A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag(CGFS)and blue algae(BA)as raw materials and used for CO_(2)capture.The CO_(2)chemisorptio...A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag(CGFS)and blue algae(BA)as raw materials and used for CO_(2)capture.The CO_(2)chemisorption capacity of the adsorbent was further enhanced by taking advantage of the nitrogenous bases contained in the BA.In the hydrothermal process,the addition of BA significantly increased the content of pyrrole nitrogen in the adsorbent.In the activation process,pyrrole nitrogen gradually changed into pyridine nitrogen and graphite nitrogen.Increased BA addition result in a higher specific surface area and microporosity of the adsorbent.The CO_(2)adsorption performance test proved that the CGFS-50%-CA sample has the strongest CO_(2)adsorption capacity at low temperature,up to 15.59 cm^(3)/g,which is mainly through physical adsorption,and the CGFS-10%-CA sample has the strongest CO_(2)adsorption capacity at high temperature,up to 7.31 cm^(3)/g,which is mainly through chemical adsorption.CO_(2)uptake of the CGFS-10%-CA sample was well maintained after 10 cycles,with regeneration efficiencies above 99%.The results indicate that the novel adsorbents with coexistence of physical and chemical adsorption have great potential for CO_(2)adsorption applications.展开更多
Nitrogen-containing organic compounds(NOCs)may potentially contribute to aqueous secondary organic aerosols,yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear.With the in-situ ...Nitrogen-containing organic compounds(NOCs)may potentially contribute to aqueous secondary organic aerosols,yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear.With the in-situ measurements performed at a mountain site(1690 m a.s.l.)in southern China,we investigated the formation of NOCs in the cloud droplets and the cloud-free particles,based on their mixing state information of NOCscontaining particles by single particle mass spectrometry.The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual(cloud RES)particles.NOCs were highly correlated with carbonyl compounds(including glyoxalate and methylglyoxal)in the cloud-free particles,however,limited correlation was observed for cloud RES particles.Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles,rather than in the cloud RES particles.The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols,rather than cloud droplets.In addition,we have identified the transport of biomass burning particles that facilitate the formation of NOCs,and that the observed NOCs is most likely contributed to the light absorption.These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.展开更多
Covalent organic frameworks(COFs)are crystalline porous polymeric materials composed of organic monomers connected by strong covalent bonds and offer high stability,good crystallinity,a large specific surface area,and...Covalent organic frameworks(COFs)are crystalline porous polymeric materials composed of organic monomers connected by strong covalent bonds and offer high stability,good crystallinity,a large specific surface area,and controllable structures.COFs are widely used in the fields of adsorption and separation,catalysis,photovoltaics,and drug-delivery.The structural regulation and performance optimization of COFs can be realized through the modification of ligands and the selection of linkage methods.In which,the types of linkage are closely related to the stability and performance of COFs.In this review,nitrogencontaining linkage-bonds(NCLBs)in COFs are divided into N-containing double bonds,N-containing conjugated rings and N-containing unconjugated rings.The association between structure and performance of COFs is elaborated and the synthesis methods of COFs are systematically summarized.Moreover,the structural design,theoretical prediction and machinable application of COFs are prospected.展开更多
The influence of nitrogen-containing polycyclic aromatic hydrocarbons(NC-PAH)on the formation of carbonaceous mesophase remains enigmatic,despite extensive research on the production of carbonaceous materials from aro...The influence of nitrogen-containing polycyclic aromatic hydrocarbons(NC-PAH)on the formation of carbonaceous mesophase remains enigmatic,despite extensive research on the production of carbonaceous materials from aromatic-rich oils.Molecular dynamics simulation was used to investigate the variations in pyrolysis behavior between PAH and NC-PAH based on the composition analysis.Through adjusting the content of NC-PAH,the influence of NC-PAH on the thermal stability of slurry oils(SOs)was evaluated by thermogravimetry,viscosity,coke value,and quinoline insoluble(QI).The morphology and structure of mesocarbon microbeads(MCMBs)prepared with SOs were measured by a polarized-light microscope,SEM,XRD,and Raman.Simulation results indicate that NC-PAH possesses much higher reactivity and tends to produce highly condensed solid and coke products.It corresponds to the QI and high viscosity in thermal stability experiments.Therefore,high concentrations of NC-PAH result in nonuniform morphology and disordered structures.In a system with low viscosity and few QIs,SO,which has a low nitrogen content(475 ppm),reacts gently to produce MCMBs with a uniform particle size(10-40μm)and an excellent spherical shape.As NC-PAH content decreases,the crystalline size of graphitization elevates,as evidenced by parallel layers(10.472-11.764)and stack height(3.269-3.701 nm).The graphitization degree becomes worse and nonuniform with the increase of the content of NC-PAH,and the best is 20.58%evaluated by Raman spectra area ratio(AG/Aall).Overall,this work suggests a nitrogen content reference and a controlling technology of nitrogen for the preparation of superior MCMB.展开更多
Many nitrogen-containing aromatic compounds （NACs）, such as nitrobenzene （NB）, 4-nitrophenol （4-NP）, aniline （AN）, and 2,4-dinitrophenol （2,4-DNP）, are environmentally hazardous, and their removal from conta...Many nitrogen-containing aromatic compounds （NACs）, such as nitrobenzene （NB）, 4-nitrophenol （4-NP）, aniline （AN）, and 2,4-dinitrophenol （2,4-DNP）, are environmentally hazardous, and their removal from contaminated water is one of the main challenges facing wastewater treatment plants. In this study, synthetic wastewater containing NB, 4-NP, 2,4-DNP, and AN at concentrations ranging from 50 to 180 mg/L was fed into a sequencing batch reactor （SBR）. Analyses of the SBR system indicated that it simultaneously removed more than 99% of the NACs at loading rates of 0.36 kg NB/（m^3·d）, 0.3 kg 4-NP/（m^3·d）, 0.25 kg AN/（m^3·d）, and 0.1 kg 2,4-DNP/（m^3·d）. Bacterial groups of Bacteriodetes, Candidate division TM7, α-Proteobacteria, and β-Proteobacteria were dominant in the clone libraries of 16S rRNA genes retrieved from the microbial communities in the SBR system. ＂Cycle tests＂ designed to alter feeding and aeration parameters of the SBR system demonstrated that the resident microbial biome of the SBR system responded rapidly to changing conditions. Consumption of O2 was concomitant with the apparent mineralization of NACs. Aromatic ring-cleaving dioxygenase activities suggested that （1） AN and NB were degraded via catechol 2,3-dioxygenase; （2） 4-NP was degraded via 1,2,4-benzentriol 1,2-dioxygenase; and （3） 2,4-DNP was degraded via an unresolved pathway.展开更多
