For decades micoorganisms have been engineered for the utilization of lignocellulose-based second-generation (2G) feedstocks, but with theconcerns of increased levels of atmospheric CO_(2) causing global warming there...For decades micoorganisms have been engineered for the utilization of lignocellulose-based second-generation (2G) feedstocks, but with theconcerns of increased levels of atmospheric CO_(2) causing global warming there is an emergent need to transition from the utilization of 2Gfeedstocks to third-generation (3G) feedstocks such as CO_(2) and its derivatives. Here, we established a yeast platform that is capable ofsimultaneously converting 2G and 3G feedstocks into bulk and value-added chemicals. We demonstrated that by adopting 3G substrates such asCO_(2) and formate, the conversion of 2G feedstocks could be substantially improved. Specifically, formate could provide reducing power andenergy for xylose conversion into valuable chemicals. Simultaneously, it can form a concentrated CO_(2) pool inside the cell, providing thermodynamically and kinetically favoured amounts of precursors for CO_(2) fixation pathways, e.g., the Calvin–Benson–Bassham (CBB) cycle.Furthermore, we demonstrated that formate could directly be utilized as a carbon source by yeast to synthesize endogenous amino acids. Theengineered strain achieved a one-carbon (C1) assimilation efficiency of 9.2%, which was the highest efficiency observed in the co-utilization of2G and 3G feedstocks. We applied this strategy for productions of both bulk and value-added chemicals, including ethanol, free fatty acids(FFAs), and longifolene, resulting in yield enhancements of 18.4%, 49.0%, and ~100%, respectively. The strategy demonstrated here for coutilization of 2G and 3G feedstocks sheds lights on both basic and applied research for the up-coming establishment of 3G biorefineries.展开更多
With the application of HIGEE process intensification technology, petroleum sulfonate surfactant used for enhanced oil recovery was synthesized from petroleum fraction of Shengli crude oil with three sulfonating agent...With the application of HIGEE process intensification technology, petroleum sulfonate surfactant used for enhanced oil recovery was synthesized from petroleum fraction of Shengli crude oil with three sulfonating agents, including diluted liquid sulfur trioxide, diluted gaseous sulfur trioxide and fuming sulfuric acid. For each sulfonating agent, different operation modes (liquid-liquid or gas-liquid reaction with semi-continuous or continuous operation) were applied. The effects of various experimental conditions, such as solvent/oil mass ratio, sulfonating agent/oil mass ratio, gas/liquid ratio, gas concentration, reaction temperature, rotating speed, circulation ratio, reaction time and aging time, on the content of active matter and unsulfonated oil were investigated. Under relatively optimal reaction conditions, the target product was prepared with high mass content of active matter (up to 45.3%) and extremely low oil/water interfacial tension (4.5×10 –3 mN·m –1 ). The product quality and process efficiency are higher compared with traditional sulfonation technology.展开更多
NiOOH was prepared by one-step electrolysis of spherical Ni(OH)2 and the effects of electrolysis parameters were examined. The highly pure NiOOH was obtained after electrolysis at a current density of 60mA.g^-1 and...NiOOH was prepared by one-step electrolysis of spherical Ni(OH)2 and the effects of electrolysis parameters were examined. The highly pure NiOOH was obtained after electrolysis at a current density of 60mA.g^-1 and 30℃ with anodic potential controlled in the range of 1.73-1.85V (vs. Zn/ZnO) for 360min. The NiOOH samriles were characterized bv X-ray oowder diffraction (XRD) and scanning electron microscope (SEM) analysis.Resuits indicate that the electrolysis product is spherical NiOOH doped with graphite. Charge and discharge tests show that the prepared NiOOH offers a discharge capacity of over 270mAh·g^-1 at current density of 30mA·g^-1 and can be directly used as cathode material of alkaline Zn/NiOOH batteries. Galvanostatic charge/discharge and cyclic voltammetry (CV) tests reveal good cycling reversibility, of the NiOOH electrode.展开更多
Electrochemical dechlorination of chloroform in neutral aqueous solution was investigated using palladium-loaded electrodes at ambient temperature. Palladium/foam-nickel (Pd/foam-Ni) and palladium/polymeric pyrrole ...Electrochemical dechlorination of chloroform in neutral aqueous solution was investigated using palladium-loaded electrodes at ambient temperature. Palladium/foam-nickel (Pd/foam-Ni) and palladium/polymeric pyrrole film/foam-nickel (Pd/PPy/foam-Ni) composite electrodes which provided catalytic surface for reductive dechlorination of chloroform in aqueous solution were prepared using an electrodepositing method. Scanning electron microscope (SEM) micrographs showed that polymeric pyrrole film modified the electrode-surface characteristics and resulted in the uniform dispersion of needle-shaped palladium particles on foam-Ni supporting electrode. The experimental results of dechlorination indicated that the removal efficiency of chloroform and current efficiency in neutral aqueous solution on Pd/PPy/foam-Ni electrode could be up to 36.8% and 33.0% at dechlorination current of 0.1 mA and dechlorination time of 180 min, which is much higher than that of Pd/foam-Ni electrode.展开更多
Rice straw physicochemical characteristics and anaerobic digestion(AD)performance via ammonia pretreatment at varying ammonia concentrations(2%,4%,and 6%)and moisture contents(30%,50%,70%,and 90%)under a mild conditio...Rice straw physicochemical characteristics and anaerobic digestion(AD)performance via ammonia pretreatment at varying ammonia concentrations(2%,4%,and 6%)and moisture contents(30%,50%,70%,and 90%)under a mild condition were investigated.The results showed that the ammonia pretreatment effectively damaged the rice straw structure,increased the soluble organic concentration,and improved rice straw hydrolysis and AD performance.After pretreatment,the ester bond and ether bond were ruptured in lignocellulose and the volatile fatty acids(VFAs)were within the range of 1457.81–1823.67 mg·L-1.In addition,ammonia pretreatment had high selectivity on lignin removal,resulting in a maximum lignin removal rate of 50.80%.The highest methane yield of rice straw was 250.34 ml·(g VS)-1 at a 4%ammonia concentration coupled with a 70%moisture content,which was 28.55%higher than that of the control.The result showed that ammonia pretreatment of rice straw is technically suitable to enhance AD performance for further application.展开更多
