Inertinite-rich coal is widely distributed in the Ordos Basin,represented by the No.2 coal seam of the Middle Jurassic Yan'an Formation.This paper combined coal petrology and geochemistry to analyze the origin of ...Inertinite-rich coal is widely distributed in the Ordos Basin,represented by the No.2 coal seam of the Middle Jurassic Yan'an Formation.This paper combined coal petrology and geochemistry to analyze the origin of inertinite,changes in the coal-forming environment and control characteristics of wildfire.Research has shown that there are two forms of inertinite sources in the study area.Alongside typical fusinization,wildfire events also play a substantial role in inertinite formation.There are significant fluctuations in the coal-forming environment of samples at different depths.Coal samples were formed in dry forest swamp with low water levels and strong oxidation,which have a high inertinite content,and the samples formed in wet forest swamp and limnic showed low inertinite content.Conversely,the inertinite content of different origins does not fully correspond to the depositional environment characterized by dryness and oxidation.Nonpyrogenic inertinites were significantly influenced by climatic conditions,while pyrofusinite was not entirely controlled by climatic conditions but rather directly impacted by wildfire events.The high oxygen level was the main factor causing widespread wildfire events.Overall,the combination of wildfire activity and oxidation generates a high content of inertinite in the Middle Jurassic coal of the Ordos Basin.展开更多
In the realm of proton exchange membrane fuel cells(PEMFCs),the bipolar plates(BPs)are indispensable and serve pivotal roles in distributing reactant gases,collecting current,facilitating product water removal,and coo...In the realm of proton exchange membrane fuel cells(PEMFCs),the bipolar plates(BPs)are indispensable and serve pivotal roles in distributing reactant gases,collecting current,facilitating product water removal,and cooling the stack.Metal BPs,characterized by outstanding manufacturability,cost-effectiveness,higher power density,and mechanical strength,are emerging as viable alternatives to traditional graphite BPs.The foremost challenge for metal BPs lies in enhancing their corrosion resistance and conductivity under acidic conditions,necessitating the application of various coatings on their surfaces to ensure superior performance.This review summarizes and compares recent advancements in the research of eight distinct types of coatings for BPs in PEMFCs,including noble metal,carbide,ni-tride,and amorphous carbon(a-C)/metal compound composite coatings.The various challenges encountered in the manufacturing and fu-ture application of these coatings are also delineated.展开更多
The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly...The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly affected by mass transfer. In this study, CoTPP-mediated(CoTPP: cobalt(II) mesotetraphenylporphyrin) selective benzyl alcohol oxidation with oxygen was conducted in a membrane microchannel(MMC) reactor and a bubble column(BC) reactor, respectively. We observed that 83% benzyl alcohol was converted within 6.5 min in the MMC reactor, but only less than 10% benzyl alcohol was converted in the BC reactor. Hydrodynamic characteristics and gas–liquid mass transfer performances were compared for the MMC and BC reactors. The MMC reactor was assumed to be a plug flow reactor,and the dimensionless variance was 0.29. Compared to the BC reactor, the gas–liquid mass transfer was intensified significantly in MMC reactor. It could be ascribed to the high gas holdup(2.9 times higher than that of BC reactor), liquid film mass transfer coefficient(8.2 times higher than that of BC reactor), and mass transfer coefficient per unit interfacial area(3.8 times higher than that of BC reactor). Moreover,the Hatta number for the MMC reactor reached up to 0.61, which was about 15 times higher than that of the BC reactor. The computational fluid dynamics calculations for mass fractions in both liquid and gas phases were consistent with the experimental data.展开更多
