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Catalytic performance of Co-Mo-Ce-K/γ-Al

Yuqiong ZHAO, Yongfa ZHANG

《化学科学与工程前沿（英文）》 2010年 第4卷 第4期   页码 457-460 doi: 10.1007/s11705-010-0524-7

摘要： The catalytic performance of Co-Mo-Ce-K/γ-Al O catalyst for the shift reaction of CO in coke oven gas is investigated using X-ray diffraction (XRD) and temperature-programmed reduction (TPR). The results indicate that Ce and K have a synergistic effect on promoting the catalytic activity, and the Co-Mo-Ce-K/γ-Al O catalyst with 3.0 wt-% CeO and 6.0 wt-% K O exhibits the highest activity. CeO favors Co dispersion and mainly produces an electronic effect. TPR characterization results indicate that the addition of CeO -K O in the Co-Mo-Ce-K/γ-Al O catalyst decreases the reduction temperature of active components, and part of octahedrally coordinated Mo transforms into tetrahedrally coordinated Mo , which has a close relationship with the catalytic activity.

关键词： coke oven gas     water gas shift reaction     sulfur-tolerant catalyst     cerium dioxide    

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Effects of seed particles Al

Xiao Zhang, Biwu Chu, Junhua Li, Chaozhi Zhang

《环境科学与工程前沿（英文）》 2017年 第11卷 第4期 doi: 10.1007/s11783-017-0936-4

摘要： Seed particles Al O , Al (SO ) and H SO were selected to investigate their effects on secondary aerosol (SA) formation in toluene/NO photooxidation under sulfur dioxide (SO ) and ammonia (NH ). Effect of seed particles on SA formation was related to their acid-base properties and the presence of acid or alkaline gases. Under NH -poor condition, SA formation increased with increasing SO concentration due to the acid-catalyzing effect of the oxidation products of SO (i.e. H SO ). The enhancing effect of SO became unobvious under NH -rich condition, because NH would eliminate the acid-catalyzing effect by neutralizing the acid products. Acidic seeds H SO accelerated SA formation under either SO or NH condition. Weak acidic Al (SO ) seeds didn’t affect obviously on SA formation. The inhibiting effect of amphoteric seeds Al O on SA formation was related to the presence of SO / NH due to their acid-base property. Under NH -poor condition, the inhibiting effect of Al O on SA formation decreased with increasing concentration of SO , while under NH -rich condition, the inhibiting effect wasn’t remarkable.

关键词： Seed particle     Secondary aerosol     Sulfur dioxide     Ammonia     Acid-catalyzing effect    

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NO oxidation over Co-La catalysts and NO

Tiejun Zhang,Jian Li,Hong He,Qianqian Song,Quanming Liang

《环境科学与工程前沿（英文）》 2017年 第11卷 第2期 doi: 10.1007/s11783-017-0906-x

摘要： The Co-La catalyst (pH= 1) exhibited maximum NO conversion of 43% at 180°C. Acid modified catalyst enhanced the resistance to SO . The formed sulfates may block the pore structure of the catalyst. The NO conversion of compact SCR was 91% at 180°C at the highest space velocity. A series of Co-La catalysts were prepared using the wet impregnation method and the synthesis of catalysts were modified by controlling pH with the addition of ammonium hydroxide or oxalic solution. All the catalysts were systematically investigated for NO oxidation and SO resistance in a fixed bed reactor and were characterized by Brunanuer–Emmett–Teller (BET) method, Fourier Transform infrared spectroscopy (FTIR), X–ray diffraction (XRD), Thermogravimetric (TG) and Ion Chromatography (IC). Among the catalysts, the one synthesized at pH= 1 exhibited the maximum NO conversion of 43% at 180°C. The activity of the catalyst was significantly suppressed by the existence of SO (300 ppm) at 220°C. Deactivation may have been associated with the generation of cobalt sulfate, and the SO adsorption quantity of the catalyst might also have effected sulfur resistance. In the case of the compact selective catalytic reduction (SCR), the activity increased from 74% to 91% at the highest gas hourly space velocity (GHSV) of 300000 h when the NO catalyst maintained the highest activity, in excess of 50% more than that of the standard SCR.

