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Mechanism of methanol decomposition on the Pd/WC(0001) surface unveiled by first-principles calculations

Jinhua Zhang, Yuanbin She

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 1052-1064 doi: 10.1007/s11705-019-1908-y

摘要： In this study, the decomposition of methanol into the CO and H species on the Pd/tungsten carbide (WC)(0001) surface is systematically investigated using periodic density functional theory (DFT) calculations. The possible reaction pathways and intermediates are determined. The results reveal that saturated molecules, i.e., methanol and formaldehyde, adsorb weakly on the Pd/WC(0001) surface. Both CO and H prefer three-fold sites, with adsorption energies of ‒1.51 and ‒2.67 eV, respectively. On the other hand, CH O stably binds at three-fold and bridge sites, with an adsorption energy of ‒2.58 eV. However, most of the other intermediates tend to adsorb to the surface with the carbon and oxygen atoms in their sp and hydroxyl-like configurations, respectively. Hence, the C atom of CH OH preferentially attaches to the top sites, CHOH and CH O adsorb at the bridge sites, while COH and CHO occupy the three-fold sites. The DFT calculations indicate that the rupture of the initial C–H bond promotes the decomposition of CH OH and CH OH, whereas in the case of CHOH, O–H bond scission is favored over the C–H bond rupture. Thus, the most probable methanol decomposition pathway on the Pd/WC(0001) surface is CH OH → CH OH → -CHOH → CHO → CO. The present study demonstrates that the synergistic effect of WC (as carrier) and Pd (as catalyst) alters the CH OH decomposition pathway and reduces the noble metal utilization.

关键词： density functional theory     methanol     direct methanol fuel cells     WC(0001)-supported Pd monolayer     decomposition mechanism    

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Preparation and influence of performance of anodic catalysts for direct methanol fuel cell

WANG Zhenbo, YIN Geping, SHI Pengfei

《化学科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 20-25 doi: 10.1007/s11705-007-0005-9

摘要： This research aims at increasing the utilization of platinum-ruthenium alloy (Pt-Ru) catalysts and thus lowering the catalyst loading in anodes for methanol electrooxidation. The direct methanol fuel cell s (DMFC) anodic catalysts, Pt-Ru/C, were prepared by chemical reduction with a reducing agent added in two kinds of solutions under different circumstances. The reducing agent was added in hot solution with the protection of inert gases or just air, and in cold solution with inert gases. The catalysts were treated at different temperatures. Their performance was tested by cyclic voltammetry and potentiostatic polarization by utilizing their inherent powder microelectrode in 0.5 mol/L CHOH and 0.5 mol/L HSO solution. The structures and micro-surface images of the catalysts were determined and observed by X-ray diffraction and transmission electron microscopy, respectively. The catalyst prepared in inert gases showed a better catalytic performance for methanol electrooxidation than that prepared in air. It resulted in a more homogeneous distribution of the Pt-Ru alloy in carbon. Its size is small, only about 4.5 nm. The catalytic performance is affected by the order of the reducing agent added. The performance of the catalyst prepared by adding the reductant at constant temperature of the solution is better than that prepared by adding it in the solution at 0?C and then heating it up to the reducing temperature. The structure of the catalyst was modified, and there was an increase in the conversion of ruthenium into the alloyed state and an increase in particle size with the ascension of heat treatment temperature. In addition, the stability of the catalyst was improved after heat treatment.

关键词： catalyst prepared     stability     ascension     potentiostatic polarization     platinum-ruthenium    

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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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poly(ether ether ketone)/zirconium tricarboxybutylphosphonate composite proton-exchange membranes for directmethanol fuel cells

