During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure o...During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure of phytoplankton community,resulting in algal blooms and seriously threatening the ecological security of the reservoir.It is of great significance to understand the continuous changes of phytoplankton in the initial impoundment period for the protection of reservoir water quality.Therefore,a two-year in-situ monitoring study was conducted on water quality and phytoplankton in a representative canyonshaped reservoir named Sanhekou and the interannual changes of phytoplankton community and its response to environmental changes during the initial impoundment period were discussed at taxonomic versus functional classification levels.The results showed that the total nitrogen and permanganate index levels were relatively high in the first year due to rapid water storage and heavy rainfall input,and the more stable hydrological conditions in the second year promoted the increase of algae density and the transformation of community,and the proportion of cyanobacteria increased significantly.The succession order of phytoplankton in the first year of the initial impoundment periodwas Chlorophyta-Bacillariophyta-Chlorophyta,or J/F/X1-P/MP/W1-A/X1/MP,respectively.And the succession order in the second year was Cyanobacteria/Chlorophyta-Bacillariophyta-Chlorophyta,or L_(M)/G/P-P/A/X1-X1/J/G.Water temperature,relativewater column stability,mixing depth,and pHwere crucial factors affecting phytoplankton community succession.This study revealed the interannual succession law and driving factors of phytoplankton in the initial impoundment period and provided an important reference for the operation management and ecological protection of canyon-shaped reservoirs.展开更多
As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC...As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC)were synthesized as CDI electrode material for removing Na^(+)and Cl^(−)in salty water.Results showed that the average diameter of HC was approximately 180 nm,and the infrared spectrum showed that its surface was successfully modified with sulfonic and amino groups,respectively.The sulfonic acid functionalized HC(HC-S)showed better electrochemical and desalting performance than the amino-functionalized HC(HC–N),with a maximum Faradic capacity of 287.4 F/g and an adsorptive capacity of 112.97 mg/g for NaCl.Additionally,92.63%capacity retention after 100 adsorption/desorption cycles demonstrates the excellent stability of HC-S.The main findings prove that HC-S is viable as an electrodematerial for desalination by high-performance CDI applications.展开更多
Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional g...Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional groups of different types and occurrences of organic matter.Combined with the quantitative evaluation of pore development via scanning electron microscopy(SEM),the response of organic pore formation and evolution mechanisms to chemical composition and structural evolution of organic matter in overmature marine shale is investigated.The results indicate that the AFM-IR spectra of graptolite periderms and pyrobitumen in shale are dominated by the stretching vibrations of conjugated C=C bonds in aromatic compounds at approximately 1600 cm-1,with weak absorption peaks near 1375,1450 and 1720 cm-1,corresponding to aliphatic chains and carbonyl/carboxyl functional groups.Overall,the AFM-IR structural indices(A and C factors)of organic matter show a strong correlation with visible porosity in shales of equivalent maturity.Lower A and C factor values correlate with enhanced development of organic pores,which is associated with the detachment of more aliphatic chains and oxygen-containing functional groups during thermal evolution.Pyrobitumen-clay mineral composites generally exhibit superior pore development,likely attributable to clay mineral dehydration participating in hydrocarbon generation reactions that promote the removal of more functional groups.Additionally,hydrocarbon generation within organic-clay composites during high-over mature stages may induce volumetric expansion,resulting in microfracturing and hydrocarbon expulsion.The associated higher hydrocarbon expulsion rates promote the formation of larger pores and fracture-shaped pores along the flake-shaped clay minerals.This study highlights that the research of submicron-scale molecular functional groups provides a deeper understanding of organic matter evolution and pores development mechanisms in overmature shales,thereby offering critical theoretical parameters for reservoir evaluation in shale oil and gas exploration.展开更多
To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation betwe...To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.展开更多
Anthropogenic disturbances are widespread in tropical forests and influence the species composition in the overstory.However,the impacts of historical disturbance on tropical forest overstory recovery are unclear due ...Anthropogenic disturbances are widespread in tropical forests and influence the species composition in the overstory.However,the impacts of historical disturbance on tropical forest overstory recovery are unclear due to a lack of disturbance data,and previous studies have focused on understory species.In this study,the purpose was to deter-mine the influence of historical disturbance on the diver-sity,composition and regeneration of overstory species in present forests.In the 20-ha Xishuangbanna tropical sea-sonal rainforest dynamics plot in southwestern China,the historical disturbance boundaries were delineated based on panchromatic photographs from 1965.Factors that drove species clustering in the overstory layer(DBH≥40 cm)were analyzed and the abundance,richness and composition of these species were compared among different tree groups based on multiple regression tree analysis.The coefficient of variation of the brightness value in historical panchro-matic photographs from 1965 was the primary driver of spe-cies clustering in the overstory layer.The abundance and richness of overstory species throughout the regeneration process were similar,but species composition was always different.Although the proportion of large-seeded and vigorous-sprouting species showed no significant differ-ence between disturbed and undisturbed forests in the tree-let layer(DBH<20 cm),the difference became significant when DBH increased.The findings highlight that historical disturbances have strong legacy effects on functional group composition in the overstory and the recovery of overstory species was multidimensional.Functional group composi-tion can better indicate the dynamics of overstory species replacement during secondary succession.展开更多
