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Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis

Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA

《化学科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 415-422 doi: 10.1007/s11705-012-1214-4

摘要： The catalysts supported on LiAl O (spinel) for vapor phase synthesis of dimethyl carbonate (DMC) from methyl nitrite (MN) have been studied. Their catalytic activities on supports prepared by different methods were evaluated in a continuous reactor. The samples were characterized by powder X-ray diffraction, N adsorption-desorption isotherms, fourier transform infrared spectroscopy and temperature-programmed reduction of H . Li/Al molar ratio and calcination temperature greatly influence the structure of crystalline phase of Li-Al-O oxides. Desirable LiAl O (spinel) was formed at 800°C, while LiAl O (primitive cube) formed at 900°C is undesirable for the reaction. A high Li/Al molar ratio, which was related with LiAlO , also slowed the reaction rate. The electron transfer ability and the interaction with active component are the important properties of the spinel-based supports. The CuCl -PdCl /LiAl O (spinel) with better electron transfer ability and low Pd reduction temperature exhibited a better catalytic ability.

关键词： Wacker-type catalyst     dimethyl carbonate     methyl nitrite     spinel    

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Mayenite supported perovskite monoliths for catalytic combustion of methyl methacrylate

Zekai ZHANG, Zhijian KONG, Huayan LIU, Yinfei CHEN

《化学科学与工程前沿（英文）》 2014年 第8卷 第1期   页码 87-94 doi: 10.1007/s11705-014-1410-5

摘要： To improve their thermal stability, La Sr MnO cordierite monoliths are washcoated with mayenite, which is a novel Al-based material with the crystal structure of 12MO·7Al O (M= Ca, Sr). The monoliths are characterized by means of nitrogen adsorption/desorption, scanning electron microscopy, and X-ray diffraction. Catalytic performances of the monoliths are tested for methyl methacrylate combustion. The results show that mayenite obviously improves both the physic-chemical properties and the catalytic performance of the monoliths. Because mayenite improves the dispersity of La Sr MnO and also prevents the interaction between La Sr MnO and cordierite or -Al O , both crystal structure and surface morphology of La Sr MnO phase can thereby be stable on the mayenite surface even at high temperature up to 1050 oC. Under the given reaction conditions, La Sr MnO monolith washcoated with 12SrO·7Al O shows the best catalytic activity for methyl methacrylate combustion among all the tested monoliths.

关键词： mayenite     perovskite     catalytic combustion     methyl methacrylate     monolith    

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HPLC determination of glyoxal in aldehyde solution with 3-methyl-2-benzothiazolinone hydrazone

Yamei ZHU, Xiaoli YAO, Shaohui CHEN, Qun CUI, Haiyan WANG

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 117-121 doi: 10.1007/s11705-010-0535-4

摘要： Based on the absorption property of a diazine that can be formed by reaction of glyoxal and 3-methyl-2-benzothiazolinone hydrazone (MBTH) in the Ultraviolet-visible (UV-vis) spectral region, a HPLC method was developed for the determination of glyoxal in acetaldehyde solution. Glyoxal was derivatised from MBTH and the derivatives (diazine) were analyzed by HPLC for identification and quantification. The determination was performed on a ZORBAX Eclipse XDB-C18 column (4.6 × 250 mm, 5 mm) at 35°C with an injection volume of 10 mL, using a mixture of acetonitrile-water solvent (99∶5, v∶v) as a mobile phase with a flow rate of 0.8 mL·min . The proper derivative reaction conditions were the temperature of 70°C, MBTH to carbonyl molar ratio of 12, and reaction time of 110 min. The glyoxal diazine was a yellow dye with a maximum molar absorptivity at 401 nm and its retention time was 5.2 min under optimal HPLC conditions. The standard curve for glyoxal had a strong linear relationship with a regression coefficient ( = 0.999) in the range of 0.002–0.020 g·L . The analysis of glyoxal in an oxidising solution gave accurate results with a relative standard deviation (RSD) value of 0.55%. The average relative recovery was 102%. This efficient HPLC technique is also proposed for detecting other dicarbonyl compounds besides glyoxal.

