The magnetization reduction of hematite using biomass waste can effectively utilize waste and reduce CO_(2) emission to achieve the goals of carbon peaking and carbon neutrality.The effects of temperatures on suspensi...The magnetization reduction of hematite using biomass waste can effectively utilize waste and reduce CO_(2) emission to achieve the goals of carbon peaking and carbon neutrality.The effects of temperatures on suspension magnetization roasting of hematite using biomass waste for evolved gases have been investigated using TG-FTIR,Py-GC/MS and gas composition analyzer.The mixture reduction process is divided into four stages.In the temperature range of 200-450℃ for mixture,the release of CO_(2),acids,and ketones is dominated in gases products.The yield and concentration of small molecules reducing gases increase when the temperature increases from 450 to 900℃.At 700℃,the volume concentrations of CO,H_(2) and CH_(4) peak at 8.91%,8.90% and 4.91%,respectively.During the suspension magnetization roasting process,an optimal iron concentrate with an iron grade of 70.86%,a recovery of 98.66% and a magnetic conversion of 45.70% is obtained at 700℃.Therefore,the magnetization reduction could react greatly in the temperature range of 600 to 700℃ owing to the suitable reducing gases.This study shows a detail gaseous evolution of roasting temperature and provides a new insight for studying the reduction process of hematite using biomass waste.展开更多
Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin f...Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.展开更多
The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge...The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.展开更多
A gold catalyst of Au/pyrenyl‑graphdiyne(Pyr‑GDY)was prepared by anchoring small size of gold nanoparticles(Au NPs)on the surface of Pyr‑GDY for electrocatalytic nitrogen reduction reaction(eNRR),in which Au NPs with ...A gold catalyst of Au/pyrenyl‑graphdiyne(Pyr‑GDY)was prepared by anchoring small size of gold nanoparticles(Au NPs)on the surface of Pyr‑GDY for electrocatalytic nitrogen reduction reaction(eNRR),in which Au NPs with a size of approximately 3.69 nm was evenly distributed on spongy‑like porous Pyr‑GDY.The catalyst exhibited a good electrocatalytic activity for N_(2)reduction in a nitrogen‑saturated electrolyte,with an ammonia yield of 32.1μg·h^(-1)·mg_(cat)^(-1)at-0.3 V(vs RHE),3.5 times higher than that of Au/C(Au NPs anchored on carbon black).In addition,Au/Pyr‑GDY showed a Faraday efficiency(FE)of 26.9%for eNRR,and a good catalysis durability for over 22 h.展开更多
The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely reported.However,most of metal single atoms in these c...The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely reported.However,most of metal single atoms in these catalysts were buried in the carbon matrix,resulting in a low metal utilization and inaccessibility for adsorption of reactants during the catalytic process.Herein,we reported a facile synthesis based on the hard-soft acid-base(HSAB)theory to fabricate Co single-atom catalysts with highly exposed metal atoms ligated to the external pyridinic-N sites of a nitrogen-doped carbon support.Benefiting from the highly accessible Co active sites,the prepared Co−N−C SAC exhibited a superior oxygen reduction reactivity comparable to that of the commercial Pt/C catalyst,showing a high turnover frequency(TOF)of 0.93 e^(−)·s^(-1)·site^(-1)at 0.85 V vs.RHE,far exceeding those of some representative SACs with a ultra-high metal content.This work provides a rational strategy to design and prepare M−N−C single-atom catalysts featured with high site-accessibility and site-density.展开更多
Manganese oxide ores from Gabon and Xiangxi were leached with waste tea as reductant in dilute sulfuric acid solution. The effects of waste tea dosage, concentration of sulfuric acid, liquid-to-solid ratio, leaching t...Manganese oxide ores from Gabon and Xiangxi were leached with waste tea as reductant in dilute sulfuric acid solution. The effects of waste tea dosage, concentration of sulfuric acid, liquid-to-solid ratio, leaching temperature and reaction time on leaching process were explored. The leaching efficiency of Gabonese manganese oxide ore reached almost 100% under the optimal condition which was determined as follows: manganese oxide ore to waste tea mass ratio of 10:1, sulfuric acid concentration of 2.5 molFL, liquid-to-solid ratio of 7.5:1, leaching temperature of 368 K, time of 8 h. The leaching efficiency of Xiangxi manganese oxide ore reached 99.8% under the optimal condition which was determined as follows: manganese oxide ore to waste tea mass ratio of 10:1, sulfuric acid concentration of 1.7 mol/L, liquid-to-solid ratio of 7.5:1, leaching temperature of 368 K, time of 8 h. The leaching process followed the internal diffusion controlled kinetic model, and the apparent activation energies of Gabonese manganese oxide ore and Xiangxi manganese oxide ore were calculated to be 38.2 kJ/mol and 20.4 kJ/mol, respectively. The morphological changes and mineralogical forms of the ore before and after the chemical treatment were discussed with the support of XRD analysis and SEM analysis.展开更多
