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Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

《化学科学与工程前沿（英文）》 2017年 第11卷 第4期   页码 586-593 doi: 10.1007/s11705-017-1659-6

摘要： Hexagonal CePO nanorods were prepared by a precipitation method and hexagonal CePO nanowires were prepared by hydrothermal synthesis at 150 °C. Rh(NO ) was then used as a precursor for the impregnation of Rh O onto these CePO materials. The Rh O supported on the CePO nanowires was much more active for the catalytic decomposition of N O than the Rh O supported on CePO nanorods. The stability of both catalysts as a function of time on stream was studied and the influence of the co-feed (CO , O , H O or O /H O) on the N O decomposition was also investigated. The samples were characterized by N adsorption-desorption, inductively coupled plasma optical emission spectroscopy, X-ray diffraction, transmission electron microscopy, X-ray photoelectron microscopy, hydrogen temperature-programmed reduction, oxygen temperature-programmed desorption, and CO temperature-programmed desorption in order to correlate the physicochemical and catalytic properties.

关键词： Rh2O3     CePO4     N2O decomposition    

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Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

《化学科学与工程前沿（英文）》 2023年 第17卷 第10期   页码 1412-1422 doi: 10.1007/s11705-023-2312-1

摘要： In this paper, Cu-doped Bi2WO6 was synthesized via a solvothermal method and applied it in photocatalytic N2 immobilization. Characterization results showed the presence of a small amount of metallic Bi in the photocatalyst, indicating that the synthesized photocatalyst is actually Bi/Cu-Bi2WO6 composite. The doped Cu had a valence state of +2 and most likely substituted the position of Bi3+. The introduced Cu did not affect the metallic Bi content, but mainly influenced the energy band structure of Bi2WO6. The band gap was slightly narrowed, the conduction band was elevated, and the work function was reduced. The reduced work function improved the transfer and separation of charge carriers, which mainly caused the increased photoactivity. The optimized NH3 generation rates of Bi/Cu-Bi2WO6 reached 624 and 243 μmol·L–1·g–1·h–1 under simulated solar and visible light, and these values were approximately 2.8 and 5.9 times higher those of Bi/Bi2WO6, respectively. This research provides a method for improving the photocatalytic N2 fixation and may provide more information on the design and preparation of heteroatom-doped semiconductor photocatalysts for N2-to-NH3 conversion.

关键词： Bi2WO6     Cu doping     work function     photocatalytic N2 fixation     charge separation    

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grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

《能源前沿（英文）》 2021年 第15卷 第3期   页码 721-731 doi: 10.1007/s11708-021-0766-8

摘要： Titanium nitride (TiN) decorated N-doped titania (N-TiO2) composite (TiN/N-TiO2) is fabricated via an in situ nitridation using a hydrothermally synthesized TiO2 and melamine (MA) as raw materials. After the optimization of the reaction condition, the resultant TiN/N-TiO2 composite delivers a hydrogen evolution activity of up to 703 μmol/h under the full spectrum irradiation of Xe-lamp, which is approximately 2.6 and 32.0 times more than that of TiO2 and TiN alone, respectively. To explore the underlying photocatalytic mechanism, the crystal phase, morphology, light absorption, energy band structure, element composition, and electrochemical behavior of the composite material are characterized and analyzed. The results indicate that the superior activity is mainly caused by the in situ formation of plasmonic TiN and N-TiO2 with intimate interface contact, which not only extends the spectral response range, but also accelerates the transfer and separation of the photoexcited hot charge carrier of TiN. The present study provides a fascinating approach to in situ forming nonmetallic plasmonic material/N-doped TiO2 composite photocatalysts for high-efficiency water splitting.