Soluble portions(SPs) 1-4(SP1-SP4) were afforded from sequentially dissolution and alkanolyses of Baiyinhua lignite(BL) in cyclohexane,CH3OH,CH3CH2OH,and(CH3)2CHOH at 300℃.They were analyzed with a gas chromatograph/...Soluble portions(SPs) 1-4(SP1-SP4) were afforded from sequentially dissolution and alkanolyses of Baiyinhua lignite(BL) in cyclohexane,CH3OH,CH3CH2OH,and(CH3)2CHOH at 300℃.They were analyzed with a gas chromatograph/mass spectrometer and quadrupole exactive orbitrap mass spectrometer(QEOTMS) with an atmosphere pressure chemical ionization source in positive-ion mode,while BL was characterized with an X-ray photoelectron spectrometer(XRPES).The results show that the yields of SP2 and SP3 are much higher than those of SP1 and SP4,and the total SP yield is ca.39.0%.According to the analysis with XRPES,pyrrolic nitrogen atoms are the most abundant nitrogen existing forms in BL.Thousands of nitrogen-containing aromatics(NCAs) were resolved with QEOTMS and their molecular masses are mainly in the range of 200-450 u.The main NCAs are N1O1 and N1O2 class species with double bond equivalent values of 4-18 and carbon numbers of 7-30.The nitrogen atoms appear in pyridine s,quinolines,benzoquinolines or acridine,and dibenzoquinolines or naphthoquinolines,while the oxygen atoms exist in methoxy and furan rings.展开更多
Nitrogen-containing organic pollutants(quinoline,pyridine and indole)are widely distributed in coking wastewater,and bioaugmentation with specific microorganisms may enhance the removal of these recalcitrant pollutant...Nitrogen-containing organic pollutants(quinoline,pyridine and indole)are widely distributed in coking wastewater,and bioaugmentation with specific microorganisms may enhance the removal of these recalcitrant pollutants.The bioaugmented system(group B)was constructed through inoculation of two aromatics-degrading bacteria,Comamonas sp.Z1(quinoline degrader)and Acinetobacter sp.JW(indole degrader),into the activated sludge for treatment of quinoline,indole and pyridine,and the non-bioaugmented activated sludge was used as the control(group C).Both groups maintained high efficiencies(>94%)for removal of nitrogen-containing organic pollutants and chemical oxygen demand(COD)during the long-term operation,and group B was highly effective at the starting period and the operation stage fed with raw wastewater.High-throughput sequencing analysis indicated that nitrogen-containing organic pollutants could shape the microbial community structure,and communities of bioaugmented group B were clearly separated from those of non-bioaugmented group C as observed in non-metric multidimensional scaling(NMDS)plot.Although the inoculants did not remain their dominance in group B,bioaugmentation could induce the formation of effective microbial community,and the indigenous microbes might play the key role in removal of nitrogen-containing organic pollutants,including Dokdonella,Comamonas and Pseudoxanthomonas.Phylogenetic Investigation of Communities by Reconstruction of Unobserved States(PICRUSt)analysis suggested that bioaugmentation could facilitate the enrichment of functional genes related to xenobiotics biodegradation and metabolism,probably leading to the improved performance in group B.This study indicated that bioaugmentation could promote the removal of nitrogen-containing organic pollutants,which should be an effective strategy for wastewater treatment.展开更多
The adsorptive denitrogenation from fuels over three metal-organic frameworks(MIL-96(Al),MIL-53(Al)and MIL-101(Cr))was studied by batch adsorption experiments.Four nitrogen-containing compounds(NCCs)pyridine,pyrrole,q...The adsorptive denitrogenation from fuels over three metal-organic frameworks(MIL-96(Al),MIL-53(Al)and MIL-101(Cr))was studied by batch adsorption experiments.Four nitrogen-containing compounds(NCCs)pyridine,pyrrole,quinoline and indole were used as model NCCs in fuels to study the adsorption mechanism.The physicochemical properties of the adsorbents were characterized by XRD,N2physical adsorption,FT-IR spectrum and Hammett indicator method.The metal-organic frameworks(MOFs),especially the MIL-101(Cr)containing Lewis acid sites as well as high specific surface area,can adsorb large quantities of NCCs from fuels.In addition,the adsorptive capacity over MIL-101(Cr)will be different for NCCs with different basicity.The stronger basicity of the NCC is,the more it can be absorbed over MIL-101(Cr).Furthermore,pore size and shape also affect the adsorption capacity for a given adsorbate,which can be proved by the adsorption over MIL-53(Al)and MIL-96(Al).The pseudo-second-order kinetic model and Langmuir equation can be used to describe kinetics and thermodynamics of the adsorption process,respectively.Finally,the regeneration of the used adsorbent has been conducted successfully by just washing it with ethanol.展开更多
Stress corrosion cracking （SCC） of stainless steels and Ni-based alloys in high temperature water coolant is one of the key problems affecting the safe operation of nuclear power plants （NPPs）. The nitrogen-added ...Stress corrosion cracking （SCC） of stainless steels and Ni-based alloys in high temperature water coolant is one of the key problems affecting the safe operation of nuclear power plants （NPPs）. The nitrogen-added stainless steel is a kind of possible candidate materials for mitigating SCC since reducing the carbon content and adding nitrogen to offset the loss in strength caused by the decrease in carbon content can mitigate the problem of sensitization. However, the reports of SCC of nitrogen-added stainless steels in high temperature water are few available. The effects of applied potential and sensitization treatment on the SCC of a newly developed nitrogen-containing stainless steel （SS） 316LN in high temperature water doped with chloride at 250 ℃ were studied by using slow strain rate tests （SSRTs）. The SSRT results are compared with our data previously published for 316 SS without nitrogen and 304NG SS with nitrogen, and the possible mechanism affecting the SCC behaviors of the studied steels is also discussed based on SSRT and microstucture analysis results. The susceptibility to cracking of 316LN SS normally increases with increasing potential. The susceptibility to SCC of 316LN SS was less than that of 316 SS and 304NG SS. Sensitization treatment at 700℃ for 30 h showed little effect on the S CC of 316LN S S and significant effect on the S CC of 316 S S. The predominant cracking mode for the 316LN S S in both annealed state and the state after the sensitization treatment was transgranular. The presented conditions of mitigating stress corrosion cracking are some useful information for the safe use of 316LN SS in NPPs.展开更多