GAO Qijun, HUANG Mianyan, WANG Yuxin, CAI Yuquan, XU Li

《化学科学与工程前沿（英文）》 2008年 第2卷 第1期   页码 95-101 doi: 10.1007/s11705-008-0012-5

摘要： Sulfonated poly(ether ether ketone) (SPEEK) is a very promising alternative membrane material for direct methanol fuel cells. However, with a fairly high degree of sulfonation (DS), SPEEK membranes can swell excessively and even dissolve at high temperature. This restricts membranes from working above a high tolerable temperature to get high proton conductivity. To deal with this contradictory situation, insolvable zirconium tricarboxybutylphosphonate (Zr(PBTC)) powder was employed to make a composite with SPEEK polymer in an attempt to improve temperature tolerance of the membranes. SPEEK/Zr(PBTC) composite membranes were obtained by casting a homogeneous mixture of Zr(PBTC) and SPEEK in N,N-dimethylacetamide on a glass plate and then evaporating the solvent at 60°C. Many characteristics were investigated, including thermal stability, liquid uptake, methanol permeability and proton conductivity. Results showed significant improvement not only in temperature tolerance, but also in methanol resistance of the SPEEK/Zr(PBTC) composite membranes. The membranes containing 30 wt-% ∼ 40 wt-% of Zr(PBTC) had their methanol permeability around 10 cm·s at room temperature to 80°C, which was one order of magnitude lower than that of Nafion115. High proton conductivity of the composite membranes, however, could also be achieved from higher temperature applied. At 100% relative humidity, above 90°C the conductivity of the composite membrane containing 40 wt-% of Zr(PBTC) exceeded that of the Nafion115 membrane and even reached a high value of 0.36 S·cm at 160°C. Improved applicable temperature and high conductivity of the composite membrane indicated its promising application in DMFC operations at high temperature.

关键词： homogeneous mixture     PBTC     zirconium tricarboxybutylphosphonate     Nafion115     DMFC    

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Impacts of methanol fuel on vehicular emissions: A review

《环境科学与工程前沿（英文）》 2022年 第16卷 第9期 doi: 10.1007/s11783-022-1553-4

摘要：

● Methanol effectively reduces CO, HC, CO2, PM, and PN emissions of gasoline vehicles.

关键词： Methanol fuel     Vehicular emission     Emission reduction     Cleaner fuel     Gasoline substitute    

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Design and analysis of dual fuel methanol-power poly-generation

Minghua WANG , Zheng LI , Weidou NI ,

《能源前沿（英文）》 2009年 第3卷 第3期   页码 341-347 doi: 10.1007/s11708-009-0023-z

摘要： A dual fuel head poly-generation flowsheet was designed based on coal gas and coke oven gas. To help clearly understand the system performance, a 1.2×10−3.2×10kg methanol and 274―496MW power poly-generation system was simulated by using the commercially available software ASPEN Plus and GT Pro. The technology scheme, the operating parameters, and the efficiency of the system were also analyzed and evaluated, which will be used for building industrial devices.

关键词： dual fuel     methanol-power poly-generation     CO2 and CH4 reforming     splitting ratio    

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Ignition delay of dual fuel engine operating with methanol ignited by pilot diesel

ZOU Hongbo, WANG Lijun, LIU Shenghua, LI Yu

《能源前沿（英文）》 2008年 第2卷 第3期   页码 285-290 doi: 10.1007/s11708-008-0060-z

摘要： An investigation on the ignition delay of a dual fuel engine operating with methanol ignited by pilot diesel was conducted on a TY1100 direct-injection diesel engine equipped with an electronic controlled methanol low-pressure injection system. The experimental results show that the polytropic index of compression process of the dual fuel engine decreases linearly while the ignition delay increases with the increase in methanol mass fraction. Compared with the conventional diesel engine, the ignition delay increment of the dual fuel engine is about 1.5° at a methanol mass fraction of 62%, an engine speed of 1600 r/min, and full engine load. With the elevation of the intake charge temperature from 20°C to 40°C and then to 60°C, the ignition delay of the dual fuel engine decreases and is more obvious at high temperature. Moreover, with the increase in engine speed, the ignition delay of the dual fuel engine by time scale (ms) decreases clearly under all engine operating conditions. However, the ignition delay of the dual fuel engine increases remarkably by advancing the delivery timing of pilot diesel, especially at light engine loads.
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Numerical investigation of the chemical and electrochemical characteristics of planar solid oxide fuelcell with direct internal reforming

Yuzhang WANG, Shilie WENG, Yiwu WENG

《能源前沿（英文）》 2011年 第5卷 第2期   页码 195-206 doi: 10.1007/s11708-011-0148-8

摘要： A fully three-dimensional mathematical model of a planar solid oxide fuel cell (SOFC) with complete direct internal steam reforming was constructed to investigate the chemical and electrochemical characteristics of the porous-electrode-supported (PES)-SOFC developed by the Central Research Institute of Electric Power Industry of Japan. The effective kinetic models developed over the Ni/YSZ anode takes into account the heat transfer and species diffusion limitations in this porous anode. The models were used to simulate the methane steam reforming processes at the co- and counter-flow patterns. The results show that the flow patterns of gas and air have certain effects on cell performance. The cell at the counter-flow has a higher output voltage and output power density at the same operating conditions. At the counter-flow, however, a high hotspot temperature is observed in the anode with a non-fixed position, even when the air inlet flow rate is increased. This is disadvantageous to the cell. Both cell voltage and power density decrease with increased air flow rate.