An active balancing technology has been applied to solve the severe vibration caused by sudden unbalance in rotating machineries during their working process. First, based on the generation principle of sudden unbalan...An active balancing technology has been applied to solve the severe vibration caused by sudden unbalance in rotating machineries during their working process. First, based on the generation principle of sudden unbalance, a simulation test stand with a sudden unbalance generation device was set up. Then, the balancing planes were optimized by using the finite element method (FEM) to determine the position for balancing device installation. Finally, the active balancing experiments were carried out on the test stand. The experimental results indicate that the vibration response caused by sudden unbalance can be decreased from 77μm to 8μm by using the active balancing device, and the vibration amplitude reduction was up to 89.6%. From this example, it can be concluded that the active balancing device, which is installed on a proper position of the rotor, can effectively control the random transient synchronous vibration, demonstrating its high value in engineering practice.展开更多
Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties.Herein,halogen anion(X-)-incorporated β-FeOOH(β-FeOOH(X),X=F-,Cl-,and Br...Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties.Herein,halogen anion(X-)-incorporated β-FeOOH(β-FeOOH(X),X=F-,Cl-,and Br-) was investigated with a spontaneous adsorption process,which realized a great improvement of supercapacitor performances by adjusting the coordination geometry.Experiments coupled with theoretical calculations demonstrated that the change of Fe-O bond length and structural distortion of β-FeOOH,which is rooted in halogen ions embedment,led to the relatively narrow band gap.Because of the strong electronegativity of X-,the Fe element in β-FeOOH(X)s presented the unexpected high valence state(3+δ),which is facilitating to adsorb S032-species.Consequently,the designed β-FeOOH(X)s exhibited the good electric conductivity and enhanced the contact between electrode and electrolyte.When used as a negative electrode,the β-FeOOH(F) showed the excellent specific capacity of 391.9 F g-1 at 1 A g-1 current density,almost tenfold improvement compared with initial β-FeOOH,with the superior rate capacity and cyclic stability.This combinational design principle of electronic structure and electrochemical performances provides a promising way to develop advanced electrode materials for supercapacitor.展开更多
Ti-Ce, Ti-Si binary and Ti-Ce-Si ternary novel nanocomposite oxide photocatalysts were prepared with cheap inorganic salts TiCI4, Na2SiO3·9H2O and Ce(NO3)3·6H2O as precursors by supercritical fluid drying ...Ti-Ce, Ti-Si binary and Ti-Ce-Si ternary novel nanocomposite oxide photocatalysts were prepared with cheap inorganic salts TiCI4, Na2SiO3·9H2O and Ce(NO3)3·6H2O as precursors by supercritical fluid drying (SCFD) technology. The catalysts were characterized by means of XRD and TEM. The particle size of nanocomposite oxide photocatalysts synthesized by SCFD method is about 6 - 11 nm, which is smaller than those obtained by common drying method (CD). The phase transformation from anatase to rutile was inhibited by SCFD technology. The peaks of SiO2 and CeO2 in XRD patterns indicate that a SiO2 amorphorous phase exists in all the samples and CeO2 is well dispersed on the surface of TiO2. The orthogonal test was designed to optimize the preparing conditions. It is found that ceria dop;.ng enhances the photocatalyric activity markedly, and the optimum doping of CeO2 is 0.1%. The thermal stability of photocatalyst can be improved ; the growth of particle-size and the decrease of surface area can be prohibited by doping of SlOe. Heat-treatment is a necessary factor to induce chemistry change of Ti-Si surface. The optimum heat-treating temperature is 600℃. A novel and efficient Ti-Ce-Si ternary nanocomposite was prepared by SCFI) method with strong thermal stability and high photoactivity in the photodegratation of phenol.展开更多
The elimination of toxic materials in sealing methods for anodic films on 1070 aluminum alloy was studied. The new process uses chemical treatments in cerium solution and an electrochemical treatment in a molybdate so...The elimination of toxic materials in sealing methods for anodic films on 1070 aluminum alloy was studied. The new process uses chemical treatments in cerium solution and an electrochemical treatment in a molybdate solution. Potentiodynamic polarization and electrochemical impedance spectroscopy(EIS) were used to study the influences of sealing methods on the corrosion behavior of anodic films in NaCl solutions. The results show that the Ce-Mo sealing makes the surface structure and morphology of anodic films uniform and compact. Ce and Mo produce a cooperative effect to improve the corrosion resistance of anodic films. Anodic films sealed by Ce-Mo provide high corrosion resistance both in acidic and basic solutions.展开更多
The use of traditional chemical catalysis to produce chemicals has a series of drawbacks,such as high dependence on fossil resources,high energy consumption,and environmental pollution.With the development of syntheti...The use of traditional chemical catalysis to produce chemicals has a series of drawbacks,such as high dependence on fossil resources,high energy consumption,and environmental pollution.With the development of synthetic biology and metabolic engineering,the use of renewable biomass raw materials for chemicals synthesis by constructing efficient microbial cell factories is a green way to replace traditional chemical catalysis and traditional microbial fermentation.This review mainly summarizes several types of bulk chemicals and high value-added chemicals using metabolic engineering and synthetic biology strategies to achieve efficient microbial production.In addition,this review also summarizes several strategies for effectively regulating microbial cell metabolism.These strategies can achieve the coupling balance of material and energy by regulating intracellular material metabolism or energy metabolism,and promote the efficient production of target chemicals by microorganisms.展开更多