A new nitrogen-containing epoxy resin (XT resin) was synthesized from chain extension of xylenephenolformaldehyde resin (XPF) and triglycidyl isocyanurate (TGIC) in the presence of base catalyst. FT-IR and H-NMR ana...A new nitrogen-containing epoxy resin (XT resin) was synthesized from chain extension of xylenephenolformaldehyde resin (XPF) and triglycidyl isocyanurate (TGIC) in the presence of base catalyst. FT-IR and H-NMR analysis confirmed the chemical structure of XT resin. It was 1 cured with dicyandiamide (DICY) and diaminodiphenyl sulfone (DDS). Dynamic mechanical analysis (DMA) results showed that the introduction of triazine ring provides epoxy polymer with good thermal stability. Furthermore, high char yields at 800℃ in thermogravimetric (TGA) analysis indicated that XT resin had potential flame retardance.展开更多
Green light-emitting polyfluorenes containing 3,7-bis（4-hexylthiophen-2-yl）dibenzo[b,d]thiophene 5,5-dioxide（DHTSO）unit were synthesized.All the resulted polymers show high thermal stability with the decomposition...Green light-emitting polyfluorenes containing 3,7-bis（4-hexylthiophen-2-yl）dibenzo[b,d]thiophene 5,5-dioxide（DHTSO）unit were synthesized.All the resulted polymers show high thermal stability with the decomposition temperatures（T_d）over 420°C and the glass transition temperatures（T_g）over 75°C.The polymers exhibit the enhanced highest occupied molecular orbital（HOMO）energy levels and the depressed lowest unoccupied molecular orbital（LUMO）energy levels with the increase of DHTSO unit in polymers.The photoluminescence（PL）spectra of the polymers show positive solvatochromism in solution with the variation of solution polarities,indicating remarkable intramolecular charge transfer（ICT）effect in the polymers containing DHTSO moiety.The fluorescence quantum yields（（37）_（PL））are in the range of 34%-67%for PF-DHTSOs in film.All polymers possess two photon absorption（TPA）properties,and the TPA cross sections（？_2）are enhanced with increasing DHTSO unit in polymers.The highest？_2 is 2392 GM for PF-DHTSO15 in chloroform solution upon 740 nm excitation.The device of PF-DHTSO15 shows green emission with the Commission Internationale de L’.Eclairage（CIE）coordinates of（0.26,0.59）,and the maximum luminous efficiency（LE_（max））of 10.8 cd·A^（-1） with the configuration of ITO/PEDOT：PSS/EL/Cs F/Al.These results indicate that introducing DHTSO unit into polyfluorene backbone could be a promising molecular design strategy for TPA and effective green-light emission.展开更多
Two kinds of polyfluorenes 19earing two lateral pyrene terminated alkyl chains and two alkyl chains per repeating unit were synthesized by Suzuki polycondensation and used to disperse single-walled carbon nanotubes （...Two kinds of polyfluorenes 19earing two lateral pyrene terminated alkyl chains and two alkyl chains per repeating unit were synthesized by Suzuki polycondensation and used to disperse single-walled carbon nanotubes （SWCNT） in organic solvents. Stable polymer-SWCNT complex can be formed via the multivalent π-π stacking in＂.eraction of the lateral pyrene functional groups and the polyfluorene backbone with the outer surface of carbon nanotubes; meanwhile the lateral alkyl chains can impart good solubility to the complex. As expected, polyfluorenes bearing lateral pyrene functional groups and octyl chains exhibited much higher ,zarbon nanotube solubility in common organic solvents than the corresponding polyfluorenes bearing only octyl chains. Photophysical studies indicated that the formation ofpalymer-SWCNT complex can effectively quench the fluorescence of polyfluorenes.展开更多
The DFT-based （density fimctional theory） ab initio quantum mechanical methods have been applied to study the basicity of the nitrogen-containing compounds in petroleum. The results have indicated that there is a di...The DFT-based （density fimctional theory） ab initio quantum mechanical methods have been applied to study the basicity of the nitrogen-containing compounds in petroleum. The results have indicated that there is a distinct relationship between the protonation energy of nitrogen-containing compounds and their basicity. The more negative the protonation energy, the stronger the basicity is. It has been also found that aliphatic amines are more basic than pyridines or aromatic amines, and all these compounds are more basic than pyrroles. The addition of the aromatic rings can influence the basicity of anilines, while the 5- and 6-membered heterocyclic compounds function differently. The solvent properties may affect the basicity of these nitrogen-containing compounds.展开更多
To elucidate the effects of Fe_(2)O_(3) on nitrogen transformation during sludge pyrolysis,thermogravimetry coupled with mass spectrometry(TG-MS)was used to investigate the influences of Fe_(2)O_(3) on the pyrolysis c...To elucidate the effects of Fe_(2)O_(3) on nitrogen transformation during sludge pyrolysis,thermogravimetry coupled with mass spectrometry(TG-MS)was used to investigate the influences of Fe_(2)O_(3) on the pyrolysis characteristics and the release of important gaseous NO_(x) precursors such as HCN and NH_(3) during pyrolysis of three typical amino acids in urban sludge.The results show that after Fe_(2)O_(3) addition,the total weight loss rate of the three amino acids and the initial decomposition temperature of proline are reduced.The release amounts of NH_(3),HCN,CH_(3)CN,and HNCO from these three representative amino acids—glumatic,arginine,and proline,decrease in the order of arginine,glutamic,proline.The generation of Fe-N complexes,reduces the generation of NH_(3),HCN,CH_(3)CN,and HNCO while the catalysis effects of Fe_(2)O_(3) on the formation of H and H2 play a promoting role in the generation of NH_(3),HCN,CH_(3)CN,and HNCO.The results would provide an experimental and theoretical basis for subsequent research on the NOx precursor formation mechanisms during pyrolysis or combustion of Fe-containing sludge or sludge with additives containing Fe.展开更多