关键词： HPLC     glyoxal     3-methyl-2-benzothiazolinone hydrazone     diazine     dicarbonyl compounds    

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Polymerization of methyl methacrylate catalyzed by mono-/bis-salicylaldiminato nickel(II) complexes and

Jihong LU, Danfeng ZHANG, Qian CHEN, Buwei YU

《化学科学与工程前沿（英文）》 2011年 第5卷 第1期   页码 19-25 doi: 10.1007/s11705-010-0546-1

摘要： Two types of salicylaldiminato-based nickel complexes, mono-ligated Ni(II) complexes ([O-C H - - C(H)=N-Ar]Ni(PPh )(Ph) ( ), [O-(3,5-Br )C H - -C(H)=N-Ar]Ni(PPh )(Ph) ( ), [O-(3- -Bu)C H - -C(H)=N-Ar]Ni(PPh )(Ph) ( )) and bis-ligated Ni(II) complexes ([O-(3,5-Br )C H - -C(H)=N-Ar] Ni ( ), [O-(3,5-Br )C H - -C(H)=N-2-C H (PhO)] Ni ( ), Ar=2,6-C H ( -Pr) ) were synthesized and characterized by Fourier transform infrared spectroscopy (FT-IR), nuclear magnetic resonance (NMR), mass spectrography (MS) and elemental analysis (EA). In the presence of methylaluminoxane (MAO) as cocatalyst, all the nickel complexes exhibited high activities for the polymerization of methyl methacrylate (MMA) and syndiotactic-rich poly(methyl methacrylate) (PMMA) was obtained. The complexes with less bulky substituents on salicylaldiminato framework possessed higher activities, while with the same salicylaldiminato, the mono-ligated nickel complexes showed higher catalytic activity than bis-ligated ones.

关键词： late transition metal catalyst     methyl methacrylate     polymerization     salicylaldiminato nickel complexes     methylaluminoxane     syndiotactic structure    

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Effect of alkyl nitrite decomposition on catalytic performance of CO coupling reaction over supported

Zhenhua LI, Weihan WANG, Dongxue YIN, Jing LV, Xinbin MA

《化学科学与工程前沿（英文）》 2012年 第6卷 第4期   页码 410-414 doi: 10.1007/s11705-012-1213-5

摘要： The syntheses of dimethyl oxalate (DMO) and diethyl oxalate (DEO) by CO coupling reaction in gaseous phase were investigated in a fixed bed reactor over Pd-Fe/Al O catalyst. The catalytic performance was characterized by CO conversion, space-time yield (STY) and selectivity of DMO (or DEO). The results showed that over Pd-Fe/Al O catalyst, the STY of DMO was higher than that of DEO under the same reaction conditions. The optimum reaction temperatures for synthesizing DMO and DEO were 403 K and 393 K, respectively, at the molar ratio 1 ∶ 1 of alkyl nitrite to CO. The difference in synthesizing DMO and DEO on the same catalyst was attributed to the decomposition performances of methyl nitrite (MN) and ethyl nitrite (EN), as density functional theory (DFT) calculation showed that EN decomposed more easily than MN.

关键词： palladium     CO coupling     dialkyl oxalate     alkyl nitrite     decomposition    

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Denitrification and phosphorus uptake by DPAOs using nitrite as an electron acceptor by step-feed strategies

Bin MA, Shuying WANG, Guibing ZHU, Shijian GE, Junmin WANG, Nanqi Ren, Yongzhen PENG