A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.The...A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.Theoretically,the activation of CH_(4) and the selectivity to the CH_(3)OH product are challenging due to the extreme stability of CH_(4) and relatively high reactivity of CH_(3)OH.The state-of-the-art‘methane reforming-methanol synthesis’process adopts a two-step strategy to avoid the further reaction of CH_(3)OH under the harsh conditions required for CH_(4) activation.In the electrochemical field,researchers are trying to develop conversion pathways under mild conditions.They have found suitable catalysts to activate the C–H bonds in methane with the help of external charge and have designed the electrode reactions to continuously generate certain active oxygen species.These active oxygen species attack the activated methane and convert it to CH_(3)OH,with the benefit of avoiding over-oxidation of CH_(3)OH,and thus obtain a high conversion efficiency of CH_(4) to CH_(3)OH.This mini-review focuses on the advantages and challenges of electrochemical conversion of CH4 to CH_(3)OH,especially the strategies for supplying electro-generated active oxygen species in-situ to react with the activated methane.展开更多
Based on online observations of fine particulate matter(PM2.5) for five consecutive years from January 2013 to December 2017 in Beijing, combined with simultaneous measurement of gaseous precursors and meteorological ...Based on online observations of fine particulate matter(PM2.5) for five consecutive years from January 2013 to December 2017 in Beijing, combined with simultaneous measurement of gaseous precursors and meteorological parameters, the evolution and meteorological causes of fineparticle explosive growth(FPEG) events were analyzed. During the 5-year observation period,132 FPEG events were observed and these events were further divided into three types(3-, 6-, and 9-h events) according to their evolution duration. The majority of FPEG events were observed in winter under the conditions of higher gas precursor concentrations and unfavorable meteorological conditions. The average concentration of PM2.5 during winter FPEG events changed little from 2013 to 2016, whereas it decreased significantly in 2017, in accordance with the similar variation of gaseous species(SO2, NO2, and CO). In addition, the higher wind speeds and lowest relative humidity observed in 2017 were also conducive to the decrease in PM2.5. The evolutions of FPEG events and normal haze episodes were analyzed, revealing that the rate of increase in NO2 was much greater than that of SO2, suggesting more of a contribution from mobile sources than stationary sources. The polar Plot results suggest that the transportation from the southeast area of Beijing plays a major role in the formation of 3-h events, whereas local emissions is the main contributory factor for 9-h events and normal haze episodes. However, further quantitative analysis regarding the contributions of these factors is still needed.展开更多
Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical...Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical reaction of CaC_(2) and a carbonate(CaCO_(3),Na2CO_(3),or NaHCO_(3))at ambient temperature.The resultant OACMs are micro mesoporous carbon nanomaterials with high specific area(>648 m2 g^(-1)),highly crosslinked texture,and rich alkynyl and oxygenated groups.The OACMs exhibit excellent Hg(Ⅱ)adsorption due to the soft acid-soft base interaction between alkynyl and Hg(Ⅱ),and OACM-3 derived from CaC_(2) and NaHCO_(3) has the saturated Hg(Ⅱ)adsorbance of 483.9 mg g^(-1)along with good selectivity and recyclability.The adsorption is mainly chemisorption following the Langmuir mode.OACM-3 also shows high adsorbance for other heavy metal ions,e.g.256.6 mg g^(-1)for Pb(II),232.4 mg g^(-1)for Zn(II),and 198.7 mg g^(-1)for Cu(II).This work expands the mechnochemical reaction of CaC_(2)with carbonates and possibly other oxyanionic salts,provides a new synthesis approach for functional alkynyl carbon materials with excellent adsorption performance for heavy metal ions,as well as a feasible approach for CO2 resource utilization.展开更多
To explore the problems of monitoring chemical processes with large numbers of input parameters, a method based on Auto-associative Hierarchical Neural Network(AHNN) is proposed. AHNN focuses on dealing with datasets ...To explore the problems of monitoring chemical processes with large numbers of input parameters, a method based on Auto-associative Hierarchical Neural Network(AHNN) is proposed. AHNN focuses on dealing with datasets in high-dimension. AHNNs consist of two parts: groups of subnets based on well trained Autoassociative Neural Networks(AANNs) and a main net. The subnets play an important role on the performance of AHNN. A simple but effective method of designing the subnets is developed in this paper. In this method,the subnets are designed according to the classification of the data attributes. For getting the classification, an effective method called Extension Data Attributes Classification(EDAC) is adopted. Soft sensor using AHNN based on EDAC(EDAC-AHNN) is introduced. As a case study, the production data of Purified Terephthalic Acid(PTA) solvent system are selected to examine the proposed model. The results of the EDAC-AHNN model are compared with the experimental data extracted from the literature, which shows the efficiency of the proposed model.展开更多
In this study,ultrasonic field was applied during potassium hydroxide(KOH) pretreatment of wheat straw(WS).Three concentrations of KOH(2%,4%,and 6%) were tested during pretreatment.The results showed that there was a ...In this study,ultrasonic field was applied during potassium hydroxide(KOH) pretreatment of wheat straw(WS).Three concentrations of KOH(2%,4%,and 6%) were tested during pretreatment.The results showed that there was a significant influence of the ultrasonic assisted KOH pretreatment(KOH(Upt)) on physiochemical characteristics of WS during pretreatment as well as on digester performance.The pretreatment time was optimized to 36 h for all KOH concentrations.The highest total volatile fatty acid(TVFA) productions(3189 mg·L^-1) from 6%KOHupt samples were observed.Similarly,the SEM analysis and FTIR observation revealed that KOH(Upt) effectively disrupted the physical morphology of WS and successful breaking of lignin and hemicellulose linkage between carboxyl groups.Moreover,the highest biogasification(555 ml·(g VS(loaded))^-1) and biomethane productions(282 ml·(g VS(loaded))^-1) from 4%KOH(Upt) digesters,with 69% of biodegradability,indicated significant availability of organic matter from KOH(Upt).The R^2 values(0.993-0.998) in Modified Gompertz Model indicated that the model was feasible to predict methane yield for this study.Similarly,the Bo values for 4%KOH(Upt)(283.30±2.74 ml·(gVS(loaded))^-1) were also in agreement to the experimental methane yield.These results suggested that ultrasonic addition during KOH pretreatment of WS can effectively increase the organic yield during pretreatment.Moreover,the increase in methane production from 4% KOH(Upt) suggested that digester performance can be improved with lower KOH concentrations using this pretreatment.展开更多
