Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study inves...Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant group.Collectively,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.展开更多
Hydroxylamine sulfate （HAS） and sodium nitrite are used as the accelerators for zinc phos- phate coating on high carbon steel. Phase evolution of phosphate coating was investigated by X-ray diffraction. It is found ...Hydroxylamine sulfate （HAS） and sodium nitrite are used as the accelerators for zinc phos- phate coating on high carbon steel. Phase evolution of phosphate coating was investigated by X-ray diffraction. It is found that the phosphating coatings are mainly composed of hopeite Zn3Fe（PO4）2.4H2O and phosphophyllite Zn2Fe（PO4）2.4H2O. The microstructural changes of the phosphate coating, as a function of phosphating time, were evaluated by scanning elec- tron microscopy. Four-ball friction experiments reveal that hydroxylamine sulfate instead of sodium nitrite can effectively reduce the friction coefficient of lubricated phosphating coat- ing. Therefore, it may be expected that HAS will be widely used as a fast and ECO-friendly accelerator in phosphate industry.展开更多
The promoting effect of ethanol on the synthesis of N-（2-methylphenyl）hydroxylamine from o-nitrotoluene in Zn/H2O/CO2 system was observed.By adding appropriate amount of ethanol,the selectivity of N-（2-methylphenyl...The promoting effect of ethanol on the synthesis of N-（2-methylphenyl）hydroxylamine from o-nitrotoluene in Zn/H2O/CO2 system was observed.By adding appropriate amount of ethanol,the selectivity of N-（2-methylphenyl）hydroxylamine increased from 71%to 90%when the reduction was carried out at 25℃under normal pressure of CO2.展开更多
Objective To purify a low-temperature hydroxylamine oxidase （HAO） from a heterotrophic nitrifying bacterium Acinetobacter sp. Y26 and investigate the enzyme property. Methods A HAO was purified by an anion-exchange ...Objective To purify a low-temperature hydroxylamine oxidase （HAO） from a heterotrophic nitrifying bacterium Acinetobacter sp. Y26 and investigate the enzyme property. Methods A HAO was purified by an anion-exchange and gel-filtration chromatography from strain Y16. The purity and molecular mass were determined by RP-HPLC and SDS-PAGE. The HAO activity was detected by monitoring the reduction of potassium ferricyanide using hydroxylamine as substrate and ferricyanide as electron acceptor. The partial amino acid sequence was determined by mass spectrometry. Results The low-temperature HAO with a molecular mass of 61 kDa was purified from strain Y26 by an anion-exchange and gel-filtration chromatography. The enzyme exhibited an ability to oxidize hydroxylamine in wide temperature range （4-40 ℃） in vitro using hydroxylamine as substrate and ferricyanide as electron acceptor. It was stable in the temperature range of 4 to 25 ℃ and pH range of 6.0 to 8.5 with less than 30% change in its activity. The optimal temperature and pH were 15 ℃ and 7.5, respectively. Three peptides were determined by mass spectrometry which were shown to be not identical to other reported HAOs. Conclusion This is the first study to purify a low-temperature HAO from a heterotrophic nitrifier Acinetobecter sp. It differs from other reported HAOs in molecular mass and enzyme properties. The findings of the present study have suggested that the strain Y26 passes through a hydroxylamine-oxidizing process catalyzed by a low-temperature HAO for ammonium removal.展开更多
It is the first reported that a new nitrogen-containing non-amino acid type organiccomponent 1 isolated from one of the well known traditional chinese herb medicines. Gastrodiaelela BI. Structure elucidation and unamb...It is the first reported that a new nitrogen-containing non-amino acid type organiccomponent 1 isolated from one of the well known traditional chinese herb medicines. Gastrodiaelela BI. Structure elucidation and unambiguous NMR assignments for the title compound werecarried out mainly Oil the basis of' 1D and 2D NMR experiments.展开更多
This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H_(2)O_(2) Fenton-like system. Sulfamethoxazole (SMX) could be efficient...This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H_(2)O_(2) Fenton-like system. Sulfamethoxazole (SMX) could be efficiently degraded at near neutral pH. Conditional parameters affecting the SMX degradation in the ZVI/H_(2)O_(2)/HA/MF system, e.g., pH and the dosages of ZVI, HA and H_(2)O_(2), were investigated. Unlike the acid-favorable ZVI/H_(2)O_(2) and ZVI/H_(2)O_(2)/HA systems, the MF-assisted system exhibited good performances even at pH up to 6.0 and highest degradation rate at pH of 5.0. ^(·)OH was still identified as the responsible oxidant. A mechanism involving the MF-enhanced heterogeneous-homogeneous iron cycle was proposed in the near-neutral ZVI/H_(2)O_(2)/HA system. Without MF, HA-induced reductive dissolution of the surface iron oxides occurred and thus leaded to homogeneous Fenton reactions. After the introduction of MF, the gradient magnetic field formed on the ZVI particles would induce the generation of concentration cells of Fe(II) and local corrosion of iron. Large amounts of aqueous and bounded Fe(II) catalyzed H_(2)O_(2) to efficiently produce ^(·)OH, while HA maintained the surface and bulk cycles of Fe(II)/Fe(III). The result of study is expected to provide a green, energy-free method in improving the effectiveness of ZVI-based Fenton-like technologies at weak-acidic circumstances.展开更多
Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone（BQ） and hydroxylamine hydrochloride（HA） as Fenton enha...Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone（BQ） and hydroxylamine hydrochloride（HA） as Fenton enhancers for the removal of glycerin from saline water under ambient temperature by accelerating the ferric system.It was found that organics removal was not obviously affected by chloride ions of low concentration（less than 0.1 mol/L）,while the mineralization rate was strongly inhibited in the presence of a large amount of chloride ions.In addition,ferric hydrolysis-precipitation was significantly alleviated in the presence of HA and BQ,and HA was more effective in reducing ferric ions into ferrous ions than HA,while the H_2O_2 decomposition rate was higher in the BQ-Fenton system.Electron spin resonance analysis revealed that OH production was reduced in high salinity conditions,while it was enhanced after the addition of HA and BQ（especially HA）.This study provided a possible solution to control and alleviate the inhibitory effect of chloride ions on the Fenton process for organics removal.展开更多
2,5-Dicyanofuran(DCF)is an important biomass-derived platform compound primarily used to prepare bio-based adiponitrile,which is the key precursor for the synthesis of nylon 66 and 1,6-hexanediisocyanate(HDI).In this ...2,5-Dicyanofuran(DCF)is an important biomass-derived platform compound primarily used to prepare bio-based adiponitrile,which is the key precursor for the synthesis of nylon 66 and 1,6-hexanediisocyanate(HDI).In this study,one-pot,green and safe synthesis of DCF from 2,5-diformylfuran(DFF)and hydroxylamine ionic liquid salts was proposed.Eco-friendly hydroxylamine ionic liquid salts were used as the nitrogen source.Ionic liquid exhibited three-fold function of cosolvent,catalysis and phase separation.The conversion of DFF and yield of DCF reached 100%under the following optimum reaction conditions:temperature of 120℃ for 70 min,volume ratio of paraxylene:[HSO_(3)-b-Py]HSO4 of 2:1,and molar ratio of DFF:(NH_(2)OH)_(2)[HSO_(3)-b-Py]HSO4 of 1:1.5.The reaction mechanism for the synthesis of DCF was proposed,and the kinetic model was established.The reaction order with respect to DFF and intermediate product 2,5-diformylfuran dioxime(DFFD)was 1.06 and 0.16,and the reaction activation energy was 64.07 kJ·mol^(-1) and 59.37 kJ·mol^(-1) respectively.After the reaction,the ionic liquid was easy to separate,recover and recycle.展开更多
A novel chemiluminescence(CL) sensor, which can be used for hydroxylamine determination in combination with flow injection analysis, was developed by electrostatically immobilizing luminol and periodate on anion exch...A novel chemiluminescence(CL) sensor, which can be used for hydroxylamine determination in combination with flow injection analysis, was developed by electrostatically immobilizing luminol and periodate on anion exchange resin respectively. Hydroxylamine was sensed by its enhancing effect on the weak CL reaction between luminol and periodate, which were eluted from the ion exchange column. The response of the sensor to hydroxylamine was linear in the concentration range of 8.0×10^(-8)-2.0×10^(-6)mol/L with a detection limit of 4.0×10^(-8)mol/L hydroxylamine(3σ).The relative standard deviation(RSD) was 2.0% for 9 repetitive determinations at a hydroxylamine concentration of 5.0×10^(-7) mol/L. The sensor could be reused for over 400 times with a good reproducibility and was used to determine hydroxylamine in wastewater.展开更多
In this paper the reaction of vinyl triazole derivatives with hydroxylamine hydrochloride under the action of sodium carbonate was studied. The result indicated that cyclization took place and new heterocyclic compoun...In this paper the reaction of vinyl triazole derivatives with hydroxylamine hydrochloride under the action of sodium carbonate was studied. The result indicated that cyclization took place and new heterocyclic compounds of 1,2-oxazocyclopentanes were obtained.展开更多
In the presence of ethyl alcohol or emulsifier OP,molybdenum(Ⅵ) forms 1∶1∶1'water soluble colored coordination com- pound with both of 2-(2-thiazolylazo)-5-diethylaminophenol (abbreviation TAE) and hydroxylamin...In the presence of ethyl alcohol or emulsifier OP,molybdenum(Ⅵ) forms 1∶1∶1'water soluble colored coordination com- pound with both of 2-(2-thiazolylazo)-5-diethylaminophenol (abbreviation TAE) and hydroxylamine.This deep blue coordination compound is inert characteristically and remains stable in 1.7 mol/L sulfuric acid,2.4 mol/L hydrochloric or ni- tric acid.It will not be decomposed by masking agents even on boiled,while in that case,almost all the colored coordination com- pounds formed by other metal ions will be decomposed completely.This inert character of the coordination compound of molybdenum(Ⅵ) and its utilization in improving the analytical selectivity have been discussed.In the coexistence of various for- eign ions,especially in the presence of a great quantity of tungsten,which always interferes with the determination of molybdenum,the direct determination of molybdenum in the aqueous solution by applying this system has shown an acceptable sensitivity and reproducibility.From the results of determination in some synthetic and standard samples,it seems feasible to use this system in the determination of molybdenum in nonferrous alloys.展开更多