With the advantages of the multiple oxidation states and highly open crystal structures,vanadium-based composites have been considered as the promising cathode materials for aqueous zinc-ion batteries(ZIBs).However,th...With the advantages of the multiple oxidation states and highly open crystal structures,vanadium-based composites have been considered as the promising cathode materials for aqueous zinc-ion batteries(ZIBs).However,the inherent inferior electrical conductivity,low specific surface area,and sluggish Zn^(2+)diffusion kinetics of the traditional vanadium-based oxides have greatly impeded their development.Herein,a novel hierarchical porous spindle-shaped Ag-V_(2)O_(5) with unique heterostructures was rationally designed via a simple MOF-assisted synthetic method and applied as stable cathode for aqueous ZIBs.The high specific surface area and hierarchically porous superstructures endowed Ag-V_(2)O_(5) with sufficient electrochemical active sites and shortened the diffusion pathways of Zn^(2+),which was beneficial to accelerate the reversible transport of Zn^(2+)and deliver a high specific capacity(426 mA h g^(-1) at 0.1 A g^(-1) and 96.5%capacity retention after 100 cycles).Meanwhile,the self-built-in electric fields at the heterointerface of Ag-V_(2)O_(5) electrode could strengthen the synergistic coupling interaction between Ag and V_(2)O_(5),which can effectively enhance the electric conductivity and maintain the structural integrity,resulting in superb rate capability(326.1 mA h g^(-1) at 5.0 A g^(-1))and remarkable cycling stability(89.7%capacity retention after 2000 cycles at 5.0 A g^(-1)).Moreover,the reversible Zn^(2+)storage mechanism was further investigated and elucidated by kinetics analysis and DFT calculations.展开更多
In the process of green and smart mine construction under the context of carbon neutrality,China's coal safety situation has been continuously improved in recent years.In order to recognize the development of coal...In the process of green and smart mine construction under the context of carbon neutrality,China's coal safety situation has been continuously improved in recent years.In order to recognize the development of coal production in China and prepare for future monitoring and prevention of safety incidents,this study mainly elaborated on the basic situation of coal resources and national mining accidents over the past five years(2017-2021),from four dimensions(accident level,type,region,and time),and then proposed the preventive measures based on accident statistical laws.The results show that the storage of coal resources has obvious geographic characteristics,mainly concentrated in the Midwest,with coal resources in Shanxi and Shaanxi accounting for about 49.4%.The proportion of coal consumption has dropped from 70.2%to 56%between 2011 and 2021,but still accounts for more than half of the all.Meanwhile,the accident-prone areas are positively correlated with the amount of coal production.Among different levels of coal mine accidents,general accidents had the highest number of accidents and deaths,with 692 accidents and 783 deaths,accounting for 87.6%and 54.64%respectively.The frequency of roof,gas,and transportation accidents is relatively high,and the number of single fatalities caused by gas accidents is the largest,about 4.18.In terms of geographical distribution of accidents,the safety situation in Shanxi Province is the most severe.From the time distribution of coal mine accidents,the accidents mainly occurred in July and August,and rarely occurred in February and December.Finally,the"4+4"safety management model is proposed,combining the statistical results with coal production in China.Based on the existing health and safety management systems,the manage-ments are divided into four sub-categories,and more specific measures are suggested.展开更多
Photocatalytic CO_(2)reduction to valuable product exhibit promising prospect for solving the energy crisis and the greenhouse effect.Herein,Co-Ti_(3)C_(2)T_(x)/g-C_(3)N_(4)(Co-TC/CN)composite with enhanced photocatal...Photocatalytic CO_(2)reduction to valuable product exhibit promising prospect for solving the energy crisis and the greenhouse effect.Herein,Co-Ti_(3)C_(2)T_(x)/g-C_(3)N_(4)(Co-TC/CN)composite with enhanced photocatalytic performance for converting CO_(2)to CO and CH_(4)was constructed by electrostatic self-assembly method.The close contact interface between Co-Ti_(3)C_(2)T_(x)and g-C_(3)N_(4)nanosheets can be used as fast transport channels of photogenerated electrons and effectively promote the separation of photogenerated electrons and holes,and the interface between the Co and Ti_(3)C_(2)T_(x)might be the active sites for CO_(2)adsorption and activation.The optimized Co-Ti_(3)C_(2)T_(x)/g-C_(3)N_(4)composite exhibited the highest photocatalytic performance with the CO and CH_(4)production of 55.04 μmol·g^(-1)and 2.29 μmol·g^(-1),respectively,which were 7.5 times and 5.8 times than those of g-C_(3)N_(4).Furthermore,the stability of g-C_(3)N_(4)was improved after coupling with Co-Ti_(3)C_(2)T_(x).展开更多