This study presents a novel technique for the controllable preparation of photoluminescent substrates to enhance the photochemical microfluidic synthesis of vitamin D_3.The dip-coating method to prepare the substrates...This study presents a novel technique for the controllable preparation of photoluminescent substrates to enhance the photochemical microfluidic synthesis of vitamin D_3.The dip-coating method to prepare the substrates was experimentally optimized,and the corresponding emission behaviors were systematically investigated.The substrates were successfully used to enhance the ultraviolet B(UVB) emission of a low-power light source(e.g.,an 8 W lamp),whose UVB emission intensity was increased by approximately 11 times.By virtue of the novel light source,the productivity of a single set of photochemical microreactor with a 12-meter-long channel(0.6 mm i.d.) was increased to 1.83 kg·a^(-1),which was 42% higher than that of a 100 W lamp,and no cooling devices were used.The method is simple and has great potential to replace traditional medium-pressure mercury lamps for UVB-irradiated photochemical reactions.展开更多
Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utiliza...Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utilization efficiency.However,there is still a lack of systematic screening and optimization of local structures surrounding active centers of SACs for ORR as the local coordination has an essential impact on their electronic structures and catalytic performance.Herein,we systematic study the ORR catalytic performance of M-NC SACs with different central metals and environmental atoms in the first and second coordination sphere by using density functional theory(DFT)calculation and machine learning(ML).The geometric and electronic informed overpotential model(GEIOM)based on random forest algorithm showed the highest accuracy,and its R^(2) and root mean square errors(RMSE)were 0.96 and 0.21,respectively.30 potential high-performance catalysts were screened out by GEIOM,and the RMSE of the predicted result was only 0.12 V.This work not only helps us fast screen high-performance catalysts,but also provides a low-cost way to improve the accuracy of ML models.展开更多
Ciprofloxacin(CIP), moxifoxacin(MOX) and enrofloxacin(ENR) were selected as typical fluoroquinolones(FQs) to analyze the excitation-enhancing effect and mechanism of solvents on FQs' electron transition based...Ciprofloxacin(CIP), moxifoxacin(MOX) and enrofloxacin(ENR) were selected as typical fluoroquinolones(FQs) to analyze the excitation-enhancing effect and mechanism of solvents on FQs' electron transition based on quantum chemical calculations. The UV spectra of three FQs in gas and five different solvents(water, cyclohexane, dimethylsulfoxide, methanol, acetone) were calculated using Gaussian 09 software. The transition mechanisms of FQs' main electron transitions were analyzed by natural bond orbital(NBO) theory, and the solvent effect on each electron transition was assessed qualitatively and quantitatively by sensitivity analysis and an established index system. The excitation enhancing mechanism of solvent on electron transitions of FQs was analyzed from the view of photo-induced reactions between solvent and FQs molecules. The results show that there are two main transitions located in the spectrum ranges of 300~380 and 240~300 nm for each FQ in any medium, which are assigned as n →π* and π→π* electron transitions, respectively. By comparison, the n →π* transition is more sensitive to solvent because of the energy transfer between solvent molecules and FQs, but the solvent effect on the π→π* transition is stronger than on the n →π* transition. The sequence of affected extent of solvent effect on electron transition was CIP 〉 MOX 〉 ENR, and the sequence of solvent effect was water 〉 DMSO 〉 methanol 〉 acetone 〉 cyclohexane(stronger solvent effect with increasing the dielectric constant of solvent). From the view of photo-induced reactions, the reaction between FQs*T1 and solvent*T1 has the decisive regulatory effect on the n →π* transition of FQs in solvent, and the reaction between FQsS0 and solvent*TI has an enhancing effect on the π→π* transition.展开更多
The use of carbon‐based materials is an appealing strategy to solve the issue of excessive CO_(2) emis‐sions.In particular,metal‐free nitrogen‐doped carbon materials(mf‐NCs)have the advantages of convenient synth...The use of carbon‐based materials is an appealing strategy to solve the issue of excessive CO_(2) emis‐sions.In particular,metal‐free nitrogen‐doped carbon materials(mf‐NCs)have the advantages of convenient synthesis,cost‐effectiveness,and high conductivity and are ideal electrocatalysts for the CO_(2) reduction reaction(CO_(2)RR).However,the unclear identification of the active N sites and the low intrinsic activity of mf‐NCs hinder the further development of high‐performance CO_(2)RR electrocat‐alysts.Achieving precise control over the synthesis of mf‐NC catalysts with well‐defined active N‐species sites is still challenging.To this end,we adopted a facile synthesis method to construct a set of mf‐NCs as robust catalysts for CO_(2)RR.The resulting best‐performing catalyst obtained a Far‐adaic efficiency of CO of approximately 90%at−0.55 V(vs.reversible hydrogen electrode)and good stability.The electrocatalytic performance and in situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy measurements collectively revealed that graphitic and pyridinic N can synergistically adsorb CO_(2) and H_(2)O and thus promote CO_(2) activation and protonation.展开更多
The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was e...The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.展开更多
基金supported by the National Key R&D Program of China[2021YFC2103500]National Natural Science Foundation of China(22211530047)+1 种基金Tianjin Synthetic Biotechnology Innovation Capacity Improvement Project[grant numbers:TSBICIP-KJGG-009]the Beijing Advanced Innovation Center for Soft Matter Science and Engineering,Beijing University of Chemical Technology.