To search for more wider absorption and higher charge carriers mobilities materials of polymer solar cell, a series of soluble alternating polyfluorene copolymers were synthesized by palladium-catalyzed Suzuki couplin...To search for more wider absorption and higher charge carriers mobilities materials of polymer solar cell, a series of soluble alternating polyfluorene copolymers were synthesized by palladium-catalyzed Suzuki coupling reaction. Their structures were determined by 1H NMR, IR and UV-vis. And their UV-vis absorption spectra indicated that they had strong absorption over 600 nm spectral range and nearly cover 400-700 nm visible region. The band gaps of copolymers calculated according to cyclic voltammetry （CV） were between 1.96 and 2.03 eV. Polymer：TiO2 bulk-heterojunction films were made from mixtures of polymer and titanium isopropoxide, a precursor for TiO2, via hydrolysis in air overnight. The photoluminescence at 380-800 nm of the blend film of PT-TPP20 （5 mg/mL）：Ti（OC3H7）4 （80 μL/mL） （20% volume fraction） was significantly quenched in the 50% Ti（OC3H7）4 blend film, indicating that rapid and efficient separation of photoinduced electron-hole pairs.展开更多
Conjugated ployfluorene with 2-（2-（2-methoxyethoxy）ethoxy）ethyl groups （EO-PF） is prepared by the palladium- catalyzed Suzuki coupling reaction. The polymer is purified carefully by a simple chemical procedure. ...Conjugated ployfluorene with 2-（2-（2-methoxyethoxy）ethoxy）ethyl groups （EO-PF） is prepared by the palladium- catalyzed Suzuki coupling reaction. The polymer is purified carefully by a simple chemical procedure. The inductively coupled plasma （ICP） test shows palladium-catalyst in the polymer can be removed by this procedure. The thermal properties, electrochemical properties, UV-Vis absorption properties, photoluminescence properties and electroluminescent properties of the polymer without （EO-PF1） or with purification （EO-PF2） are studied. EO-PF2 shows better PL CIE coordinates in THF solutions as blue light-emitting materials and better photoluminescence stability in thin solid films. Polymer light emitting diodes and electrochemical cells based on EO-PF2 exhibit somewhat improved optoelectronic performance than control devices of EO-PF 1.展开更多
The density functional theory was employed to study the structures, ionization potentials（IPs）, electron affinities（EAs）, and HOMO-LUMO gaps（ΔH-L） of the oligomers. The time-dependent density functional theory...The density functional theory was employed to study the structures, ionization potentials（IPs）, electron affinities（EAs）, and HOMO-LUMO gaps（ΔH-L） of the oligomers. The time-dependent density functional theory（TD-DFT） and ZINDO were employed to study the lowest excitation energies（Egs） and the absorption and emission spectra of the oligomers of polyfluorene（PF） and poly（fluorene-co-thiophene）（PFT）. By extrapolating ΔH-L and Egs to those of infinite chain length, band gaps and effective conjugation lengths of the corresponding polymers were obtained. The IPs, EAs and 2abs of the polymers were obtained by extrapolating those of the oligomers to the inverse chain length equal to zero（I/n=0）. The outcome shows the decreased dihedral angle between fluorene and thiophene units in the PFT compared to that between fluorene units in the PF results in the increased efficient conjugation of PFT. These cause both the maximal absorption and emission wavelengths of PFT red-shifted compared with those of PF.展开更多
A block copolymer consisting of polyfluorene (PF) and polytriarylamine (PTAA) functionalized with green emitting phenoxazine moiety at the junction point of two blocks was designed and prepared for electroluminescent ...A block copolymer consisting of polyfluorene (PF) and polytriarylamine (PTAA) functionalized with green emitting phenoxazine moiety at the junction point of two blocks was designed and prepared for electroluminescent application. PF homopolymer was synthesized by Suzuki coupling polymerization, and was reacted with brominated phenoxazine. In the presence of the resulting PF functionalized with phenoxazine, C-N coupling polymerization of 4-(4’-bromophenyl)-4’’-butyldiphenylamine was carried out to afford a triblock copolymer, PTAA-phenoxazine-PF-phenoxazine-PTAA (PF-Ph-PTAA). Two types of random copolymers were also synthesized with fluorene and phenoxazine (PF2) by Suzuki coupling polymerization for comparison. All the polymers were soluble in common organic solvents and readily formed thin films by a solution processing. Prepared polymers exhibited similar UV absorption and PL emission in chloroform solutions. In a film state, the existence of phenoxazine unit drastically changed PL spectra. Although the content of phenoxazine unit in PF-Ph-PTAA was relatively high (13 mol%), it showed similar PL spectrum to that of PF2(phenoxazine content, 0.2 mol%) indicating that phenoxazine unit is isolated in single polymer chain nevertheless the high content. EL device based on PF-Ph-PTAA showed green-emission, suggesting that emission sites predominantly located in the vicinity of phenoxazine moiety because of its shallow HOMO level.展开更多
We synthesized a series of hydrazones,a novel type of nitrogen-containing prostaglandins,from different aromatic hydrazines and variant 2-substituted amino-3-hydroxy bicycle[3.2.0]hept-6-ones IV.
The inorganic-organic hybrid junction was synthesized on ITO glass substrate, which was consisted of an n-type ZnO nanorods （NRs） grown by low-temperature aqueous chemical growth method and a p-type polyfluorene （P...The inorganic-organic hybrid junction was synthesized on ITO glass substrate, which was consisted of an n-type ZnO nanorods （NRs） grown by low-temperature aqueous chemical growth method and a p-type polyfluorene （PF） organic film fabricated by spin-coating. The experimental results indicate that densely and uniformly distributed ZnO nanorods are successfully grown on the PF layer. The thickness of the PF layer plays a dominant role for the current-voltage （I-V） characteristic of the ZnO NRs/PF inorganic-organic hybrid junction device, and a p-n junction with obviously rectifying behavior is achieved with optimal PF layer thickness. The photoluminescence （PL） spectrum covering the broad visible range was obtained from the n-ZnO nanorods/p-polyfluorene （PF） structure, which was originated from the combination of the PF-related blue emission and the ZnO-related deep level emission.展开更多
基金supported by the National Natural Science Foundation of China(22168032)the National Key Research and Development Program of China(2023YFC3904302,2023YFB4103500)the Key Projects of Ning Dong Energy and Chemical Industry Base(2023NDKJXMLX022).
