The influence of high concentration Zn^(2+) on the floatability of sphalerite in an acidic system was investigated via flotation experiments,zeta potential measurements,contact angle measurements,and X-ray photoelectr...The influence of high concentration Zn^(2+) on the floatability of sphalerite in an acidic system was investigated via flotation experiments,zeta potential measurements,contact angle measurements,and X-ray photoelectron spectroscopy.The results indicated that Zn^(2+) was adsorbed on the sphalerite surface and a Zn-hydroxyl complex was formed at a pH of 4 and a Zn^(2+) concentration of 4×10^(-2) mol/L.The zeta potential increased and the contact angle decreased from 84.80°to 36.48°,strongly inhibiting the floatability of sphalerite.When S^(2−) or Cu^(2+) activator was used alone,sphalerite was not activated after Zn^(2+) was adsorbed,and its contact angle did not change significantly.However,by using a combination of S^(2−) and Cu^(2+) activators,its floatability was realized after Zn^(2+) adsorption.This result was attributed to the removal of the Zn-hydroxyl complex on the surface of sphalerite by S^(2-).After this removal,Cu^(2+) was adsorbed on the sphalerite surface to form a Cu_(2)S·S^(0) hydrophobic film.展开更多
The high-efficiency conversion of biomass resources to biofuels has attracted widespread attention, and the active sites and synergistic effect of catalysts significantly impact their surface arrangement and electroni...The high-efficiency conversion of biomass resources to biofuels has attracted widespread attention, and the active sites and synergistic effect of catalysts significantly impact their surface arrangement and electronic structure. Here, a nickel-based transition metal carbide catalyst(Ni/TMC) with high Lewis acidity was prepared by self-assembly of transition metal carbide(TMC) and nickel, which exhibited excellent performance on synergistic hydrogenation and hydrogenolysis of 5-hydroxymethylfurfural(HMF) into liquid biofuel 2,5-dimethylfuran(DMF).Notably, Ni/WC with the highest Lewis acidity(4728.3 μmol g^(-1)) can achieve 100% conversion of HMF to 97.6% yield of DMF, with a turnover frequency of up to 46.5 h^(-1). The characterization results demonstrate that the rich Lewis acid sites yielded by the synergistic effect between Ni species and TMC are beneficial for the C=O hydrogenation and C–O cleavage, thereby accelerating the process of hydrodeoxygenation(HDO). Besides, a kinetic model for the HDO of HMF to DMF process has been established based on the experimental results, which elucidated a significant correlation between the measured and the predicted data(R~2> 0.97). Corresponding to the adsorption configuration of Ni/WC and substrate determined by in-situ FTIR characterization, this study provides a novel insight into the selective conversion of HMF process for functional biofuel and bio-chemicals.展开更多
The conversion process of chitin,one of the abundant biomass resources on the earth,not only follows the principles of green chemistry,but also has significant value in industrial applications.However,it is a great ch...The conversion process of chitin,one of the abundant biomass resources on the earth,not only follows the principles of green chemistry,but also has significant value in industrial applications.However,it is a great challenge to directly convert insoluble and rigid structured chitin to 5-hydroxymethylfurfural(HMF).To address this issue,we developed a green conversion process combining pretreatment and catalytic system.Chitin was first pretreated by hexafluoro isopropanol(HFIP),which somewhat disrupted the hydrogen bonding network within the chitin structure.Subsequently,formic acid(FA)and silicotungstic acid(STA)synergistically catalyzed the conversion to HMF in a biphasic system of 2-methyltetrahydrofuran(2-Me-THF)/H2O,and high yields(40.2%)HMF was obtained under the optimism conditions.The product distribution was analyzed by HPLC-MS and the co-catalysis of FA with STA was evidenced.A dual-function catalytic system with both Lewis and Br?nsted acids was created,the catalytic system that significantly improved the efficiency of complex tandem catalytic reactions with chitin.Based on the experimental results,a possible pathway for chitin conversion was deduced,providing a new catalytic idea for the efficient conversion of chitin to HMF.展开更多
The electrochemical reduction of CO_(2)holds considerable promise in combating global climate change while yielding valuable chemical commodities.Membrane electrode assemblies operating within acidic electrolyte have ...The electrochemical reduction of CO_(2)holds considerable promise in combating global climate change while yielding valuable chemical commodities.Membrane electrode assemblies operating within acidic electrolyte have exhibited noteworthy advancements in CO_(2)utilization efficiency,albeit encountering formidable competition from the hydrogen evolution reaction.In our investigation,we introduced a silicate buffer layer,which yielded exceptional outcomes even using strong acid electrolyte.Notably,our approach yielded a CO Faradic efficiency of 90%and reached a substantial current density of 400 mA cm^(-2).Furthermore,our system displayed remarkable stability over a 12-hour duration,and achieved a high single-pass-conversion efficiency of 67%.Leveraging in-situ Raman analysis,we attributed these performance enhancements to the augmented CO_(2)adsorption and localized alkaline environment facilitated by the incorporation of the silicate buffer layer.We think the addition of buffer layer to adjust the microenvironment is essential to achieve high performance and keep stable in acid condition.展开更多