The transformation of renewable nitrogen feedstock to nitrogenous chemicals plays a significant role in our modern society,considering the crucial impact of nitrogenous chemicals on life sciences,biomedicine,agricultu...The transformation of renewable nitrogen feedstock to nitrogenous chemicals plays a significant role in our modern society,considering the crucial impact of nitrogenous chemicals on life sciences,biomedicine,agriculture,and manufacture.Hydroxylamine(NH_(2)OH),a typical nucleophile,has been widely served as the nitrogenous feedstock to produce nitrogenous chemicals.Conventional NH_(2)OH synthesis methods rely on harsh reaction conditions,leading to an unfavorable environmental footprint.In contrast,nitric oxide electroreduction promises to produce NH_(2)OH powered by renewable electricity.Some achievements have revealed the possibility of this process,but have also identified significant challenges.The activity and selectivity are fundamentally limited by competing hydrogenation reactions,while the performance evaluation with high accuracy and reproducibility is challenging.Herein,this review aims to provide insight into the mechanism of NH_(2)OH electrosynthesis,especially regarding understanding reaction pathways and the design principle towards efficient electrocatalyst.Then,the performance evaluation parameters and standard measurement methods for NH_(2)OH synthesis are summarized to screen efficient electrocatalysts.Finally,the prospects and emerging opportunities to synthesize nitrogen-containing organic compounds by tandem reaction are proposed.This review aims to provide a guide for evaluating and exploring efficient electrocatalytic systems for NH_(2)OH production and utilization technology.展开更多
With the rapid evolution of contemporary society,there is an increasing demand for the production of bulk chemicals such as fertilizers,fuels,and pharmaceuticals.However,current synthetic approaches for these bulk che...With the rapid evolution of contemporary society,there is an increasing demand for the production of bulk chemicals such as fertilizers,fuels,and pharmaceuticals.However,current synthetic approaches for these bulk chemicals predominantly depend on conventional fossil fuel-based chemical refining processes.This dependence poses a substantial challenge to both environmental sustainability and energy resources[1].An example of this issue is the synthesis of hydroxylamine(NH2OH).展开更多
Sulfapyridine(SPY)is a ubiquitous environmental contaminant belonging to the sulfonamide antibiotics.Previous studies showed that hydroxylamine(HA)can improve the performance of advanced oxidation processes(AOPs)by pr...Sulfapyridine(SPY)is a ubiquitous environmental contaminant belonging to the sulfonamide antibiotics.Previous studies showed that hydroxylamine(HA)can improve the performance of advanced oxidation processes(AOPs)by promoting Fe(Ⅱ)regeneration,yet the reaction mechanisms were not elucidated.Therefore,the role of HA and the degradation mechanisms of SPY were systematically studied therein.The SPY degradation efficiency increased from 77.5%to 91.6%after HA was added.With radical scav-enger experiment,a function of HA to promote·OH production for SPY degradation was clarified.The major radical from SO_(4)^(·-) and·OH to·OH with addition of HA in Fe(Ⅱ)/potassium peroxydisulfate(PDS).Results showed that alkali,acid condition and high PDS concentration all contributed to SPY degradation.According to experimental results,density functional theory(DFT)was used to calculate the degradation pathway of SPY.Rate-limiting path was obtained by comparing the rate constants calculated from the transition-state theory.The cleavage of CeC bond in benzene ring with the slowest rate was essential to degrade SPY,which not only promotes the mineralization of SPY,but also prevent the production of toxic TPs effectively.This study provides valuable insight into the SPY degradation in HA/Fe(Ⅱ)/PDS.展开更多
Comprehensive Summary A general and efficient strategy for the synthesis ofγ-lactams has been reported.The hydroxylamines form Lossen rearrangement products of electron-deficient group migration with base and then un...Comprehensive Summary A general and efficient strategy for the synthesis ofγ-lactams has been reported.The hydroxylamines form Lossen rearrangement products of electron-deficient group migration with base and then undergo[3+2]cycloaddition reaction with vinyl cyclopropane,which could be performed with broad substrate scope,excellent functional group tolerance and high efficiency to produce the desired products.It also allowed further modification to other derivatives of theseγ-lactams.展开更多
Hydroxyl radicals(HO*)show low reactivity with perchlorinated hydrocarbons,such as carbon tetrachloride(CT),in conventional Fenton reactions,therefore,the generation of reductive radicals has attracted increasing atte...Hydroxyl radicals(HO*)show low reactivity with perchlorinated hydrocarbons,such as carbon tetrachloride(CT),in conventional Fenton reactions,therefore,the generation of reductive radicals has attracted increasing attention.This study investigated the enhancement of CT degradation by the synergistic effects of hydroxylamine(HA)and formic acid(FA)(initial[CT]=0.13 mmol/L)in a Fe(il)activated calcium peroxide(CP)fenton process.CT degradation increased from 56.6%to 99.9%with the addition of 0.78 mmol/L HA to the CP/Fe(II)/FA/CT process in a molar ratio o f 12/6/12/1.The results also showed that the presence of HA enhanced the regeneration of Fe(II)from Fe(III),and the production of HO*increased one-fold when employing benzoic acid as the HO*probe.Additionally,FA slightly improves the production of HO*.A study of the mechanism confirmed that the carbon dioxide radical(C02·),a strong reductant generated by the reaction between FA and HO*,was the dominant radical responsible for CT degradation.Almost complete CT dechlorination was achieved in the process.The presence of humic acid and chloride ion slightly decreased CT removal,while high doses of bicarbonate and high pH inhibited CT degradation.This study helps us to better understand the synergistic roles of FA and HA for HO·and C02·^-generation and the removal of perchlorinated hydrocarbons in modified Fenton systems.展开更多