文摘A new adsorbent was successfully prepared by hydrothermal treatment and chemical activation through coal gasification fine slag(CGFS)and blue algae(BA)as raw materials and used for CO_(2)capture.The CO_(2)chemisorption capacity of the adsorbent was further enhanced by taking advantage of the nitrogenous bases contained in the BA.In the hydrothermal process,the addition of BA significantly increased the content of pyrrole nitrogen in the adsorbent.In the activation process,pyrrole nitrogen gradually changed into pyridine nitrogen and graphite nitrogen.Increased BA addition result in a higher specific surface area and microporosity of the adsorbent.The CO_(2)adsorption performance test proved that the CGFS-50%-CA sample has the strongest CO_(2)adsorption capacity at low temperature,up to 15.59 cm^(3)/g,which is mainly through physical adsorption,and the CGFS-10%-CA sample has the strongest CO_(2)adsorption capacity at high temperature,up to 7.31 cm^(3)/g,which is mainly through chemical adsorption.CO_(2)uptake of the CGFS-10%-CA sample was well maintained after 10 cycles,with regeneration efficiencies above 99%.The results indicate that the novel adsorbents with coexistence of physical and chemical adsorption have great potential for CO_(2)adsorption applications.
基金supported by the National Key Research and Development Program of China(No.2022YFC3701103)the National Natural Science Foundation of China(No.42222705)+1 种基金the Youth Innovation Promotion Association CAS(No.2021354)Guangdong Foundation for Program of Science and Technology Research(No.2023B1212060049).
文摘Nitrogen-containing organic compounds(NOCs)may potentially contribute to aqueous secondary organic aerosols,yet the different formation of NOCs in aerosol particles and cloud droplets remains unclear.With the in-situ measurements performed at a mountain site(1690 m a.s.l.)in southern China,we investigated the formation of NOCs in the cloud droplets and the cloud-free particles,based on their mixing state information of NOCscontaining particles by single particle mass spectrometry.The relative abundance of NOCs in the cloud-free particles was significantly higher than those in cloud residual(cloud RES)particles.NOCs were highly correlated with carbonyl compounds(including glyoxalate and methylglyoxal)in the cloud-free particles,however,limited correlation was observed for cloud RES particles.Analysis of their mixing state and temporal variations highlights that NOCs was mainly formed from the carbonyl compounds and ammonium in the cloud-free particles,rather than in the cloud RES particles.The results support that the formation of NOCs from carbonyl compounds is facilitated in concentrated solutions in wet aerosols,rather than cloud droplets.In addition,we have identified the transport of biomass burning particles that facilitate the formation of NOCs,and that the observed NOCs is most likely contributed to the light absorption.These findings have implications for the evaluation of NOCs formation and their contribution to light absorption.
基金supported by the National Key Research and Development Program of China(Nos.2022YFD1700800 and 2023YFC3905903)the Science and Technology Project of Education Department of Jiangxi Province(No.GJJ2201103)+2 种基金the Fund of Nanchang Hangkong University(Nos.EA202201110 and EA202201065)National Undergraduate Innovation and Entrepreneurship Training Program(No.202310406023)the National Natural Science Foundation of China(No.52470149)。
文摘Covalent organic frameworks(COFs)are crystalline porous polymeric materials composed of organic monomers connected by strong covalent bonds and offer high stability,good crystallinity,a large specific surface area,and controllable structures.COFs are widely used in the fields of adsorption and separation,catalysis,photovoltaics,and drug-delivery.The structural regulation and performance optimization of COFs can be realized through the modification of ligands and the selection of linkage methods.In which,the types of linkage are closely related to the stability and performance of COFs.In this review,nitrogencontaining linkage-bonds(NCLBs)in COFs are divided into N-containing double bonds,N-containing conjugated rings and N-containing unconjugated rings.The association between structure and performance of COFs is elaborated and the synthesis methods of COFs are systematically summarized.Moreover,the structural design,theoretical prediction and machinable application of COFs are prospected.
基金support of National Natural Science Foundation of P.R.China(22308104).
文摘The influence of nitrogen-containing polycyclic aromatic hydrocarbons(NC-PAH)on the formation of carbonaceous mesophase remains enigmatic,despite extensive research on the production of carbonaceous materials from aromatic-rich oils.Molecular dynamics simulation was used to investigate the variations in pyrolysis behavior between PAH and NC-PAH based on the composition analysis.Through adjusting the content of NC-PAH,the influence of NC-PAH on the thermal stability of slurry oils(SOs)was evaluated by thermogravimetry,viscosity,coke value,and quinoline insoluble(QI).The morphology and structure of mesocarbon microbeads(MCMBs)prepared with SOs were measured by a polarized-light microscope,SEM,XRD,and Raman.Simulation results indicate that NC-PAH possesses much higher reactivity and tends to produce highly condensed solid and coke products.It corresponds to the QI and high viscosity in thermal stability experiments.Therefore,high concentrations of NC-PAH result in nonuniform morphology and disordered structures.In a system with low viscosity and few QIs,SO,which has a low nitrogen content(475 ppm),reacts gently to produce MCMBs with a uniform particle size(10-40μm)and an excellent spherical shape.As NC-PAH content decreases,the crystalline size of graphitization elevates,as evidenced by parallel layers(10.472-11.764)and stack height(3.269-3.701 nm).The graphitization degree becomes worse and nonuniform with the increase of the content of NC-PAH,and the best is 20.58%evaluated by Raman spectra area ratio(AG/Aall).Overall,this work suggests a nitrogen content reference and a controlling technology of nitrogen for the preparation of superior MCMB.
基金Project supported by the Pilot Project of Knowledge Innovation Program of Chinese Academy of Sciences (No. KZCX2-YW-G-009)the National Natural Science Foundation of China (No. 20577067, 30230010).