关键词： NO catalytic oxidation     pH effect     Low temperature     Sulfur dioxide     High space velocity     SCR    

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Static and dynamic characteristics of SO

Shi Yin, Yan-Qiu Chen, Yue-Li Li, Wang-Lai Cen, Hua-Qiang Yin

《环境科学与工程前沿（英文）》 2018年 第12卷 第5期 doi: 10.1007/s11783-018-1058-3

摘要：

To derive liquid fuel from waste engine oil and plastics thorough pyrolysis process.

To make equal blend of waste engine oil and plastics with diesel fuel.

To find the suitability of fuel from waste in diesel engine through performance, emission and combustion characteristics.

关键词： Molecular dynamics     Flue gas desulfurization     Graphene     Sulfur dioxide     Heterogeneous catalysis    

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amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 194-205 doi: 10.1007/s11705-022-2206-7

摘要： The shuttle effect of soluble polysulfides is a serious problem impeding the development of lithium−sulfur batteries. Herein, continuous amino-functionalized University of Oslo 66 membranes supported on carbon nanotube films are proposed as ion-permselective interlayers that overcome these issues and show outstanding suppression of the polysulfide shuttle effect. The proposed membrane material has appropriately sized pores, and can act as ionic sieves and serve as barriers to polysulfides transport while allowing the passage of lithium ions during electrochemical cycles, thereby validly preventing the shuttling of polysulfides. Moreover, a fast catalytic conversion of polysulfides is also achieved with the as-developed interlayer. Therefore, lithium−sulfur batteries with this interlayer show a desirable initial capacity of 999.21 mAh·g–1 at 1 C and a durable cyclic stability with a decay rate of only 0.04% per cycle over 300 cycles. Moreover, a high area capacity of 4.82 mAh·cm–2 is also obtained even under increased sulfur loading (5.12 mg·cm–2) and a lean-electrolyte condition (E/S = 4.8 μL·mg–1).

关键词： lithium−sulfur batteries     amino-functionalized University of Oslo 66 membrane     polysulfide     interlayer    

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Tuning nitrogen defects and doping sulfur in carbon nitride for enhanced visible light photocatalytic

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 93-101 doi: 10.1007/s11705-022-2175-x

摘要： Defect construction and heteroatom doping are effective strategies for improving photocatalytic activity of carbon nitride (g-C3N4). In this work, N defects were successfully prepared via cold plasma. High-energy electrons generated by plasma can produce N defects and embed sulfur atoms into g-C3N4. The N defects obviously promoted photocatalytic degradation performance that was 7.5 times higher than that of pure g-C3N4. The concentration of N defects can be tuned by different power and time of plasma. With the increase in N defects, the photocatalytic activity showed a volcanic trend. The g-C3N4 with moderate concentration of N defects exhibited the highest photocatalytic activity. S-doped g-C3N4 exhibited 11.25 times higher photocatalytic activity than pure g-C3N4. It provided extra active sites for photocatalytic reaction and improved stability of N defects. The N vacancy-enriched and S-doped g-C3N4 are beneficial for widening absorption edge and improving the separation efficiency of electron and holes.

关键词： g-C3N4     nitrogen defect     sulfur doping     photodegradation     plasma    

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Theoretical study on the mechanism of sulfur migration to gas in the pyrolysis of benzothiophene

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 334-346 doi: 10.1007/s11705-022-2209-4