Arsenic(As)removal from smelting acidic wastewater is an urgent task.The most common method is oxidation of trivalent As(III)to pentavalent As(V)subsequently precipitated by ferric(Fe(III))salts.Foundations of redox b...Arsenic(As)removal from smelting acidic wastewater is an urgent task.The most common method is oxidation of trivalent As(III)to pentavalent As(V)subsequently precipitated by ferric(Fe(III))salts.Foundations of redox behavior and chemical species are of great importance for understanding As removal.In this work,cyclic voltammetry(CV)and UV?Vis spectroscopy were used for laboratory observation;meanwhile HSC and MINTEQ software were employed for theoretical analyses.It is found that As(III)oxidation,a multiple electron transfer reaction,is diffusion-controlled.The oxidation over-potential is very high(about0.9V)in sulfuric acid solutions(pH1.0).In addition,Fe(III)?As(V)complexes are evidenced by UV?Vis spectra and chemical species analyses in series of Fe(III)?As(V)?H2SO4?H2O solutions.Therefore,the Fe(III)and As(V)species distribution against pH values are determined and a newφ?pH diagram with inclusion of Fe?As complexes is consequently compiled based on thermodynamic data predicted by other researchers.展开更多
Olefin oligomerization reaction catalyzed by new catalyst systems（a Br？nsted‐acidic ionic liquid as the main catalyst and tricaprylylmethylammonium chloride as the co‐catalyst） has been investigat‐ed. The synthe...Olefin oligomerization reaction catalyzed by new catalyst systems（a Br？nsted‐acidic ionic liquid as the main catalyst and tricaprylylmethylammonium chloride as the co‐catalyst） has been investigat‐ed. The synthesized Br？nsted acidic ionic liquids were characterized by Fourier transform infrared spectroscopy（FT‐IR）, ultraviolet‐visible spectroscopy（UV）, ^1H nuclear magnetic resonance（NMR）, and ^13 C NMR to analyze their structures and acidities. The influence of different ionic liquids, ionic liquid loading, different co‐catalysts, catalyst ratios（mole ratio of ionic liquid to co‐catalyst）, reac‐tion time, pressure, temperature, solvent, source of reactants, and the recycling of catalyst systems was studied. Among the synthesized ionic liquids, 1‐（4‐sulfonic acid）butyl‐3‐hexylimidazolium hydrogen sulfate（[HIMBs]HSO4） exhibited the best catalytic activity under the tested reaction con‐ditions. The conversion of isobutene and selectivity of trimers were 83.21% and 35.80%, respec‐tively, at the optimum reaction conditions. Furthermore, the catalyst system can be easily separated and reused; a feasible reaction mechanism is proposed on the basis of the distribution of experi‐mental products.展开更多
Based on the semi-quantitative approach, four environmental factors of sites (i.e. bedrock lithology, soil type, land use, and rainfall) were categorized, weighted and combined to determine and assess the relative sen...Based on the semi-quantitative approach, four environmental factors of sites (i.e. bedrock lithology, soil type, land use, and rainfall) were categorized, weighted and combined to determine and assess the relative sensitivity of the terrestrial ecosystems to acidic deposition in Fujian Province. Then the factors have been digitized and combined to assign an overall value for each mesh square (16.77 km×18.39 km) by using the geographic information system (GIS) The results indicated that the most sensitive area in Fujian was mainly located in the southeast, and the least: ensitive area was distributed sporadically in the east along the coast. Due to slow weathering rate of siliceous rocks, acid to weakly acid reactions of the soils, along with the greater percent of coniferous forests, more than 80 percent of the total area exhibits higher sensitivity classes (4–7).展开更多
Six Brnsted acidic ionic liquids（ILs） 1a―1f were synthesized and used as the dual solvent-catalyst systems for Beckmann rearrangement reactions. Among ILs 1a―1f, IL 1a exhibited the highest catalytic activity and ...Six Brnsted acidic ionic liquids（ILs） 1a―1f were synthesized and used as the dual solvent-catalyst systems for Beckmann rearrangement reactions. Among ILs 1a―1f, IL 1a exhibited the highest catalytic activity and successfully catalyzed the Beckmann rearrangement of ketoximes, and the corresponding amides were obtained in good to excellent yields（74%―92%）. In addition, IL 1a could be recovered easily and reused at least three times without any loss of catalytic activity.展开更多
This study investigated the promotion effect of A.ferrooxidans on complex heavy metals coprecipitation process.A.ferrooxidans significantly enhanced the ferrous oxidation,which also promoted the formation of iron-oxyh...This study investigated the promotion effect of A.ferrooxidans on complex heavy metals coprecipitation process.A.ferrooxidans significantly enhanced the ferrous oxidation,which also promoted the formation of iron-oxyhydroxysulphate.Cu(II)concentration reduced to0.058mmol/L in A.ferrooxidans inoculated system,and Cd also reduced to the lowest concentration(0.085mmol/L).Pb was mainly immobilized as anglesite and iron-oxyhydroxysulphate promoted the removal of remanent Pb in solution.The precipitates are characterized by XRD,SEM,and FTIR analysis.The main component of the iron-oxyhydroxysulphate was well crystallized jarosite.A.ferrooxidans contributed to the formation of schwertmannite in later monovalent cation lack stage.Higher ferrous iron oxidation rate and Fe(III)supply rate in A.ferrooxidans inoculated system facilitated polyhedron crystal formation and the increase of particle diameter.Complex heavy metals could be incorporated into iron oxyhydroxysulphate crystal,and efficiently removed from acidic wastewater through A.ferrooxidans mediated coprecipitation.展开更多