关键词： planar solid oxide fuel cell (SOFC)     direct internal reforming     chemical reaction     methane     electrochemical    

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Microbial electrolysis cells with biocathodes and driven by microbial fuel cells for simultaneous enhanced

Jingya SHEN,Yuliang SUN,Liping HUANG,Jinhui YANG

《环境科学与工程前沿（英文）》 2015年 第9卷 第6期   页码 1084-1095 doi: 10.1007/s11783-015-0805-y

摘要： Cobalt and copper recovery from aqueous Co(II) and Cu(II) is one critical step for cobalt and copper wastewaters treatment. Previous tests have primarily examined Cu(II) and Co(II) removal in microbial electrolysis cells (MECs) with abiotic cathodes and driven by microbial fuel cell (MFCs). However, Cu(II) and Co(II) removal rates were still slow. Here we report MECs with biocathodes and driven by MFCs where enhanced removal rates of 6.0±0.2 mg?L ?h for Cu(II) at an initial concentration of 50 mg?L and 5.3±0.4 mg?L h for Co(II) at an initial 40 mg?L were achieved, 1.7 times and 3.3 times as high as those in MECs with abiotic cathodes and driven by MFCs. Species of Cu(II) was reduced to pure copper on the cathodes of MFCs whereas Co(II) was removed associated with microorganisms on the cathodes of the connected MECs. Higher Cu(II) concentrations and smaller working volumes in the cathode chambers of MFCs further improved removal rates of Cu(II) (115.7 mg?L ?h ) and Co(II) (6.4 mg?L ?h ) with concomitantly achieving hydrogen generation (0.05±0.00 mol?mol COD). Phylogenetic analysis on the biocathodes indicates dominantly accounted for 67.9% of the total reads, followed by (14.0%), (6.1%), (2.5%), (1.4%), and (1.0%). This study provides a beneficial attempt to achieve simultaneous enhanced Cu(II) and Co(II) removal, and efficient Cu(II) and Co(II) wastewaters treatment without any external energy consumption.

关键词： biocathode     microbial electrolysis cell     microbial fuel cell     Cu(II) removal     Co(II) removal    

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Latest development of double perovskite electrode materials for solid oxide fuel cells: a review

Shammya AFROZE, AfizulHakem KARIM, Quentin CHEOK, Sten ERIKSSON, Abul K. AZAD

《能源前沿（英文）》 2019年 第13卷 第4期   页码 770-797 doi: 10.1007/s11708-019-0651-x

摘要： Recently, the development and fabrication of electrode component of the solid oxide fuel cell (SOFC) have gained a significant importance, especially after the advent of electrode supported SOFCs. The function of the electrode involves the facilitation of fuel gas diffusion, oxidation of the fuel, transport of electrons, and transport of the byproduct of the electrochemical reaction. Impressive progress has been made in the development of alternative electrode materials with mixed conducting properties and a few of the other composite cermets. During the operation of a SOFC, it is necessary to avoid carburization and sulfidation problems. The present review focuses on the various aspects pertaining to a potential electrode material, the double perovskite, as an anode and cathode in the SOFC. More than 150 SOFCs electrode compositions which had been investigated in the literature have been analyzed. An evaluation has been performed in terms of phase, structure, diffraction pattern, electrical conductivity, and power density. Various methods adopted to determine the quality of electrode component have been provided in detail. This review comprises the literature values to suggest possible direction for future research.

关键词： double perovskites     electrode materials     hydrocarbon fuel     solid oxide fuel cells    

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Plasma spray coating on interconnector toward promoted solid oxide fuel cells and solid oxide electrolysiscells