To understand the distribution of phytoplankton functional groups(PFGs)and key factors on their compositions in different watersheds of the Huanghe(Yellow)River basin,25 river sites and 25 lake-reservoirs sites were s...To understand the distribution of phytoplankton functional groups(PFGs)and key factors on their compositions in different watersheds of the Huanghe(Yellow)River basin,25 river sites and 25 lake-reservoirs sites were selected.The contents of nephelometric turbidity(NTU),total nitrogen(TN),and total phosphorus(TP)were significantly higher in rivers than that in lakes or reservoirs,whereas the pH and CODMn(chemical oxygen demand or potassium permanganate index)were lower.Results show that,27 PFGs,namely,assemblages A,B,C,D,E,F,G,H,J,K,LM,Lo,M,MP,N,P,S1,S2,T,TC,W1,W2,X1,X2,X3,XPh,and Y,were identified.Additionally,ANOSIM correlation analysis demonstrated significant differences in PFG composition between the riverine and lake-reservoir sections in the Huanghe River basin.In the riverine watersheds,the group MP was dominant,while assemblages B and J were prevalent in lakes and reservoirs.The Mantel correlation tests and RDA analysis showed that environmental variables,such as NTU,water temperature(WT),conductivity(Cond),and TP,were key driving factors of shaping the dominant PFGs of the study area.Using the Venn diagram based on variation partitioning analysis,PFGs were mainly influenced by WT and TP in lake-reservoir sites,while in the river sites were affected mainly by geo-climatic variables.This study helps understanding the PFGs in river ecosystems,and unraveling the key driving factors in different watersheds,which shall be important for the protection and management of entire Huanghe River basin.展开更多
Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary...Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area(SSA),pore volume/size,and surface functional groups(SFGs).The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported.However,the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine.To address in this gap in the literature,this review introduces a new perspective on the adsorption mechanisms of aromatics.Through collecting previously-reported results,the parameters log P(logarithm of the Kow),polar surface area,and the positive/negative charges were carefully calculated using Chem Draw3D,which allowed the hydrophobicity/hydrophilicity properties,electron donor-acceptor interactions,Hbonding,and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively.These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights,chemical structures,and polarities of the target aromatics.Overall,this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates,which may provide useful guidance for the preparing of highly-efficient,functional BCs for the adsorption of aromatics.展开更多
The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and a...The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption isotherms.The morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration method.Cr（VI） removal by the activated carbons from aqueous solution was investigated at different pH values.The results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated carbon.The pH value of the solution plays a key role in the Cr（VI） removal.The ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional groups.At higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated carbons.At lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.展开更多
Variations in the fractions of biomass allocated to functional components are widely considered as plant responses to resource availability for grassland plants. Observations indicated shoots isometrically relates to ...Variations in the fractions of biomass allocated to functional components are widely considered as plant responses to resource availability for grassland plants. Observations indicated shoots isometrically relates to roots at the community level but allometrically at the species level in Tibetan alpine grasslands. These differences may result from the specific complementarity of functional groups between functional components, such as leaf, root, stem and reproductive organ. To test the component complementary responses to regional moisture variation, we conducted a multi-site transect survey to measure plant individual size and component biomass fractions of common species belonging to the functional groups： forbs, grasses, legumes and sedges on the Northern Tibetan Plateau in peak growing season in 2010. Along the mean annual precipitation （MAP） gradient, we sampled 7o species, in which 2o are in alpine meadows, 20 in alpine steppes, 15 in alpine desert-steppes and 15 in alpine deserts, respectively. Our results showed that the size of alpine plants is small with individual biomass mostly lower than 1.0 g. Plants keep relative conservative component individual responses moisture functional fractions across alpine grasslands at the level. However, the complementary between functional components to variations specifically differ among groups. These results indicate that functional group diversity may be an effective tool for scaling biomass allocation patterns from individual up to community level. Therefore, it is necessary andvaluable to perform intensive and systematic studies on identification and differentiation the influences of compositional changes in functional groups on ecosystem primary services and processes.展开更多
Reservoirs are an important water source in many densely populated areas in southwest China.Phytoplankton play an essential role in maintaining the structure and function of reservoir ecosystems.Understanding the succ...Reservoirs are an important water source in many densely populated areas in southwest China.Phytoplankton play an essential role in maintaining the structure and function of reservoir ecosystems.Understanding the succession in phytoplankton communities and the factors driving it are essential for eff ective water quality management in drinking water reservoirs.In this study,water samples were collected monthly at the surface layers from March 2016 to December 2019 in Hongfeng Reservoir,southwest China.The relationship between functional group succession was analyzed based on nonmetric multidimensional scaling analysis(NMDS),redundancy analysis(RDA),succession rate,and other analysis methods.The results showed distinct shifts in the community structure of phytoplankton functional groups within study period.The Cyclotella sp.was dominant in 2016 and 2017,and Pseudanabaena limnetica was the dominant group in 2018 and 2019.It appears that the phytoplankton composition and biomass are closely related to the water temperature and nutrient status in this reservoir.The results clearly showed that the permanganate index(COD_(Mn))was the key factor of dramatic phytoplankton functional group succession,and the change in succession rates was closely caused by total nitrogen concentration(TN).Therefore,the succession pattern and key factors of Hongfeng Reservoir revealed in this study were important guidance for the management of drinking water reservoirs in southwest China.A reasonable limit on exogenous nutrient input should be a priority,especially in high water temperature period.展开更多