Hydroxylamine(NH_(2)OH),a vital but unstable industrial feedstock,is presently prepared under harsh conditions that cause environmental and energy concerns.Here,we report an electrochemical method to prepare oximes,wh...Hydroxylamine(NH_(2)OH),a vital but unstable industrial feedstock,is presently prepared under harsh conditions that cause environmental and energy concerns.Here,we report an electrochemical method to prepare oximes,which serve as precursors for NH_(2)OH after facile hydrolysis.The carbon-supported amorphous Mn electrocatalyst delivers a current density of~100 mA cm^(-2) with a Faradaic efficiency of 40.92%and a yield rate of 0.251 mmol cm^(-2)h^(-1) for formaldoxime(CH_(2)NOH)generation by using nitrate and formaldehyde as reactants.Formaldoxime can be easily released to produce NH_(2)OH via hydrolysis.Impressively,this method exhibits an economic advantage over conventional manufacturing based on techno-economic analysis.A series of control experiments,in situ characterizations,and theoretical simulations unveil the reaction mechanism via the spontaneous reaction between an aldehyde and*NH_(2)OH intermediate derived from nitrate electroreduction.The high activity of Mn originates from its inhibitory effects on the further reduction of key*NH_(2)OH intermediate.This strategy opens a sustainable and green way for NH_(2)OH synthesis under mild conditions using renewable energy.展开更多
Transition metal-catalyzed diamination by hydroxylamines is a common approach for making three-membered aziridines,while its use for building the larger N-heterocycles is still underdeveloped.Herein,we report an effic...Transition metal-catalyzed diamination by hydroxylamines is a common approach for making three-membered aziridines,while its use for building the larger N-heterocycles is still underdeveloped.Herein,we report an efficient Pd(0)-catalyzed intermolecular[4+1]annulation of o-bromo(or chloro)-biaryls with bifunctional secondary hydroxylamines for the one-step assembly of synthetically useful carbazoles.Noteworthily,a linchpin for this domino reaction was the judicious selection of both the amino-sources and Pd(0)-catalysts for enabling the prerequisite oxidative addition of aryl halides to Pd(0)-species in the presence of hydroxylamines with a labile N-O bond.展开更多
Two pairs of structural isomers isolated from Aconitum nagarum var.lasiandrum have been differentiated by ESI MS using hydroxylamine hydrochloride(NH2OH·HCl) derivative method.
This paper focused on investigating high-efficient reductants of recovering selenium and tellurium from degoldizedsolution of copper anode slimes.Firstly,the effect of various reductants on recovery rates of Se and Te...This paper focused on investigating high-efficient reductants of recovering selenium and tellurium from degoldizedsolution of copper anode slimes.Firstly,the effect of various reductants on recovery rates of Se and Te was investigated based onthermodynamic analysis of various metallic ions in degoldized solution.Secondly,the single factor experiments were made toinvestigate the effect of the process parameters on recovering Se and Te with hydrazine hydrate.Finally,the hydroxylaminehydrochloride was added to intensify the extraction efficiencies of Se and Te.The results indicated that hydrazine hydrate was themost suitable reductant,and the recovery rates of Se and Te are71.23%and76.50%,respectively;the recovery rates of Se and Tewere92.07%and97.81%,respectively,under the optimal process conditions of hydrazine hydrate dosage of0.2133mol/L,H+concentration of4.305mol/L,reaction temperature of85°C and reaction time of5h;the recovery rate of Se was97.59%,and that Tereached up to100%when hydroxylamine hydrochloride dosage was1.5116mol/L.展开更多
文摘Partial nitrification is a key aspect of efficient nitrogen removal,although practically it suf-fers from long start-up cycles and unstable long-term operational performance.To address these drawbacks,this study investigated the effect of low intensity ultrasound treatment combined with hydroxylamine(NH2OH)on the performance of partial nitrification.Results showthat compared with the control group,low-intensity ultrasound treatment(0.10W/mL,15 min)combined with NH2OH(5 mg/L)reduced the time required for partial nitrification initiation by 6 days,increasing the nitrite accumulation rate(NAR)and ammonia nitro-gen removal rate(NRR)by 20.4% and 6.7%,respectively,achieving 96.48% NRR.Mechanis-tic analysis showed that NH2OH enhanced ammonia oxidation,inhibited nitrite-oxidizing bacteria(NOB)activity and shortened the time required for partial nitrification initiation.Furthermore,ultrasonication combined with NH2OH dosing stimulated EPS(extracellular polymeric substances)secretion,increased carbonyl,hydroxyl and amine functional group abundances and enhanced mass transfer.In addition,16S rRNA gene sequencing results showed that ultrasonication-sensitive Nitrospira disappeared from the ultrasound+NH_(2)OH system,while Nitrosomonas gradually became the dominant group.Collectively,the results of this study provide valuable insight into the enhancement of partial nitrification start-up during the process of wastewater nitrogen removal.
