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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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Experimental and DFT insights into nitrogen and sulfur co-doped carbon nanotubes for effective desulfurization

《环境科学与工程前沿（英文）》 2021年 第15卷 第5期 doi: 10.1007/s11783-021-1397-3

摘要：

• Synthesis of NS-CNTS is used in a high desulfurization performance.

关键词： Dibenzothiophene (DBT)     Tertiary methyl mercaptan     Adsorption     Carbon nano tube (CNT)     Desulfurization     Doping    

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Combined biologic aerated filter and sulfur/ceramisite autotrophic denitrification for advanced wastewaternitrogen removal at low temperatures

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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S-enriched porous polymer derived N-doped porous carbons for electrochemical energy storage and conversion

Chao Zhang, Chenbao Lu, Shuai Bi, Yang Hou, Fan Zhang, Ming Cai, Yafei He, Silvia Paasch, Xinliang Feng, Eike Brunner, Xiaodong Zhuang

《化学科学与工程前沿（英文）》 2018年 第12卷 第3期   页码 346-357 doi: 10.1007/s11705-018-1727-6

摘要：

Porous polymers have been recently recognized as one of the most important precursors for fabrication of heteroatom-doped porous carbons due to the intrinsic porous structure, easy available heteroatom-containing monomers and versatile polymerization methods. However, the heteroatom elements in as-produced porous carbons are quite relied on monomers. So far, the manipulating of heteroatom in porous polymer derived porous carbons are still very rare and challenge. In this work, a sulfur-enriched porous polymer, which was prepared from a diacetylene-linked porous polymer, was used as precursor to prepare S-doped and/or N-doped porous carbons under nitrogen and/or ammonia atmospheres. Remarkably, S content can sharply decrease from 36.3% to 0.05% after ammonia treatment. The N content and specific surface area of as-fabricated porous carbons can reach up to 1.32% and 1508 m2·g−1, respectively. As the electrode materials for electrical double-layer capacitors, as-fabricated porous carbons exhibit high specific capacitance of up to 431.6 F·g−1 at 5 mV·s−1 and excellent cycling stability of 99.74% capacitance retention after 3000 cycles at 100 mV·s−1. Furthermore, as the electrochemical catalysts for oxygen reduction reaction, as-fabricated porous carbons presented ultralow half-wave-potential of 0.78 V versus RHE. This work not only offers a new strategy for manipulating S and N doping features for the porous carbons derived from S-containing porous polymers, but also paves the way for the structure-performance interrelationship study of heteroatoms co-doped porous carbon for energy applications.

关键词： porous polymers     porous carbons     sulfur and nitrogen doping     supercapacitor    

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Boron and nitrogen co-doped porous carbon derived from sodium alginate enhanced capacitive deionization

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 2014-2024 doi: 10.1007/s11705-023-2346-4

摘要： Capacitive deionization can alleviate water shortage and water environmental pollution, but performances are greatly determined by the electrochemical and desalination properties of its electrode materials. In this work, B and N co-doped porous carbon with micro-mesoporous structures is derived from sodium alginate by a carbonization, activation, and hydrothermal doping process, which exhibits large specific surface area (2587 m2·g‒1) and high specific capacitance (190.7 F·g‒1) for adsorption of salt ions and heavy metal ions. Furthermore, the materials provide a desalination capacity of 26.9 mg·g−1 at 1.2 V in 500 mg·L‒1 NaCl solution as well as a high removal capacity (239.6 mg·g‒1) and adsorption rate (7.99 mg·g‒1·min‒1) for Pb2+ with an excellent cycle stability. This work can pave the way to design low-cost porous carbon with high-performances for removal of salt ions and heavy metal ions.

关键词： capacitance deionization     porous carbon     B/N co-doping     heavy metal ions     water purification    

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Effect of metal ion-doping on characteristics and photocatalytic activity of TiO

Rongfang YUAN,Beihai ZHOU,Duo HUA,Chunhong SHI

《环境科学与工程前沿（英文）》 2015年 第9卷 第5期   页码 850-860 doi: 10.1007/s11783-014-0737-y

摘要： The effect of ion-doping on TiO nanotubes were investigated to obtain the optimal TiO nanotubes for the effective decomposition of humic acids (HA) through O /UV/ion-doped TiO process. The experimental results show that changing the calcination temperature, which changed the weight fractions of the anatase phase, the average crystallite sizes, the Brunauer-Emmett-Teller surface area, and the energy band gap of the catalyst, affected the photocatalytic activity of the catalyst. The ionic radius, valence state, and configuration of the dopant also affected the photocatalytic activity. The photocatalytic activities of the catalysts on HA removal increased when Ag , Al , Cu , Fe , V , and Zn were doped into the TiO nanotubes, whereas such activities decreased as a result of Mn - and Ni -doping. In the presence of 1.0 at.% Fe -doped TiO nanotubes calcined at 550°C, the removal efficiency of HA was 80% with a pseudo-first-order rate constant of 0.158 min . Fe in TiO could increase the generation of ·OH, which could remove HA. However, Fe in water cannot function as a shallow trapping site for electrons or holes.