The synthesis of a continuous IMF zeolite membrane was fabricated on tubular substrates by seeded growth for the first time. The straight channels of IMF zeolite with diameters of 0.53–0.59 nm are distinguishable for...The synthesis of a continuous IMF zeolite membrane was fabricated on tubular substrates by seeded growth for the first time. The straight channels of IMF zeolite with diameters of 0.53–0.59 nm are distinguishable for p-xylene from o-xylene molecules. Pure IMF-phase high-silica IM-5 zeolite seeds with uniform and fine crystal size were fabricated by a new sonication-assisted aging process. The seeds were coated on the support by dipcoating and induced the formation of continuous membrane. Separation performance in p-/o-xylene mixture was investigated at various temperature and pressure. The typical IM-5zeolite membrane had p-/o-xylene separation factor of 3.7. Our results suggest that IM-5 zeolite is a potentially good membrane material for the separation of xylene mixtures.展开更多
The utilization of single atoms(SAs)as trifunctional electrocatalyst for nitro-gen reduction,oxygen reduction,and oxygen evolution reactions(NRR,ORR,and OER)is still a formidable challenge.Herein,we devise one-pot syn...The utilization of single atoms(SAs)as trifunctional electrocatalyst for nitro-gen reduction,oxygen reduction,and oxygen evolution reactions(NRR,ORR,and OER)is still a formidable challenge.Herein,we devise one-pot synthesized palladium SAs stabilized on nitrogen-doped carbon palladium SA electrocat-alyst(Pd-SA/NC)as efficient trifunctional electrocatalyst for NRR,ORR,and OER.Pd-SA/NC performs a robust catalytic activity toward NRR with faradaic efficiency of 22.5%at-0.25 V versus reversible hydrogen electrode(RHE),and the relative Pd utilization efficiency is enhanced by 17-fold than Pd-NP/NC.In addition,the half-wave potential reaches 0.876 V versus RHE,amounting to a 58-time higher mass activity than commercial Pt/C.Moreover,the overpotential at 10 mA cm-2 is as low as 287 mV for Pd-SA/NC,outperforming the commer-cial IrO2 by 360 times in turnover frequency at 1.6 V versus RHE.Accordingly,the assembled rechargeable zinc-air battery(ZAB)achieves a maximum power den-sity of 170 mW cm-2,boosted by 2.3 times than Pt/C–IrO2.Two constructed ZABs efficiently power the NRR-OER system to electrochemically generate ammonia implying its superior trifunctionality.展开更多
Four strains of the Q biotype and one of the B biotype of the whitefly Bemisia tabaci collected from China were characterised for resistance to four neonicotinoid insecticides and pymetrozine.Q biotype strains showed ...Four strains of the Q biotype and one of the B biotype of the whitefly Bemisia tabaci collected from China were characterised for resistance to four neonicotinoid insecticides and pymetrozine.Q biotype strains showed moderate to strong resistance to imidacloprid,thiamethoxam and acetamiprid,but little or no cross-resistance to dinotefuron.Resistance to neonicotinoids was consistently associated with resistance to pymetrozine,despite the latter having a distinct(though unresolved)mode of action.The single B biotype strain proved largely susceptible to all the insecticides investigated.Resistance in the Q biotype strains was associated with over-expression of a cytochrome P450 monooxygenase gene,CYP6CM1,whose substrate specificity presumably accounts for the observed cross-resistance profiles.展开更多
Magnetic starch microspheres(AAM-MSM)were synthesized via an inverse emulsion graft copolymerization by using mechanically activated cassava starch(MS)as a crude material,acrylic acid(AA)and acrylamide(AM)as graft cop...Magnetic starch microspheres(AAM-MSM)were synthesized via an inverse emulsion graft copolymerization by using mechanically activated cassava starch(MS)as a crude material,acrylic acid(AA)and acrylamide(AM)as graft copolymer monomers,and methyl methacrylate(MMA)as the dispersing agent and used as an adsorbent for the removal of Cd(Ⅱ)ions from aqueous solution.Fourier-transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),scanning electron microscopy(SEM),and vibrating sample magnetometry(VSM)were used to characterize the AAM-MSM adsorbent.The results