关键词： photocatalytic H2 evolution     TiN/N-TiO2 composite     plasmonic effect     in-situ nitridation    

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CH<sub>4sub> and N<sub>2sub>O emissions from double-rice cropping system as affected by Chinese milk

Heshui XU,Dengyun LI,Bo ZHU,Kai ZHANG,Yadong YANG,Chen WANG,Ying JIANG,Zhaohai ZENG

《农业科学与工程前沿（英文）》 2017年 第4卷 第1期   页码 59-68 doi: 10.15302/J-FASE-2017137

摘要： Chinese milk vetch (CMV) and rice straw (RS) were incorporated into soil to substitute for synthetic N fertilizers and to maintain soil fertility. However, little is known about the integrated impacts of CMV and RS incorporation on CH and N O emissions in double-rice cropping systems in southern China. A field experiment was conducted to estimate the integrated impacts of CMV and RS incorporation in the early- and late-rice seasons on CH and N O emissions. All treatments received uniform N inputs, 6%–37% of which was replaced by CMV and RS crop residue. CMV and/or RS incorporation produced equivalent or slightly more grain yield, while reducing N O emissions by 3%–43%. However, both CMV and RS incorporation increased CH emissions. Annual CH emissions ranged from 321 to 614 kg·hm from CMV and RS amendment treatments, which were 1.5–2.9 times higher than that from synthetic N. Compared with single synthetic N fertilizer, incorporation of CMV and/or RS increased GWP and yield-scaled GWP by 45%–164% and 45%–153%, respectively. Our results demonstrate CMV and RS amendments replacing N fertilizer, maintained stable yield, mitigated N O emission, but enhanced CH emission. Further study is needed on crop residue management in double-cropping rice systems.

关键词： Chinese milk vetch     CH4     double-rice cropping system     grain yield     N2O     rice straw    

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基于实时CT扫描技术的CO<sub>2sub>和N<sub>2sub>交替注入条件下煤吸附膨胀和解吸收缩规律研究 Article

张广磊, P.G. Ranjith, Herbert E. Huppert

《工程（英文）》 2022年 第18卷 第11期   页码 88-95 doi: 10.1016/j.eng.2022.03.010

摘要：

深部煤层是分布最广泛的适宜二氧化碳（CO<sub>2sub>）地质封存的地层之一，且通常位于大型CO<sub>2sub>排放源附近。将CO<sub>2sub>注入到煤层中具有巨大的CO<sub>2sub>封存潜力，同时可以提高煤层气的采收率（CO<sub>2sub>-ECBM）。本文采用原位同步辐射X射线显微CT扫描技术，首次在原位条件下直接证明了注入氮气（N<sub>2sub>）可以置换解吸CO<sub>2sub>并减小因CO<sub>2sub>吸附引起的煤基质膨胀研究结果表明，煤层中注入经过简单处理的烟道气（主要成分为N<sub>2sub>和CO<sub>2sub>），是技术上可行的CO<sub>2sub>-ECBM 替代方案。其次，N<sub>2sub>的存在可以使煤层保持较高的渗透率，实现长期CO<sub>2sub>注入封存和煤层气增产。

关键词： CCS     CO<sub>2sub>-ECBM     碳中和     X 射线成像     煤渗透率    

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Inexpensive synthesis of a high-performance Fe

Nadir Abbas, Godlisten N. Shao, Syed M. Imran, Muhammad S. Haider, Hee Taik Kim

《化学科学与工程前沿（英文）》 2016年 第10卷 第3期   页码 405-416 doi: 10.1007/s11705-016-1579-x

摘要： A sol-gel technique has been developed for the synthesis of a magnetite-silica-titania (Fe O -SiO -TiO ) tertiary nanocomposite with improved photocatalytic properties based on the use of inexpensive titania and silica precursors. The exceptional photocatalytic activity of the resulting materials was demonstrated by using them to photocatalyze the degradation of methylene blue solution. The best formulation achieved 98% methylene blue degradation. An interesting feature of the present work was the ability to magnetically separate and reuse the catalyst. The efficiency of the catalyst remained high during two reuses. The synthesized nanomaterials were characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM), Fourier transform infrared (FTIR) spectroscopy, ultra-violet-visible spectroscopy, diffuse reflectance spectroscopy, and thermogravimetric analysis. XRD analysis revealed the formation of multicrystalline systems of cubic magnetite and anatase titania crystals. SEM and TEM characterization revealed well-developed and homogeneously dispersed particles of size less than 15 nm. FTIR spectra confirmed the chemical interaction of titania and silica. It was further noticed that the optical properties of the prepared materials were dependent on the relative contents of their constituent metal oxides.