文摘Many nitrogen-containing aromatic compounds （NACs）, such as nitrobenzene （NB）, 4-nitrophenol （4-NP）, aniline （AN）, and 2,4-dinitrophenol （2,4-DNP）, are environmentally hazardous, and their removal from contaminated water is one of the main challenges facing wastewater treatment plants. In this study, synthetic wastewater containing NB, 4-NP, 2,4-DNP, and AN at concentrations ranging from 50 to 180 mg/L was fed into a sequencing batch reactor （SBR）. Analyses of the SBR system indicated that it simultaneously removed more than 99% of the NACs at loading rates of 0.36 kg NB/（m^3·d）, 0.3 kg 4-NP/（m^3·d）, 0.25 kg AN/（m^3·d）, and 0.1 kg 2,4-DNP/（m^3·d）. Bacterial groups of Bacteriodetes, Candidate division TM7, α-Proteobacteria, and β-Proteobacteria were dominant in the clone libraries of 16S rRNA genes retrieved from the microbial communities in the SBR system. ＂Cycle tests＂ designed to alter feeding and aeration parameters of the SBR system demonstrated that the resident microbial biome of the SBR system responded rapidly to changing conditions. Consumption of O2 was concomitant with the apparent mineralization of NACs. Aromatic ring-cleaving dioxygenase activities suggested that （1） AN and NB were degraded via catechol 2,3-dioxygenase; （2） 4-NP was degraded via 1,2,4-benzentriol 1,2-dioxygenase; and （3） 2,4-DNP was degraded via an unresolved pathway.
基金Supported by the Key Project of Joint Fund from National Natural Science Foundation of China and the Government of Xinjiang Uygur Autonomous Region(U1503293)the National Key Research and Development Program of China(2018YFB0604602)the Priority Academic Program Development of Jiangsu Higher Education Institutions.
文摘Soluble portions(SPs) 1-4(SP1-SP4) were afforded from sequentially dissolution and alkanolyses of Baiyinhua lignite(BL) in cyclohexane,CH3OH,CH3CH2OH,and(CH3)2CHOH at 300℃.They were analyzed with a gas chromatograph/mass spectrometer and quadrupole exactive orbitrap mass spectrometer(QEOTMS) with an atmosphere pressure chemical ionization source in positive-ion mode,while BL was characterized with an X-ray photoelectron spectrometer(XRPES).The results show that the yields of SP2 and SP3 are much higher than those of SP1 and SP4,and the total SP yield is ca.39.0%.According to the analysis with XRPES,pyrrolic nitrogen atoms are the most abundant nitrogen existing forms in BL.Thousands of nitrogen-containing aromatics(NCAs) were resolved with QEOTMS and their molecular masses are mainly in the range of 200-450 u.The main NCAs are N1O1 and N1O2 class species with double bond equivalent values of 4-18 and carbon numbers of 7-30.The nitrogen atoms appear in pyridine s,quinolines,benzoquinolines or acridine,and dibenzoquinolines or naphthoquinolines,while the oxygen atoms exist in methoxy and furan rings.
基金supported by the National Natural Science Foundation of China(Nos.31970107 and 51508068)the Fundamental Research Funds for the Central Universities(No.DUT19JC17)the Open Project of State Key Laboratory of Urban Water Resource and Environment,Harbin Institute of Technology(No.QAK201943)。
文摘Nitrogen-containing organic pollutants(quinoline,pyridine and indole)are widely distributed in coking wastewater,and bioaugmentation with specific microorganisms may enhance the removal of these recalcitrant pollutants.The bioaugmented system(group B)was constructed through inoculation of two aromatics-degrading bacteria,Comamonas sp.Z1(quinoline degrader)and Acinetobacter sp.JW(indole degrader),into the activated sludge for treatment of quinoline,indole and pyridine,and the non-bioaugmented activated sludge was used as the control(group C).Both groups maintained high efficiencies(>94%)for removal of nitrogen-containing organic pollutants and chemical oxygen demand(COD)during the long-term operation,and group B was highly effective at the starting period and the operation stage fed with raw wastewater.High-throughput sequencing analysis indicated that nitrogen-containing organic pollutants could shape the microbial community structure,and communities of bioaugmented group B were clearly separated from those of non-bioaugmented group C as observed in non-metric multidimensional scaling(NMDS)plot.Although the inoculants did not remain their dominance in group B,bioaugmentation could induce the formation of effective microbial community,and the indigenous microbes might play the key role in removal of nitrogen-containing organic pollutants,including Dokdonella,Comamonas and Pseudoxanthomonas.Phylogenetic Investigation of Communities by Reconstruction of Unobserved States(PICRUSt)analysis suggested that bioaugmentation could facilitate the enrichment of functional genes related to xenobiotics biodegradation and metabolism,probably leading to the improved performance in group B.This study indicated that bioaugmentation could promote the removal of nitrogen-containing organic pollutants,which should be an effective strategy for wastewater treatment.
基金supported by the Program for New Century Excellent Talents in University (NCET-04-0270)National Basic Research Program of China (2011CB201301)
文摘The adsorptive denitrogenation from fuels over three metal-organic frameworks(MIL-96(Al),MIL-53(Al)and MIL-101(Cr))was studied by batch adsorption experiments.Four nitrogen-containing compounds(NCCs)pyridine,pyrrole,quinoline and indole were used as model NCCs in fuels to study the adsorption mechanism.The physicochemical properties of the adsorbents were characterized by XRD,N2physical adsorption,FT-IR spectrum and Hammett indicator method.The metal-organic frameworks(MOFs),especially the MIL-101(Cr)containing Lewis acid sites as well as high specific surface area,can adsorb large quantities of NCCs from fuels.In addition,the adsorptive capacity over MIL-101(Cr)will be different for NCCs with different basicity.The stronger basicity of the NCC is,the more it can be absorbed over MIL-101(Cr).Furthermore,pore size and shape also affect the adsorption capacity for a given adsorbate,which can be proved by the adsorption over MIL-53(Al)and MIL-96(Al).The pseudo-second-order kinetic model and Langmuir equation can be used to describe kinetics and thermodynamics of the adsorption process,respectively.Finally,the regeneration of the used adsorbent has been conducted successfully by just washing it with ethanol.