《能源前沿（英文）》 doi: 10.1007/s11708-023-0901-9

摘要： Interconnector is a critical component to construct solid oxide cells (SOCs) stack. Oxidation of metallic interconnectors and Cr poisoning caused by oxidation are important factors that lead to long-term performance degradation of SOCs. Coating on the interconnector surface is an important approach to inhibit the oxidation and Cr migration of the interconnector. Herein, (La0.75Sr0.25)0.95MnO3–δ (LSM) and Mn1.5Co1.5O4 (MCO) are used to fabricate the coatings of interconnector. Two advanced thermal spray technology, atmospheric plasma spraying (APS) and low-pressure plasma spray (LPPS), are adopted for the coating preparation. The electrochemical performance, rising and cooling cycle stability, and Cr diffusion inhibition performance of the coatings are tested and evaluated. The result indicates that MCO can generate more uniform and denser coatings than LSM. In addition, MCO coatings prepared by LPPS shows the best electrochemical performance, rising and cooling cycle stability, and Cr diffusion inhibition. The initial area specific resistance (ASR) is 0.0027 Ω·cm2 at 800 °C. After 4 cooling cycle tests, the ASR increases to 0.0032 Ω·cm2 but lower than other samples. Meanwhile, the relative intense of Cr at the interface of SUS430 with MCO coatings fabricated by LPPS is lower than that of MCO fabricated by APS after 4 rising and cooling cycle operations, showing more favorable Cr diffusion inhibition performance.

关键词： interconnector coating     plasma spray     electrochemical performance     Cr diffusion inhibition     solid oxide cells (SOCs)    

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Study on direct alcohol/ether fuel synthesis process in bubble column slurry reactor

Zhen CHEN, Haitao ZHANG, Weiyong YING, Dingye FANG

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 461-471 doi: 10.1007/s11705-010-0517-6

摘要： The recent studies of direct alcohol/ether synthesis process in slurry reactors were reviewed, and the research work in our laboratory was carried out in this paper. a global kinetics model for direct dimethyl ether (DME) synthesis from syngas over a novel Cu-Zn-Al-Zr slurry catalyst was established according to the total of 25 experimental data, and a steady-state one-dimensional mathematical model was further developed in bubble column slurry reactor (BCSR), which was assumed that the bubble phase was plug flow, and the liquid phase was fully mixed flow. The numerical simulations of reactor design of 100000 t/a dimethyl ether pilot plant indicate that higher pressure and lower temperature were favorable to the increase of CO conversion, selectivity of dimethyl ether, product yield and height of slurry bed. The optimal operating conditions for DME synthesis process were obtained: reaction temperature at 240°C, reactor pressure at 5 MPa and reactor diameter of 2.5 m.

关键词： syngas     alcohol/ether fuel     slurry catalyst     bubble column slurry reactor     global kinetics     mathematical model    

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Effects of Fischer-Tropsch diesel fuel on combustion and emissions of direct injection diesel engine

HUANG Yongcheng, WANG Shangxue, ZHOU Longbao

《能源前沿（英文）》 2008年 第2卷 第3期   页码 261-267 doi: 10.1007/s11708-008-0062-x

摘要： Effects of Fischer-Tropsch (F-T) diesel fuel on the combustion and emission characteristics of a single-cylinder direct injection diesel engine under different fuel delivery advance angles were investigated. The experimental results show that F-T diesel fuel exhibits shorter ignition delay, lower peak values of premixed burning rate, lower combustion pressure and pressure rise rate, and higher peak value of diffusion burning rate than conventional diesel fuel when the engine remains unmodified. In addition, the unmodified engine with F-T diesel fuel has lower brake specific fuel consumption and higher effective thermal efficiency, and presents lower HC, CO, NO and smoke emissions than conventional diesel fuel. When fuel delivery advance angle is retarded by 3 crank angle degrees, the combustion duration is obviously shortened; the peak values of premixed burning rate, the combustion pressure and pressure rise rate are further reduced; and the peak value of diffusion burning rate is further increased for F-T diesel fuel operation. Moreover, the retardation of fuel delivery advance angle results in a further significant reduction in NO emissions with no penalty on specific fuel consumption and with much less penalty on HC, CO and smoke emissions.

关键词： combustion pressure     further     HC     operation     single-cylinder    

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Sensitivity analysis of a methanol and power polygeneration system fueled with coke oven gas and coal

Guoqiang ZHANG, Lin GAO, Hongguang JIN, Rumou LIN, Sheng LI

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 491-497 doi: 10.1007/s11705-010-0511-z

摘要： The sensitivity analysis of a polygeneration energy system fueled with duo fuel of coke oven gas and coal gas is performed in the study, and the focus is put on the relations among syngas composition, conversation rate and performance. The impacts of the system configuration together with the fuel composition on the performance are investigated and discussed from the point of cascading utilization of fuel chemical energy. First, the main parameters affecting the performance are derived along with the analysis of the system configuration and the syngas composition. After the performance is being simulated by means of the Aspen Plus process simulator of version 11.1, the variation of the performance due to the composition of syngas and the conversion rate of chemical subsystem is obtained and discussed. It is obtained from the result that the proper conversion rate of the chemical subsystem according to the specific syngas composition results in better performance. And the syngas composition affects the optimal conversion rate of the chemical subsystem, the optimal point of which is around the stoichiometric composition for methanol production (CO/H = 0.5). In all, the polygeneration system fueled with coke oven gas and coal gas, which can realize the reasonable conversion of syngas to power and chemical product according to the syngas composition, is a promising method for coal energy conversion and utilization.