The extraction of manganese from low-grade manganese oxide ores using Ca S derived from Ca SO4 as reductant was investigated. The effects of mass ratio of Ca S to ore, reduction temperature, reduction time, liquid to ...The extraction of manganese from low-grade manganese oxide ores using Ca S derived from Ca SO4 as reductant was investigated. The effects of mass ratio of Ca S to ore, reduction temperature, reduction time, liquid to solid ratio(L/S ratio), stirring speed, leaching temperature, leaching time and H2SO4 concentration on the leaching rates of Mn and Fe during the reduction–acid leaching process were discussed. The leaching rates of 96.47% for Mn and 19.24% for Fe were obtained under the optimized conditions of mass ratio of Ca S to manganese oxide ore 1:6.7, L/S ratio 5:1, stirring speed 300 r/min, reduction temperature of 95 °C for 2.0 h in the reduction process and leaching stirring speed of 200 r/min, H2SO4 concentration of 1.5 mol/L, leaching temperature of 80 °C for 5 min in the leaching process. In addition, this process can be employed in the recovery of manganese from various manganese oxide ores, and Mn leaching rate above 95% is obtained.展开更多
Iron and titanium were recovered from beach titanomagnetite(TTM) concentrate by embedding direct reduction and magnetic separation. The reduction products and the effects of the reductant type and reduction temperatur...Iron and titanium were recovered from beach titanomagnetite(TTM) concentrate by embedding direct reduction and magnetic separation. The reduction products and the effects of the reductant type and reduction temperature on the reduction behavior were investigated. The results showed that the reduction of TTM concentrate was strongly related to the gasification reactivity of the reductant. Bitumite presented a better product index than wheat-straw biochar and coke, mainly because the gasification reactivity of bitumite was better than that of the other reductants. In addition, high temperatures were not beneficial to embedding direct reduction because of the emergence of a molten phase and iron-joined crystals, which in turn reduced the diffusion rate of the reducing gas and impeded the reduction reaction in the central area of the roasted briquette. The use of bitumite as the reductant at a C/Fe molar ratio of 1.4 and a reduction temperature of 1200°C for 120 min resulted in direct-reduction iron powder assaying 90.28 wt% TFe and 0.91 wt% TiO_2 with an iron recovery of 91.83% and titanium concentrate assaying 46.01 wt% TiO_2 with a TiO_2 recovery of 91.19%. Titanium existed mainly in the form of anosovite and ilmenite in the titanium concentrate.展开更多
The present investigation examines the viability of dolochar, a sponge iron industry waste material, as a reductant in the reduction roasting of iron ore slimes, which are another waste generated by iron ore beneficia...The present investigation examines the viability of dolochar, a sponge iron industry waste material, as a reductant in the reduction roasting of iron ore slimes, which are another waste generated by iron ore beneficiation plants. Under statistically determined optimum conditions, which include a temperature of 900°C, a reductant-to-feed mass ratio of 0.35, and a reduction time of 30–45 min, the roasted mass, after being subjected to low-intensity magnetic separation, yielded an iron ore concentrate of approximately 64 wt% Fe at a mass recovery of approximately 71% from the feed iron ore slime assaying 56.2 wt% Fe. X-ray diffraction analyses indicated that the magnetic products contain magnetite and hematite as the major phases, whereas the nonmagnetic fractions contain quartz and hematite.展开更多
Measuring the dust explosion characteristics of aluminum-based activated fuels was a prerequisite for developing effective prevention and control measures.In this paper,ignition sensitivity,flame propagation behaviors...Measuring the dust explosion characteristics of aluminum-based activated fuels was a prerequisite for developing effective prevention and control measures.In this paper,ignition sensitivity,flame propagation behaviors and explosion severity of aluminum/polytetrafluoroethylene(Al/PTFE)compositions including 2 PT(2.80 wt.%F),4 PT(7.18 wt.%F)and 8 PT(11.90 wt.%F)were studied.When the content of F increased from 2.80 wt.%to 11.90 wt.%,the minimum explosive concentration MEC decreased from380 g/m^(3)to 140 g/m^(3),due to the dual effects of increased internal active aluminum and enhanced reactivity.The average flame propagation velocities increased as the percentage of F increased.The maximum explosion pressure Pmof 500 g/m3aluminum-based activated fuels increased from 247 k Pa to299 kPa.Scanning electron microscopy demonstrated that with the increase of PTFE content,the reaction was more complete.On this basis,the explosion mechanism of aluminum-based activated fuels was revealed.展开更多
The chemiluminescence reaction between luminol and reductant was investigated by a flow-injection system. The results show that this reaction can be used for the determination of the reductant which is active to chemi...The chemiluminescence reaction between luminol and reductant was investigated by a flow-injection system. The results show that this reaction can be used for the determination of the reductant which is active to chemiluminescence in alkaline lumminol, and of the substance which can, in appropriate manner, be converted into the active reductant. The mechanism of the chemiluminescence reaction may be that the reductant reduces dissolved oxygen to O2 , then O2 reacts with alkaline luminol to generate chemiluminescence.展开更多