indicated that AA,AM,and MMA were grafted to the MS,and the Fe_(3)O_(4) nanoparticles were encapsulated in the AAM-MSM adsorbent microspheres.The adsorbent exhibited a smooth surface,uniform size,and good sphericity because of the addition of the MMA and provided more adsorption sites for the Cd(Ⅱ)ions.The maximum adsorption capacity of Cd(Ⅱ)on the AAM-MSM was 39.98 mg·g^(-1).The adsorbents were superparamagnetic,and the saturation magnetization was 16.7 A·m^(2)·kg^(-1).Additionally,the adsorption isotherms and kinetics of the adsorption process were further investigated.The process of Cd(Ⅱ)ions adsorbed onto the AAM-MSM could be described more favorably by the pseudo-second-order kinetic and Langmuir isothermal adsorption models,which suggested that the chemical reaction process dominated the adsorption process for the Cd(Ⅱ)and chemisorption was the rate-controlling step during the Cd(Ⅱ)removal process.展开更多
Cation substitution in spinel cobaltites(e.g.,ACo2O4,in which A=Mn,Fe,Co,Ni,Cu,or Zn)is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemic...Cation substitution in spinel cobaltites(e.g.,ACo2O4,in which A=Mn,Fe,Co,Ni,Cu,or Zn)is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemical performance for water splitting.However,the fundamental principles and mechanisms are not fully understood.This research aims to systematically investigate the effects of cation substitution in spinel cobaltites derived from mixed-metal-organic frameworks on the oxygen evolution reaction(OER).Among the obtained ACo2O4 catalysts,FeCo2O4 showed excellent OER performance with a current density of 10 mA·cm^-2 at an overpotential of 164 mV in alkaline media.Both theoretical calculations and experimental results demonstrate that the Fe substitution in the crystal lattice of ACo2O4 can significantly accelerate charge transfer,thereby achieving enhanced electrochemical properties.The crystal field of spinel ACo2O4,which determines the valence states of cations A,is identified as the key factor to dictate the OER performance of these spinel cobaltites.展开更多
A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loa...A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loading NHPI on h-BN not only benefits to the dispersion and utilization of NHPI,but also can significantly promote the catalytic performance.By employing NHPI/h-BN as the catalyst,azodiisobutyronitrile(AIBN)as the metal-free initiator,a 95%conversion of dibenzothiophene(DBT)can be acquired under the reaction conditions of 120°C and atmospheric pressure with molecular oxygen(O_(2))as oxidant.Moreover,the heterogenization is convenient for the regeneration of the catalyst with>94%DBT conversion after being recycled seven times.Characterizations illustrate that the promoted catalytic activity along with the regenerability originate from the interactions between NHPI and h-BN.The catalytic mechanism study shows that molecular oxygen is readily activated by the NHPI/h-BN to form a superoxide radical(O_(2)^(·-)),which oxidize DBT to DBTO2 for desulfurization.展开更多
Propylene molecule owns two active sites,the direct epoxidation of propylene by dioxygen is still a challenge due to the limitation of selectivity.In this work,the direct liquid-phase propylene aerobic epoxidation pro...Propylene molecule owns two active sites,the direct epoxidation of propylene by dioxygen is still a challenge due to the limitation of selectivity.In this work,the direct liquid-phase propylene aerobic epoxidation protocol by chloride manganese meso-tetraphenylporphyrin(MnTPPCl)was developed.The conversion of propylene was 12.7%,and the selectivity towards PO(propylene oxide)reached up to 80.5%.The formation of PO was attributed to the mechanism via high-valent Mn species,which was confirmed by means of in situ UV–vis spectrum.展开更多