基金This work was supported by the Bengbu Yucheng New Materials Science and Technology Ltd. （No.2012QTXM0375） and the Natural Science Foundation of Anhui Province （No.1208085QE99）.
文摘Hydroxylamine sulfate （HAS） and sodium nitrite are used as the accelerators for zinc phos- phate coating on high carbon steel. Phase evolution of phosphate coating was investigated by X-ray diffraction. It is found that the phosphating coatings are mainly composed of hopeite Zn3Fe（PO4）2.4H2O and phosphophyllite Zn2Fe（PO4）2.4H2O. The microstructural changes of the phosphate coating, as a function of phosphating time, were evaluated by scanning elec- tron microscopy. Four-ball friction experiments reveal that hydroxylamine sulfate instead of sodium nitrite can effectively reduce the friction coefficient of lubricated phosphating coat- ing. Therefore, it may be expected that HAS will be widely used as a fast and ECO-friendly accelerator in phosphate industry.
基金supported by the Doctoral Fund of Ministry of Education of China(No.20070141046)the Fund of Education Department of Liaoning Province(No.[2006]124)
文摘The promoting effect of ethanol on the synthesis of N-（2-methylphenyl）hydroxylamine from o-nitrotoluene in Zn/H2O/CO2 system was observed.By adding appropriate amount of ethanol,the selectivity of N-（2-methylphenyl）hydroxylamine increased from 71%to 90%when the reduction was carried out at 25℃under normal pressure of CO2.
基金supported by grants from National Natural Science Foundation of China(51078106)Heilongjiang Provincial Science Foundation for Distinguished Youth Scholar(JC200708)Heilongjiang Provincial Finance Foundation for Basic Sciences(CZ12BZSM06)
文摘Objective To purify a low-temperature hydroxylamine oxidase （HAO） from a heterotrophic nitrifying bacterium Acinetobacter sp. Y26 and investigate the enzyme property. Methods A HAO was purified by an anion-exchange and gel-filtration chromatography from strain Y16. The purity and molecular mass were determined by RP-HPLC and SDS-PAGE. The HAO activity was detected by monitoring the reduction of potassium ferricyanide using hydroxylamine as substrate and ferricyanide as electron acceptor. The partial amino acid sequence was determined by mass spectrometry. Results The low-temperature HAO with a molecular mass of 61 kDa was purified from strain Y26 by an anion-exchange and gel-filtration chromatography. The enzyme exhibited an ability to oxidize hydroxylamine in wide temperature range （4-40 ℃） in vitro using hydroxylamine as substrate and ferricyanide as electron acceptor. It was stable in the temperature range of 4 to 25 ℃ and pH range of 6.0 to 8.5 with less than 30% change in its activity. The optimal temperature and pH were 15 ℃ and 7.5, respectively. Three peptides were determined by mass spectrometry which were shown to be not identical to other reported HAOs. Conclusion This is the first study to purify a low-temperature HAO from a heterotrophic nitrifier Acinetobecter sp. It differs from other reported HAOs in molecular mass and enzyme properties. The findings of the present study have suggested that the strain Y26 passes through a hydroxylamine-oxidizing process catalyzed by a low-temperature HAO for ammonium removal.
文摘It is the first reported that a new nitrogen-containing non-amino acid type organiccomponent 1 isolated from one of the well known traditional chinese herb medicines. Gastrodiaelela BI. Structure elucidation and unambiguous NMR assignments for the title compound werecarried out mainly Oil the basis of' 1D and 2D NMR experiments.