Hydrazine sulfate was used as a reducing agent for the leaching of Li,Ni,Co and Mn from spent lithium-ion batteries.The effects of the reaction conditions on the leaching mechanism and kinetics were characterized and ...Hydrazine sulfate was used as a reducing agent for the leaching of Li,Ni,Co and Mn from spent lithium-ion batteries.The effects of the reaction conditions on the leaching mechanism and kinetics were characterized and examined.97%of the available Li,96%of the available Ni,95%of the available Co,and 86%of the available Mn are extracted under the following optimized conditions:sulfuric acid concentration of 2.0 mol/L,hydrazine sulfate dosage of 30 g/L,solid-to-liquid ratio of 50 g/L,temperature of 80℃,and leaching time of 60 min.The activation energies of the leaching are determined to be 44.32,59.37 and 55.62 k J/mol for Li,Ni and Co,respectively.By performing X-ray diffraction and scanning electron microscopy in conjunction with energy dispersive X-ray spectroscopy,it is confirmed that the main phase in the leaching residue is MnO2.The results show that hydrazine sulfate is an effective reducing agent in the acid leaching process for spent lithium-ion batteries.展开更多
The chemiluminescence reactions between lucigenin and reductants such as Mo(LII),V( II), U(III), W(III), Cr(II), Ti(III) and Fe( II), which were produced on-line by passing Mo(VI),V(V),U(VI), W(VI), Cr(VI,III),Ti(IV) ...The chemiluminescence reactions between lucigenin and reductants such as Mo(LII),V( II), U(III), W(III), Cr(II), Ti(III) and Fe( II), which were produced on-line by passing Mo(VI),V(V),U(VI), W(VI), Cr(VI,III),Ti(IV) and Fe(III) through a micro Jones column, are studied in detail. Results show that the reactions can be used directly for the determination of these substances. The mechanism of the reactions is also investigated.展开更多
The kinetics of reductive leaching of manganese from a low-grade manganese oxide ore were studied using cellulose as reductant in dilute sulfuric acid medium.It was found that when the stirring speed was higher than 2...The kinetics of reductive leaching of manganese from a low-grade manganese oxide ore were studied using cellulose as reductant in dilute sulfuric acid medium.It was found that when the stirring speed was higher than 200 r/min,the effect of gas film diffusion on manganese extraction efficiency could be neglected,and the kinetic behavior was investigated under the condition of elimination of external diffusion influence on the leaching process.Effects of leaching temperature,mass ratio of cellulose and ore,and the sulfuric acid concentration on manganese extraction efficiency were discussed.The kinetic data were analyzed based on the shrinking core model,which indicated that the leaching process was dominated by both ash layer diffusion and chemical reaction at the initial stage,with the progress of leaching reaction,the rate-controlling step switched to the ash layer diffusion.It was also concluded that the sulfuric acid concentration had the most significant influence on the leaching rate,the reaction orders with respect to the sulfuric acid concentration were 2.102 in the first 60 min,and 3.642 in the later 90 min,while the reaction orders for mass ratio of cellulose and ore were 0.660 and 0.724,respectively.An Arrhenius relationship was used to relate the temperature to the rate of leaching,from which apparent activation energies were calculated to be 46.487 kJ/mol and 62.290 kJ/mol at the two stages,respectively.Finally,the overall leaching rate equations for the manganese dissolution reaction with cellulose in sulphuric acid solution were developed.The morphological changes and mineralogical forms of the ore before and after the chemical treatment were discussed with the support of SEM and XRD analyses.展开更多
To improve the thermal properties of aluminum(Al)in the energetic system,a coated structure with ammonium perchlorate(AP)was prepared by a facile approach.And N,N-Dimethylformamide(DMF)was chosen as an ideal solvent b...To improve the thermal properties of aluminum(Al)in the energetic system,a coated structure with ammonium perchlorate(AP)was prepared by a facile approach.And N,N-Dimethylformamide(DMF)was chosen as an ideal solvent based on heterogeneous nucleation theory and molecular dynamics simulation.This coated structure could enlarge the contact area and improve the reaction environment to enhance the thermal properties.The addition of AP could accelerate oxidation temperature of Al with around 17.5°C.And the heat release of 85@15 composition rises to 26.13 k J/g and the reaction degree is97.6%with higher peak pressure(254.6 k Pa)and rise rate(1.397 MPa/s).An ideal ratio with 15 wt%AP was probed primarily.The high energy laser-induced shockwave experiment was utilized to simulate the reaction behavior in hot field.And the larger activated mixture of coated powder could release more energy to promote the growth of shockwave with higher speed up to 518.7±55.9 m/s.In conclusion,85@15 composition is expected to be applied in energetic system as a novel metal fuel.展开更多