关键词： TiO2 nanotubes     ion-doping     humic acids     pseudo-first-order     mechanism    

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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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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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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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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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Tuning the electronic structure of NiCoP arrays through V doping for pH-universal hydrogen evolution

Yu Lin, Jinlei Wang, Duanlin Cao, Yaqiong Gong

《化学科学与工程前沿（英文）》 2021年 第15卷 第5期   页码 1134-1146 doi: 10.1007/s11705-020-2014-x

摘要： The exploration of cost-effective, high-performance, and stable electrocatalysts for the hydrogen evolution reaction (HER) over wide pH range (0–14) is of paramount importance for future renewable energy conversion technologies. Regulation of electronic structure through doping vanadium atoms is a feasible construction strategy to enhance catalytic activities, electron transfer capability, and stability of the HER electrode. Herein, V-doped NiCoP nanosheets on carbon fiber paper (CFP) (denoted as V -NiCoP/CFP) were constructed by doping V modulation on NiCoP nanosheets on CFP and used for pH-universal HER. Benefiting from the abundant catalytic sites and optimized hydrogen binding thermodynamics, the resultant V -NiCoP/CFP demonstrates a significantly improved HER catalytic activity, requiring overpotentials of 46.5, 52.4, and 85.3 mV to reach a current density of 10 mA·cm in 1 mol·L KOH, 0.5 mol·L H SO , and 1 mol·L phosphate buffer solution (PBS) electrolytes, respectively. This proposed cation-doping strategy provides a new inspiration to rationally enhance or design new-type nonprecious metal-based, highly efficient, and pH-universal electrocatalysts for various energy conversion systems.

关键词： hydrogen evolution reaction     transition metal phosphides     pH-universal     vanadium doping     carbon fiber paper    

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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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Highly uniform Ni particles with phosphorus and adjacent defects catalyze 1,5-dinitronaphthalene hydrogenation with excellent catalytic performance

Wei Xiong, Susu Zhou, Zeyong Zhao, Fang Hao, Zhihui Cai, Pingle Liu, Hailiang Zhang, Hean Luo

《化学科学与工程前沿（英文）》 2021年 第15卷 第4期   页码 998-1007 doi: 10.1007/s11705-020-1994-x

摘要： This work proposes a modified activated carbon support, with defects and heteroatoms (N,P-ACs) by nitrogen and phosphorus doping to load non-noble nickel to catalyze aromatic compound hydrogenation. The Ni/N,P-ACs-900 (prepared at 900 °C) showed promising catalytic activity in liquid-phase 1,5-dinitronaphthalene hydrogenation with a 1,5-diaminonaphthalene yield of 95.8% under the mild condition of 100 °C, which is comparable to the commercial Pd/C catalyst. The nitrogen species were burned off at 900 °C, causing more defects for nickel metal loading, facilitating the interaction between the supports and the nickel metal, and resulting in highly dispersed metal particles. The computational study of the nickel binding energy has been conducted using density functional theory. It exhibits that the defects formed by heteroatom doping are beneficial to nickel anchoring and deposition to form highly uniform nickel particles. The phosphorus species in combination with the defects are suitable for H adsorption and dissociation. These results reveal that the heteroatomic doping on the active carbon shows significant effects in the hydrogenation of the liquid-phase aromatic compounds. These findings could provide a promising route for the rational design of aromatic compound hydrogenation catalysts to significantly decrease the cost by instead using noble metal catalysts in the industry.

关键词： nitrogen and phosphorus doping     non-noble nickel catalyst     aromatic compounds hydrogenation    

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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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标题 作者 时间 类型 操作

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

期刊论文

Experimental and DFT insights into nitrogen and sulfur co-doped carbon nanotubes for effective desulfurization

期刊论文

Combined biologic aerated filter and sulfur/ceramisite autotrophic denitrification for advanced wastewaternitrogen removal at low temperatures

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

期刊论文

S-enriched porous polymer derived N-doped porous carbons for electrochemical energy storage and conversion

Chao Zhang, Chenbao Lu, Shuai Bi, Yang Hou, Fan Zhang, Ming Cai, Yafei He, Silvia Paasch, Xinliang Feng, Eike Brunner, Xiaodong Zhuang

期刊论文

Boron and nitrogen co-doped porous carbon derived from sodium alginate enhanced capacitive deionization

期刊论文

Effect of metal ion-doping on characteristics and photocatalytic activity of TiO

Rongfang YUAN,Beihai ZHOU,Duo HUA,Chunhong SHI

期刊论文

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

期刊论文

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

期刊论文

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

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

Tuning the electronic structure of NiCoP arrays through V doping for pH-universal hydrogen evolution

Yu Lin, Jinlei Wang, Duanlin Cao, Yaqiong Gong

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

Highly uniform Ni particles with phosphorus and adjacent defects catalyze 1,5-dinitronaphthalene hydrogenation with excellent catalytic performance

Wei Xiong, Susu Zhou, Zeyong Zhao, Fang Hao, Zhihui Cai, Pingle Liu, Hailiang Zhang, Hean Luo

期刊论文

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

期刊论文