《环境科学与工程前沿（英文）》 2013年 第7卷 第2期   页码 267-272 doi: 10.1007/s11783-012-0439-2

摘要： Denitrifying phosphorus accumulating organisms (DPAOs) using nitrite as an electron acceptor can reduce more energy. However, nitrite has been reported to have an inhibition on denitrifying phosphorus removal. In this study, the step-feed strategy was proposed to achieve low nitrite concentration, which can avoid or relieve nitrite inhibition. The results showed that denitrification rate, phosphorus uptake rate and the ratio of the phosphorus uptaken to nitrite denitrified (anoxic P/N ratio) increased when the nitrite concentration was 15 mg·L after step-feeding nitrite. The maximum denitrification rate and phosphorus uptake rate was 12.73 mg and 18.75 mg , respectively. These rates were higher than that using nitrate (15 mg·L ) as an electron acceptor. The maximum anoxic P/N ratio was 1.55 mg . When the nitrite concentration increased from 15 to 20 mg after addition of nitrite, the anoxic phosphorus uptake was inhibited by 64.85%, and the denitrification by DPAOs was inhibited by 61.25%. Denitrification rate by DPAOs decreased gradually when nitrite (about 20 mg·L ) was added in the step-feed SBR. These results indicated that the step-feed strategy can be used to achieve denitrifying phosphorus removal using nitrite as an electron acceptor, and nitrite concentration should be maintained at low level (<15 mg·L in this study).

关键词： denitrifying phosphate accumulating organisms (DPAOs)     denitrification     phosphorus uptake     nitrite     step-feed     enhanced biological phosphorus removal    

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Photocatalytic degradation of methyl orange using ZnO/TiO composites

Ming GE , Changsheng GUO , Xingwang ZHU , Lili MA , Wei HU , Yuqiu WANG , Zhenan HAN ,

《环境科学与工程前沿（英文）》 2009年 第3卷 第3期   页码 271-280 doi: 10.1007/s11783-009-0035-2

摘要： ZnO/TiO composites were synthesized by using the solvothermal method and ultrasonic precipitation followed by heat treatment in order to investigate their photocatalytic degradation of methyl orange (MO) in aqueous suspension under UV irradiation. The composition and surface structure of the catalyst were characterized by X-ray diffraction (XRD), field emission scanning electron microscope (FE-SEM), and transmission electron microscopy (TEM). The degradation efficiencies of MO at various pH values were obtained. The highest degradation efficiencies were obtained before 30min and after 60min at pH 11.0 and pH 2.0, respectively. A sample analysis was conducted using liquid chromatography coupled with electrospray ionization ion-trap mass spectrometry. Six intermediates were found during the photocatalytic degradation process of quinonoid MO. The degradation pathway of quinonoid MO was also proposed.

关键词： photocatalytic degradation     methyl orange     ZnO/TiO2 composites     high performance liquid chromatography mass spectrometry (HPLC-MS)    

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of activated sludge aggregates using microelectrodes in completely autotrophic nitrogen removal over nitrite

Yongtao LV,Xuan CHEN,Lei WANG,Kai JU,Xiaoqiang CHEN,Rui MIAO,Xudong WANG

《环境科学与工程前沿（英文）》 2016年 第10卷 第2期   页码 390-398 doi: 10.1007/s11783-015-0818-6

摘要： Microsensor measurements and fluorescence in situ hybridization (FISH) analysis were combined to investigate the microbial populations and activities in a laboratory-scale sequencing batch reactor (SBR) for completely autotrophic nitrogen removal over nitrite (CANON). Fed with synthetic wastewater rich in ammonia, the SBR removed 82.5±5.4% of influent nitrogen and a maximum nitrogen-removal rate of 0.52 kgN·m ·d was achieved. The FISH analysis revealed that aerobic ammonium-oxidizing bacteria (AerAOB) and anaerobic ammonium-oxidizing bacteria (AnAOB) dominated the community. To quantify the microbial activities inside the sludge aggregates, microprofiles were measured using pH, dissolved oxygen (DO), , and microelectrodes. In the outer layer of sludge aggregates (0–700 μm), nitrite-oxidizing bacteria (NOB) showed high activity with 4.1 μmol·cm ·h of maximum nitrate production rate under the condition of DO concentration higher than 3.3 mg·L . Maximum AerAOB activity was detected in the middle layer (depths around 1700 μm) where DO concentration was 1.1 mg·L . In the inner layer (2200–3500 μm), where DO concentration was below 0.9 mg·L , AnAOB activity was detected. We thus showed that information obtained from microscopic views can be helpful in optimizing the SBR performance.