Reduction roasting-acid leaching process was utilized to process high-iron-content manganese oxide ore using black charcoal as reductant. The results indicate that, compared with the traditional reductant of anthracit...Reduction roasting-acid leaching process was utilized to process high-iron-content manganese oxide ore using black charcoal as reductant. The results indicate that, compared with the traditional reductant of anthracite, higher manganese extraction efficiency is achieved at lower roasting temperature and shorter residence time. The effects of roasting parameters on the leaching efficiency of Mn and Fe were studied, and the optimal parameters are determined as follows: roasting temperature is 650 °C, residence time is 40 min, and black charcoal dosage is 10%(mass fraction). Under these conditions, the leaching efficiency of Mn reaches 82.37% while that of Fe is controlled below 7%. XRD results show that a majority of MnO2 and Fe2O3 in the raw ore are reduced to MnO and Fe3O4, respectively.展开更多
Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utiliz...Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.展开更多
The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production...The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production of high-loading SACs is still challenging.Herein,a facile and green boron acid(H_(3)BO_(3))-assisted pyrolysis strategy is put forward to synthesize SACs by only using chitosan,cobalt salt and H_(3)BO_(3)as precursor,and the effect of H_(3)BO_(3)is deeply investigated.The results show that molten boron oxide derived from H_(3)BO_(3)as ideal high-temperature carbonization media and blocking media play important role in the synthesis process.As a result,the acquired Co/N/B tri-doped porous carbon framework(Co-N-B-C)not only presents hierarchical porous structure,large specific surface area and abundant carbon edges but also possesses high-loading single Co atom(4.2 wt.%),thus giving rise to outstanding oxygen catalytic performance.When employed as a catalyst for air cathode in Zn-air batteries,the resultant Co-N-B-C catalyst shows remarkable power density and long-term stability.Clearly,our work gains deep insight into the role of H_(3)BO_(3)and provides a new avenue to synthesis of high-performance SACs.展开更多
Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for ca...Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.展开更多
From atom economy of green chemistry,two principles of selecting reductant were gotten: the smaller consumption of reductant material quantity per Mole-electron,and the lighter load on environment. On the basis of the...From atom economy of green chemistry,two principles of selecting reductant were gotten: the smaller consumption of reductant material quantity per Mole-electron,and the lighter load on environment. On the basis of these two principles,experimental research was done on organic compounds. Alcohol,ketone,amine,ester,acid,and alcohol,ketone,amine were selected to act as green reductants,whose optimal process parameters were obtained. Compared with the traditional method,researched method decreases not only the amount of reductants by about 90%,but also the amount of acid medium and solid waste,where the by-products are carbon dioxide and water. The acid medium is recycled.展开更多
基金Project(52022019)supported by the National Natural Science Foundation of China。
文摘The magnetization reduction of hematite using biomass waste can effectively utilize waste and reduce CO_(2) emission to achieve the goals of carbon peaking and carbon neutrality.The effects of temperatures on suspension magnetization roasting of hematite using biomass waste for evolved gases have been investigated using TG-FTIR,Py-GC/MS and gas composition analyzer.The mixture reduction process is divided into four stages.In the temperature range of 200-450℃ for mixture,the release of CO_(2),acids,and ketones is dominated in gases products.The yield and concentration of small molecules reducing gases increase when the temperature increases from 450 to 900℃.At 700℃,the volume concentrations of CO,H_(2) and CH_(4) peak at 8.91%,8.90% and 4.91%,respectively.During the suspension magnetization roasting process,an optimal iron concentrate with an iron grade of 70.86%,a recovery of 98.66% and a magnetic conversion of 45.70% is obtained at 700℃.Therefore,the magnetization reduction could react greatly in the temperature range of 600 to 700℃ owing to the suitable reducing gases.This study shows a detail gaseous evolution of roasting temperature and provides a new insight for studying the reduction process of hematite using biomass waste.
基金supported by the Fundamental Research Funds for the Central Universities(QNTD202302)National Natural Science Foundation of China(22378024)the Foreign expert program(G2022109001L).
文摘Developing a cost-effective and environmentally friendly process for the production of valuable chemicals from abundant herbal biomass receives great attentions in recent years.Herein,taking advantage of the“lignin first”strategy,corn straw is converted to valuable chemicals including lignin monomers,furfural and 5-methoxymethylfurfural via a two steps process.The key of this research lies in the development of a green and low-cost catalytic process utilizing magnetic Raney Ni catalyst and high boiling point ethylene glycol.The utilization of neat ethylene glycol as the sole slovent under atmospheric conditions obviates the need for additional additives,thereby facilitating the entire process to be conducted in glass flasks and rendering it highly convenient for scaling up.In the initial step,depolymerization of corn straw lignin resulted in a monomer yield of 18.1 wt%.Subsequently,in a dimethyl carbonate system,the carbohydrate component underwent complete conversion in a one-pot process,yielding furfural and 5-methoxymethylfurfural as the primary products with an impressive yield of 47.7%.