关键词： sol-gel     photocatalysis     magnetic recovery     TiO2     Fe3O4     SiO2    

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Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance in N

《化学科学与工程前沿（英文）》 2023年 第17卷 第12期   页码 1949-1961 doi: 10.1007/s11705-023-2360-6

摘要： This study aimed to prepare and apply a novel Pt/CdMoO4 composite photocatalyst for photocatalytic N2 fixation and tetracycline degradation. The Pt/CdMoO4 composite was subjected to comprehensive investigation on the morphology, structure, optical properties, and photoelectric chemical properties. The results demonstrate the dispersion of Pt nanoparticles on the CdMoO4 surface. Close contact between CdMoO4 and Pt was observed, resulting in the formation of a heterojunction structure at their contact region. Density functional theory calculation and Mott-Schottky analysis revealed that Pt possesses a higher work function value than CdMoO4, resulting in electron drift from CdMoO4 to Pt and the formation of a Schottky barrier. The presence of this barrier increases the separation efficiency of electron-hole pairs, thereby improving the performance of the Pt/CdMoO4 composite in photocatalysis. When exposed to simulated sunlight, the optimal Pt/CdMoO4 catalyst displayed a photocatalytic nitrogen fixation rate of 443.7 μmol·L‒1·g‒1·h‒1, which is 3.2 times higher than that of pure CdMoO4. In addition, the composite also exhibited excellent performance in tetracycline degradation, with hole and superoxide species identified as the primary reactive species. These findings offer practical insights into designing and synthesizing efficient photocatalysts for photocatalytic nitrogen fixation and antibiotics removal.

关键词： photocatalytic N2 fixation     Pt/CdMoO4     tetracycline degradation     Schottky barrier    

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N<sub>2sub>O emission from a sequencing batch reactor for biological N and P removal from wastewater

Lei SHEN,Yuntao GUAN,Guangxue WU,Xinmin ZHAN

《环境科学与工程前沿（英文）》 2014年 第8卷 第5期   页码 776-783 doi: 10.1007/s11783-013-0586-0

摘要： Nitrous oxide (N O) is a greenhouse gas that can be released during biological nitrogen removal from wastewater. N O emission from a sequencing batch reactor (SBR) for biological nitrogen and phosphorus removal from wastewater was investigated, and the aims were to examine which process, nitrification or denitrification, would contribute more to N O emission and to study the effects of heterotrophic activities on N O emission during nitrification. The results showed that N O emission was mainly attributed to nitrification rather than to denitrification. N O emission during denitrification mainly occurred with stored organic carbon as the electron donor. During nitrification, N O emission was increased with increasing initial ammonium or nitrite concentrations. The ratio of N O emission to the removed ammonium nitrogen (N O-N/NH -N) was 2.5% in the SBR system with high heterotrophic activities, while this ratio was in the range from 0.14% to 1.06% in batch nitrification experiments with limited heterotrophic activities.

关键词： biological nutrient removal     denitrification     greenhouse gas     nitrification     nitrous oxide    

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NiCo2O4@quinone-rich N–C core–shell nanowires as composite electrode for electric double layer capacitor

《化学科学与工程前沿（英文）》 2023年 第17卷 第4期   页码 373-386 doi: 10.1007/s11705-022-2223-6

摘要： The bind-free carbon cloth-supported electrodes hold the promises for high-performance electrochemical capacitors with high specific capacitance and good cyclic stability. Considering the close connection between their performance and the amount of carbon material loaded on the electrodes, in this work, NiCo2O4 nanowires were firstly grown on the substrate of active carbon cloth to provide the necessary surface area in the longitudinal direction. Then, the quinone-rich nitrogen-doped carbon shell structure was formed around NiCo2O4 nanowires, and the obtained composite was used as electrode for electric double layer capacitor. The results showed that the composite electrode displayed an area-specific capacitance of 1794 mF∙cm–2 at the current density of 1 mA∙cm–2. The assembled symmetric electric double layer capacitor achieved a high energy density of 6.55 mW∙h∙cm–3 at a power density of 180 mW∙cm–3. The assembled symmetric capacitor exhibited a capacitance retention of 88.96% after 10000 charge/discharge cycles at the current density of 20 mA∙cm–2. These results indicated the potentials in the preparation of the carbon electrode materials with high energy density and good cycling stability.