关键词： microelectrodes     CANON     aerobic ammonium-oxidizing bacteria     anaerobic ammonium-oxidizing bacteria     nitrite-oxidizing bacteria    

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Effects of nitrite on phosphate uptake in anaerobic-oxic process

LI Jie, XIONG Biyong, ZHANG Shude, YANG Hong, ZHANG Jie

《环境科学与工程前沿（英文）》 2007年 第1卷 第1期   页码 39-42 doi: 10.1007/s11783-007-0007-3

摘要： An anaerobic-oxic (A/O) biological phosphorus removal reactor was operated to study the effect of nitrite on phosphate uptake. The phosphorus uptake profile was determined under different operating conditions. The results indicated that in addition to oxygen and nitrate (DPB, nitrate denitrifying phosphorus removal), to some extent, nitrite could also serve as an electron acceptor to achieve nitrite denitrifying phosphorus removal (DPB). The quantity and rate of phosphorus uptake of DPB, however, were evidently lower than that of DPB The experiment results revealed that nitrite would bring toxic action to phosphate-accumulating organisms (PAOs) when NO-N"e93.7 mg/L. The nitrite existing in the anoxic reactor made no difference to the quantity and rate of denitrifying phosphorus removal, but it could reduce the consumption of nitrate. Moreover, the data showed that the aerobic phosphate uptake of DPB was lower than that of anaerobic phosphorus-released sludge in a traditional A/O process. However, there was not much difference between these two kinds of sludge in terms of the total phosphorus uptake quantity and the effluent quality.

关键词： effluent     PAOs     experiment     phosphate-accumulating     phosphorus removal    

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Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation of methyl

《化学科学与工程前沿（英文）》 2022年 第16卷 第3期   页码 443-460 doi: 10.1007/s11705-021-2079-1

摘要： Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d-band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n-pentadecane and n-C6–n-C16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO2 recovered the catalyst reactivity.

关键词： Stöber method     carbon-coated Ni-Co alloy     in-situ hydrodeoxygenation     methyl palmitate     decarbonylation/decarboxylation    

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method for efficient control of hydrogen sulfide and methane in gravity sewers: Combination of NaOH and Nitrite

《环境科学与工程前沿（英文）》 2022年 第16卷 第6期 doi: 10.1007/s11783-021-1509-0

摘要：

• The combination of NaOH and nitrite was used to control harmful gas in sewers.

关键词： Sewer corrosion     Sulfide control     Combination treatment     NaOH     Nitrite    

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A simple, azulene-based colorimetric probe for the detection of nitrite in water

Lloyd C. Murfin, Carlos M. López-Alled, Adam C. Sedgwick, Jannis Wenk, Tony D. James, Simon E. Lewis

《化学科学与工程前沿（英文）》 2020年 第14卷 第1期   页码 90-96 doi: 10.1007/s11705-019-1790-7

摘要： We describe the synthesis and evaluation of an azulene-based chemodosimeter for nitrite. The probe was found to undergo two distinct color changes upon introduction aqueous nitrite ion. A near-instant formation of a grey color provides a qualitative indication of the presence of nitrite, followed by the formation of a deep-yellow/orange color, the endpoint from which quantitative data can be derived. The azulene probe exhibits 1:1 stoichiometry of reaction with nitrite in water, and is selective for nitrite over other anions. The azulene probe was applied to determine nitrite content in cured meat, and compared with the British Standard testing procedure (Griess test). The value obtained from the azulene-based probe agreed closely with the standard test. Our procedure only requires the preparation of one standard solution, instead of the three required for the standard Griess test.