文摘The use of visible-light responsive photocatalysts for removing heavy metal ions in wastewater has received great attention.However,the development of photocatalysts with high activity and recyclability remains a huge challenge.Herein,a recyclable carbon fiber cloth-supported porous CdS nanorod photocatalyst was fabricated by a two-step hydrothermal treatment using AgVO_(3) nanowires as templates.The results indicated that under visible-light illumination,the carbon cloth-supported porous CdS nanorods showed improved photocatalytic activity for the reduction of Cr(Ⅵ),with an apparent rate constant exceeding that of carbon cloth-supported CdS nanospheres by a factor of 1.65 times.Moreover,the carbon cloth-supported porous CdS nanorods can be easily separated and be reused.This brings a new perspective for developing photocatalysts with high efficiency and recyclability for wastewater treatment.
文摘A gold catalyst of Au/pyrenyl‑graphdiyne(Pyr‑GDY)was prepared by anchoring small size of gold nanoparticles(Au NPs)on the surface of Pyr‑GDY for electrocatalytic nitrogen reduction reaction(eNRR),in which Au NPs with a size of approximately 3.69 nm was evenly distributed on spongy‑like porous Pyr‑GDY.The catalyst exhibited a good electrocatalytic activity for N_(2)reduction in a nitrogen‑saturated electrolyte,with an ammonia yield of 32.1μg·h^(-1)·mg_(cat)^(-1)at-0.3 V(vs RHE),3.5 times higher than that of Au/C(Au NPs anchored on carbon black).In addition,Au/Pyr‑GDY showed a Faraday efficiency(FE)of 26.9%for eNRR,and a good catalysis durability for over 22 h.
基金supported by Shanxi Province Science Foundation for Youths(202203021212300)Taiyuan University of Science and Technology Scientific Research Initial Funding(20212064)Outstanding Doctoral Award Fund in Shanxi Province(20222060).
文摘The nitrogen-coordinated metal single-atom catalysts(M−N−C SACs)with an ultra-high metal loading synthetized by direct high-temperature pyrolysis have been widely reported.However,most of metal single atoms in these catalysts were buried in the carbon matrix,resulting in a low metal utilization and inaccessibility for adsorption of reactants during the catalytic process.Herein,we reported a facile synthesis based on the hard-soft acid-base(HSAB)theory to fabricate Co single-atom catalysts with highly exposed metal atoms ligated to the external pyridinic-N sites of a nitrogen-doped carbon support.Benefiting from the highly accessible Co active sites,the prepared Co−N−C SAC exhibited a superior oxygen reduction reactivity comparable to that of the commercial Pt/C catalyst,showing a high turnover frequency(TOF)of 0.93 e^(−)·s^(-1)·site^(-1)at 0.85 V vs.RHE,far exceeding those of some representative SACs with a ultra-high metal content.This work provides a rational strategy to design and prepare M−N−C single-atom catalysts featured with high site-accessibility and site-density.
基金Project(2010FJ1011)supported by the Major Project of Hunan Science and Technology,ChinaProject(cstc2012ggB90002)supported by the Chongqing Key Science and Technology Program,China
文摘Manganese oxide ores from Gabon and Xiangxi were leached with waste tea as reductant in dilute sulfuric acid solution. The effects of waste tea dosage, concentration of sulfuric acid, liquid-to-solid ratio, leaching temperature and reaction time on leaching process were explored. The leaching efficiency of Gabonese manganese oxide ore reached almost 100% under the optimal condition which was determined as follows: manganese oxide ore to waste tea mass ratio of 10:1, sulfuric acid concentration of 2.5 molFL, liquid-to-solid ratio of 7.5:1, leaching temperature of 368 K, time of 8 h. The leaching efficiency of Xiangxi manganese oxide ore reached 99.8% under the optimal condition which was determined as follows: manganese oxide ore to waste tea mass ratio of 10:1, sulfuric acid concentration of 1.7 mol/L, liquid-to-solid ratio of 7.5:1, leaching temperature of 368 K, time of 8 h. The leaching process followed the internal diffusion controlled kinetic model, and the apparent activation energies of Gabonese manganese oxide ore and Xiangxi manganese oxide ore were calculated to be 38.2 kJ/mol and 20.4 kJ/mol, respectively. The morphological changes and mineralogical forms of the ore before and after the chemical treatment were discussed with the support of XRD analysis and SEM analysis.
