized Cu

Kasra Pirzadeh, Ali Asghar Ghoreyshi, Mostafa Rahimnejad, Maedeh Mohammadi

期刊论文

Abundance and distribution of ammonia-oxidizing archaea in Tibetan and Yunnan plateau agricultural soils

Kun DING,Xianghua WEN,Liang CHEN,Daishi HUANG,Fan FEI,Yuyang LI

期刊论文

Heat and mass transfer of ammonia-water in falling film evaporator

Xianbiao BU, Weibin MA, Huashan LI

期刊论文

Facile synthesis of hierarchical flower-like Ag/Cu

Mengyun Wang, Shengbo Zhang, Mei Li, Aiguo Han, Xinli Zhu, Qingfeng Ge, Jinyu Han, Hua Wang

期刊论文

Simulation on thermodynamic state of ammonia carbonation at low temperature and low pressure

Jingcai ZHAO, Xingfu SONG, Ze SUN, Jianguo YU

期刊论文

Design guidelines for urea hydrolysers for ammonia demand of the SCR DENOX project in coal-fired power

Peng ZHENG, Xuan YAO, Wei ZHENG

期刊论文

Recent advances in electrochemical decontamination of perfluorinated compounds from water: a review

期刊论文

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

期刊论文

Research progress in tribo-electrochemistry and tribo-electrochemical polishing

ZHAI Wenjie

期刊论文

Enhanced electrochemical performance of CoNiS@TiCT electrode material through doping of cobalt element

期刊论文