Objective: To investigate the distribution and contents of vimentin(Vim) and glial fibrillary acidic protein(GFAP) immunoreactivities in the central nervous system(CNS)of normal newborn, adult and aged rats.Methods: I...Objective: To investigate the distribution and contents of vimentin(Vim) and glial fibrillary acidic protein(GFAP) immunoreactivities in the central nervous system(CNS)of normal newborn, adult and aged rats.Methods: In this study, thirty healthy and normal Sprague–Dawley rats were simply classified into three groups: Newborn(7 days aged), adult(5 months aged) and aged(24 months aged) rats. Brains and spinal cord were dissected and cut into frozen sections. The expression of Vim and GFAP in CNS were detected by confocal immunofluorescence.Results: In each group, Vim was expressed in all the regions of CNS including the hippocampal, cerebral cortex, the third ventricle and spinal cord, and the expression was highest in neuron-like cell of newborn rats, while Vim was mainly expressed in cell bodies in adult and aged rats. GFAP was expressed in all the regions of CNS including the hippocampal, cerebral cortex, the third ventricle and spinal cord, and the expression was in astrocytes of aged rats. In the third ventricle, Vim was detected in all groups, and only observed in neuron-like cells of newborn. Meanwhile, the GFAP expression showed no significant differences between adult and aged rats in this region. The co-localization of Vim and GFAP were mainly observed in hippocampus and cerebral cortex of newborn,but this co-localization was found in the third ventricle of the rats in all groups.Conclusion: Our data demonstrate for the first time that the expression of Vim and GFAP in the rat's CNS during development. This data may provide a foundation for the further mechanistic studies of these two main intermediate filaments during development of CNS.展开更多
An efficient metal-free strategy for the synthesis of pharmaceutically relevant benzo[α]carbazoles from the derivatives of readily available 2-phenylindole and bio-renewable acetol in an aqueous biphasic system was d...An efficient metal-free strategy for the synthesis of pharmaceutically relevant benzo[α]carbazoles from the derivatives of readily available 2-phenylindole and bio-renewable acetol in an aqueous biphasic system was developed. This protocol employed a sulfone-containing Bronsted acidic ionic liquid as the catalyst, which could be used for five times without a noticeable decrease in its activity and selectivity. Various substituted 2-phenylindoles and α-hydroxyketones participated in the reaction smoothly, with water as the sole byproduct. Mechanistically, the reaction involved the conventional carbon-nucleophile-induced Heyns-type rearrangement and downstream intramolecular olefination.展开更多
The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct ...The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.展开更多
In accordance with principles and methods of ecology, the effects of acidic deposition on productivity and volume increment of masson pine and Cinnamomum campora forest which are widely distributed in southern sub...In accordance with principles and methods of ecology, the effects of acidic deposition on productivity and volume increment of masson pine and Cinnamomum campora forest which are widely distributed in southern suburbs of Chongqing, China were studied. Based on the field data and measurements, a multivariable stepwise regression model was established to analyze the effects of multiple environmental factors on the productivity of the forest ecosystems. This model was used to assess the volume and economic losses of these two forest ecosystems caused by acidic deposition. The result showed that, among the environmental factors, pH value of precipitation, soil depth, soil organic contents and slope are the dominant ones influencing the growth of masson pine forest. It was also shown that the acidic deposition has no clear relation to the growth of C.Campora forest, so development of such broad leaved forest is suitable in the area.展开更多
2-Methyl-4-methoxyaniline （MMA） was synthesized by one-pot method through the hydrogenation and Bamberger rearrangement of o-nitrotoluene in methanol using acidic ionic liquid and 3% Pt/C as catalyst system. The eff...2-Methyl-4-methoxyaniline （MMA） was synthesized by one-pot method through the hydrogenation and Bamberger rearrangement of o-nitrotoluene in methanol using acidic ionic liquid and 3% Pt/C as catalyst system. The effects of ionic liquid type, dosage of ionic liquid and 3% Pt/C, reaction temperature and reaction pressure on o-nitrotoluene conversion and MMA selectivity were investigated. The results indicated that the imidazolium-based acidic ionic liquid which contains SO3H-functionalized cation showed higher selectivity to MMA than other acidic ionic liquids used in this work. Using 1-（propyl-3-sulfonate）-3-methylimidazolium hydrosulfate （[HSO3-pmim][HSO4]） as the acid catalyst, the selectivity to MMA was as high as 67.6% at 97.8% of o-nitrotoluene conversion. As 3% Pt/C increased from 0.01 g to 0.025 g, the selectivity to MMA decreased from 73.4% to 62.5%, because of the hydrogenation of intermediate o-methyl-phenylhydroxylamine to o-toluidine becoming more dominant. An increase in hydrogen pressure also had obviously dramatic effect in lowering the MMA selectivity. After easy separation from the products, the catalyst system could be reused at least 3 times.展开更多
Na2WO4‐acidic ionic liquid was used as a simple, ecofriendly, recyclable and efficient catalytic system for the one‐pot conversion of cyclohexanol to ε‐caprolactam. The effect of the structure of the ionic liquid ...Na2WO4‐acidic ionic liquid was used as a simple, ecofriendly, recyclable and efficient catalytic system for the one‐pot conversion of cyclohexanol to ε‐caprolactam. The effect of the structure of the ionic liquid on the catalytic activity of this system was investigated, and the results revealed that sulfonic acid‐functionalized ionic liquids with HSO4? as an anion gave the best results. The highly efficient performance of this catalyst system was attributed to the phase‐transfer behavior of the cation of the ionic liquid, the improved coordination of the substrate to bisperoxotungstate duringthe oxidation reaction, and the stabilization of the intermediate formed during the Beckmann rearrangement.展开更多
Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we r...Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.展开更多
CD36 is a highly glycosylated integral membrane protein that belongs to the scavenger receptor class B family and regulates the pathological progress of metabolic diseases.CD36 was recently found to be widely expresse...CD36 is a highly glycosylated integral membrane protein that belongs to the scavenger receptor class B family and regulates the pathological progress of metabolic diseases.CD36 was recently found to be widely expressed in various cell types in the nervous system,including endothelial cells,pericytes,astrocytes,and microglia.CD36 mediates a number of regulatory processes,such as endothelial dysfunction,oxidative stress,mitochondrial dysfunction,and inflammatory responses,which are involved in many central nervous system diseases,such as stroke,Alzheimer’s disease,Parkinson’s disease,and spinal cord injury.CD36 antagonists can suppress CD36 expression or prevent CD36 binding to its ligand,thereby achieving inhibition of CD36-mediated pathways or functions.Here,we reviewed the mechanisms of action of CD36 antagonists,such as Salvianolic acid B,tanshinone IIA,curcumin,sulfosuccinimidyl oleate,antioxidants,and small-molecule compounds.Moreover,we predicted the structures of binding sites between CD36 and antagonists.These sites can provide targets for more efficient and safer CD36 antagonists for the treatment of central nervous system diseases.展开更多
A novel BrФnsted acidic ionic liquid（IL） based on the cyclic guanidinium cation has been synthesized. This IL, as a strong BrФnsted acid catalyst or solvent, shows high catalytic activity and biphsaic behavor in t...A novel BrФnsted acidic ionic liquid（IL） based on the cyclic guanidinium cation has been synthesized. This IL, as a strong BrФnsted acid catalyst or solvent, shows high catalytic activity and biphsaic behavor in the esterifications of carboxylic acids and alcohols. The produced esters as a separate phase can be conveniently decanted out from the IL and the IL is recyclable without any loss of catalytic activity.展开更多
Generally, the tolerance of yeasts to acid is stronger than that of bacteria. In addition, some of the yeasts are able to neutralize acidic media, which is called acid-neutralizing yeast. An acid-neutralizing yeast, C...Generally, the tolerance of yeasts to acid is stronger than that of bacteria. In addition, some of the yeasts are able to neutralize acidic media, which is called acid-neutralizing yeast. An acid-neutralizing yeast, Cryptococcus sp. strain T1, was previously isolated from Lake Tazawa in Japan. Here we investigated the effect of several types of acid on the neutralizing ability of strain T1, and we improved an existing bioreactor model to effectively neutralize acidic water. First we carried out a neutralizing test with strain T1 using casamino acid solution adjusted to pH 3.0 - 5.0 with each inorganic or organic acid. The solutions adjusted to pH 3.0 with nitric acid, phosphoric acid, sulfuric acid, and citric acid were neutralized by strain T1. The pH 3.0 solutions with lactic acid, formic acid, and acetic acid were not neutralized. These results demonstrated that some types of organic acid avoid neutralization by strain T1, and we hypothesized that this might be due to the sterilizing function of non-dissociative organic acid. We then constructed a bioreactor system with a column filled with T1-immobilized alginate beads. The previous research identified a problem in this bioreactor system: the high level of ammonium ions (NH+4) in the neutralized water might pollute water environments, and aluminum ions (Al3+) included in acidic water prevent the neutralization. Here, we used zeolite to get rid of the NH+4 and Al3+, and the addition of a zeolite reactor enabled the bioreactor system to neutralize the acidic water with a decrease of NH+4 in the water.展开更多
The adsorption state and catalytic properties of pepsin and acidic protease from microorganisms Asp. awamori and Asp. oryzae were studied in solid phase system （in presence of sorsilen, DEAE- and CM-cellulose）. Acco...The adsorption state and catalytic properties of pepsin and acidic protease from microorganisms Asp. awamori and Asp. oryzae were studied in solid phase system （in presence of sorsilen, DEAE- and CM-cellulose）. According to the results, adsorption capacity and catalytic activity of enzymes depend on the physical nature of surface groups of the solid phase. Changing the stability of enzymes in the system with solid phase is observed even the adsorption bond is less stable （in the case of DEAE- and CM-cellulose in acidic media）. Injection to the medium ethanol, surfactants, sodium chloride and changing the temperature of the incubation medium could prevent the negative effects of the solid phases. When sorsilen is used as solid phase, pepsin and acidic protease from Asp. awamori suffer from high surface inactivation. Various surfactants influence adsorption state of enzymes differently. Non-ionic surfactants （Triton X-100） prevent adsorption and restore catalytic properties of enzymes.展开更多
基金the financial supports from the National Key R&D Program of China(Nos.2018YFC0903404,2018YFC1903400)the National Natural Science Foundation of China(No.51974138)+1 种基金the Natural Science Foundation of Jiangxi Province,China(No.20202BABL214022)the Research Startup Fund Project of JXUST,China(Nos.jxxjbs17032,jxxjbs19019).