The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) i...The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) ion adsorption onto AC-T.The modified activated carbon is characterized by scanning electron microscopy,Fourier transform infrared spectroscopy(FT-IR) and X-ray photoelectron spectroscopy(XPS).The results of batch experiments indicate that the maximal adsorption could be achieved over the broad pH range of 4.5 to 6.5.Adsorption isotherms and kinetic study suggest that the sorption of Cd(Ⅱ) onto AC-T produces monolayer coverage and that adsorption is controlled by chemical adsorption.And the adsorbent has a good reusability.According to the FT-IR and XPS analyses,electrostatic attraction and cation exchange between Cd(Ⅱ) and oxygen-containing functional groups on AC-T are dominant mechanisms for Cd(Ⅱ) adsorption.展开更多
The relationship between trace elements in coal and organic functional groups of coal, also some of aromatic structure, was investigated by using curve fitting of infrared spectra. Cluster analysis was also performed ...The relationship between trace elements in coal and organic functional groups of coal, also some of aromatic structure, was investigated by using curve fitting of infrared spectra. Cluster analysis was also performed according to the degree of affinity of organic groups to the trace elements. The results show that there is a possibility that trace elements, especially LREE, were bound to peripheral organic functional groups of middle rank coal macromolecule. The most possible functional group that binds trace element is the hydroxyl, and to the less degree, the asymmetric -CH3 and 〉CH2 stretching, -CH3 stretching, etc. The degree of affinity of trace elements to different functional groups varies. The tendency obeys the natural structural changing law of trace elements-- the periodic law. The deviation of some trace elements from this regular trend is attributed to the deviation of intrinsic ＂confusion degree＂ （conventional molar entropy） of the matter system of coal basin, which is affected by the inner and outer factors during the evolution.展开更多
Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were ...Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were prepared by using the fresh urea and the urea kept for five years,respectively,for the first time.Experimental results show that the H2 production rate of the C-GCN is 39.06μmol/h,which is about 5 times of the Y-GCN.Meantime,in terms of apparent quantum efficiency(AQ.E)at 420 nm,C-GCN has a value of 6.3%and nearly 7.3 times higher than that of Y-GCN(0.86%).The results of XRD,IR,DRS,and NMR show,different from Y-GCN,a new kind of functional group of—N=CH—was firstly in-situ introduced into the C-GCN,resulting in good visible light absorption,and then markedly improving the photocatalytic performance.DFT calculation also confirms the effect of the—N=CH—group band structure of g-C3N4.Furthermore,XPS results demonstrate that the existence of—N=CH—groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles,and then improves the charge separation and photocatalytic performance.The present work demonstrates a good example of"defect engineering"to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.展开更多
In order to explore the influence of modification sites of functional groups on landfill gas （CO2/CH4） separation performance of metal-organic frameworks （MOFs）, six types of or- ganic linkers and three types of f...In order to explore the influence of modification sites of functional groups on landfill gas （CO2/CH4） separation performance of metal-organic frameworks （MOFs）, six types of or- ganic linkers and three types of functional groups （i.e. -F, -NH2, -CH3） were used to construct 36 MOFs of pcu topology based on copper paddlewheel. Grand canonical Monte Carlo sim- ulations were performed in this work to evaluate the separation performance of MOFs at low （vacuum swing adsorption） and high （pressure swing adsorption） pressures, respectively. Simulation results demonstrated that CO2 working capacity of the unfunctionalized MOFs generally exhibits pore-size dependence at 1 bar, which increases with the decrease in pore sizes. It was also found that -NH2 funetionalized MOFs exhibit the highest CO2 uptake due to the enhanced Coulombic interactions between the polar -NH2 groups and the quadrupole moment of CO2 molecules, which is followed by -CH3 and -F functionalized ones. Moreover, positioning the functional groups -NH2 and -CH3 at sites far from the metal node （site b） exhibits more significant enhancement on CO2/CH4 separation performance compared to that adjacent to the metal node （site a）.展开更多
MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their p...MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries.In this work,a robust strategy is developed to control the functional groups of Nb_2 CT_x MXene.The capacity of pristine Nb_2 CT_x MXene can be significantly increased by Li~+ intercalation and surface modification.The specific capacity of the treated Nb_2 CT_x is up to 448 mAh g^(-1) at 0.05 A g^(-1),and at a large current density of 2 A g^(-1) remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles.These values exceed most of the reported pristine MXenes(including the most studied Ti_3 C_2 T_x) and carbon-based materials.It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene,and the results enhance the promise of MXenes in the application of lithium-ion batteries.展开更多
In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for ...In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.展开更多
Correlations among free radicals, apparent activation energy, and functional groups during lowtemperature oxidation of Jurassic coal in Northern Shaanxi were investigated by examining three coal samples collected from...Correlations among free radicals, apparent activation energy, and functional groups during lowtemperature oxidation of Jurassic coal in Northern Shaanxi were investigated by examining three coal samples collected from the Ningtiaota, Jianxin, and Shigetai coal mines. Free radical concentrations at less than 120 ℃ were investigated by electron spin resonance experiments while the thermogravimetric experiments were conducted to analyze apparent activation energies. In addition, Fourier transform infrared spectroscopy was employed to study the spectrum of functional groups generated in coal. The results indicated that, in decreasing order, the apparent activation energies were Shigetai 〉Jianxin 〉 Ningtiaota, indicating that, from 50 to 120 ℃, the Ningtiaota coal sample most easily absorbed and reacted with oxygen while the most resistant was the Shigetai coal sample. Free radical concentrations and line heights increased with increased temperature, and the line width and Lande factor showed irregular fluctuations. Functional group variations were different among these coals, and the phenol and alcohol-associated OHs, carboxyls, and aromatic ring double bonds might have had a major impact on free radical concentrations. These results were meaningful for better consideration and management of coal oxidation at low temperatures.展开更多
