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Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional

《化学科学与工程前沿（英文）》 2023年 第17卷 第11期   页码 1707-1717 doi: 10.1007/s11705-023-2308-x

摘要： Water electrolysis technology is considered to be one of the most promising means to produce hydrogen. Herein, aiming at the problems of high overpotential and slow kinetics in water splitting, N-doped porous carbon nanofibers-coupled CoNi2S4 nanoparticles are prepared as bifunctional electrocatalyst. In the strategy, NaCl is used as the template to prepare porous carbon nanofibers with a large surface area, and sulfur vacancies are created to modulate the electronic structure of CoNi2S4. Electron spin resonance confirms the formation of abundant sulfur vacancies, which largely reduce the bandgap of CoNi2S4 from 1.68 to 0.52 eV. The narrowed bandgap is conducive to the migration of valence electrons and decreases the charge transfer resistance for electrocatalytic reaction. Moreover, the uniform distribution of CoNi2S4 nanoparticles on carbon nanofibers can prevent the aggregation and facilitate the exposure of electrochemical active sites. Therefore, the composite catalyst exhibits low overpotentials of 340 mV@100 mA·cm–2 for oxygen evolution reaction and 380 mV@100 mA·cm–2 for hydrogen evolution reaction. The assembled electrolyzer requires 1.64 V to achieve 10 mA·cm–2 for overall water-splitting with good long-term stability. The excellent performance results from the synergistic effect of porous structures, sulfur deficiency, nitrogen doping, and the well-dispersed active component.

关键词： nanoparticle     sulfur vacancy     porous carbon nanofiber     transition metal sulfides     electrolysis    

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Role of oxygen vacancy inducer for graphene in graphene-containing anodes

《化学科学与工程前沿（英文）》 2023年 第17卷 第3期   页码 326-333 doi: 10.1007/s11705-022-2213-8

摘要： Currently, graphene is only considered as a conductive additive and expansion inhibitor in oxides/graphene composite anodes. In this study, a new graphene role (oxygen vacancy inducer) in graphene/oxides composites anodes, which are treated at high-temperature, is proposed and verified using experiments and density functional theory calculations. During high-temperature processing, graphene forms carbon vacancies due to increased thermal vibration, and the carbon vacancies capture oxygen atoms, facilitating the formation of oxygen vacancies in oxides. Moreover, the induced oxygen vacancy concentrations can be regulated by sintering temperatures, and the behavior is unaffected by oxide crystal structures (crystalline and amorphous) and morphology (size and shape). According to density functional theory calculations and electrochemical measurements, the oxygen vacancies enhance the lithium-ion storage performance. The findings can result in a better understanding of graphene’s roles in graphene/oxide composite anodes, and provide a new method for designing high-performance oxide anodes.

关键词： oxide     oxygen vacancy     graphene     anode     density functional theory calculation    

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Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide

《化学科学与工程前沿（英文）》 2021年 第15卷 第6期   页码 1524-1536 doi: 10.1007/s11705-021-2106-2

摘要： The effects of Zr doping on the existence of Cu and the catalytic performance of Ce0.7−xZrxCu0.3O2 for CO oxidation were investigated. The characterization results showed that all samples have a cubic structure, and a small amount of Zr doping facilitates Cu2+ ions entering the CeO2 lattice, but excessive Zr doping leads to the formation of surface CuO crystals again. Thus, the number of oxygen vacancies caused by the Cu2+ entering the lattice (e.g., Cu2+–□–Ce4+; □: oxygen vacancy), and the amount of reducible copper species caused by CuO crystals, varies with the Zr doping. Catalytic CO oxidation tests indicated that the oxygen vacancy and the reducible copper species were the adsorption and activation sites of O2 and CO, respectively, and the cooperative effects between them accounted for the high CO oxidation activity. Thus, the samples x = 0.1 and 0.3, which possessed the most oxygen vacancy or reducible copper species, showed the best activity for CO oxidation, with full CO conversion obtained at 110 °C. The catalyst is also stable and has good resistance to water during the reaction.

关键词： Ce–Zr–Cu–O     CO oxidation     reducible copper species     oxygen vacancy     cooperative effect    

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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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Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1937-1948 doi: 10.1007/s11705-023-2353-5

摘要： In this study, Bi2MoO6 with adjustable rich oxygen vacancies was prepared by a novel and simple solvothermal-photoreduction method which might be suitable for a large-scale production. The experiment results show that Bi2MoO6 with rich oxygen vacancies is an excellent photocatalyst. The photocatalytic ability of BMO-10 is 0.3 and 3.5 times higher than that of the pristine Bi2MoO6 for Rhodamine B degradation and Cr(VI) reduction, respectively. The results display that the band energy of the samples with oxygen vacancies was narrowed and the light absorption was broadened. Meanwhile, the efficiency of photogenerated electron-holes was increased and the separation and transfer speed of photogenerated carriers were improved. Therefore, this work provides a convenient and efficient method to prepare potential adjustable oxygen vacancy based photocatalysts to eliminate the pollution of dyes and Cr(VI) in water.