文摘The influence of high concentration Zn^(2+) on the floatability of sphalerite in an acidic system was investigated via flotation experiments,zeta potential measurements,contact angle measurements,and X-ray photoelectron spectroscopy.The results indicated that Zn^(2+) was adsorbed on the sphalerite surface and a Zn-hydroxyl complex was formed at a pH of 4 and a Zn^(2+) concentration of 4×10^(-2) mol/L.The zeta potential increased and the contact angle decreased from 84.80°to 36.48°,strongly inhibiting the floatability of sphalerite.When S^(2−) or Cu^(2+) activator was used alone,sphalerite was not activated after Zn^(2+) was adsorbed,and its contact angle did not change significantly.However,by using a combination of S^(2−) and Cu^(2+) activators,its floatability was realized after Zn^(2+) adsorption.This result was attributed to the removal of the Zn-hydroxyl complex on the surface of sphalerite by S^(2-).After this removal,Cu^(2+) was adsorbed on the sphalerite surface to form a Cu_(2)S·S^(0) hydrophobic film.
基金Fundamental Research Foundation of CAF (CAFYBB2022QB001)National Nature Science Foundation of China for Excellent Young Scientists Fund (32222058)。
文摘The high-efficiency conversion of biomass resources to biofuels has attracted widespread attention, and the active sites and synergistic effect of catalysts significantly impact their surface arrangement and electronic structure. Here, a nickel-based transition metal carbide catalyst(Ni/TMC) with high Lewis acidity was prepared by self-assembly of transition metal carbide(TMC) and nickel, which exhibited excellent performance on synergistic hydrogenation and hydrogenolysis of 5-hydroxymethylfurfural(HMF) into liquid biofuel 2,5-dimethylfuran(DMF).Notably, Ni/WC with the highest Lewis acidity(4728.3 μmol g^(-1)) can achieve 100% conversion of HMF to 97.6% yield of DMF, with a turnover frequency of up to 46.5 h^(-1). The characterization results demonstrate that the rich Lewis acid sites yielded by the synergistic effect between Ni species and TMC are beneficial for the C=O hydrogenation and C–O cleavage, thereby accelerating the process of hydrodeoxygenation(HDO). Besides, a kinetic model for the HDO of HMF to DMF process has been established based on the experimental results, which elucidated a significant correlation between the measured and the predicted data(R~2> 0.97). Corresponding to the adsorption configuration of Ni/WC and substrate determined by in-situ FTIR characterization, this study provides a novel insight into the selective conversion of HMF process for functional biofuel and bio-chemicals.
基金Supported by the National Natural Science Foundation of China(No.42076126)the Shandong Key R&D Plan+2 种基金Major Scientific and Technological Innovation Project(No.2022CXGC020413)the Natural Science Foundation of Shandong Province(Nos.ZR2020MD072,ZR2021QD014)the Liaoning Provincial Natural Science Foundation:Joint Open Fund of the State Key Laboratory for the Creation and Development of New Pesticides(No.2022-KF-25-03)。
文摘The conversion process of chitin,one of the abundant biomass resources on the earth,not only follows the principles of green chemistry,but also has significant value in industrial applications.However,it is a great challenge to directly convert insoluble and rigid structured chitin to 5-hydroxymethylfurfural(HMF).To address this issue,we developed a green conversion process combining pretreatment and catalytic system.Chitin was first pretreated by hexafluoro isopropanol(HFIP),which somewhat disrupted the hydrogen bonding network within the chitin structure.Subsequently,formic acid(FA)and silicotungstic acid(STA)synergistically catalyzed the conversion to HMF in a biphasic system of 2-methyltetrahydrofuran(2-Me-THF)/H2O,and high yields(40.2%)HMF was obtained under the optimism conditions.The product distribution was analyzed by HPLC-MS and the co-catalysis of FA with STA was evidenced.A dual-function catalytic system with both Lewis and Br?nsted acids was created,the catalytic system that significantly improved the efficiency of complex tandem catalytic reactions with chitin.Based on the experimental results,a possible pathway for chitin conversion was deduced,providing a new catalytic idea for the efficient conversion of chitin to HMF.
文摘The electrochemical reduction of CO_(2)holds considerable promise in combating global climate change while yielding valuable chemical commodities.Membrane electrode assemblies operating within acidic electrolyte have exhibited noteworthy advancements in CO_(2)utilization efficiency,albeit encountering formidable competition from the hydrogen evolution reaction.In our investigation,we introduced a silicate buffer layer,which yielded exceptional outcomes even using strong acid electrolyte.Notably,our approach yielded a CO Faradic efficiency of 90%and reached a substantial current density of 400 mA cm^(-2).Furthermore,our system displayed remarkable stability over a 12-hour duration,and achieved a high single-pass-conversion efficiency of 67%.Leveraging in-situ Raman analysis,we attributed these performance enhancements to the augmented CO_(2)adsorption and localized alkaline environment facilitated by the incorporation of the silicate buffer layer.We think the addition of buffer layer to adjust the microenvironment is essential to achieve high performance and keep stable in acid condition.