A series of new chelating resins with incorporating heterocyclic functional groups： pyridine, thiadizole, benzothizole into macroporous chloromethylated polystyrene were synthesized via hydrophilic spacer arm of poly...A series of new chelating resins with incorporating heterocyclic functional groups： pyridine, thiadizole, benzothizole into macroporous chloromethylated polystyrene were synthesized via hydrophilic spacer arm of polyethylene glycol containing sulfur. These chelating resins were found to show high adsorption capacities for Ag^＋, Hg^2＋, Au^3＋ and Pd^2＋, and the presence of spacer arm can enhance adsorption ability due to increase the hydrophilicity of the chelating resins.展开更多
The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters(DPFs).This work focused on the changes in the surface functio...The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters(DPFs).This work focused on the changes in the surface functional groups,carbon chemical state,and graphitization degree during thermal treatment in an inert gas environment at intermediate temperatures of 600℃,800℃,and 1000℃ and explore the chemical species that were desorbed from the diesel soot surface during thermal treatment using a thermogravimetric analyser coupled with a gas-chromatograph mass spectrometer(TGA-GC/MS).The surface functional groups and carbon chemical statewere characterized using Fourier transform infrared spectroscopy(FT-IR)and X-ray photoelectron spectroscopy(XPS).The graphitization degree was evaluated by means of Raman spectroscopy(RS).The concentrations of aliphatic C–H,C–OH,C=O,and O–C=O groups are reduced for diesel soot and carbon black when increasing the thermal treatment temperature,while the sp^(2)/sp^(3) hybridized ratio and graphitization degree enhance.These results provide comprehensive evidence of the decreased reactivity of soot samples.Among oxygenated functional groups,the percentage reduction during thermal treatment is the largest for the O–C=O groups owing to its worst thermodynamic stability.TGA-GC/MS results show that the aliphatic and aromatic chains and oxygenated species would be desorbed from the soot surface during 1000℃ thermal treatment of diesel soot.展开更多
The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination.In addition,poor perovskite crystallization and incomplete conversion of PbI_(2) to perovskite restrict further en...The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination.In addition,poor perovskite crystallization and incomplete conversion of PbI_(2) to perovskite restrict further enhancement of the photovoltaic performance of the devices using sequential deposition.Herein,a buried interface stabilization strategy that relies on the synergy of fluorine(F)and sulfonyl(S=O)functional groups is proposed.A series of potassium salts containing halide and non-halogen anions are employed to modify SnO_(2)/perovskite buried interface.Multiple chemical bonds including hydrogen bond,coordination bond and ionic bond are realized,which strengthens interfacial contact and defect passivation effect.The chemical interaction between modification molecules and perovskite along with SnO_(2) heightens incessantly as the number of S=O and F augments.The chemical interaction strength between modifiers and perovskite as well as SnO_(2) gradually increases with the increase in the number of S=O and F.The defect passivation effect is positively correlated with the chemical interaction strength.The crystallization kinetics is regulated through the compromise between chemical interaction strength and wettability of substrates.Compared with Cl−,all non-halogen anions perform better in crystallization optimization,energy band regulation and defect passivation.The device with potassium bis(fluorosulfonyl)imide achieves a tempting efficiency of 24.17%.展开更多
基金supported by the National Key R&D Program of China(No.2022YFC3203602)the Natural Science Foundation of China(No.52370018)+1 种基金Shaanxi Provincial Youth Innovation Team Project(No.22JP040)Shaanxi Provincial Key Scientific and Technological Innovation Team(No.2023-CX-TD-32).
文摘During the initial impoundment period of a canyon-shaped reservoir,the water body fluctuated violently regarding water level,hydrological condition,and thermal stratification.These variations may alter the structure of phytoplankton community,resulting in algal blooms and seriously threatening the ecological security of the reservoir.It is of great significance to understand the continuous changes of phytoplankton in the initial impoundment period for the protection of reservoir water quality.Therefore,a two-year in-situ monitoring study was conducted on water quality and phytoplankton in a representative canyonshaped reservoir named Sanhekou and the interannual changes of phytoplankton community and its response to environmental changes during the initial impoundment period were discussed at taxonomic versus functional classification levels.The results showed that the total nitrogen and permanganate index levels were relatively high in the first year due to rapid water storage and heavy rainfall input,and the more stable hydrological conditions in the second year promoted the increase of algae density and the transformation of community,and the proportion of cyanobacteria increased significantly.The succession order of phytoplankton in the first year of the initial impoundment periodwas Chlorophyta-Bacillariophyta-Chlorophyta,or J/F/X1-P/MP/W1-A/X1/MP,respectively.And the succession order in the second year was Cyanobacteria/Chlorophyta-Bacillariophyta-Chlorophyta,or L_(M)/G/P-P/A/X1-X1/J/G.Water temperature,relativewater column stability,mixing depth,and pHwere crucial factors affecting phytoplankton community succession.This study revealed the interannual succession law and driving factors of phytoplankton in the initial impoundment period and provided an important reference for the operation management and ecological protection of canyon-shaped reservoirs.
基金supported by the National Science Foundation of China(No.21606191)the Natural Science Foundation of Shandong Province(No.ZR2020ME024).
文摘As a new electrochemical technology,capacitive deionization(CDI)has been increasingly applied in environmental water treatment and seawater desalination.In this study,functional groups modified porous hollow carbon(HC)were synthesized as CDI electrode material for removing Na^(+)and Cl^(−)in salty water.Results showed that the average diameter of HC was approximately 180 nm,and the infrared spectrum showed that its surface was successfully modified with sulfonic and amino groups,respectively.The sulfonic acid functionalized HC(HC-S)showed better electrochemical and desalting performance than the amino-functionalized HC(HC–N),with a maximum Faradic capacity of 287.4 F/g and an adsorptive capacity of 112.97 mg/g for NaCl.Additionally,92.63%capacity retention after 100 adsorption/desorption cycles demonstrates the excellent stability of HC-S.The main findings prove that HC-S is viable as an electrodematerial for desalination by high-performance CDI applications.