关键词： azulene     nitrite     diazoquinone    

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Experimental study of nitrite accumulation in pre-denitrification biological nitrogen removal process

WU Xuelei, CHEN Lunqiang, PENG Yongzhen, WANG Pu, WANG Yayi

《环境科学与工程前沿（英文）》 2008年 第2卷 第2期   页码 236-240 doi: 10.1007/s11783-008-0008-x

摘要： The effect of dissolved oxygen (DO) concentration on nitrite accumulation was investigated in a pilot-scale pre-denitrification process at room temperature for 100 days. In the first 10 days, due to the instability of the system, the DO concentration fluctuated between 1.0 and 2.0 mg/L. In the next 14 days, the DO concentration was kept at 0.5 mg/L and nitrite accumulation occurred, with the average nitrite accumulation rate at 91%. From the 25th day, the DO concentration was increased to 2.0 mg/L to destroy the nitrite accumulation, but nitrite accumulation rate was still as high as 90%. From the 38th day the nitrite accumulation rate decreased to 15%–30% linearly. From the 50th day, DO concentration was decreased to 0.5 mg/L to resume nitrite accumulation. Until the 83rd day the nitrite accumulation rate began to increase to 80%. Dissolved oxygen was the main cause of nitrite accumulation, taking into account other factors such as pH, free ammonia concentration, temperature, and sludge retention time. Because of the different affinity for oxygen between nitrite oxidizing bacteria and ammonia oxidizing bacteria when DO concentration was kept at 0.5 mg/L, nitrite accumulation occurred.
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Performance of completely autotrophic nitrogen removal over nitrite process under different aeration

GUO Jinsong, YANG Guohong, FANG Fang, QIN Yu

《环境科学与工程前沿（英文）》 2008年 第2卷 第4期   页码 439-445 doi: 10.1007/s11783-008-0046-4

摘要： In this study, three sequential batch biofilm reactors (SBBRs) were operated for 155 days to evaluate the performance of completely autotrophic nitrogen removal over nitrite (CANON) process under different aeration modes and dissolved oxygen (DO). Synthetic wastewater with 160-mg NH-N/L was fed into the reactors. In the continuously-aerated reactor, the efficiency of the ammonium nitrogen conversion and total nitrogen (TN) removal reached 80% and 70%, respectively, with DO between 0.8–1.0 mg/L. Whereas in the intermittently-aerated reactor, at the aeration/non-aeration ratio of 1.0, ammonium was always under the detection limit and 86% of TN was removed with DO between 2.0–2.5 mg/L during the aeration time. Results show that CANON could be achieved in both continuous and intermittent aeration pattern. However, to achieve the same nitrogen removal efficiency, the DO needed in the intermittently-aerated sequential batch biofilm reactor (SBBR) during the aeration period was higher than that in the continuously-aerated SBBR. In addition, the DO in the CANON system should be adjusted to the aeration mode, and low DO was not a prerequisite to CANON process.

关键词： Synthetic wastewater     process     Whereas     biofilm     detection    

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Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

《化学科学与工程前沿（英文）》 2023年 第17卷 第2期   页码 139-155 doi: 10.1007/s11705-022-2217-4

摘要： Porous carbon-encapsulated Ni and Ni–Sn intermetallic compound catalysts were prepared by the one-pot extended Stöber method followed by carbonization and tested for in-situ hydrothermal deoxygenation of methyl palmitate with methanol as the hydrogen donor. During the catalyst preparation, Sn doping reduces the size of carbon spheres, and the formation of Ni–Sn intermetallic compounds restrain the graphitization, contributing to larger pore volume and pore diameter. Consequently, a more facile mass transfer occurs in carbon-encapsulated Ni–Sn intermetallic compound catalysts than in carbon-encapsulated Ni catalysts. During the in-situ hydrothermal deoxygenation, the synergism between Ni and Sn favors palmitic acid hydrogenation to a highly reactive hexadecanal that easily either decarbonylate to n-pentadecane or is hydrogenated to hexadecanol. At high reaction temperature, hexadecanol undergoes dehydrogenation–decarbonylation, generating n-pentadecane. Also, the C–C bond hydrolysis and methanation are suppressed on Ni–Sn intermetallic compounds, favorable for increasing the carbon yield and reducing the H2 consumption. The n-pentadecane and n-hexadecane yields reached 88.1% and 92.8% on carbon-encapsulated Ni3Sn2 intermetallic compound at 330 °C. After washing and H2 reduction, the carbon-encapsulated Ni3Sn2 intermetallic compound remains stable during three recycling cycles. This is ascribed to the carbon confinement that effectively suppresses the sintering and loss of metal particles under harsh hydrothermal conditions.