基金Projects (51304251,51374237) supported by the National Natural Science Foundation of ChinaProject (201509050) supported by Special Program on Environmental Protection for Public Welfare,China
文摘Arsenic(As)removal from smelting acidic wastewater is an urgent task.The most common method is oxidation of trivalent As(III)to pentavalent As(V)subsequently precipitated by ferric(Fe(III))salts.Foundations of redox behavior and chemical species are of great importance for understanding As removal.In this work,cyclic voltammetry(CV)and UV?Vis spectroscopy were used for laboratory observation;meanwhile HSC and MINTEQ software were employed for theoretical analyses.It is found that As(III)oxidation,a multiple electron transfer reaction,is diffusion-controlled.The oxidation over-potential is very high(about0.9V)in sulfuric acid solutions(pH1.0).In addition,Fe(III)?As(V)complexes are evidenced by UV?Vis spectra and chemical species analyses in series of Fe(III)?As(V)?H2SO4?H2O solutions.Therefore,the Fe(III)and As(V)species distribution against pH values are determined and a newφ?pH diagram with inclusion of Fe?As complexes is consequently compiled based on thermodynamic data predicted by other researchers.
基金supported by the National Natural Science Foundation of China(21473225)
文摘Olefin oligomerization reaction catalyzed by new catalyst systems（a Br？nsted‐acidic ionic liquid as the main catalyst and tricaprylylmethylammonium chloride as the co‐catalyst） has been investigat‐ed. The synthesized Br？nsted acidic ionic liquids were characterized by Fourier transform infrared spectroscopy（FT‐IR）, ultraviolet‐visible spectroscopy（UV）, ^1H nuclear magnetic resonance（NMR）, and ^13 C NMR to analyze their structures and acidities. The influence of different ionic liquids, ionic liquid loading, different co‐catalysts, catalyst ratios（mole ratio of ionic liquid to co‐catalyst）, reac‐tion time, pressure, temperature, solvent, source of reactants, and the recycling of catalyst systems was studied. Among the synthesized ionic liquids, 1‐（4‐sulfonic acid）butyl‐3‐hexylimidazolium hydrogen sulfate（[HIMBs]HSO4） exhibited the best catalytic activity under the tested reaction con‐ditions. The conversion of isobutene and selectivity of trimers were 83.21% and 35.80%, respec‐tively, at the optimum reaction conditions. Furthermore, the catalyst system can be easily separated and reused; a feasible reaction mechanism is proposed on the basis of the distribution of experi‐mental products.
文摘Based on the semi-quantitative approach, four environmental factors of sites (i.e. bedrock lithology, soil type, land use, and rainfall) were categorized, weighted and combined to determine and assess the relative sensitivity of the terrestrial ecosystems to acidic deposition in Fujian Province. Then the factors have been digitized and combined to assign an overall value for each mesh square (16.77 km×18.39 km) by using the geographic information system (GIS) The results indicated that the most sensitive area in Fujian was mainly located in the southeast, and the least: ensitive area was distributed sporadically in the east along the coast. Due to slow weathering rate of siliceous rocks, acid to weakly acid reactions of the soils, along with the greater percent of coniferous forests, more than 80 percent of the total area exhibits higher sensitivity classes (4–7).
基金Supported by the National Natural Science Foundation of China(Nos.20771030,20671025)
文摘Six Brnsted acidic ionic liquids（ILs） 1a―1f were synthesized and used as the dual solvent-catalyst systems for Beckmann rearrangement reactions. Among ILs 1a―1f, IL 1a exhibited the highest catalytic activity and successfully catalyzed the Beckmann rearrangement of ketoximes, and the corresponding amides were obtained in good to excellent yields（74%―92%）. In addition, IL 1a could be recovered easily and reused at least three times without any loss of catalytic activity.
基金Project(51174239)supported by the National Natural Science Foundation of ChinaProject supported by the Shanghai Tongji Gao Tingyao Environment Protection Science&Technology Development Foundation,China+2 种基金Project supported by the Hunan Provincial Co-Innovation Center for Clean and Efficient Utilization of Strategic Metal Mineral Resources,ChinaProject(2017M610506)supported by Postdoctoral Foundation for MG from Chinese PD Science Foundation,ChinaProject(185690)supported by PD Research Funding Plan in Hunan and Central South University,China
文摘This study investigated the promotion effect of A.ferrooxidans on complex heavy metals coprecipitation process.A.ferrooxidans significantly enhanced the ferrous oxidation,which also promoted the formation of iron-oxyhydroxysulphate.Cu(II)concentration reduced to0.058mmol/L in A.ferrooxidans inoculated system,and Cd also reduced to the lowest concentration(0.085mmol/L).Pb was mainly immobilized as anglesite and iron-oxyhydroxysulphate promoted the removal of remanent Pb in solution.The precipitates are characterized by XRD,SEM,and FTIR analysis.The main component of the iron-oxyhydroxysulphate was well crystallized jarosite.A.ferrooxidans contributed to the formation of schwertmannite in later monovalent cation lack stage.Higher ferrous iron oxidation rate and Fe(III)supply rate in A.ferrooxidans inoculated system facilitated polyhedron crystal formation and the increase of particle diameter.Complex heavy metals could be incorporated into iron oxyhydroxysulphate crystal,and efficiently removed from acidic wastewater through A.ferrooxidans mediated coprecipitation.