关键词： carbon cloth     NiCo2O4 nanowires     core−shell structure     quinone-rich     electric double layer capacitor    

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Effects of Pd doping on N

Mingxin Dong, Jun Wang, Jinxin Zhu, Jianqiang Wang, Wulin Wang, Meiqing Shen

《环境科学与工程前沿（英文）》 2017年 第11卷 第6期 doi: 10.1007/s11783-017-0976-9

摘要： N O is a powerful greenhouse gas and plays an important role in destructing the ozone layer. This present work investigated the effects of Pd doping on N O formation over Pt/BaO/Al O catalyst. Three types of catalysts, Pt/BaO/Al O , Pt/Pd mechanical mixing catalyst (Pt/BaO/Al O +Pd/Al O ) and Pt-Pd co-impregnation catalyst (Pt-Pd/BaO/Al O ) were prepared by incipient wetness impregnation method. These catalysts were first evaluated in NSR activity tests using H /CO as reductants and then carefully characterized by BET, CO chemisorption, CO-DRIFTs and H -TPR techniques. In addition, temperature programmed reactions of NO with H /CO were conducted to obtain further information about N O formation mechanism. Compared with Pt/BaO/Al O , (Pt/BaO/Al O +Pd/Al O ) produced less N O and more NH during NO storage and reduction process, while an opposite trend was found over (Pt-Pd/BaO/Al O +Al O ). Temperature programmed reactions of NO with H /CO results showed that Pd/Al O component in (Pt/BaO/Al O +Pd/Al O ) played an important role in NO reduction to NH , and the formed NH could reduce NO to N leading to a decrease in N O formation. Most of N O formed over (Pt-Pd/BaO/Al O +Al O ) was originated from Pd/BaO/Al O component. H -TPR results indicated Pd-Ba interaction resulted in more difficult-to-reduce PdO species over Pd/BaO/Al O , which inhibits the NO dissociation and thus drives the selectivity to N O in NO reduction.

关键词： NOx storage reduction     Pt/BaO/Al2O3     Pd doping     N2O formation     Optimization    

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过硫酸盐诱导的缺陷氮化碳中三配位氮（N3<sub>Csub>）空位增强光催化产过氧化氢 Article

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

《工程（英文）》 2023年 第25卷 第6期   页码 214-221 doi: 10.1016/j.eng.2021.12.016

摘要： 其中石墨氮化碳（g-C<sub>3sub>N<sub>4sub>）被认为是最有前途的合成过氧化氢的光催化剂之一；并且，在g-C<sub>3sub>N<sub>4sub>中引入氮空位已被证明是提高其光催化活性的有效策略在此，本文提出了一种简便的过硫酸钠共晶聚合方法，制备了具有丰富三配位氮空位（N3<sub>Csub>）的g-C<sub>3sub>N<sub>4sub>。本研究的结果表明，在g-C<sub>3sub>N<sub>4sub>中引入N3<sub>Csub>空位可以成功地拓宽光吸收范围，抑制光激发电荷的重组，增强O<sub>2sub>的吸附和活化富含N3<sub>Csub>空位的g-C<sub>3sub>N<sub>4sub>的光催化过氧化氢产量是原始g-C<sub>3sub>N<sub>4sub>的4.5倍。本研究提出了在g-C<sub>3sub>N<sub>4sub>中引入N3<sub>Csub>空位的新策略，为开发光催化产过氧化氢的活性催化剂提供了一种新方法。

关键词： 氮化碳     N3<sub>Csub>空位     过氧化氢     光催化     过硫酸盐    

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Physical and chemical processes of wintertime secondary nitrate aerosol formation