基金supported by the National Natural Science Foundation of China (Nos. 21677055 and 22006045)the China Postdoctory Science Foundation (No. 2020M672361)the Project of Three Gorges Corporation (No. JD-ZC-FW-20-001)。
文摘This study has demonstrated an interesting amplification effect of magnetic field (MF) on the hydroxylamine (HA)-promoted zero valent iron (ZVI)/H_(2)O_(2) Fenton-like system. Sulfamethoxazole (SMX) could be efficiently degraded at near neutral pH. Conditional parameters affecting the SMX degradation in the ZVI/H_(2)O_(2)/HA/MF system, e.g., pH and the dosages of ZVI, HA and H_(2)O_(2), were investigated. Unlike the acid-favorable ZVI/H_(2)O_(2) and ZVI/H_(2)O_(2)/HA systems, the MF-assisted system exhibited good performances even at pH up to 6.0 and highest degradation rate at pH of 5.0. ^(·)OH was still identified as the responsible oxidant. A mechanism involving the MF-enhanced heterogeneous-homogeneous iron cycle was proposed in the near-neutral ZVI/H_(2)O_(2)/HA system. Without MF, HA-induced reductive dissolution of the surface iron oxides occurred and thus leaded to homogeneous Fenton reactions. After the introduction of MF, the gradient magnetic field formed on the ZVI particles would induce the generation of concentration cells of Fe(II) and local corrosion of iron. Large amounts of aqueous and bounded Fe(II) catalyzed H_(2)O_(2) to efficiently produce ^(·)OH, while HA maintained the surface and bulk cycles of Fe(II)/Fe(III). The result of study is expected to provide a green, energy-free method in improving the effectiveness of ZVI-based Fenton-like technologies at weak-acidic circumstances.
基金supported by the National Natural Science Foundation of China(Nos.51025830,41201498 and 51178360)
文摘Fenton oxidation is generally inhibited in the presence of a high concentration of chloride ions.This study investigated the feasibility of using benzoquinone（BQ） and hydroxylamine hydrochloride（HA） as Fenton enhancers for the removal of glycerin from saline water under ambient temperature by accelerating the ferric system.It was found that organics removal was not obviously affected by chloride ions of low concentration（less than 0.1 mol/L）,while the mineralization rate was strongly inhibited in the presence of a large amount of chloride ions.In addition,ferric hydrolysis-precipitation was significantly alleviated in the presence of HA and BQ,and HA was more effective in reducing ferric ions into ferrous ions than HA,while the H_2O_2 decomposition rate was higher in the BQ-Fenton system.Electron spin resonance analysis revealed that OH production was reduced in high salinity conditions,while it was enhanced after the addition of HA and BQ（especially HA）.This study provided a possible solution to control and alleviate the inhibitory effect of chloride ions on the Fenton process for organics removal.
基金support from the National Natural Science Foundation of China(Nos.U20A20152,21236001 and 21878069).
文摘2,5-Dicyanofuran(DCF)is an important biomass-derived platform compound primarily used to prepare bio-based adiponitrile,which is the key precursor for the synthesis of nylon 66 and 1,6-hexanediisocyanate(HDI).In this study,one-pot,green and safe synthesis of DCF from 2,5-diformylfuran(DFF)and hydroxylamine ionic liquid salts was proposed.Eco-friendly hydroxylamine ionic liquid salts were used as the nitrogen source.Ionic liquid exhibited three-fold function of cosolvent,catalysis and phase separation.The conversion of DFF and yield of DCF reached 100%under the following optimum reaction conditions:temperature of 120℃ for 70 min,volume ratio of paraxylene:[HSO_(3)-b-Py]HSO4 of 2:1,and molar ratio of DFF:(NH_(2)OH)_(2)[HSO_(3)-b-Py]HSO4 of 1:1.5.The reaction mechanism for the synthesis of DCF was proposed,and the kinetic model was established.The reaction order with respect to DFF and intermediate product 2,5-diformylfuran dioxime(DFFD)was 1.06 and 0.16,and the reaction activation energy was 64.07 kJ·mol^(-1) and 59.37 kJ·mol^(-1) respectively.After the reaction,the ionic liquid was easy to separate,recover and recycle.
基金Supported by the National Natural Science Foundation of China(No.2 9975 0 13,9835 110 )
文摘A novel chemiluminescence(CL) sensor, which can be used for hydroxylamine determination in combination with flow injection analysis, was developed by electrostatically immobilizing luminol and periodate on anion exchange resin respectively. Hydroxylamine was sensed by its enhancing effect on the weak CL reaction between luminol and periodate, which were eluted from the ion exchange column. The response of the sensor to hydroxylamine was linear in the concentration range of 8.0×10^(-8)-2.0×10^(-6)mol/L with a detection limit of 4.0×10^(-8)mol/L hydroxylamine(3σ).The relative standard deviation(RSD) was 2.0% for 9 repetitive determinations at a hydroxylamine concentration of 5.0×10^(-7) mol/L. The sensor could be reused for over 400 times with a good reproducibility and was used to determine hydroxylamine in wastewater.
文摘In this paper the reaction of vinyl triazole derivatives with hydroxylamine hydrochloride under the action of sodium carbonate was studied. The result indicated that cyclization took place and new heterocyclic compounds of 1,2-oxazocyclopentanes were obtained.