基金Supported by the National Natural Science Foundation of China(42172148,42172142)。
文摘Taking the Lower Silurian Longmaxi Formation shale in the Sichuan Basin as an example,this study employs atomic force microscopy-based infrared(AFM-IR)spectroscopy to analyze the submicron-scale molecular functional groups of different types and occurrences of organic matter.Combined with the quantitative evaluation of pore development via scanning electron microscopy(SEM),the response of organic pore formation and evolution mechanisms to chemical composition and structural evolution of organic matter in overmature marine shale is investigated.The results indicate that the AFM-IR spectra of graptolite periderms and pyrobitumen in shale are dominated by the stretching vibrations of conjugated C=C bonds in aromatic compounds at approximately 1600 cm-1,with weak absorption peaks near 1375,1450 and 1720 cm-1,corresponding to aliphatic chains and carbonyl/carboxyl functional groups.Overall,the AFM-IR structural indices(A and C factors)of organic matter show a strong correlation with visible porosity in shales of equivalent maturity.Lower A and C factor values correlate with enhanced development of organic pores,which is associated with the detachment of more aliphatic chains and oxygen-containing functional groups during thermal evolution.Pyrobitumen-clay mineral composites generally exhibit superior pore development,likely attributable to clay mineral dehydration participating in hydrocarbon generation reactions that promote the removal of more functional groups.Additionally,hydrocarbon generation within organic-clay composites during high-over mature stages may induce volumetric expansion,resulting in microfracturing and hydrocarbon expulsion.The associated higher hydrocarbon expulsion rates promote the formation of larger pores and fracture-shaped pores along the flake-shaped clay minerals.This study highlights that the research of submicron-scale molecular functional groups provides a deeper understanding of organic matter evolution and pores development mechanisms in overmature shales,thereby offering critical theoretical parameters for reservoir evaluation in shale oil and gas exploration.
基金funding of the National Key Research and Development Plan(Grant 2017YFB0306600)the Project of SINOPEC(NO.117006).
文摘To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.
基金supported by the Natural Science Foundation of Yunnan Province(Grant No:202301AT070356)the Open Fund of the Key Laboratory of Tropical Forest Ecology,Chinese Academy of Sciences,National Science Foundation of China(Grant No.32061123003)+1 种基金the Joint Fund of the National Natural Science Foundation of China-Yunnan Province(Grant No.U1902203)the Field Station Foundation of the Chinese Academy of Sciences.
文摘Anthropogenic disturbances are widespread in tropical forests and influence the species composition in the overstory.However,the impacts of historical disturbance on tropical forest overstory recovery are unclear due to a lack of disturbance data,and previous studies have focused on understory species.In this study,the purpose was to deter-mine the influence of historical disturbance on the diver-sity,composition and regeneration of overstory species in present forests.In the 20-ha Xishuangbanna tropical sea-sonal rainforest dynamics plot in southwestern China,the historical disturbance boundaries were delineated based on panchromatic photographs from 1965.Factors that drove species clustering in the overstory layer(DBH≥40 cm)were analyzed and the abundance,richness and composition of these species were compared among different tree groups based on multiple regression tree analysis.The coefficient of variation of the brightness value in historical panchro-matic photographs from 1965 was the primary driver of spe-cies clustering in the overstory layer.The abundance and richness of overstory species throughout the regeneration process were similar,but species composition was always different.Although the proportion of large-seeded and vigorous-sprouting species showed no significant differ-ence between disturbed and undisturbed forests in the tree-let layer(DBH<20 cm),the difference became significant when DBH increased.The findings highlight that historical disturbances have strong legacy effects on functional group composition in the overstory and the recovery of overstory species was multidimensional.Functional group composi-tion can better indicate the dynamics of overstory species replacement during secondary succession.
基金Supported by the Young Backbone Teachers Project of Henan Province (No. 2020GGJS064)the Key Scientific and Technological Project of Henan Province (No. 232102321056)+1 种基金the Scientific Fund of Henan Normal University (No. 2020QK02)the Project of Huanghe River Fisheries Resources and Environment Investigation from the MARA,China,and the Observation and Research Station on Water Ecosystem in Danjiangkou Reservoir of Henan Province
文摘To understand the distribution of phytoplankton functional groups(PFGs)and key factors on their compositions in different watersheds of the Huanghe(Yellow)River basin,25 river sites and 25 lake-reservoirs sites were selected.The contents of nephelometric turbidity(NTU),total nitrogen(TN),and total phosphorus(TP)were significantly higher in rivers than that in lakes or reservoirs,whereas the pH and CODMn(chemical oxygen demand or potassium permanganate index)were lower.Results show that,27 PFGs,namely,assemblages A,B,C,D,E,F,G,H,J,K,LM,Lo,M,MP,N,P,S1,S2,T,TC,W1,W2,X1,X2,X3,XPh,and Y,were identified.Additionally,ANOSIM correlation analysis demonstrated significant differences in PFG composition between the riverine and lake-reservoir sections in the Huanghe River basin.In the riverine watersheds,the group MP was dominant,while assemblages B and J were prevalent in lakes and reservoirs.The Mantel correlation tests and RDA analysis showed that environmental variables,such as NTU,water temperature(WT),conductivity(Cond),and TP,were key driving factors of shaping the dominant PFGs of the study area.Using the Venn diagram based on variation partitioning analysis,PFGs were mainly influenced by WT and TP in lake-reservoir sites,while in the river sites were affected mainly by geo-climatic variables.This study helps understanding the PFGs in river ecosystems,and unraveling the key driving factors in different watersheds,which shall be important for the protection and management of entire Huanghe River basin.
基金funded by the National Natural Science Foundation of China(No.51961165104)Project of Thousand Youth Talents(No.AUGA2160100917)+1 种基金University Nursing Program for Young Scholars with Creative Talents in Heilongjiang Province(No.UNPYSCT-2020050)Provincial Leading Talent Echelon Cultivation Project of Heilongjiang Institute of Technology(No.2020LJ04)。
文摘Biochar(BC)are widely used as highly efficient adsorbents to alleviate aromatics-based contaminants due to their ease of preparation,wide availability,and high sustainability.The surface properties of BCs usually vary greatly due to their complex chemical constituents and different preparation processes and are reflected in the values of parameters such as the specific surface area(SSA),pore volume/size,and surface functional groups(SFGs).The effects of SSA and pore volume/size on the adsorption of aromatics have been widely reported.However,the corresponding mechanisms of BC SFGs towards aromatics adsorption remains unclear as the compositions of the SFGs are usually complex and hard to determine.To address in this gap in the literature,this review introduces a new perspective on the adsorption mechanisms of aromatics.Through collecting previously-reported results,the parameters log P(logarithm of the Kow),polar surface area,and the positive/negative charges were carefully calculated using Chem Draw3D,which allowed the hydrophobicity/hydrophilicity properties,electron donor-acceptor interactions,Hbonding,and electrostatic interactions between SFGs and aromatics-based contaminates to be inferred intuitively.These predictions were consistent with the reported results and showed that tailor-made BCs can be designed according to the molecular weights,chemical structures,and polarities of the target aromatics.Overall,this review provides new insight into predicting the physicochemical properties of BCs through revealing the relationship between SFGs and adsorbates,which may provide useful guidance for the preparing of highly-efficient,functional BCs for the adsorption of aromatics.