基金supported by National Natural Science Foundation of China(No:81500377)the Joint Special Fund between Yunnan Provincial Science and Technology Department and Kunming Medical University(No:2015FB009,2015FB153)Program for Students Innovation in Kunming Medical University
文摘Objective: To investigate the distribution and contents of vimentin(Vim) and glial fibrillary acidic protein(GFAP) immunoreactivities in the central nervous system(CNS)of normal newborn, adult and aged rats.Methods: In this study, thirty healthy and normal Sprague–Dawley rats were simply classified into three groups: Newborn(7 days aged), adult(5 months aged) and aged(24 months aged) rats. Brains and spinal cord were dissected and cut into frozen sections. The expression of Vim and GFAP in CNS were detected by confocal immunofluorescence.Results: In each group, Vim was expressed in all the regions of CNS including the hippocampal, cerebral cortex, the third ventricle and spinal cord, and the expression was highest in neuron-like cell of newborn rats, while Vim was mainly expressed in cell bodies in adult and aged rats. GFAP was expressed in all the regions of CNS including the hippocampal, cerebral cortex, the third ventricle and spinal cord, and the expression was in astrocytes of aged rats. In the third ventricle, Vim was detected in all groups, and only observed in neuron-like cells of newborn. Meanwhile, the GFAP expression showed no significant differences between adult and aged rats in this region. The co-localization of Vim and GFAP were mainly observed in hippocampus and cerebral cortex of newborn,but this co-localization was found in the third ventricle of the rats in all groups.Conclusion: Our data demonstrate for the first time that the expression of Vim and GFAP in the rat's CNS during development. This data may provide a foundation for the further mechanistic studies of these two main intermediate filaments during development of CNS.
基金supported by the National Natural Science Foundation of China(21761132014,21872060)the Fundamental Research Funds for the Central Universities of China(2016YXZD033)+1 种基金the Fundamental Research Funds for the Central Universities(2019kfyXJJS072)Opening fund of Hubei Key Laboratory of Material Chemistry and Service Failure(2017MCF01K)~~
文摘An efficient metal-free strategy for the synthesis of pharmaceutically relevant benzo[α]carbazoles from the derivatives of readily available 2-phenylindole and bio-renewable acetol in an aqueous biphasic system was developed. This protocol employed a sulfone-containing Bronsted acidic ionic liquid as the catalyst, which could be used for five times without a noticeable decrease in its activity and selectivity. Various substituted 2-phenylindoles and α-hydroxyketones participated in the reaction smoothly, with water as the sole byproduct. Mechanistically, the reaction involved the conventional carbon-nucleophile-induced Heyns-type rearrangement and downstream intramolecular olefination.
基金supported by the Taishan Scholar Program of Shandong Province,China (tsqn202211162)the National Natural Science Foundation of China (22102079)the Natural Science Foundation of Shandong Province of China (ZR2021YQ10,ZR2022QB163)。
文摘The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.
文摘In accordance with principles and methods of ecology, the effects of acidic deposition on productivity and volume increment of masson pine and Cinnamomum campora forest which are widely distributed in southern suburbs of Chongqing, China were studied. Based on the field data and measurements, a multivariable stepwise regression model was established to analyze the effects of multiple environmental factors on the productivity of the forest ecosystems. This model was used to assess the volume and economic losses of these two forest ecosystems caused by acidic deposition. The result showed that, among the environmental factors, pH value of precipitation, soil depth, soil organic contents and slope are the dominant ones influencing the growth of masson pine forest. It was also shown that the acidic deposition has no clear relation to the growth of C.Campora forest, so development of such broad leaved forest is suitable in the area.
基金Supported by the National Natural Science Foundation of China （21106134） and the Natural Science Foundation of Zlaejlang Province （Y4100671）.
文摘2-Methyl-4-methoxyaniline （MMA） was synthesized by one-pot method through the hydrogenation and Bamberger rearrangement of o-nitrotoluene in methanol using acidic ionic liquid and 3% Pt/C as catalyst system. The effects of ionic liquid type, dosage of ionic liquid and 3% Pt/C, reaction temperature and reaction pressure on o-nitrotoluene conversion and MMA selectivity were investigated. The results indicated that the imidazolium-based acidic ionic liquid which contains SO3H-functionalized cation showed higher selectivity to MMA than other acidic ionic liquids used in this work. Using 1-（propyl-3-sulfonate）-3-methylimidazolium hydrosulfate （[HSO3-pmim][HSO4]） as the acid catalyst, the selectivity to MMA was as high as 67.6% at 97.8% of o-nitrotoluene conversion. As 3% Pt/C increased from 0.01 g to 0.025 g, the selectivity to MMA decreased from 73.4% to 62.5%, because of the hydrogenation of intermediate o-methyl-phenylhydroxylamine to o-toluidine becoming more dominant. An increase in hydrogen pressure also had obviously dramatic effect in lowering the MMA selectivity. After easy separation from the products, the catalyst system could be reused at least 3 times.