Adsorptive recovery of valuable components from industrial wastewater is highly desirable for avoiding resource wastage but remains a challenge.Herein,we develop an efficient continuous adsorption process for recoveri...Adsorptive recovery of valuable components from industrial wastewater is highly desirable for avoiding resource wastage but remains a challenge.Herein,we develop an efficient continuous adsorption process for recovering aromatic compounds in wastewater from styrene monomer and propylene oxide coproduction(SMPO)plant.Based on our insight into the potential of bio-based porous materials for adsorption application,starch-graft-polystyrene(SPS)and aryl-modifiedβ-cyclodextrin(ACD)were prepared,and novel hypercrosslinked porous polymers combined SPS with ACD(HSPS-ACDs)were synthesized through external crosslinking approach.In a binary-component system,the best-performing one HSPS-ACD(H)with high ACD content and large specific surface area possessed superior capacities for the representative aromatic compounds,acetophenone(AP,2.81 mmol·g^(-1))and 1-phenylethanol(1-PE,1.35 mmol·g^(-1))compared with the previously reported materials.Further,the adsorption properties of aromatic compounds on HSPS-ACD(H)were investigated in batch mode.For practical application,continuous adsorption experiments were conducted in a HSPS-ACD(H)-packed fixed bed,where the target aromatic components in wastewater were effectively retained and further released by elution.Besides showing the reversible adsorption and efficient enrichment effect,the HSPS-ACD(H)-packed fixed bed also maintained great stability in multiple cycles.Moreover,quantum chemical calculations were performed to elucidate the potential mechanism of adsorption of AP and 1-PE onto HSPS-ACD(H).展开更多
Temperature variation and gas generation at diferent depths and positions in the coal combustion process were studied to determine the propagation and evolution of high temperature regions in the process of coal spont...Temperature variation and gas generation at diferent depths and positions in the coal combustion process were studied to determine the propagation and evolution of high temperature regions in the process of coal spontaneous combustion.This study selected coal samples from Mengcun,Shaanxi Province,People’s Republic of China,and developed a semi-enclosed experimental system(furnace)for simulating coal combustion.The thermal mass loss of coal samples under various heating rates(5,10,and 15℃/min)was analyzed through thermogravimetric analysis,and the dynamic characteristics of the coal samples were analyzed;the reliability of the semi-enclosed experimental system was verifed through the equal proportional method of fuzzy response.The results reveal that the high-temperature zone is distributed nonlinearly from the middle to the front end of the furnace,and the temperatures of points in this zone decreased gradually as the layer depth increased.The apparent activation energy of the coal samples during combustion frst increased and then decreased as the conversion degree increased.Furthermore,the proportion of mass loss and the mass loss rate in the coal samples observed in the thermogravimetric experiment is consistent with that observed in the frst and second stages of the experiment conducted using the semi-enclosed system.The research fndings can provide a theoretical basis for the prevention and control of hightemperature zones in coal combustion.展开更多
The underground brine resource along the coast of Laizhou Bay is the world’s rare shallow underground brine resource,which occurs in the Laizhou city in the east,and extends to the coastal area of the Binzhou city in
Four naturally rare 5,6,7-trimethoxy-2,3-cis-dihydroflavonols (3-6) and two 5,6,7-trimethoxy-2,3-trans-dihydroflavonols (7-8) were designed and synthesized. Their antioxidative properties were evaluated by way of ...Four naturally rare 5,6,7-trimethoxy-2,3-cis-dihydroflavonols (3-6) and two 5,6,7-trimethoxy-2,3-trans-dihydroflavonols (7-8) were designed and synthesized. Their antioxidative properties were evaluated by way of examining their scavenging capacities towards DPPH and O2^*- free radicals, as well as by measuring their inhibitory ability against LPO. Both the 2,3-trans and the 2,3- cis conformers exhibited certain quenching abilities to DPPH and O2^*- radicals, while most of the synthetic dihydroflavonols demonstrated remarkable inhibition to LPO.展开更多
Multiple hetero-interfaces would strengthen interfacial polarization and boost electromagnetic wave absorption,but still remain the formidable challenges in decreasing filler loadings.Herein,sandwich NC@Co/NC@MnO_(2)c...Multiple hetero-interfaces would strengthen interfacial polarization and boost electromagnetic wave absorption,but still remain the formidable challenges in decreasing filler loadings.Herein,sandwich NC@Co/NC@MnO_(2)composites with hollow cavity,multiple hetero-interfaces,and hierarchical structures have been fabricated via the cooperative processes of self-sacrifice strategy and sequential hydrothermal reaction.In the sandwich composites,middle magnetic components(Co/NC)are wrapped by inner N-doped carbon(NC)matrix and outer hierarchical MnO_(2)nanosheets.Importantly,hollow engineering of sandwich composites with multiple hetero-interfaces greatly facilitates the enhancement of absorption bandwidth without sacrificing the absorption intensity.The maximum reflection loss of sandwich NC@Co/NC@MnO_(2)composites reaches-44.8 dB at 2.5 mm and the effective bandwidths is achieved as wide as 9.6 GHz at 2.3 mm.These results provide us a new insight into preparing efficient electromagnetic wave absorbers by interface engineering and hollow construction.展开更多