文摘The activated carbon with high surface area was prepared by KOH activation.It was further modified by H2SO4 and HNO3 to introduce more surface functional groups.The pore structure of the activated carbons before and after modification was analyzed based on the nitrogen adsorption isotherms.The morphology of those activated carbons was characterized using scanning electronic microscopy （SEM）.The surface functional groups were determined by Fourier transform infrared spectroscopy （FTIR）.The quantity of those groups was measured by the Boehm titration method.Cr（VI） removal by the activated carbons from aqueous solution was investigated at different pH values.The results show that compared with H2SO4,HNO3 destructs the original pore of the activated carbon more seriously and induces more acidic surface functional groups on the activated carbon.The pH value of the solution plays a key role in the Cr（VI） removal.The ability of reducing Cr（VI） to Cr（III） by the activated carbons is relative to the acidic surface functional groups.At higher pH values,the Cr（VI） removal ratio is improved by increasing the acidic surface functional groups of the activated carbons.At lower pH values,however,the acidic surface functional groups almost have no effect on the Cr（VI） removal by the activated carbon from aqueous solution.
基金supported by the Strategic Priority Research Program of the Chinese Academy of Sciences (Grant No. XDB03030401 & XDA05060700)the National Natural Science Foundation of China (Grant Nos. 41171044, 31070391, 41271067)the General Financial Grant from the China Postdoctoral Science Foundation (Grant No. 2013M530716)
文摘Variations in the fractions of biomass allocated to functional components are widely considered as plant responses to resource availability for grassland plants. Observations indicated shoots isometrically relates to roots at the community level but allometrically at the species level in Tibetan alpine grasslands. These differences may result from the specific complementarity of functional groups between functional components, such as leaf, root, stem and reproductive organ. To test the component complementary responses to regional moisture variation, we conducted a multi-site transect survey to measure plant individual size and component biomass fractions of common species belonging to the functional groups： forbs, grasses, legumes and sedges on the Northern Tibetan Plateau in peak growing season in 2010. Along the mean annual precipitation （MAP） gradient, we sampled 7o species, in which 2o are in alpine meadows, 20 in alpine steppes, 15 in alpine desert-steppes and 15 in alpine deserts, respectively. Our results showed that the size of alpine plants is small with individual biomass mostly lower than 1.0 g. Plants keep relative conservative component individual responses moisture functional fractions across alpine grasslands at the level. However, the complementary between functional components to variations specifically differ among groups. These results indicate that functional group diversity may be an effective tool for scaling biomass allocation patterns from individual up to community level. Therefore, it is necessary andvaluable to perform intensive and systematic studies on identification and differentiation the influences of compositional changes in functional groups on ecosystem primary services and processes.
基金Supported by the National Natural Science Foundation of China(No.U1612442)the Science and Technology Foundation of Guizhou Province(Nos.[2020]6009,[2020]4Y009)Anton Brancelj was supported by Slovenian Research Agency(ARRS)(No.P1-0255)。
文摘Reservoirs are an important water source in many densely populated areas in southwest China.Phytoplankton play an essential role in maintaining the structure and function of reservoir ecosystems.Understanding the succession in phytoplankton communities and the factors driving it are essential for eff ective water quality management in drinking water reservoirs.In this study,water samples were collected monthly at the surface layers from March 2016 to December 2019 in Hongfeng Reservoir,southwest China.The relationship between functional group succession was analyzed based on nonmetric multidimensional scaling analysis(NMDS),redundancy analysis(RDA),succession rate,and other analysis methods.The results showed distinct shifts in the community structure of phytoplankton functional groups within study period.The Cyclotella sp.was dominant in 2016 and 2017,and Pseudanabaena limnetica was the dominant group in 2018 and 2019.It appears that the phytoplankton composition and biomass are closely related to the water temperature and nutrient status in this reservoir.The results clearly showed that the permanganate index(COD_(Mn))was the key factor of dramatic phytoplankton functional group succession,and the change in succession rates was closely caused by total nitrogen concentration(TN).Therefore,the succession pattern and key factors of Hongfeng Reservoir revealed in this study were important guidance for the management of drinking water reservoirs in southwest China.A reasonable limit on exogenous nutrient input should be a priority,especially in high water temperature period.
基金Supported by the Fundamental Research Funds for the Central Universities(TD2013-2,2012LYB33)the National Natural Science Foundation of China(51278053,21373032)grant-in-aid from Kochi University of Technology and China Scholarship Council
文摘The adsorption of aqueous cadmium ions(Cd(Ⅱ)) have been investigated for modified activated carbon(AC-T)with oxygen-containing functional groups.The oxygen-containing groups of AC-T play an important role in Cd(Ⅱ) ion adsorption onto AC-T.The modified activated carbon is characterized by scanning electron microscopy,Fourier transform infrared spectroscopy(FT-IR) and X-ray photoelectron spectroscopy(XPS).The results of batch experiments indicate that the maximal adsorption could be achieved over the broad pH range of 4.5 to 6.5.Adsorption isotherms and kinetic study suggest that the sorption of Cd(Ⅱ) onto AC-T produces monolayer coverage and that adsorption is controlled by chemical adsorption.And the adsorbent has a good reusability.According to the FT-IR and XPS analyses,electrostatic attraction and cation exchange between Cd(Ⅱ) and oxygen-containing functional groups on AC-T are dominant mechanisms for Cd(Ⅱ) adsorption.