摘要： The release and control of sulfur species in the pyrolysis of fossil fuels and solid wastes have attracted attention worldwide. Particularly, thiophene derivatives are important intermediates for the sulfur gas release from organic sulfur, but the underlying migration mechanisms remain unclear. Herein, the mechanism of sulfur migration during the release of sulfur-containing radicals in benzothiophene pyrolysis was explored through quantum chemistry modeling. The C1-to-C2 H-transfer has the lowest energy barrier of 269.9 kJ·mol–1 and the highest rate constant at low temperatures, while the elevated temperature is beneficial for C−S bond homolysis. 2-Ethynylbenzenethiol is the key intermediate for the formation of S and SH radicals with the overall energy barriers of 408.0 and 498.7 kJ·mol–1 in favorable pathways. The generation of CS radicals is relatively difficult because of the high energy barrier (551.8 kJ·mol–1). However, it can be significantly promoted by high temperatures, where the rate constant exceeds that for S radical generation above 930 °C. Consequently, the strong competitiveness of S and SH radicals results in abundant H2S during benzothiophene pyrolysis, and the high temperature is more beneficial for CS2 generation from CS radicals. This study lays a foundation for elucidating sulfur migration mechanisms and furthering the development of pyrolysis techniques.

关键词： benzothiophene     sulfur migration     pyrolysis     density functional theory    

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Kombucha SCOBY-based carbon and graphene oxide wrapped sulfur/polyacrylonitrile as a high-capacity cathodein lithium-sulfur batteries

Krishnaveni Kalaiappan, Subadevi Rengapillai, Sivakumar Marimuthu, Raja Murugan, Premkumar Thiru

《化学科学与工程前沿（英文）》 2020年 第14卷 第6期   页码 976-987 doi: 10.1007/s11705-019-1897-x

摘要： Hierarchically-porous carbon nano sheets were prepared as a conductive additive for sulfur/polyacrylonitrile (S/PAN) composite cathodes using a simple heat treatment. In this study, kombucha (that was derived from symbiotic culture of bacteria and yeast) carbon (KC) and graphene oxide (GO) were used as a carbon host matrix. These rational-designed S/PAN/KC/GO hybrid composites greatly suppress the diffusion of polysulfides by providing strong physical and chemical adsorption. The cathode delivered an initial discharge capacity of 1652 mAh·g at a 0.1 C rate and a 100 cycle capacity of 1193 mAh·g . The nano sheets with embedded hierarchical pores create a conductive network that provide effective electron transfer and fast electrochemical kinetics. Further, the nitrogen component of PAN can raise the affinity/interaction of the carbon host with lithium polysulfides, supporting the cyclic performance. The results exploit the cumulative contribution of both the conductive carbon matrix and PAN in the enhanced performance of the positive electrode.

关键词： sulfur cathode     kombucha SCOBY     graphene oxide     polyacrylonitrile     lithium-sulfur battery    

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Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

《化学科学与工程前沿（英文）》 2023年 第17卷 第5期   页码 617-633 doi: 10.1007/s11705-022-2258-8

摘要： MnOx and Sm–Mn catalysts were prepared with the coprecipitation method, and they showed excellent activities and sulfur resistances for the selective catalytic reduction of NOx by NH3 between 50 and 300 °C in the presence of excess oxygen. 0.10Sm–Mn catalyst indicated better catalytic activity and sulfur resistance. Additionally, the Sm doping led to multi-aspect impacts on the phases, morphology structures, gas adsorption, reactions process, and specific surface areas. Therefore, it significantly enhances the NO conversion, N2 selectivity, and sulfur resistance. Based on various experimental characterization results, the reaction mechanism of catalysts and the effect of SO2 on the reaction process about the catalysts were extensively explored. For 0.10Sm–Mn catalyst, manganese sulfate and sulfur ammonium cannot be generated broadly under the influence of SO2 and the amount of surface adsorbed oxygen. The Bronsted acid sites strengthen significantly due to the addition of SO2, enhancing the sulfur resistance of the 0.10Sm–Mn catalyst.