文摘In the presence of ethyl alcohol or emulsifier OP,molybdenum(Ⅵ) forms 1∶1∶1'water soluble colored coordination com- pound with both of 2-(2-thiazolylazo)-5-diethylaminophenol (abbreviation TAE) and hydroxylamine.This deep blue coordination compound is inert characteristically and remains stable in 1.7 mol/L sulfuric acid,2.4 mol/L hydrochloric or ni- tric acid.It will not be decomposed by masking agents even on boiled,while in that case,almost all the colored coordination com- pounds formed by other metal ions will be decomposed completely.This inert character of the coordination compound of molybdenum(Ⅵ) and its utilization in improving the analytical selectivity have been discussed.In the coexistence of various for- eign ions,especially in the presence of a great quantity of tungsten,which always interferes with the determination of molybdenum,the direct determination of molybdenum in the aqueous solution by applying this system has shown an acceptable sensitivity and reproducibility.From the results of determination in some synthetic and standard samples,it seems feasible to use this system in the determination of molybdenum in nonferrous alloys.
基金supported by the National Natural Science Foundation of China(21925203 and 22402110)the National Key Research and Development Program of China(2021YFC2101900)+3 种基金the Program for Youth Sanjin Scholarthe 100 Talent Project of Shanxi Provincethe Program for Young Scholar Talents of Wenying in Shanxi Universitythe Fund for Shanxi“1331 Project”。
文摘The transformation of renewable nitrogen feedstock to nitrogenous chemicals plays a significant role in our modern society,considering the crucial impact of nitrogenous chemicals on life sciences,biomedicine,agriculture,and manufacture.Hydroxylamine(NH_(2)OH),a typical nucleophile,has been widely served as the nitrogenous feedstock to produce nitrogenous chemicals.Conventional NH_(2)OH synthesis methods rely on harsh reaction conditions,leading to an unfavorable environmental footprint.In contrast,nitric oxide electroreduction promises to produce NH_(2)OH powered by renewable electricity.Some achievements have revealed the possibility of this process,but have also identified significant challenges.The activity and selectivity are fundamentally limited by competing hydrogenation reactions,while the performance evaluation with high accuracy and reproducibility is challenging.Herein,this review aims to provide insight into the mechanism of NH_(2)OH electrosynthesis,especially regarding understanding reaction pathways and the design principle towards efficient electrocatalyst.Then,the performance evaluation parameters and standard measurement methods for NH_(2)OH synthesis are summarized to screen efficient electrocatalysts.Finally,the prospects and emerging opportunities to synthesize nitrogen-containing organic compounds by tandem reaction are proposed.This review aims to provide a guide for evaluating and exploring efficient electrocatalytic systems for NH_(2)OH production and utilization technology.
基金supported by the National Natural Science Foundation of China(Nos.22175174 and 52332007).
文摘With the rapid evolution of contemporary society,there is an increasing demand for the production of bulk chemicals such as fertilizers,fuels,and pharmaceuticals.However,current synthetic approaches for these bulk chemicals predominantly depend on conventional fossil fuel-based chemical refining processes.This dependence poses a substantial challenge to both environmental sustainability and energy resources[1].An example of this issue is the synthesis of hydroxylamine(NH2OH).
基金supported by the China Postdoctoral Science Foundation(No.2023M733167)the National Natural Science Foundation of China(No.52170093)+5 种基金by the Zhejiang Provincial Natural Science Foundation(No.LY22E080010)the Science and Technology Project of Zhejiang Province(No.2022C02038)the Basic Public Welfare Research Program of Zhejiang Province(LZJWZ22C030002)the Joint Funds of the Zhejiang Provincial Natural Science Foundation of China(LZJWZ23E090007)the Science Foundation of President of the Zhejiang Institute of Hy-draulics and Estuary(ZIHE 22Q009)the Zhejiang Province Science and Technology Plan Project(RC2223,RC2224).
文摘Sulfapyridine(SPY)is a ubiquitous environmental contaminant belonging to the sulfonamide antibiotics.Previous studies showed that hydroxylamine(HA)can improve the performance of advanced oxidation processes(AOPs)by promoting Fe(Ⅱ)regeneration,yet the reaction mechanisms were not elucidated.Therefore,the role of HA and the degradation mechanisms of SPY were systematically studied therein.The SPY degradation efficiency increased from 77.5%to 91.6%after HA was added.With radical scav-enger experiment,a function of HA to promote·OH production for SPY degradation was clarified.The major radical from SO_(4)^(·-) and·OH to·OH with addition of HA in Fe(Ⅱ)/potassium peroxydisulfate(PDS).Results showed that alkali,acid condition and high PDS concentration all contributed to SPY degradation.According to experimental results,density functional theory(DFT)was used to calculate the degradation pathway of SPY.Rate-limiting path was obtained by comparing the rate constants calculated from the transition-state theory.The cleavage of CeC bond in benzene ring with the slowest rate was essential to degrade SPY,which not only promotes the mineralization of SPY,but also prevent the production of toxic TPs effectively.This study provides valuable insight into the SPY degradation in HA/Fe(Ⅱ)/PDS.
基金the National Natural Science Foundation of China(21925108,21901203,21901204)for financial support.
文摘Comprehensive Summary A general and efficient strategy for the synthesis ofγ-lactams has been reported.The hydroxylamines form Lossen rearrangement products of electron-deficient group migration with base and then undergo[3+2]cycloaddition reaction with vinyl cyclopropane,which could be performed with broad substrate scope,excellent functional group tolerance and high efficiency to produce the desired products.It also allowed further modification to other derivatives of theseγ-lactams.