基金Project(21376273)supported by the National Natural Science Foundation of ChinaProject(2010FJ1011)supported by the Key Program of Science and Technology of Hunan Province,China
文摘The extraction of manganese from low-grade manganese oxide ores using Ca S derived from Ca SO4 as reductant was investigated. The effects of mass ratio of Ca S to ore, reduction temperature, reduction time, liquid to solid ratio(L/S ratio), stirring speed, leaching temperature, leaching time and H2SO4 concentration on the leaching rates of Mn and Fe during the reduction–acid leaching process were discussed. The leaching rates of 96.47% for Mn and 19.24% for Fe were obtained under the optimized conditions of mass ratio of Ca S to manganese oxide ore 1:6.7, L/S ratio 5:1, stirring speed 300 r/min, reduction temperature of 95 °C for 2.0 h in the reduction process and leaching stirring speed of 200 r/min, H2SO4 concentration of 1.5 mol/L, leaching temperature of 80 °C for 5 min in the leaching process. In addition, this process can be employed in the recovery of manganese from various manganese oxide ores, and Mn leaching rate above 95% is obtained.
基金financially supported by the National Natural Science Foundation of China (Nos. 51474018 and 51674018)
文摘Iron and titanium were recovered from beach titanomagnetite(TTM) concentrate by embedding direct reduction and magnetic separation. The reduction products and the effects of the reductant type and reduction temperature on the reduction behavior were investigated. The results showed that the reduction of TTM concentrate was strongly related to the gasification reactivity of the reductant. Bitumite presented a better product index than wheat-straw biochar and coke, mainly because the gasification reactivity of bitumite was better than that of the other reductants. In addition, high temperatures were not beneficial to embedding direct reduction because of the emergence of a molten phase and iron-joined crystals, which in turn reduced the diffusion rate of the reducing gas and impeded the reduction reaction in the central area of the roasted briquette. The use of bitumite as the reductant at a C/Fe molar ratio of 1.4 and a reduction temperature of 1200°C for 120 min resulted in direct-reduction iron powder assaying 90.28 wt% TFe and 0.91 wt% TiO_2 with an iron recovery of 91.83% and titanium concentrate assaying 46.01 wt% TiO_2 with a TiO_2 recovery of 91.19%. Titanium existed mainly in the form of anosovite and ilmenite in the titanium concentrate.
文摘The present investigation examines the viability of dolochar, a sponge iron industry waste material, as a reductant in the reduction roasting of iron ore slimes, which are another waste generated by iron ore beneficiation plants. Under statistically determined optimum conditions, which include a temperature of 900°C, a reductant-to-feed mass ratio of 0.35, and a reduction time of 30–45 min, the roasted mass, after being subjected to low-intensity magnetic separation, yielded an iron ore concentrate of approximately 64 wt% Fe at a mass recovery of approximately 71% from the feed iron ore slime assaying 56.2 wt% Fe. X-ray diffraction analyses indicated that the magnetic products contain magnetite and hematite as the major phases, whereas the nonmagnetic fractions contain quartz and hematite.
基金financially supported by National Natural Science Foundation of China(No.51922025 and No.51874066)China Postdoctoral Science Foundation(No.2020M670759)the Fundamental Research Funds for the Central Universities(No.DUT20GJ201)。
文摘Measuring the dust explosion characteristics of aluminum-based activated fuels was a prerequisite for developing effective prevention and control measures.In this paper,ignition sensitivity,flame propagation behaviors and explosion severity of aluminum/polytetrafluoroethylene(Al/PTFE)compositions including 2 PT(2.80 wt.%F),4 PT(7.18 wt.%F)and 8 PT(11.90 wt.%F)were studied.When the content of F increased from 2.80 wt.%to 11.90 wt.%,the minimum explosive concentration MEC decreased from380 g/m^(3)to 140 g/m^(3),due to the dual effects of increased internal active aluminum and enhanced reactivity.The average flame propagation velocities increased as the percentage of F increased.The maximum explosion pressure Pmof 500 g/m3aluminum-based activated fuels increased from 247 k Pa to299 kPa.Scanning electron microscopy demonstrated that with the increase of PTFE content,the reaction was more complete.On this basis,the explosion mechanism of aluminum-based activated fuels was revealed.
基金Supported by the National Natural Science Foundation of China
文摘The chemiluminescence reaction between luminol and reductant was investigated by a flow-injection system. The results show that this reaction can be used for the determination of the reductant which is active to chemiluminescence in alkaline lumminol, and of the substance which can, in appropriate manner, be converted into the active reductant. The mechanism of the chemiluminescence reaction may be that the reductant reduces dissolved oxygen to O2 , then O2 reacts with alkaline luminol to generate chemiluminescence.
基金Project(51674298)supported by the National Natural Science Foundation of ChinaProject supported by Anhui Province Research and Development Innovation Program,China。
文摘Hydrazine sulfate was used as a reducing agent for the leaching of Li,Ni,Co and Mn from spent lithium-ion batteries.The effects of the reaction conditions on the leaching mechanism and kinetics were characterized and examined.97%of the available Li,96%of the available Ni,95%of the available Co,and 86%of the available Mn are extracted under the following optimized conditions:sulfuric acid concentration of 2.0 mol/L,hydrazine sulfate dosage of 30 g/L,solid-to-liquid ratio of 50 g/L,temperature of 80℃,and leaching time of 60 min.The activation energies of the leaching are determined to be 44.32,59.37 and 55.62 k J/mol for Li,Ni and Co,respectively.By performing X-ray diffraction and scanning electron microscopy in conjunction with energy dispersive X-ray spectroscopy,it is confirmed that the main phase in the leaching residue is MnO2.The results show that hydrazine sulfate is an effective reducing agent in the acid leaching process for spent lithium-ion batteries.