关键词： MnOx     Sm–Mn     catalyst     NH3-SCR     sulfur resistance    

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zirconium-based metal-organic framework-801 films on carbon cloth as shuttle-inhibiting interlayers for lithium-sulfur

《化学科学与工程前沿（英文）》 2022年 第16卷 第4期   页码 511-522 doi: 10.1007/s11705-021-2068-4

摘要： Lithium-sulfur batteries have been regarded as the next-generation rechargeable batteries due to their high theoretical energy density and specific capacity. Nevertheless, the shuttle effect of lithium polysulfides has hindered the development of lithium-sulfur batteries. Herein, a novel zirconium-based metal-organic framework-801 film on carbon cloth was developed as a versatile interlayer for lithium-sulfur batteries. This interlayer has a hierarchical porous structure, suitable for the immobilization of lithium polysulfides and accommodating volume expansion on cycling. Moreover, the MOF-801 material is capable of strongly adsorbing lithium polysulfides and promoting their catalytic conversion, which can be enhanced by the abundant active sites provided by the continuous structure of the MOF-801 films. Based on the above advantages, the lithium-sulfur battery, with the proposed interlayer, delivers an initial discharge capacity of 927 mAh·g–1 at 1 C with an extremely low decay rate of 0.04% over 500 cycles. Additionally, a high area capacity of 4.3 mAh·cm–2 can be achieved under increased S loading.

关键词： lithium-sulfur batteries     metal-organic framework-801 film     interlayer     shuttle effect    

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Effects of sulfur on variations in the chemical speciation of heavy metals from fly ash glass

《环境科学与工程前沿（英文）》 2023年 第17卷 第10期 doi: 10.1007/s11783-023-1728-7

摘要：

● A higher sulfur content reduced the curing rate of Cr in glass.

关键词： Dechlorinated fly ash     SO3     Heavy metal     Chemical speciation     Glass solidification    

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An investigation of reaction furnace temperatures and sulfur recovery

S. ASADI, M. PAKIZEH, M. POURAFSHARI CHENAR

《化学科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 362-371 doi: 10.1007/s11705-011-1106-z

摘要： In a modern day sulfur recovery unit (SRU), hydrogen sulfide (H S) is converted to elemental sulfur using a modified Claus unit. A process simulator called TSWEET has been used to consider the Claus process. The effect of the H S concentration, the H S/CO ratio, the input air flow rate, the acid gas flow of the acid gas (AG) splitter and the temperature of the acid gas feed at three different oxygen concentrations (in the air input) on the main burner temperature have been studied. Also the effects of the tail gas ratio and the catalytic bed type on the sulfur recovery were studied. The bed temperatures were optimized in order to enhance the sulfur recovery for a given acid gas feed and air input. Initially when the fraction of AG splitter flow to the main burner was increased, the temperature of the main burner increased to a maximum but then decreased sharply when the flow fraction was further increased; this was true for all three concentrations of oxygen. However, if three other parameters (the concentration of H S, the ratio H S/CO and the flow rate of air) were increased, the temperature of the main burner increased monotonically. This increase had different slopes depending on the oxygen concentration in the input air. But, by increasing the temperature of the acid gas feed, the temperature of the main burner decreased. In general, the concentration of oxygen in the input air into the Claus unit had little effect on the temperature of the main burner (This is true for all parameters). The optimal catalytic bed temperature, tail gas ratio and type of catalytic bed were also determined and these conditions are a minimum temperature of 300°C, a ratio of 2.0 and a hydrolysing Claus bed.

关键词： Claus unit     concentration of H2S     tail gas ratio     sulfur recovery     catalytic bed    

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Investigation of carbon dioxide photoreduction process in a laboratory-scale photoreactor by computational