文摘For decades micoorganisms have been engineered for the utilization of lignocellulose-based second-generation (2G) feedstocks, but with theconcerns of increased levels of atmospheric CO_(2) causing global warming there is an emergent need to transition from the utilization of 2Gfeedstocks to third-generation (3G) feedstocks such as CO_(2) and its derivatives. Here, we established a yeast platform that is capable ofsimultaneously converting 2G and 3G feedstocks into bulk and value-added chemicals. We demonstrated that by adopting 3G substrates such asCO_(2) and formate, the conversion of 2G feedstocks could be substantially improved. Specifically, formate could provide reducing power andenergy for xylose conversion into valuable chemicals. Simultaneously, it can form a concentrated CO_(2) pool inside the cell, providing thermodynamically and kinetically favoured amounts of precursors for CO_(2) fixation pathways, e.g., the Calvin–Benson–Bassham (CBB) cycle.Furthermore, we demonstrated that formate could directly be utilized as a carbon source by yeast to synthesize endogenous amino acids. Theengineered strain achieved a one-carbon (C1) assimilation efficiency of 9.2%, which was the highest efficiency observed in the co-utilization of2G and 3G feedstocks. We applied this strategy for productions of both bulk and value-added chemicals, including ethanol, free fatty acids(FFAs), and longifolene, resulting in yield enhancements of 18.4%, 49.0%, and ~100%, respectively. The strategy demonstrated here for coutilization of 2G and 3G feedstocks sheds lights on both basic and applied research for the up-coming establishment of 3G biorefineries.
基金Supported by the National Natural Science Foundation of China (20821004 20990221) the National High Technology Research and Development Program of China (2006AA030202)
文摘With the application of HIGEE process intensification technology, petroleum sulfonate surfactant used for enhanced oil recovery was synthesized from petroleum fraction of Shengli crude oil with three sulfonating agents, including diluted liquid sulfur trioxide, diluted gaseous sulfur trioxide and fuming sulfuric acid. For each sulfonating agent, different operation modes (liquid-liquid or gas-liquid reaction with semi-continuous or continuous operation) were applied. The effects of various experimental conditions, such as solvent/oil mass ratio, sulfonating agent/oil mass ratio, gas/liquid ratio, gas concentration, reaction temperature, rotating speed, circulation ratio, reaction time and aging time, on the content of active matter and unsulfonated oil were investigated. Under relatively optimal reaction conditions, the target product was prepared with high mass content of active matter (up to 45.3%) and extremely low oil/water interfacial tension (4.5×10 –3 mN·m –1 ). The product quality and process efficiency are higher compared with traditional sulfonation technology.
文摘NiOOH was prepared by one-step electrolysis of spherical Ni(OH)2 and the effects of electrolysis parameters were examined. The highly pure NiOOH was obtained after electrolysis at a current density of 60mA.g^-1 and 30℃ with anodic potential controlled in the range of 1.73-1.85V (vs. Zn/ZnO) for 360min. The NiOOH samriles were characterized bv X-ray oowder diffraction (XRD) and scanning electron microscope (SEM) analysis.Resuits indicate that the electrolysis product is spherical NiOOH doped with graphite. Charge and discharge tests show that the prepared NiOOH offers a discharge capacity of over 270mAh·g^-1 at current density of 30mA·g^-1 and can be directly used as cathode material of alkaline Zn/NiOOH batteries. Galvanostatic charge/discharge and cyclic voltammetry (CV) tests reveal good cycling reversibility, of the NiOOH electrode.
文摘Electrochemical dechlorination of chloroform in neutral aqueous solution was investigated using palladium-loaded electrodes at ambient temperature. Palladium/foam-nickel (Pd/foam-Ni) and palladium/polymeric pyrrole film/foam-nickel (Pd/PPy/foam-Ni) composite electrodes which provided catalytic surface for reductive dechlorination of chloroform in aqueous solution were prepared using an electrodepositing method. Scanning electron microscope (SEM) micrographs showed that polymeric pyrrole film modified the electrode-surface characteristics and resulted in the uniform dispersion of needle-shaped palladium particles on foam-Ni supporting electrode. The experimental results of dechlorination indicated that the removal efficiency of chloroform and current efficiency in neutral aqueous solution on Pd/PPy/foam-Ni electrode could be up to 36.8% and 33.0% at dechlorination current of 0.1 mA and dechlorination time of 180 min, which is much higher than that of Pd/foam-Ni electrode.
基金the funding support from the Tianjin City Science and Technology Planning Project of the People’s Republic of China(grant number 18ZXSZSF00120).
文摘Rice straw physicochemical characteristics and anaerobic digestion(AD)performance via ammonia pretreatment at varying ammonia concentrations(2%,4%,and 6%)and moisture contents(30%,50%,70%,and 90%)under a mild condition were investigated.The results showed that the ammonia pretreatment effectively damaged the rice straw structure,increased the soluble organic concentration,and improved rice straw hydrolysis and AD performance.After pretreatment,the ester bond and ether bond were ruptured in lignocellulose and the volatile fatty acids(VFAs)were within the range of 1457.81–1823.67 mg·L-1.In addition,ammonia pretreatment had high selectivity on lignin removal,resulting in a maximum lignin removal rate of 50.80%.The highest methane yield of rice straw was 250.34 ml·(g VS)-1 at a 4%ammonia concentration coupled with a 70%moisture content,which was 28.55%higher than that of the control.The result showed that ammonia pretreatment of rice straw is technically suitable to enhance AD performance for further application.
基金Supported by the National Natural Science Foundation of China (No. 50635010) and the National High Technology Research and Development Program of China ( No. 2007AA04Z422 ).
文摘An active balancing technology has been applied to solve the severe vibration caused by sudden unbalance in rotating machineries during their working process. First, based on the generation principle of sudden unbalance, a simulation test stand with a sudden unbalance generation device was set up. Then, the balancing planes were optimized by using the finite element method (FEM) to determine the position for balancing device installation. Finally, the active balancing experiments were carried out on the test stand. The experimental results indicate that the vibration response caused by sudden unbalance can be decreased from 77μm to 8μm by using the active balancing device, and the vibration amplitude reduction was up to 89.6%. From this example, it can be concluded that the active balancing device, which is installed on a proper position of the rotor, can effectively control the random transient synchronous vibration, demonstrating its high value in engineering practice.