基金supported by the National Science Foundation of China(Nos.41172143 and 40872101)Developmental Plan of Basic Research on Natural Science of Shanxi Province(20012JM5005)Science Research Plan of Shanxi education department(12JK0483)
文摘The relationship between trace elements in coal and organic functional groups of coal, also some of aromatic structure, was investigated by using curve fitting of infrared spectra. Cluster analysis was also performed according to the degree of affinity of organic groups to the trace elements. The results show that there is a possibility that trace elements, especially LREE, were bound to peripheral organic functional groups of middle rank coal macromolecule. The most possible functional group that binds trace element is the hydroxyl, and to the less degree, the asymmetric -CH3 and 〉CH2 stretching, -CH3 stretching, etc. The degree of affinity of trace elements to different functional groups varies. The tendency obeys the natural structural changing law of trace elements-- the periodic law. The deviation of some trace elements from this regular trend is attributed to the deviation of intrinsic ＂confusion degree＂ （conventional molar entropy） of the matter system of coal basin, which is affected by the inner and outer factors during the evolution.
基金financial support of the National Natural Science Foundation of China(NSFC,Nos.51622806,51878325,51868050,51378246 and 51720105001)the Natural Science Foundation of Jiangxi Province(Nos.20162BCB22017,20165BCB18008,20171ACB20017,20133ACB21001 and 20171BAB206049)。
文摘Rational modification by functional groups was regarded as one of efficient methods to improve the photocatalytic performance of graphitic carbon nitride(g-C3 N4).Herein,g-C3 N4 with yellow(Y-GCN)and brown(C-GCN)were prepared by using the fresh urea and the urea kept for five years,respectively,for the first time.Experimental results show that the H2 production rate of the C-GCN is 39.06μmol/h,which is about 5 times of the Y-GCN.Meantime,in terms of apparent quantum efficiency(AQ.E)at 420 nm,C-GCN has a value of 6.3%and nearly 7.3 times higher than that of Y-GCN(0.86%).The results of XRD,IR,DRS,and NMR show,different from Y-GCN,a new kind of functional group of—N=CH—was firstly in-situ introduced into the C-GCN,resulting in good visible light absorption,and then markedly improving the photocatalytic performance.DFT calculation also confirms the effect of the—N=CH—group band structure of g-C3N4.Furthermore,XPS results demonstrate that the existence of—N=CH—groups in C-GCN results in tight interaction between C-GCN and Pt nanoparticles,and then improves the charge separation and photocatalytic performance.The present work demonstrates a good example of"defect engineering"to modify the intrinsic molecular structure of g-C3N4 and provides a new avenue to enhance the photocatalytic activity of g-C3N4 via facile and environmental-friendly method.
基金supported by the National Natural Science Foundation of China(No.51606081)the Basic Research Foundation of Shenzhen(No.JCYJ20160506170043770)
文摘In order to explore the influence of modification sites of functional groups on landfill gas （CO2/CH4） separation performance of metal-organic frameworks （MOFs）, six types of or- ganic linkers and three types of functional groups （i.e. -F, -NH2, -CH3） were used to construct 36 MOFs of pcu topology based on copper paddlewheel. Grand canonical Monte Carlo sim- ulations were performed in this work to evaluate the separation performance of MOFs at low （vacuum swing adsorption） and high （pressure swing adsorption） pressures, respectively. Simulation results demonstrated that CO2 working capacity of the unfunctionalized MOFs generally exhibits pore-size dependence at 1 bar, which increases with the decrease in pore sizes. It was also found that -NH2 funetionalized MOFs exhibit the highest CO2 uptake due to the enhanced Coulombic interactions between the polar -NH2 groups and the quadrupole moment of CO2 molecules, which is followed by -CH3 and -F functionalized ones. Moreover, positioning the functional groups -NH2 and -CH3 at sites far from the metal node （site b） exhibits more significant enhancement on CO2/CH4 separation performance compared to that adjacent to the metal node （site a）.
基金Project supported by the National Science Foundation of China (No.51772070 and 51772069)。
文摘MXenes are well known for their potential application in supercapacitors due to their high-rate intercalation pseudocapacitance and long cyclability.However,the reported low capacity of pristine MXenes hinders their practical application in lithium-ion batteries.In this work,a robust strategy is developed to control the functional groups of Nb_2 CT_x MXene.The capacity of pristine Nb_2 CT_x MXene can be significantly increased by Li~+ intercalation and surface modification.The specific capacity of the treated Nb_2 CT_x is up to 448 mAh g^(-1) at 0.05 A g^(-1),and at a large current density of 2 A g^(-1) remains a high reversible capacity retention rate of 75% after an ultra-long cycle of 2000 cycles.These values exceed most of the reported pristine MXenes(including the most studied Ti_3 C_2 T_x) and carbon-based materials.It demonstrates that this strategy has great help to improve the electrochemical performance of pristine MXene,and the results enhance the promise of MXenes in the application of lithium-ion batteries.