关键词： extended Stöber method     carbon encapsulated Ni–Sn intermetallic compounds     confinement     in-situ hydrothermal deoxygenation     hydrogenation     decarbonylation    

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标题 作者 时间 类型 操作

Influence of crystalline phase of Li-Al-O oxides on the activity of Wacker-type catalysts in dimethyl carbonate synthesis

Yadong GE, Yuanyuan DONG, Shengping WANG, Yujun ZHAO, Jing LV, Xinbin MA

期刊论文

Mayenite supported perovskite monoliths for catalytic combustion of methyl methacrylate

Zekai ZHANG, Zhijian KONG, Huayan LIU, Yinfei CHEN

期刊论文

HPLC determination of glyoxal in aldehyde solution with 3-methyl-2-benzothiazolinone hydrazone

Yamei ZHU, Xiaoli YAO, Shaohui CHEN, Qun CUI, Haiyan WANG

期刊论文

Polymerization of methyl methacrylate catalyzed by mono-/bis-salicylaldiminato nickel(II) complexes and

Jihong LU, Danfeng ZHANG, Qian CHEN, Buwei YU

期刊论文

Effect of alkyl nitrite decomposition on catalytic performance of CO coupling reaction over supported

Zhenhua LI, Weihan WANG, Dongxue YIN, Jing LV, Xinbin MA

期刊论文

Denitrification and phosphorus uptake by DPAOs using nitrite as an electron acceptor by step-feed strategies

Bin MA, Shuying WANG, Guibing ZHU, Shijian GE, Junmin WANG, Nanqi Ren, Yongzhen PENG

期刊论文

Photocatalytic degradation of methyl orange using ZnO/TiO composites

Ming GE , Changsheng GUO , Xingwang ZHU , Lili MA , Wei HU , Yuqiu WANG , Zhenan HAN ,

期刊论文

of activated sludge aggregates using microelectrodes in completely autotrophic nitrogen removal over nitrite

Yongtao LV,Xuan CHEN,Lei WANG,Kai JU,Xiaoqiang CHEN,Rui MIAO,Xudong WANG

期刊论文

Effects of nitrite on phosphate uptake in anaerobic-oxic process

LI Jie, XIONG Biyong, ZHANG Shude, YANG Hong, ZHANG Jie

期刊论文

Carbon-coated Ni-Co alloy catalysts: preparation and performance for aqueous phase hydrodeoxygenation of methyl

期刊论文

method for efficient control of hydrogen sulfide and methane in gravity sewers: Combination of NaOH and Nitrite

期刊论文

A simple, azulene-based colorimetric probe for the detection of nitrite in water

Lloyd C. Murfin, Carlos M. López-Alled, Adam C. Sedgwick, Jannis Wenk, Tony D. James, Simon E. Lewis

期刊论文

Experimental study of nitrite accumulation in pre-denitrification biological nitrogen removal process

WU Xuelei, CHEN Lunqiang, PENG Yongzhen, WANG Pu, WANG Yayi

期刊论文

Performance of completely autotrophic nitrogen removal over nitrite process under different aeration

GUO Jinsong, YANG Guohong, FANG Fang, QIN Yu

期刊论文

Efficient hydrothermal deoxygenation of methyl palmitate to diesel-like hydrocarbons on carbon encapsulated

期刊论文