基金a grant from the National Key R&D Program of China(No.2018YFC1802500)Chinese Scholar Council(CSC,No.201806740035)。
文摘Hydroxyl radicals(HO*)show low reactivity with perchlorinated hydrocarbons,such as carbon tetrachloride(CT),in conventional Fenton reactions,therefore,the generation of reductive radicals has attracted increasing attention.This study investigated the enhancement of CT degradation by the synergistic effects of hydroxylamine(HA)and formic acid(FA)(initial[CT]=0.13 mmol/L)in a Fe(il)activated calcium peroxide(CP)fenton process.CT degradation increased from 56.6%to 99.9%with the addition of 0.78 mmol/L HA to the CP/Fe(II)/FA/CT process in a molar ratio o f 12/6/12/1.The results also showed that the presence of HA enhanced the regeneration of Fe(II)from Fe(III),and the production of HO*increased one-fold when employing benzoic acid as the HO*probe.Additionally,FA slightly improves the production of HO*.A study of the mechanism confirmed that the carbon dioxide radical(C02·),a strong reductant generated by the reaction between FA and HO*,was the dominant radical responsible for CT degradation.Almost complete CT dechlorination was achieved in the process.The presence of humic acid and chloride ion slightly decreased CT removal,while high doses of bicarbonate and high pH inhibited CT degradation.This study helps us to better understand the synergistic roles of FA and HA for HO·and C02·^-generation and the removal of perchlorinated hydrocarbons in modified Fenton systems.
基金supported by the National Natural Science Foundation of China(22271213(B.Z.)and 22071173(Y.Y.))the Haihe Laboratory of Sustainable Chemical Transformationsthe National Postdoctoral Science Foundation of China(2022M722357(Y.W.))。
文摘Hydroxylamine(NH_(2)OH),a vital but unstable industrial feedstock,is presently prepared under harsh conditions that cause environmental and energy concerns.Here,we report an electrochemical method to prepare oximes,which serve as precursors for NH_(2)OH after facile hydrolysis.The carbon-supported amorphous Mn electrocatalyst delivers a current density of~100 mA cm^(-2) with a Faradaic efficiency of 40.92%and a yield rate of 0.251 mmol cm^(-2)h^(-1) for formaldoxime(CH_(2)NOH)generation by using nitrate and formaldehyde as reactants.Formaldoxime can be easily released to produce NH_(2)OH via hydrolysis.Impressively,this method exhibits an economic advantage over conventional manufacturing based on techno-economic analysis.A series of control experiments,in situ characterizations,and theoretical simulations unveil the reaction mechanism via the spontaneous reaction between an aldehyde and*NH_(2)OH intermediate derived from nitrate electroreduction.The high activity of Mn originates from its inhibitory effects on the further reduction of key*NH_(2)OH intermediate.This strategy opens a sustainable and green way for NH_(2)OH synthesis under mild conditions using renewable energy.
基金supported by the National Natural Science Foundation of China(21925108,22171225)。
文摘Transition metal-catalyzed diamination by hydroxylamines is a common approach for making three-membered aziridines,while its use for building the larger N-heterocycles is still underdeveloped.Herein,we report an efficient Pd(0)-catalyzed intermolecular[4+1]annulation of o-bromo(or chloro)-biaryls with bifunctional secondary hydroxylamines for the one-step assembly of synthetically useful carbazoles.Noteworthily,a linchpin for this domino reaction was the judicious selection of both the amino-sources and Pd(0)-catalysts for enabling the prerequisite oxidative addition of aryl halides to Pd(0)-species in the presence of hydroxylamines with a labile N-O bond.
文摘Two pairs of structural isomers isolated from Aconitum nagarum var.lasiandrum have been differentiated by ESI MS using hydroxylamine hydrochloride(NH2OH·HCl) derivative method.
基金Project(201407300993)supported by Xinjiang Autonomous Region Science and Technology Support Project,China
文摘This paper focused on investigating high-efficient reductants of recovering selenium and tellurium from degoldizedsolution of copper anode slimes.Firstly,the effect of various reductants on recovery rates of Se and Te was investigated based onthermodynamic analysis of various metallic ions in degoldized solution.Secondly,the single factor experiments were made toinvestigate the effect of the process parameters on recovering Se and Te with hydrazine hydrate.Finally,the hydroxylaminehydrochloride was added to intensify the extraction efficiencies of Se and Te.The results indicated that hydrazine hydrate was themost suitable reductant,and the recovery rates of Se and Te are71.23%and76.50%,respectively;the recovery rates of Se and Tewere92.07%and97.81%,respectively,under the optimal process conditions of hydrazine hydrate dosage of0.2133mol/L,H+concentration of4.305mol/L,reaction temperature of85°C and reaction time of5h;the recovery rate of Se was97.59%,and that Tereached up to100%when hydroxylamine hydrochloride dosage was1.5116mol/L.