基金supported by the National Natural Science Foundation of China (20636030, 2090618, 21236001)the Natural Science Foundation of Hebei Province (B2017202226)~~
文摘Na2WO4‐acidic ionic liquid was used as a simple, ecofriendly, recyclable and efficient catalytic system for the one‐pot conversion of cyclohexanol to ε‐caprolactam. The effect of the structure of the ionic liquid on the catalytic activity of this system was investigated, and the results revealed that sulfonic acid‐functionalized ionic liquids with HSO4? as an anion gave the best results. The highly efficient performance of this catalyst system was attributed to the phase‐transfer behavior of the cation of the ionic liquid, the improved coordination of the substrate to bisperoxotungstate duringthe oxidation reaction, and the stabilization of the intermediate formed during the Beckmann rearrangement.
基金This study is supported by the National Key Research and Development Program of China(2017YFB0307500).
文摘Implementing a new energy-saving electrochemical synthesis system with high commercial value is a strategy of the sustainable development for upgrading the bulk chemicals preparation technology in the future.Here,we report a multiple redox-mediated linear paired electrolysis system,combining the hydrogen peroxide mediated cathode process with the I2 mediated anode process,and realize the conversion of furfural to furoic acid in both side of the dividedflow cell simultaneously.By reasonably controlling the cathode potential,the undesired water splitting reaction and furfural reduction side reactions are avoided.Under the galvanostatic electrolysis,the two-mediated electrode processes have good compatibility,which reduce the energy consumption by about 22%while improving the electronic efficiency by about 125%.This system provides a green electrochemical synthesis route with commercial prospects.
基金supported by the National Major Project of Research and Development,No.2022YFA1105500(to SZ)the National Natural Science Foundation of China,No.81870975(to SZ)Innovation Program for Graduate Students in Jiangsu Province of China,No.KYCX223335(to MZ)。
文摘CD36 is a highly glycosylated integral membrane protein that belongs to the scavenger receptor class B family and regulates the pathological progress of metabolic diseases.CD36 was recently found to be widely expressed in various cell types in the nervous system,including endothelial cells,pericytes,astrocytes,and microglia.CD36 mediates a number of regulatory processes,such as endothelial dysfunction,oxidative stress,mitochondrial dysfunction,and inflammatory responses,which are involved in many central nervous system diseases,such as stroke,Alzheimer’s disease,Parkinson’s disease,and spinal cord injury.CD36 antagonists can suppress CD36 expression or prevent CD36 binding to its ligand,thereby achieving inhibition of CD36-mediated pathways or functions.Here,we reviewed the mechanisms of action of CD36 antagonists,such as Salvianolic acid B,tanshinone IIA,curcumin,sulfosuccinimidyl oleate,antioxidants,and small-molecule compounds.Moreover,we predicted the structures of binding sites between CD36 and antagonists.These sites can provide targets for more efficient and safer CD36 antagonists for the treatment of central nervous system diseases.
文摘A novel BrФnsted acidic ionic liquid（IL） based on the cyclic guanidinium cation has been synthesized. This IL, as a strong BrФnsted acid catalyst or solvent, shows high catalytic activity and biphsaic behavor in the esterifications of carboxylic acids and alcohols. The produced esters as a separate phase can be conveniently decanted out from the IL and the IL is recyclable without any loss of catalytic activity.
文摘Generally, the tolerance of yeasts to acid is stronger than that of bacteria. In addition, some of the yeasts are able to neutralize acidic media, which is called acid-neutralizing yeast. An acid-neutralizing yeast, Cryptococcus sp. strain T1, was previously isolated from Lake Tazawa in Japan. Here we investigated the effect of several types of acid on the neutralizing ability of strain T1, and we improved an existing bioreactor model to effectively neutralize acidic water. First we carried out a neutralizing test with strain T1 using casamino acid solution adjusted to pH 3.0 - 5.0 with each inorganic or organic acid. The solutions adjusted to pH 3.0 with nitric acid, phosphoric acid, sulfuric acid, and citric acid were neutralized by strain T1. The pH 3.0 solutions with lactic acid, formic acid, and acetic acid were not neutralized. These results demonstrated that some types of organic acid avoid neutralization by strain T1, and we hypothesized that this might be due to the sterilizing function of non-dissociative organic acid. We then constructed a bioreactor system with a column filled with T1-immobilized alginate beads. The previous research identified a problem in this bioreactor system: the high level of ammonium ions (NH+4) in the neutralized water might pollute water environments, and aluminum ions (Al3+) included in acidic water prevent the neutralization. Here, we used zeolite to get rid of the NH+4 and Al3+, and the addition of a zeolite reactor enabled the bioreactor system to neutralize the acidic water with a decrease of NH+4 in the water.
文摘The adsorption state and catalytic properties of pepsin and acidic protease from microorganisms Asp. awamori and Asp. oryzae were studied in solid phase system （in presence of sorsilen, DEAE- and CM-cellulose）. According to the results, adsorption capacity and catalytic activity of enzymes depend on the physical nature of surface groups of the solid phase. Changing the stability of enzymes in the system with solid phase is observed even the adsorption bond is less stable （in the case of DEAE- and CM-cellulose in acidic media）. Injection to the medium ethanol, surfactants, sodium chloride and changing the temperature of the incubation medium could prevent the negative effects of the solid phases. When sorsilen is used as solid phase, pepsin and acidic protease from Asp. awamori suffer from high surface inactivation. Various surfactants influence adsorption state of enzymes differently. Non-ionic surfactants （Triton X-100） prevent adsorption and restore catalytic properties of enzymes.