文摘The chemiluminescence reactions between lucigenin and reductants such as Mo(LII),V( II), U(III), W(III), Cr(II), Ti(III) and Fe( II), which were produced on-line by passing Mo(VI),V(V),U(VI), W(VI), Cr(VI,III),Ti(IV) and Fe(III) through a micro Jones column, are studied in detail. Results show that the reactions can be used directly for the determination of these substances. The mechanism of the reactions is also investigated.
基金Project(2010FJ1011)supported by the Major Project of Science and Technology of Hunan Province,China
文摘The kinetics of reductive leaching of manganese from a low-grade manganese oxide ore were studied using cellulose as reductant in dilute sulfuric acid medium.It was found that when the stirring speed was higher than 200 r/min,the effect of gas film diffusion on manganese extraction efficiency could be neglected,and the kinetic behavior was investigated under the condition of elimination of external diffusion influence on the leaching process.Effects of leaching temperature,mass ratio of cellulose and ore,and the sulfuric acid concentration on manganese extraction efficiency were discussed.The kinetic data were analyzed based on the shrinking core model,which indicated that the leaching process was dominated by both ash layer diffusion and chemical reaction at the initial stage,with the progress of leaching reaction,the rate-controlling step switched to the ash layer diffusion.It was also concluded that the sulfuric acid concentration had the most significant influence on the leaching rate,the reaction orders with respect to the sulfuric acid concentration were 2.102 in the first 60 min,and 3.642 in the later 90 min,while the reaction orders for mass ratio of cellulose and ore were 0.660 and 0.724,respectively.An Arrhenius relationship was used to relate the temperature to the rate of leaching,from which apparent activation energies were calculated to be 46.487 kJ/mol and 62.290 kJ/mol at the two stages,respectively.Finally,the overall leaching rate equations for the manganese dissolution reaction with cellulose in sulphuric acid solution were developed.The morphological changes and mineralogical forms of the ore before and after the chemical treatment were discussed with the support of SEM and XRD analyses.
基金supported by National Natural Science Foundation of China[No.21975024]。
文摘To improve the thermal properties of aluminum(Al)in the energetic system,a coated structure with ammonium perchlorate(AP)was prepared by a facile approach.And N,N-Dimethylformamide(DMF)was chosen as an ideal solvent based on heterogeneous nucleation theory and molecular dynamics simulation.This coated structure could enlarge the contact area and improve the reaction environment to enhance the thermal properties.The addition of AP could accelerate oxidation temperature of Al with around 17.5°C.And the heat release of 85@15 composition rises to 26.13 k J/g and the reaction degree is97.6%with higher peak pressure(254.6 k Pa)and rise rate(1.397 MPa/s).An ideal ratio with 15 wt%AP was probed primarily.The high energy laser-induced shockwave experiment was utilized to simulate the reaction behavior in hot field.And the larger activated mixture of coated powder could release more energy to promote the growth of shockwave with higher speed up to 518.7±55.9 m/s.In conclusion,85@15 composition is expected to be applied in energetic system as a novel metal fuel.
基金Project(2013JSJJ028)supported by the Teachers’Research Fund of Central South University,ChinaProject supported by Co-Innovation Center for Clean and Efficient Utilization of Strategic Mineral Resources,China
文摘Reduction roasting-acid leaching process was utilized to process high-iron-content manganese oxide ore using black charcoal as reductant. The results indicate that, compared with the traditional reductant of anthracite, higher manganese extraction efficiency is achieved at lower roasting temperature and shorter residence time. The effects of roasting parameters on the leaching efficiency of Mn and Fe were studied, and the optimal parameters are determined as follows: roasting temperature is 650 °C, residence time is 40 min, and black charcoal dosage is 10%(mass fraction). Under these conditions, the leaching efficiency of Mn reaches 82.37% while that of Fe is controlled below 7%. XRD results show that a majority of MnO2 and Fe2O3 in the raw ore are reduced to MnO and Fe3O4, respectively.