基金supported by the National Natural Science Foundation of China(Nos.2177060378,21627813,and 21521005)the Program for Changjiang Scholars,Innovative Research Teams in Universities(No.IRT1205)the Fundamental Research Funds for the Central Universities(Nos.12060093063 and XK1803-05).
文摘Coordination tuning electronic structure of host materials is a quite effective strategy for activating and improving the intrinsic properties.Herein,halogen anion(X-)-incorporated β-FeOOH(β-FeOOH(X),X=F-,Cl-,and Br-) was investigated with a spontaneous adsorption process,which realized a great improvement of supercapacitor performances by adjusting the coordination geometry.Experiments coupled with theoretical calculations demonstrated that the change of Fe-O bond length and structural distortion of β-FeOOH,which is rooted in halogen ions embedment,led to the relatively narrow band gap.Because of the strong electronegativity of X-,the Fe element in β-FeOOH(X)s presented the unexpected high valence state(3+δ),which is facilitating to adsorb S032-species.Consequently,the designed β-FeOOH(X)s exhibited the good electric conductivity and enhanced the contact between electrode and electrolyte.When used as a negative electrode,the β-FeOOH(F) showed the excellent specific capacity of 391.9 F g-1 at 1 A g-1 current density,almost tenfold improvement compared with initial β-FeOOH,with the superior rate capacity and cyclic stability.This combinational design principle of electronic structure and electrochemical performances provides a promising way to develop advanced electrode materials for supercapacitor.
文摘Ti-Ce, Ti-Si binary and Ti-Ce-Si ternary novel nanocomposite oxide photocatalysts were prepared with cheap inorganic salts TiCI4, Na2SiO3·9H2O and Ce(NO3)3·6H2O as precursors by supercritical fluid drying (SCFD) technology. The catalysts were characterized by means of XRD and TEM. The particle size of nanocomposite oxide photocatalysts synthesized by SCFD method is about 6 - 11 nm, which is smaller than those obtained by common drying method (CD). The phase transformation from anatase to rutile was inhibited by SCFD technology. The peaks of SiO2 and CeO2 in XRD patterns indicate that a SiO2 amorphorous phase exists in all the samples and CeO2 is well dispersed on the surface of TiO2. The orthogonal test was designed to optimize the preparing conditions. It is found that ceria dop;.ng enhances the photocatalyric activity markedly, and the optimum doping of CeO2 is 0.1%. The thermal stability of photocatalyst can be improved ; the growth of particle-size and the decrease of surface area can be prohibited by doping of SlOe. Heat-treatment is a necessary factor to induce chemistry change of Ti-Si surface. The optimum heat-treating temperature is 600℃. A novel and efficient Ti-Ce-Si ternary nanocomposite was prepared by SCFI) method with strong thermal stability and high photoactivity in the photodegratation of phenol.
基金Project(50571006) supported by the National Natural Science Foundation of China
文摘The elimination of toxic materials in sealing methods for anodic films on 1070 aluminum alloy was studied. The new process uses chemical treatments in cerium solution and an electrochemical treatment in a molybdate solution. Potentiodynamic polarization and electrochemical impedance spectroscopy(EIS) were used to study the influences of sealing methods on the corrosion behavior of anodic films in NaCl solutions. The results show that the Ce-Mo sealing makes the surface structure and morphology of anodic films uniform and compact. Ce and Mo produce a cooperative effect to improve the corrosion resistance of anodic films. Anodic films sealed by Ce-Mo provide high corrosion resistance both in acidic and basic solutions.
基金This work was financially supported by the National Natural Science Foundation of China(Grant Nos.21811530003,21861132017,U1663227,21706006)。
文摘The use of traditional chemical catalysis to produce chemicals has a series of drawbacks,such as high dependence on fossil resources,high energy consumption,and environmental pollution.With the development of synthetic biology and metabolic engineering,the use of renewable biomass raw materials for chemicals synthesis by constructing efficient microbial cell factories is a green way to replace traditional chemical catalysis and traditional microbial fermentation.This review mainly summarizes several types of bulk chemicals and high value-added chemicals using metabolic engineering and synthetic biology strategies to achieve efficient microbial production.In addition,this review also summarizes several strategies for effectively regulating microbial cell metabolism.These strategies can achieve the coupling balance of material and energy by regulating intracellular material metabolism or energy metabolism,and promote the efficient production of target chemicals by microorganisms.
基金support from National Science Foundation of China(No.22075012).
文摘A convenient method for methane(CH_(4))direct conversion to methanol(CH_(3)OH)is of great significance to use methane-rich resources,especially clathrates and stranded shale gas resources located in remote regions.Theoretically,the activation of CH_(4) and the selectivity to the CH_(3)OH product are challenging due to the extreme stability of CH_(4) and relatively high reactivity of CH_(3)OH.The state-of-the-art‘methane reforming-methanol synthesis’process adopts a two-step strategy to avoid the further reaction of CH_(3)OH under the harsh conditions required for CH_(4) activation.In the electrochemical field,researchers are trying to develop conversion pathways under mild conditions.They have found suitable catalysts to activate the C–H bonds in methane with the help of external charge and have designed the electrode reactions to continuously generate certain active oxygen species.These active oxygen species attack the activated methane and convert it to CH_(3)OH,with the benefit of avoiding over-oxidation of CH_(3)OH,and thus obtain a high conversion efficiency of CH_(4) to CH_(3)OH.This mini-review focuses on the advantages and challenges of electrochemical conversion of CH4 to CH_(3)OH,especially the strategies for supplying electro-generated active oxygen species in-situ to react with the activated methane.
基金This study was supported by The Ministry of Science and Technology of the people's Republic of China:[Grant Numbers 2017YFC0210000 and 2016YFC0202700]the National Natural Science Foundation of China:[Grant Number 41705110].