《化学科学与工程前沿（英文）》 2022年 第16卷 第7期   页码 1149-1163 doi: 10.1007/s11705-021-2096-0

摘要： The production of solar fuels via the photoreduction of carbon dioxide to methane by titanium oxide is a promising process to control greenhouse gas emissions and provide alternative renewable fuels. Although several reaction mechanisms have been proposed, the detailed steps are still ambiguous, and the limiting factors are not well defined. To improve our understanding of the mechanisms of carbon dioxide photoreduction, a multiphysics model was developed using COMSOL. The novelty of this work is the computational fluid dynamic model combined with the novel carbon dioxide photoreduction intrinsic reaction kinetic model, which was built based on three-steps, namely gas adsorption, surface reactions and desorption, while the ultraviolet light intensity distribution was simulated by the Gaussian distribution model and Beer-Lambert model. The carbon dioxide photoreduction process conducted in a laboratory-scale reactor under different carbon dioxide and water moisture partial pressures was then modeled based on the intrinsic kinetic model. It was found that the simulation results for methane, carbon monoxide and hydrogen yield match the experiments in the concentration range of 10−4 mol·m–3 at the low carbon dioxide and water moisture partial pressure. Finally, the factors of adsorption site concentration, adsorption equilibrium constant, ultraviolet light intensity and temperature were evaluated.

关键词： carbon dioxide photoreduction     computational fluid dynamic simulation     kinetic model     Langmuir adsorption    

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Scale up of reactors for carbon dioxide reduction

《化学科学与工程前沿（英文）》 2023年 第17卷 第1期   页码 116-122 doi: 10.1007/s11705-022-2178-7

摘要： In recent times there has been a great deal of interest in the conversion of carbon dioxide into more useful chemical compounds. On the other hand, the translation of these developments in electrochemical reduction of carbon dioxide from the laboratory bench to practical scale remains an underexplored topic. Here we examine some of the major challenges, demonstrating some promising strategies towards such scale-up, including increased electrode area and stacking of electrode pairs in different configurations. We observed that increasing the electrode area from 1 to 10 cm2 led to only a 4% drop in current density, with similarly small penalties realised when stacking sub-cells together.

关键词： CO2 reduction     electrochemical cell     electrosynthesis     upscaling    

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Renewable synthetic fuel: turning carbon dioxide back into fuel

《能源前沿（英文）》 2022年 第16卷 第2期   页码 145-149 doi: 10.1007/s11708-022-0828-6

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标题 作者 时间 类型 操作

Catalytic performance of Co-Mo-Ce-K/γ-Al

Yuqiong ZHAO, Yongfa ZHANG

期刊论文

Effects of seed particles Al

Xiao Zhang, Biwu Chu, Junhua Li, Chaozhi Zhang

期刊论文

NO oxidation over Co-La catalysts and NO

Tiejun Zhang,Jian Li,Hong He,Qianqian Song,Quanming Liang

期刊论文

Static and dynamic characteristics of SO

Shi Yin, Yan-Qiu Chen, Yue-Li Li, Wang-Lai Cen, Hua-Qiang Yin

期刊论文

amino-functionalized University of Oslo 66 membranes as efficacious polysulfide barriers for lithium−sulfur

期刊论文

Tuning nitrogen defects and doping sulfur in carbon nitride for enhanced visible light photocatalytic

期刊论文

Theoretical study on the mechanism of sulfur migration to gas in the pyrolysis of benzothiophene

期刊论文

Kombucha SCOBY-based carbon and graphene oxide wrapped sulfur/polyacrylonitrile as a high-capacity cathodein lithium-sulfur batteries

Krishnaveni Kalaiappan, Subadevi Rengapillai, Sivakumar Marimuthu, Raja Murugan, Premkumar Thiru

期刊论文

Denitrification performance and sulfur resistance mechanism of Sm–Mn catalyst for low temperature NH-SCR

期刊论文

zirconium-based metal-organic framework-801 films on carbon cloth as shuttle-inhibiting interlayers for lithium-sulfur

期刊论文

Effects of sulfur on variations in the chemical speciation of heavy metals from fly ash glass

期刊论文

An investigation of reaction furnace temperatures and sulfur recovery

S. ASADI, M. PAKIZEH, M. POURAFSHARI CHENAR

期刊论文

Investigation of carbon dioxide photoreduction process in a laboratory-scale photoreactor by computational

期刊论文

Scale up of reactors for carbon dioxide reduction

期刊论文

Renewable synthetic fuel: turning carbon dioxide back into fuel

期刊论文