基金supported by National Basic Research Program of China (973 Program, Grant No. 2006CB605005)Shanghai Municipal Committee of Science and Technology of china(Grant No. 005207019,Grant No. 08520708000)
文摘Stress corrosion cracking （SCC） of stainless steels and Ni-based alloys in high temperature water coolant is one of the key problems affecting the safe operation of nuclear power plants （NPPs）. The nitrogen-added stainless steel is a kind of possible candidate materials for mitigating SCC since reducing the carbon content and adding nitrogen to offset the loss in strength caused by the decrease in carbon content can mitigate the problem of sensitization. However, the reports of SCC of nitrogen-added stainless steels in high temperature water are few available. The effects of applied potential and sensitization treatment on the SCC of a newly developed nitrogen-containing stainless steel （SS） 316LN in high temperature water doped with chloride at 250 ℃ were studied by using slow strain rate tests （SSRTs）. The SSRT results are compared with our data previously published for 316 SS without nitrogen and 304NG SS with nitrogen, and the possible mechanism affecting the SCC behaviors of the studied steels is also discussed based on SSRT and microstucture analysis results. The susceptibility to cracking of 316LN SS normally increases with increasing potential. The susceptibility to SCC of 316LN SS was less than that of 316 SS and 304NG SS. Sensitization treatment at 700℃ for 30 h showed little effect on the S CC of 316LN S S and significant effect on the S CC of 316 S S. The predominant cracking mode for the 316LN S S in both annealed state and the state after the sensitization treatment was transgranular. The presented conditions of mitigating stress corrosion cracking are some useful information for the safe use of 316LN SS in NPPs.
文摘A new nitrogen-containing epoxy resin (XT resin) was synthesized from chain extension of xylenephenolformaldehyde resin (XPF) and triglycidyl isocyanurate (TGIC) in the presence of base catalyst. FT-IR and H-NMR analysis confirmed the chemical structure of XT resin. It was 1 cured with dicyandiamide (DICY) and diaminodiphenyl sulfone (DDS). Dynamic mechanical analysis (DMA) results showed that the introduction of triazine ring provides epoxy polymer with good thermal stability. Furthermore, high char yields at 800℃ in thermogravimetric (TGA) analysis indicated that XT resin had potential flame retardance.
文摘Green light-emitting polyfluorenes containing 3,7-bis（4-hexylthiophen-2-yl）dibenzo[b,d]thiophene 5,5-dioxide（DHTSO）unit were synthesized.All the resulted polymers show high thermal stability with the decomposition temperatures（T_d）over 420°C and the glass transition temperatures（T_g）over 75°C.The polymers exhibit the enhanced highest occupied molecular orbital（HOMO）energy levels and the depressed lowest unoccupied molecular orbital（LUMO）energy levels with the increase of DHTSO unit in polymers.The photoluminescence（PL）spectra of the polymers show positive solvatochromism in solution with the variation of solution polarities,indicating remarkable intramolecular charge transfer（ICT）effect in the polymers containing DHTSO moiety.The fluorescence quantum yields（（37）_（PL））are in the range of 34%-67%for PF-DHTSOs in film.All polymers possess two photon absorption（TPA）properties,and the TPA cross sections（？_2）are enhanced with increasing DHTSO unit in polymers.The highest？_2 is 2392 GM for PF-DHTSO15 in chloroform solution upon 740 nm excitation.The device of PF-DHTSO15 shows green emission with the Commission Internationale de L’.Eclairage（CIE）coordinates of（0.26,0.59）,and the maximum luminous efficiency（LE_（max））of 10.8 cd·A^（-1） with the configuration of ITO/PEDOT：PSS/EL/Cs F/Al.These results indicate that introducing DHTSO unit into polyfluorene backbone could be a promising molecular design strategy for TPA and effective green-light emission.
基金financially supported by the NSF of China(Nos.20834006 and 50821062)the National Basic Research Program of China(973 Program:2009CB623601)
文摘Two kinds of polyfluorenes 19earing two lateral pyrene terminated alkyl chains and two alkyl chains per repeating unit were synthesized by Suzuki polycondensation and used to disperse single-walled carbon nanotubes （SWCNT） in organic solvents. Stable polymer-SWCNT complex can be formed via the multivalent π-π stacking in＂.eraction of the lateral pyrene functional groups and the polyfluorene backbone with the outer surface of carbon nanotubes; meanwhile the lateral alkyl chains can impart good solubility to the complex. As expected, polyfluorenes bearing lateral pyrene functional groups and octyl chains exhibited much higher ,zarbon nanotube solubility in common organic solvents than the corresponding polyfluorenes bearing only octyl chains. Photophysical studies indicated that the formation ofpalymer-SWCNT complex can effectively quench the fluorescence of polyfluorenes.
基金supported by the"973"project envisaged in the State Key Basic R&D Program(2006CB202505).
文摘The DFT-based （density fimctional theory） ab initio quantum mechanical methods have been applied to study the basicity of the nitrogen-containing compounds in petroleum. The results have indicated that there is a distinct relationship between the protonation energy of nitrogen-containing compounds and their basicity. The more negative the protonation energy, the stronger the basicity is. It has been also found that aliphatic amines are more basic than pyridines or aromatic amines, and all these compounds are more basic than pyrroles. The addition of the aromatic rings can influence the basicity of anilines, while the 5- and 6-membered heterocyclic compounds function differently. The solvent properties may affect the basicity of these nitrogen-containing compounds.
文摘To elucidate the effects of Fe_(2)O_(3) on nitrogen transformation during sludge pyrolysis,thermogravimetry coupled with mass spectrometry(TG-MS)was used to investigate the influences of Fe_(2)O_(3) on the pyrolysis characteristics and the release of important gaseous NO_(x) precursors such as HCN and NH_(3) during pyrolysis of three typical amino acids in urban sludge.The results show that after Fe_(2)O_(3) addition,the total weight loss rate of the three amino acids and the initial decomposition temperature of proline are reduced.The release amounts of NH_(3),HCN,CH_(3)CN,and HNCO from these three representative amino acids—glumatic,arginine,and proline,decrease in the order of arginine,glutamic,proline.The generation of Fe-N complexes,reduces the generation of NH_(3),HCN,CH_(3)CN,and HNCO while the catalysis effects of Fe_(2)O_(3) on the formation of H and H2 play a promoting role in the generation of NH_(3),HCN,CH_(3)CN,and HNCO.The results would provide an experimental and theoretical basis for subsequent research on the NOx precursor formation mechanisms during pyrolysis or combustion of Fe-containing sludge or sludge with additives containing Fe.