基金the National Natural Science Foundation of China(No.21978183)。
文摘In this work,a modification method of H_(3)PO_(4)plus H_(2)O_(2)(PHP)was introduced to targetedly form abundant oxygenated functional groups(OFGs)on biochar,and methylene blue(MB)was employed as a model pollutant for adsorption to reflect the modification performance.Results indicated that parent biochars,especially derived from lower temperatures,substantially underwent oxidative modification by PHP,and OFGs were targetedly produced.Correspondingly,approximately 21.5-fold MB adsorption capacity was achieved by PHP-modified biochar comparing with its parent biochar.To evaluate the compatibility of PHP-modification,coefficient of variation(CV)based on MB adsorption capacity by the biochar from various precursors was calculated,in which the CV of PHP-modified biochars was 0.0038 comparing to0.64 of the corresponding parent biochars.These results suggested that the PHP method displayed the excellent feedstock compatibility on biochar modification.The maximum MB adsorption capacity was454.1 mg/g when the H_(3)PO_(4)and H_(2)O_(2)fraction in PHP were 65.2%and 7.0%;the modification was further intensified by promoting temperature and duration.Besides,average 94.5%H_(3)PO_(4)was recovered after 10-batch modification,implying 1.0 kg H_(3)PO_(4)(85%)in PHP can maximally modify 2.37 kg biochar.Overall,this work offered a novel method to tailor biochar towards OFGs-rich surface for efficient adsorption.
基金supported by the Key Projects of the National Natural Science Foundation of China (Nos. 51504187, 51774233, and 51704226)Shaanxi Province Industrial Science and Technology Research Project (No. 2016GY-192)the China Postdoctoral Science Foundation (No. 2016-M-590963)
文摘Correlations among free radicals, apparent activation energy, and functional groups during lowtemperature oxidation of Jurassic coal in Northern Shaanxi were investigated by examining three coal samples collected from the Ningtiaota, Jianxin, and Shigetai coal mines. Free radical concentrations at less than 120 ℃ were investigated by electron spin resonance experiments while the thermogravimetric experiments were conducted to analyze apparent activation energies. In addition, Fourier transform infrared spectroscopy was employed to study the spectrum of functional groups generated in coal. The results indicated that, in decreasing order, the apparent activation energies were Shigetai 〉Jianxin 〉 Ningtiaota, indicating that, from 50 to 120 ℃, the Ningtiaota coal sample most easily absorbed and reacted with oxygen while the most resistant was the Shigetai coal sample. Free radical concentrations and line heights increased with increased temperature, and the line width and Lande factor showed irregular fluctuations. Functional group variations were different among these coals, and the phenol and alcohol-associated OHs, carboxyls, and aromatic ring double bonds might have had a major impact on free radical concentrations. These results were meaningful for better consideration and management of coal oxidation at low temperatures.
基金The authors are grateful to the financial support by the Postdoctoral Science Foundation of China(No.2003034330)the Science Foundation for mid-youth elite of Shangdong Province+1 种基金the Natural Science Foundation of Shangdong Province(No.Q99B15)the National Natural Science Foundation of China(No.2906008)
文摘A series of new chelating resins with incorporating heterocyclic functional groups： pyridine, thiadizole, benzothizole into macroporous chloromethylated polystyrene were synthesized via hydrophilic spacer arm of polyethylene glycol containing sulfur. These chelating resins were found to show high adsorption capacities for Ag^＋, Hg^2＋, Au^3＋ and Pd^2＋, and the presence of spacer arm can enhance adsorption ability due to increase the hydrophilicity of the chelating resins.
基金supported by the National Natural Science Foundation of China (No.52006054)the State Key Laboratory of Engines at Tianjin University (No.K2021-05)+1 种基金the European Union’s projects MODALES (No.815189)nPETS (No.954377)
文摘The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters(DPFs).This work focused on the changes in the surface functional groups,carbon chemical state,and graphitization degree during thermal treatment in an inert gas environment at intermediate temperatures of 600℃,800℃,and 1000℃ and explore the chemical species that were desorbed from the diesel soot surface during thermal treatment using a thermogravimetric analyser coupled with a gas-chromatograph mass spectrometer(TGA-GC/MS).The surface functional groups and carbon chemical statewere characterized using Fourier transform infrared spectroscopy(FT-IR)and X-ray photoelectron spectroscopy(XPS).The graphitization degree was evaluated by means of Raman spectroscopy(RS).The concentrations of aliphatic C–H,C–OH,C=O,and O–C=O groups are reduced for diesel soot and carbon black when increasing the thermal treatment temperature,while the sp^(2)/sp^(3) hybridized ratio and graphitization degree enhance.These results provide comprehensive evidence of the decreased reactivity of soot samples.Among oxygenated functional groups,the percentage reduction during thermal treatment is the largest for the O–C=O groups owing to its worst thermodynamic stability.TGA-GC/MS results show that the aliphatic and aromatic chains and oxygenated species would be desorbed from the soot surface during 1000℃ thermal treatment of diesel soot.
基金supported by the Defense Industrial Technology Development Program(JCKY2017110C0654)National Natural Science Foundation of China(11974063,61904023,62274018)+1 种基金Chongqing Special Postdoctoral Science Foundation(cstc2019jcyj-bsh0026)Fundamental Research Funds for the Central Universities(2021CDJQY-022).
文摘The interfacial defects and energy barrier are main reasons for interfacial nonradiative recombination.In addition,poor perovskite crystallization and incomplete conversion of PbI_(2) to perovskite restrict further enhancement of the photovoltaic performance of the devices using sequential deposition.Herein,a buried interface stabilization strategy that relies on the synergy of fluorine(F)and sulfonyl(S=O)functional groups is proposed.A series of potassium salts containing halide and non-halogen anions are employed to modify SnO_(2)/perovskite buried interface.Multiple chemical bonds including hydrogen bond,coordination bond and ionic bond are realized,which strengthens interfacial contact and defect passivation effect.The chemical interaction between modification molecules and perovskite along with SnO_(2) heightens incessantly as the number of S=O and F augments.The chemical interaction strength between modifiers and perovskite as well as SnO_(2) gradually increases with the increase in the number of S=O and F.The defect passivation effect is positively correlated with the chemical interaction strength.The crystallization kinetics is regulated through the compromise between chemical interaction strength and wettability of substrates.Compared with Cl−,all non-halogen anions perform better in crystallization optimization,energy band regulation and defect passivation.The device with potassium bis(fluorosulfonyl)imide achieves a tempting efficiency of 24.17%.