Qi YING

《环境科学与工程前沿（英文）》 2011年 第5卷 第3期   页码 348-361 doi: 10.1007/s11783-011-0343-1

摘要： The UCD/CIT model was modified to include a process analysis (PA) scheme for gas and particulate matter (PM) to study the formation of secondary nitrate aerosol during a stagnant wintertime air pollution episode during the California Regional PM /PM Air Quality Study (CRPAQS) where detailed measurements of PM components are available at a few sites. Secondary nitrate is formed in the urban areas from near the ground to a few hundred meters above the surface during the day with a maximum modeled net increase rate of 4 μg·m ·d during the study episode. The secondary nitrate formation rate in rural areas is lower due to lower NO . In the afternoon hours, near-surface temperature can be high enough to evaporate the particulate nitrate. In the nighttime hours, both the gas phase N O reactions with water vapor and the N O heterogeneous reactions with particle-bound water are important for secondary nitrate formation. The N O reactions are most import near the surface to a few hundred meters above surface with a maximum modeled net secondary nitrate increase rate of 1 μg·m ·d and are more significant in the rural areas where the O concentrations are high at night. In general, vertical transport during the day moves the nitrate formed near the surface to higher elevations. During the stagnant days, process analysis indicates that the nitrate concentration in the upper air builds up and leads to a net downward flux of nitrate through vertical diffusion and a rapid increase of surface nitrate concentration.

关键词： secondary nitrate aerosol     N2O5 heterogeneous reaction     process analysis    

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New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

《能源前沿（英文）》 2021年 第15卷 第2期   页码 421-430 doi: 10.1007/s11708-021-0727-2

摘要： In recent years, Fe-N-C catalyst is particularly attractive due to its high oxygen reduction reaction (ORR) activity and low cost for proton exchange membrane fuel cells (PEMFCs). However, the durability problems still pose challenge to the application of Fe-N-C catalyst. Although considerable work has been done to investigate the degradation mechanisms of Fe-N-C catalyst, most of them are simply focused on the active-site decay, the carbon oxidation, and the demetalation problems. In fact, the 2e pathway in the ORR process of Fe-N-C catalyst would result in the formation of H O , which is proved to be a key degradation source. In this paper, a new insight into the effect of potential on degradation of Fe-N-C catalyst was provided by quantifying the H O intermediate. In this case, stability tests were conducted by the potential-static method in O saturated 0.1 mol/L HClO . During the tests, H O was quantified by rotating ring disk electrode (RRDE). The results show that compared with the loading voltage of 0.4 V, 0.8 V, and 1.0 V, the catalysts being kept at 0.6 V exhibit a highest H O yield. It is found that it is the combined effect of electrochemical oxidation and chemical oxidation (by aggressive radicals like H O /radicals) that triggered the highest H O release rate, with the latter as the major cause.

关键词： proton exchange membrane fuel cells (PEMFCs)     oxygen reduction reaction (ORR)     Fe-N-C catalyst     potential     H2O2     degradation    

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CO, N, and CO/N mixed gas injection for enhanced shale gas recovery and CO geological storage