文摘To search for more wider absorption and higher charge carriers mobilities materials of polymer solar cell, a series of soluble alternating polyfluorene copolymers were synthesized by palladium-catalyzed Suzuki coupling reaction. Their structures were determined by 1H NMR, IR and UV-vis. And their UV-vis absorption spectra indicated that they had strong absorption over 600 nm spectral range and nearly cover 400-700 nm visible region. The band gaps of copolymers calculated according to cyclic voltammetry （CV） were between 1.96 and 2.03 eV. Polymer：TiO2 bulk-heterojunction films were made from mixtures of polymer and titanium isopropoxide, a precursor for TiO2, via hydrolysis in air overnight. The photoluminescence at 380-800 nm of the blend film of PT-TPP20 （5 mg/mL）：Ti（OC3H7）4 （80 μL/mL） （20% volume fraction） was significantly quenched in the 50% Ti（OC3H7）4 blend film, indicating that rapid and efficient separation of photoinduced electron-hole pairs.
基金supported by the National Natural Science Foundation of China(No.50903078)Specialized Research Fund for the Doctoral Program of Higher Education(New Teachers)(No.20090132120017)+1 种基金Promotive research fund for excellent young and middle-aged scientisits of Shandong Province(No.BS2009CL036)the Fundamental Research Funds for the Central Universities(No.201113045)
文摘Conjugated ployfluorene with 2-（2-（2-methoxyethoxy）ethoxy）ethyl groups （EO-PF） is prepared by the palladium- catalyzed Suzuki coupling reaction. The polymer is purified carefully by a simple chemical procedure. The inductively coupled plasma （ICP） test shows palladium-catalyst in the polymer can be removed by this procedure. The thermal properties, electrochemical properties, UV-Vis absorption properties, photoluminescence properties and electroluminescent properties of the polymer without （EO-PF1） or with purification （EO-PF2） are studied. EO-PF2 shows better PL CIE coordinates in THF solutions as blue light-emitting materials and better photoluminescence stability in thin solid films. Polymer light emitting diodes and electrochemical cells based on EO-PF2 exhibit somewhat improved optoelectronic performance than control devices of EO-PF 1.
基金Supported by the State Basic Research Development Program of China(No.2002CB613406)the National Natural Science Foundation of China(No.20673045)the Open Project of State Key Laboratory of Superamolecular Structure and Materials of Jilin University(No.SKLSSM200716)
文摘The density functional theory was employed to study the structures, ionization potentials（IPs）, electron affinities（EAs）, and HOMO-LUMO gaps（ΔH-L） of the oligomers. The time-dependent density functional theory（TD-DFT） and ZINDO were employed to study the lowest excitation energies（Egs） and the absorption and emission spectra of the oligomers of polyfluorene（PF） and poly（fluorene-co-thiophene）（PFT）. By extrapolating ΔH-L and Egs to those of infinite chain length, band gaps and effective conjugation lengths of the corresponding polymers were obtained. The IPs, EAs and 2abs of the polymers were obtained by extrapolating those of the oligomers to the inverse chain length equal to zero（I/n=0）. The outcome shows the decreased dihedral angle between fluorene and thiophene units in the PFT compared to that between fluorene units in the PF results in the increased efficient conjugation of PFT. These cause both the maximal absorption and emission wavelengths of PFT red-shifted compared with those of PF.
文摘A block copolymer consisting of polyfluorene (PF) and polytriarylamine (PTAA) functionalized with green emitting phenoxazine moiety at the junction point of two blocks was designed and prepared for electroluminescent application. PF homopolymer was synthesized by Suzuki coupling polymerization, and was reacted with brominated phenoxazine. In the presence of the resulting PF functionalized with phenoxazine, C-N coupling polymerization of 4-(4’-bromophenyl)-4’’-butyldiphenylamine was carried out to afford a triblock copolymer, PTAA-phenoxazine-PF-phenoxazine-PTAA (PF-Ph-PTAA). Two types of random copolymers were also synthesized with fluorene and phenoxazine (PF2) by Suzuki coupling polymerization for comparison. All the polymers were soluble in common organic solvents and readily formed thin films by a solution processing. Prepared polymers exhibited similar UV absorption and PL emission in chloroform solutions. In a film state, the existence of phenoxazine unit drastically changed PL spectra. Although the content of phenoxazine unit in PF-Ph-PTAA was relatively high (13 mol%), it showed similar PL spectrum to that of PF2(phenoxazine content, 0.2 mol%) indicating that phenoxazine unit is isolated in single polymer chain nevertheless the high content. EL device based on PF-Ph-PTAA showed green-emission, suggesting that emission sites predominantly located in the vicinity of phenoxazine moiety because of its shallow HOMO level.
基金Project(39470824)was supported by the National Natural Science Foundation of China.
文摘We synthesized a series of hydrazones,a novel type of nitrogen-containing prostaglandins,from different aromatic hydrazines and variant 2-substituted amino-3-hydroxy bicycle[3.2.0]hept-6-ones IV.
基金Funded by the National Natural Science Foundation of China (Nos.10804014,11004092,60807009)the Fundamental Research Funds for the Central Universities (No.DUT10LK01)
文摘The inorganic-organic hybrid junction was synthesized on ITO glass substrate, which was consisted of an n-type ZnO nanorods （NRs） grown by low-temperature aqueous chemical growth method and a p-type polyfluorene （PF） organic film fabricated by spin-coating. The experimental results indicate that densely and uniformly distributed ZnO nanorods are successfully grown on the PF layer. The thickness of the PF layer plays a dominant role for the current-voltage （I-V） characteristic of the ZnO NRs/PF inorganic-organic hybrid junction device, and a p-n junction with obviously rectifying behavior is achieved with optimal PF layer thickness. The photoluminescence （PL） spectrum covering the broad visible range was obtained from the n-ZnO nanorods/p-polyfluorene （PF） structure, which was originated from the combination of the PF-related blue emission and the ZnO-related deep level emission.