文摘Based on online observations of fine particulate matter(PM2.5) for five consecutive years from January 2013 to December 2017 in Beijing, combined with simultaneous measurement of gaseous precursors and meteorological parameters, the evolution and meteorological causes of fineparticle explosive growth(FPEG) events were analyzed. During the 5-year observation period,132 FPEG events were observed and these events were further divided into three types(3-, 6-, and 9-h events) according to their evolution duration. The majority of FPEG events were observed in winter under the conditions of higher gas precursor concentrations and unfavorable meteorological conditions. The average concentration of PM2.5 during winter FPEG events changed little from 2013 to 2016, whereas it decreased significantly in 2017, in accordance with the similar variation of gaseous species(SO2, NO2, and CO). In addition, the higher wind speeds and lowest relative humidity observed in 2017 were also conducive to the decrease in PM2.5. The evolutions of FPEG events and normal haze episodes were analyzed, revealing that the rate of increase in NO2 was much greater than that of SO2, suggesting more of a contribution from mobile sources than stationary sources. The polar Plot results suggest that the transportation from the southeast area of Beijing plays a major role in the formation of 3-h events, whereas local emissions is the main contributory factor for 9-h events and normal haze episodes. However, further quantitative analysis regarding the contributions of these factors is still needed.
基金supports from the National Natural Science Foundation of China(No.21776015)the University Scientific Research Project of Anhui Province(No.KJ2018A0065&KJ2020A0245).
文摘Adsorptive removal of heavy metal ions from wastewater is very important,and the key is the development of efficient sorbents.In this work,oxygenated alkynyl carbon materials(OACMs)were synthesized via mechanochemical reaction of CaC_(2) and a carbonate(CaCO_(3),Na2CO_(3),or NaHCO_(3))at ambient temperature.The resultant OACMs are micro mesoporous carbon nanomaterials with high specific area(>648 m2 g^(-1)),highly crosslinked texture,and rich alkynyl and oxygenated groups.The OACMs exhibit excellent Hg(Ⅱ)adsorption due to the soft acid-soft base interaction between alkynyl and Hg(Ⅱ),and OACM-3 derived from CaC_(2) and NaHCO_(3) has the saturated Hg(Ⅱ)adsorbance of 483.9 mg g^(-1)along with good selectivity and recyclability.The adsorption is mainly chemisorption following the Langmuir mode.OACM-3 also shows high adsorbance for other heavy metal ions,e.g.256.6 mg g^(-1)for Pb(II),232.4 mg g^(-1)for Zn(II),and 198.7 mg g^(-1)for Cu(II).This work expands the mechnochemical reaction of CaC_(2)with carbonates and possibly other oxyanionic salts,provides a new synthesis approach for functional alkynyl carbon materials with excellent adsorption performance for heavy metal ions,as well as a feasible approach for CO2 resource utilization.
基金Supported by the National Natural Science Foundation of China(61074153)
文摘To explore the problems of monitoring chemical processes with large numbers of input parameters, a method based on Auto-associative Hierarchical Neural Network(AHNN) is proposed. AHNN focuses on dealing with datasets in high-dimension. AHNNs consist of two parts: groups of subnets based on well trained Autoassociative Neural Networks(AANNs) and a main net. The subnets play an important role on the performance of AHNN. A simple but effective method of designing the subnets is developed in this paper. In this method,the subnets are designed according to the classification of the data attributes. For getting the classification, an effective method called Extension Data Attributes Classification(EDAC) is adopted. Soft sensor using AHNN based on EDAC(EDAC-AHNN) is introduced. As a case study, the production data of Purified Terephthalic Acid(PTA) solvent system are selected to examine the proposed model. The results of the EDAC-AHNN model are compared with the experimental data extracted from the literature, which shows the efficiency of the proposed model.
基金supported by Yuan Yi Biomass S&T Company of China(No.H2015198)。
文摘In this study,ultrasonic field was applied during potassium hydroxide(KOH) pretreatment of wheat straw(WS).Three concentrations of KOH(2%,4%,and 6%) were tested during pretreatment.The results showed that there was a significant influence of the ultrasonic assisted KOH pretreatment(KOH(Upt)) on physiochemical characteristics of WS during pretreatment as well as on digester performance.The pretreatment time was optimized to 36 h for all KOH concentrations.The highest total volatile fatty acid(TVFA) productions(3189 mg·L^-1) from 6%KOHupt samples were observed.Similarly,the SEM analysis and FTIR observation revealed that KOH(Upt) effectively disrupted the physical morphology of WS and successful breaking of lignin and hemicellulose linkage between carboxyl groups.Moreover,the highest biogasification(555 ml·(g VS(loaded))^-1) and biomethane productions(282 ml·(g VS(loaded))^-1) from 4%KOH(Upt) digesters,with 69% of biodegradability,indicated significant availability of organic matter from KOH(Upt).The R^2 values(0.993-0.998) in Modified Gompertz Model indicated that the model was feasible to predict methane yield for this study.Similarly,the Bo values for 4%KOH(Upt)(283.30±2.74 ml·(gVS(loaded))^-1) were also in agreement to the experimental methane yield.These results suggested that ultrasonic addition during KOH pretreatment of WS can effectively increase the organic yield during pretreatment.Moreover,the increase in methane production from 4% KOH(Upt) suggested that digester performance can be improved with lower KOH concentrations using this pretreatment.
基金the National Natural Science Foundation of China (21978008, 21606008)the State Key Laboratory of Chemical Engineering (SKL-ChE-17A02)the Fundamental Research Funds for the Central Universities (JD2017)。
文摘This study presents a novel technique for the controllable preparation of photoluminescent substrates to enhance the photochemical microfluidic synthesis of vitamin D_3.The dip-coating method to prepare the substrates was experimentally optimized,and the corresponding emission behaviors were systematically investigated.The substrates were successfully used to enhance the ultraviolet B(UVB) emission of a low-power light source(e.g.,an 8 W lamp),whose UVB emission intensity was increased by approximately 11 times.By virtue of the novel light source,the productivity of a single set of photochemical microreactor with a 12-meter-long channel(0.6 mm i.d.) was increased to 1.83 kg·a^(-1),which was 42% higher than that of a 100 W lamp,and no cooling devices were used.The method is simple and has great potential to replace traditional medium-pressure mercury lamps for UVB-irradiated photochemical reactions.