关键词： Bi2MoO6     oxygen vacancies     photoreduction     Cr(VI)     RhB    

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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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Effect of a promoter on the methanation activity of a Mo-based sulfur-resistant catalyst

Can LIN, Haiyang WANG, Zhenhua LI, Baowei WANG, Xinbin MA, Shaodong QIN, Qi SUN

《化学科学与工程前沿（英文）》 2013年 第7卷 第1期   页码 88-94 doi: 10.1007/s11705-013-1301-1

摘要： The effect of adding Co, Ni or La on the methanation activity of a Mo-based sulfur-resistant catalyst was investigated. As promoters, Co, Ni and La all improved the methanation activity of a 15% MoO /Al O catalyst but to different extents. Similar improvements were also found when Co, Ni or La was added to a 15% MoO /25%-CeO -Al O catalyst. The promotion effects of Co and Ni were better than that of La. However, the catalytic methanation activity deteriorated the most with time for the Ni-promoted catalyst. The used catalysts were analyzed by nitrogen adsorption measurement, X-ray diffraction and X-ray photoelectron spectroscopy.

关键词： sulfur-resistant     methanation     promoter    

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Combined biologic aerated filter and sulfur/ceramisite autotrophic denitrification for advanced wastewater

Tian WAN,Guangming ZHANG,Fengwei DU,Junguo HE,Pan WU

《环境科学与工程前沿（英文）》 2014年 第8卷 第6期   页码 967-972 doi: 10.1007/s11783-014-0690-9

摘要： An innovative advanced wastewater treatment process combining biologic aerated filter (BAF) and sulfur/ceramisite-based autotrophic denitrification (SCAD) for reliable removal of nitrogen was proposed in this paper. In SCAD reactor, ceramisite was used as filter and Ca(HCO ) was used for supplying alkalinity and carbon source. The BAF-SCAD was used to treat the secondary treatment effluent. The performance of this process was investigated, and the impact of temperature on nitrogen removal was studied. Results showed that the combined system was effective in nitrogen removal even at low temperatures (8 °C). Removal of total nitrogen (TN), -N, N reached above 90% at room temperature. Nitrification was affected by the temperature and nitrification at low temperature (8 °C) was a limiting factor for TN removal. However, denitrification was not impacted by the temperature and the removal of -N maintained 98% during the experimental period. The reason of effective denitrification at low temperature might be the use of easily dissolved Ca(HCO ) and high-flux ceramisite, which solved the problem of low mass transfer efficiency at low temperatures. Besides, vast surface area of sulfur with diameter of 2–6 mm enhanced the rate of microbial utilization. The removal of nitrate companied with the production of , and the average concentration of was about 240 mg·L . These findings would be beneficial for the application of this process to nitrogen removal especially in the winter and cold regions.

关键词： autotrophic denitrification     biologic aerated filter (BAF)     sulfur/ceramisite-based autotrophic denitrification (SCAD)     advanced nitrogen removal    

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Sulfur mediated heavy metal biogeochemical cycles in coastal wetlands: From sediments, rhizosphere to

《环境科学与工程前沿（英文）》 2022年 第16卷 第8期 doi: 10.1007/s11783-022-1523-x

摘要：

• In sediments, the transformation of sulfides may lead to the release of heavy metals.

关键词： Coastal wetland     Heavy metal     Sulfur     Biogeochemical cycle    

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标题 作者 时间 类型 操作

Sulfur-deficient CoNi2S4 nanoparticles-anchored porous carbon nanofibers as bifunctional

期刊论文

Role of oxygen vacancy inducer for graphene in graphene-containing anodes

期刊论文

Cooperative effect between copper species and oxygen vacancy in CeZrCuO catalysts for carbon monoxide

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

Photoreduction adjusted surface oxygen vacancy of BiMoO for boosting photocatalytic redox performance

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

Effect of a promoter on the methanation activity of a Mo-based sulfur-resistant catalyst

Can LIN, Haiyang WANG, Zhenhua LI, Baowei WANG, Xinbin MA, Shaodong QIN, Qi SUN

期刊论文

Combined biologic aerated filter and sulfur/ceramisite autotrophic denitrification for advanced wastewater

Tian WAN,Guangming ZHANG,Fengwei DU,Junguo HE,Pan WU

期刊论文

Sulfur mediated heavy metal biogeochemical cycles in coastal wetlands: From sediments, rhizosphere to

期刊论文