《能源前沿（英文）》 2023年 第17卷 第3期   页码 428-445 doi: 10.1007/s11708-023-0865-9

摘要： In this work, using fractured shale cores, isothermal adsorption experiments and core flooding tests were conducted to investigate the performance of injecting different gases to enhance shale gas recovery and CO2 geological storage efficiency under real reservoir conditions. The adsorption process of shale to different gases was in agreement with the extended-Langmuir model, and the adsorption capacity of CO2 was the largest, followed by CH4, and that of N2 was the smallest of the three pure gases. In addition, when the CO2 concentration in the mixed gas exceeded 50%, the adsorption capacity of the mixed gas was greater than that of CH4, and had a strong competitive adsorption effect. For the core flooding tests, pure gas injection showed that the breakthrough time of CO2 was longer than that of N2, and the CH4 recovery factor at the breakthrough time (RCH4) was also higher than that of N2. The RCH4 of CO2 gas injection was approximately 44.09%, while the RCH4 of N2 was only 31.63%. For CO2/N2 mixed gas injection, with the increase of CO2 concentration, the RCH4 increased, and the RCH4 for mixed gas CO2/N2 = 8:2 was close to that of pure CO2, about 40.24%. Moreover, the breakthrough time of N2 in mixed gas was not much different from that when pure N2 was injected, while the breakthrough time of CO2 was prolonged, which indicated that with the increase of N2 concentration in the mixed gas, the breakthrough time of CO2 could be extended. Furthermore, an abnormal surge of N2 concentration in the produced gas was observed after N2 breakthrough. In regards to CO2 storage efficiency (Sstorage-CO2), as the CO2 concentration increased, Sstorage-CO2 also increased. The Sstorage-CO2 of the pure CO2 gas injection was about 35.96%, while for mixed gas CO2/N2 = 8:2, Sstorage-CO2 was about 32.28%.

关键词： shale gas     gas injection     competitive adsorption     enhanced shale gas recovery     CO2 geological storage    

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The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The

《环境科学与工程前沿（英文）》 2021年 第15卷 第4期 doi: 10.1007/s11783-020-1366-2

摘要：

•Bacterially-mediated coupled N and Fe processes examined in incubation experiments.

关键词： Denitrification     N2O emission     Fe(II) oxidation     Fe/N ratio     Fe minerals    

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标题 作者 时间 类型 操作

Rh<sub>2sub>O<sub>3sub>/hexagonal CePO<sub>4sub> nanocatalysts for N<sub>2sub>O decomposition

Huan Liu, Zhen Ma

期刊论文

Cu-doped Bi/Bi<sub>2sub>WO<sub>6sub> catalysts for efficient N<sub>2sub> fixation by photocatalysis

期刊论文

grown TiN/N-TiO composite for enhanced photocatalytic H evolution activity

期刊论文

CH<sub>4sub> and N<sub>2sub>O emissions from double-rice cropping system as affected by Chinese milk

Heshui XU,Dengyun LI,Bo ZHU,Kai ZHANG,Yadong YANG,Chen WANG,Ying JIANG,Zhaohai ZENG

期刊论文

基于实时CT扫描技术的CO<sub>2sub>和N<sub>2sub>交替注入条件下煤吸附膨胀和解吸收缩规律研究

张广磊, P.G. Ranjith, Herbert E. Huppert

期刊论文

Inexpensive synthesis of a high-performance Fe

Nadir Abbas, Godlisten N. Shao, Syed M. Imran, Muhammad S. Haider, Hee Taik Kim

期刊论文

Decoration of CdMoO micron polyhedron with Pt nanoparticle and their enhanced photocatalytic performance in N

期刊论文

N<sub>2sub>O emission from a sequencing batch reactor for biological N and P removal from wastewater

Lei SHEN,Yuntao GUAN,Guangxue WU,Xinmin ZHAN

期刊论文

NiCo2O4@quinone-rich N–C core–shell nanowires as composite electrode for electric double layer capacitor

期刊论文

Effects of Pd doping on N

Mingxin Dong, Jun Wang, Jinxin Zhu, Jianqiang Wang, Wulin Wang, Meiqing Shen

期刊论文

过硫酸盐诱导的缺陷氮化碳中三配位氮（N3<sub>Csub>）空位增强光催化产过氧化氢

缪蔚, 王奕杰, 刘莹, 秦贺贺, 褚成成, 毛舜

期刊论文

Physical and chemical processes of wintertime secondary nitrate aerosol formation

Qi YING

期刊论文

New insight into effect of potential on degradation of Fe-N-C catalyst for ORR

Yanyan GAO, Manman QI, Liang HE, Haiping CHEN, Wenzhe LUO, Ming HOU, Zhigang SHAO

期刊论文

CO, N, and CO/N mixed gas injection for enhanced shale gas recovery and CO geological storage

期刊论文

The performance of nitrate-reducing Fe(II) oxidation processes under variable initial Fe/N ratios: The

期刊论文