基金financially supported by the National Key Research and Development Program of China (2018YFA0702002)the Beijing Natural Science Foundation (Z210016)the National Natural Science Foundation of China (21935001)。
文摘Single atomic catalysts(SACs),especially metal-nitrogen doped carbon(M-NC)catalysts,have been extensively explored for the electrochemical oxygen reduction reaction(ORR),owing to their high activity and atomic utilization efficiency.However,there is still a lack of systematic screening and optimization of local structures surrounding active centers of SACs for ORR as the local coordination has an essential impact on their electronic structures and catalytic performance.Herein,we systematic study the ORR catalytic performance of M-NC SACs with different central metals and environmental atoms in the first and second coordination sphere by using density functional theory(DFT)calculation and machine learning(ML).The geometric and electronic informed overpotential model(GEIOM)based on random forest algorithm showed the highest accuracy,and its R^(2) and root mean square errors(RMSE)were 0.96 and 0.21,respectively.30 potential high-performance catalysts were screened out by GEIOM,and the RMSE of the predicted result was only 0.12 V.This work not only helps us fast screen high-performance catalysts,but also provides a low-cost way to improve the accuracy of ML models.
文摘Ciprofloxacin(CIP), moxifoxacin(MOX) and enrofloxacin(ENR) were selected as typical fluoroquinolones(FQs) to analyze the excitation-enhancing effect and mechanism of solvents on FQs' electron transition based on quantum chemical calculations. The UV spectra of three FQs in gas and five different solvents(water, cyclohexane, dimethylsulfoxide, methanol, acetone) were calculated using Gaussian 09 software. The transition mechanisms of FQs' main electron transitions were analyzed by natural bond orbital(NBO) theory, and the solvent effect on each electron transition was assessed qualitatively and quantitatively by sensitivity analysis and an established index system. The excitation enhancing mechanism of solvent on electron transitions of FQs was analyzed from the view of photo-induced reactions between solvent and FQs molecules. The results show that there are two main transitions located in the spectrum ranges of 300~380 and 240~300 nm for each FQ in any medium, which are assigned as n →π* and π→π* electron transitions, respectively. By comparison, the n →π* transition is more sensitive to solvent because of the energy transfer between solvent molecules and FQs, but the solvent effect on the π→π* transition is stronger than on the n →π* transition. The sequence of affected extent of solvent effect on electron transition was CIP 〉 MOX 〉 ENR, and the sequence of solvent effect was water 〉 DMSO 〉 methanol 〉 acetone 〉 cyclohexane(stronger solvent effect with increasing the dielectric constant of solvent). From the view of photo-induced reactions, the reaction between FQs*T1 and solvent*T1 has the decisive regulatory effect on the n →π* transition of FQs in solvent, and the reaction between FQsS0 and solvent*TI has an enhancing effect on the π→π* transition.
文摘The use of carbon‐based materials is an appealing strategy to solve the issue of excessive CO_(2) emis‐sions.In particular,metal‐free nitrogen‐doped carbon materials(mf‐NCs)have the advantages of convenient synthesis,cost‐effectiveness,and high conductivity and are ideal electrocatalysts for the CO_(2) reduction reaction(CO_(2)RR).However,the unclear identification of the active N sites and the low intrinsic activity of mf‐NCs hinder the further development of high‐performance CO_(2)RR electrocat‐alysts.Achieving precise control over the synthesis of mf‐NC catalysts with well‐defined active N‐species sites is still challenging.To this end,we adopted a facile synthesis method to construct a set of mf‐NCs as robust catalysts for CO_(2)RR.The resulting best‐performing catalyst obtained a Far‐adaic efficiency of CO of approximately 90%at−0.55 V(vs.reversible hydrogen electrode)and good stability.The electrocatalytic performance and in situ attenuated total reflectance surface‐enhanced infrared absorption spectroscopy measurements collectively revealed that graphitic and pyridinic N can synergistically adsorb CO_(2) and H_(2)O and thus promote CO_(2) activation and protonation.
基金Supported by the National Natural Science Foundation of China(21276013,21676008)Specialized Research Fund for the Doctoral Program of Higher Education of China(20130010110001)
文摘The study herein investigated the effectiveness of simultaneous use of ozone and hydrogen peroxide(O_3/H_2O_2 process) to degrade o-phenylenediamine(o-PDA) in a simulated wastewater. A rotor–stator reactor(RSR) was employed to create a high-gravity environment in order to enhance ozone-liquid mass transfer rate and possibly improve the degradation rate of o-PDA. The degradation efficiency of o-PDA(η) as well as the overall gas-phase volumetric mass transfer coefficient(KGa) were determined under different operating conditions of H_2O_2 concentration, initial o-PDA concentration, temperature of reaction, initial p H and rotation speed of RSR in attempt to establish the optimal conditions. Chemical oxygen demand reduction rate(rCOD) of wastewater treated at a particular set of conditions was also analyzed. Additionally, the intermediate products of degradation were identified using a gas chromatography-mass spectrometer(GC/MS) to further evaluate the extent of o-PDA degradation as well as establish its possible degradation pathway. Results were validated by comparison with those of sole use of ozone(O_3 process), and it was noted that η, KGa and rCODachieved by O_3/H_2O_2 process was 24.4%,31.6% and 25.2% respectively higher than those of O_3 process, indicating that H_2O_2 can greatly enhance ozonation of o-PDA. This work further demonstrates that an RSR can significantly intensify ozone-liquid mass transfer rate and thus provides a feasible intensification means for the ozonation of o-PDA as well as other recalcitrant organics.