基金supported by the National Natural Science Foundation of China(22234005,21974070)the Natural Science Foundation of Jiangsu Province(BK20222015)。
文摘Atomically dispersed catalysts exhibit significant influence on facilitating the sluggish oxygen reduction reaction(ORR)kinetics with high atom economy,owing to remarkable attributes including nearly 100%atomic utilization and exceptional catalytic functionality.Furthermore,accurately controlling atomic physical properties including spin,charge,orbital,and lattice degrees of atomically dispersed catalysts can realize the optimized chemical properties including maximum atom utilization efficiency,homogenous active centers,and satisfactory catalytic performance,but remains elusive.Here,through physical and chemical insight,we review and systematically summarize the strategies to optimize atomically dispersed ORR catalysts including adjusting the atomic coordination environment,adjacent electronic orbital and site density,and the choice of dual-atom sites.Then the emphasis is on the fundamental understanding of the correlation between the physical property and the catalytic behavior for atomically dispersed catalysts.Finally,an overview of the existing challenges and prospects to illustrate the current obstacles and potential opportunities for the advancement of atomically dispersed catalysts in the realm of electrocatalytic reactions is offered.
基金supported by National Natural Science Foundation of China(Nos.52274298,51974114,51672075 and 21908049)China Postdoctoral Science Foundation(2020M682560)+4 种基金International Postdoctoral Exchange Fel owship Program(Grant No.PC2022020)Science&Technology innovation program of Hunan province(2020RC2024 and 2022RC3037)Hunan Provincial Natural Science Foundation of China(No.2020JJ4175)Science&Technology talents lifting project of Hunan Province(No.2022TJ-N16)Scientific Research Fund of Hunan Provincial Education Department(No.21A0392)
文摘The emerging of single-atom catalysts(SACs)offers a great opportunity for the development of advanced energy storage and conversion devices due to their excellent activity and durability,but the actual mass production of high-loading SACs is still challenging.Herein,a facile and green boron acid(H_(3)BO_(3))-assisted pyrolysis strategy is put forward to synthesize SACs by only using chitosan,cobalt salt and H_(3)BO_(3)as precursor,and the effect of H_(3)BO_(3)is deeply investigated.The results show that molten boron oxide derived from H_(3)BO_(3)as ideal high-temperature carbonization media and blocking media play important role in the synthesis process.As a result,the acquired Co/N/B tri-doped porous carbon framework(Co-N-B-C)not only presents hierarchical porous structure,large specific surface area and abundant carbon edges but also possesses high-loading single Co atom(4.2 wt.%),thus giving rise to outstanding oxygen catalytic performance.When employed as a catalyst for air cathode in Zn-air batteries,the resultant Co-N-B-C catalyst shows remarkable power density and long-term stability.Clearly,our work gains deep insight into the role of H_(3)BO_(3)and provides a new avenue to synthesis of high-performance SACs.
基金supported by the National Natural Science Foundation of China (22178149)Jiangsu Distinguished Professor Program+4 种基金Natural Science Foundation of Jiangsu Province for Outstanding Youth Scientists (BK20211599)Key R and D Project of Zhenjiang City (CQ2022001)Scientific Research Startup Foundation of Jiangsu University (Nos. 202096 and 22JDG020)Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment of Fuzhou University (SKLPEE-KF202310)the Opening Project of Structural Optimization and Application of Functional Molecules Key Laboratory of Sichuan Province (2023GNFZ-01)。
文摘Carbon dioxide conversion into valuable products using photocatalysis and electrocatalysis is an effective approach to mitigate global environmental issues and the energy shortages. Among the materials utilized for catalytic reduction of CO_(2), Cu-based materials are highly advantageous owing to their widespread availability, cost-effectiveness, and environmental sustainability. Furthermore, Cu-based materials demonstrate interesting abilities in the adsorption and activation of carbon dioxide, allowing the formation of C_(2+) compounds through C–C coupling process. Herein, the basic principles of photocatalytic CO_(2) reduction reactions(PCO_(2)RR) and electrocatalytic CO_(2) reduction reaction(ECO_(2)RR) and the pathways for the generation C_(2+) products are introduced. This review categorizes Cu-based materials into different groups including Cu metal, Cu oxides, Cu alloys, and Cu SACs, Cu heterojunctions based on their catalytic applications. The relationship between the Cu surfaces and their efficiency in both PCO_(2)RR and ECO_(2)RR is emphasized. Through a review of recent studies on PCO_(2)RR and ECO_(2)RR using Cu-based catalysts, the focus is on understanding the underlying reasons for the enhanced selectivity toward C_(2+) products. Finally, the opportunities and challenges associated with Cu-based materials in the CO_(2) catalytic reduction applications are presented, along with research directions that can guide for the design of highly active and selective Cu-based materials for CO_(2) reduction processes in the future.
文摘From atom economy of green chemistry,two principles of selecting reductant were gotten: the smaller consumption of reductant material quantity per Mole-electron,and the lighter load on environment. On the basis of these two principles,experimental research was done on organic compounds. Alcohol,ketone,amine,ester,acid,and alcohol,ketone,amine were selected to act as green reductants,whose optimal process parameters were obtained. Compared with the traditional method,researched method decreases not only the amount of reductants by about 90%,but also the amount of acid medium and solid waste,where the by-products are carbon dioxide and water. The acid medium is recycled.