关键词： duo fuel of coke oven gas and coal gas     polygeneration of power and methanol     sensitivity analysis     the relation among energy utilization     syngas composition and chemical conversion rate    

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Numerical simulation of biodiesel fuel combustion and emission characteristics in a direct injection

Yi REN, Ehab ABU-RAMADAN, Xianguo LI,

《能源前沿（英文）》 2010年 第4卷 第2期   页码 252-261 doi: 10.1007/s11708-010-0036-7

摘要： The effect of the physical and chemical properties of biodiesel fuels on the combustion process and pollutants formation in Direct Injection (DI) engine are investigated numerically by using multi-dimensional Computational Fluid Dynamics (CFD) simulation. In the current study, methyl butanoate (MB) and -heptane are used as the surrogates for the biodiesel fuel and the conventional diesel fuel. Detailed kinetic chemical mechanisms for MB and -heptane are implemented to simulate the combustion process. It is shown that the differences in the chemical properties between the biodiesel fuel and the diesel fuel affect the whole combustion process more significantly than the differences in the physical properties. While the variations of both the chemical and the physical properties between the biodiesel and diesel fuel influence the soot formation at the equivalent level, the variations in the chemical properties play a crucial role in the NO emissions formation.

关键词： biodiesel     diesel engine     CFD simulation     combustion     pollutant formation    

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标题 作者 时间 类型 操作

Mechanism of methanol decomposition on the Pd/WC(0001) surface unveiled by first-principles calculations

Jinhua Zhang, Yuanbin She

期刊论文

Preparation and influence of performance of anodic catalysts for direct methanol fuel cell

WANG Zhenbo, YIN Geping, SHI Pengfei

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

poly(ether ether ketone)/zirconium tricarboxybutylphosphonate composite proton-exchange membranes for directmethanol fuel cells

GAO Qijun, HUANG Mianyan, WANG Yuxin, CAI Yuquan, XU Li

期刊论文

Impacts of methanol fuel on vehicular emissions: A review

期刊论文

Design and analysis of dual fuel methanol-power poly-generation

Minghua WANG , Zheng LI , Weidou NI ,

期刊论文

Ignition delay of dual fuel engine operating with methanol ignited by pilot diesel

ZOU Hongbo, WANG Lijun, LIU Shenghua, LI Yu

期刊论文

Numerical investigation of the chemical and electrochemical characteristics of planar solid oxide fuelcell with direct internal reforming

Yuzhang WANG, Shilie WENG, Yiwu WENG

期刊论文

Microbial electrolysis cells with biocathodes and driven by microbial fuel cells for simultaneous enhanced

Jingya SHEN,Yuliang SUN,Liping HUANG,Jinhui YANG

期刊论文

Latest development of double perovskite electrode materials for solid oxide fuel cells: a review

Shammya AFROZE, AfizulHakem KARIM, Quentin CHEOK, Sten ERIKSSON, Abul K. AZAD

期刊论文

Plasma spray coating on interconnector toward promoted solid oxide fuel cells and solid oxide electrolysiscells

期刊论文

Study on direct alcohol/ether fuel synthesis process in bubble column slurry reactor

Zhen CHEN, Haitao ZHANG, Weiyong YING, Dingye FANG

期刊论文

Effects of Fischer-Tropsch diesel fuel on combustion and emissions of direct injection diesel engine

HUANG Yongcheng, WANG Shangxue, ZHOU Longbao

期刊论文

Sensitivity analysis of a methanol and power polygeneration system fueled with coke oven gas and coal

Guoqiang ZHANG, Lin GAO, Hongguang JIN, Rumou LIN, Sheng LI

期刊论文

Numerical simulation of biodiesel fuel combustion and emission characteristics in a direct injection

Yi REN, Ehab ABU-RAMADAN, Xianguo LI,

期刊论文