Establishing an effective charge transfer mechanism in carbon nitride(g-C_(3)N_(4))to enhance its photocatalytic activity remains a limiting nuisance.Herein,the combination design of a single Cu atom with hollow g-C_(...Establishing an effective charge transfer mechanism in carbon nitride(g-C_(3)N_(4))to enhance its photocatalytic activity remains a limiting nuisance.Herein,the combination design of a single Cu atom with hollow g-C_(3)N_(4)nanospheres(Cu-N_(3)structure)has been proven to offer significant opportunities for this crucial challenge.Moreover,this structure endows two pathways for charge transfer in the reaction,namely,the N atoms in the three-dimensional planar structure are only bonded with a single Cu atom,and charge transfer occurs between the plane and the layered structure due to the bending of the interlayered g-C_(3)N_(4)hollow nanospheres.Notably,Cu-N_(3)and hollow nanosphere structures have been certified to greatly enhance the efficiency of photogenerated carrier separation and transfer between the layers and planes by ultrafast spectral analysis.As a result,this catalyst possesses unparalleled photocatalytic efficiency.Specifically,the hydrogen production rate up to 2040μmol h^(−1) g^(−1),which is 51 times that of pure C_(3)N_(4)under visible light conditions.The photocatalytic degradation performance of tetracycline and oxidation performance of benzene is also expressed,with a degradation rate of 100%,a conversion of 97.3%and a selectivity of 99.9%.This work focuses on the structure-activity relationship to provide the possibilities for the development of potential photocatalytic materials.展开更多
Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous catalysts.Unlike conventional organo-phosphine modification,R...Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous catalysts.Unlike conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and stability.Furthermore,a volcano curve between Ca addition ratio and catalytic activity is found.Introducing Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.42272209)the Natural Science Basic Research Program of Shaanxi(Grant No.2021JLM-12)the CNPC Major Science and Technology Project(Grant No.2021DJ3805)。
文摘Inertinite-rich coal is widely distributed in the Ordos Basin,represented by the No.2 coal seam of the Middle Jurassic Yan'an Formation.This paper combined coal petrology and geochemistry to analyze the origin of inertinite,changes in the coal-forming environment and control characteristics of wildfire.Research has shown that there are two forms of inertinite sources in the study area.Alongside typical fusinization,wildfire events also play a substantial role in inertinite formation.There are significant fluctuations in the coal-forming environment of samples at different depths.Coal samples were formed in dry forest swamp with low water levels and strong oxidation,which have a high inertinite content,and the samples formed in wet forest swamp and limnic showed low inertinite content.Conversely,the inertinite content of different origins does not fully correspond to the depositional environment characterized by dryness and oxidation.Nonpyrogenic inertinites were significantly influenced by climatic conditions,while pyrofusinite was not entirely controlled by climatic conditions but rather directly impacted by wildfire events.The high oxygen level was the main factor causing widespread wildfire events.Overall,the combination of wildfire activity and oxidation generates a high content of inertinite in the Middle Jurassic coal of the Ordos Basin.
基金the support from the Shenzhen Science and Technology Program of China(No.JCYJ20220530161614031)National Natural Science Foundation of China(No.52471094)Shaanxi Coal Chemical Industry Technology Research Institute Co.,Ltd.
文摘In the realm of proton exchange membrane fuel cells(PEMFCs),the bipolar plates(BPs)are indispensable and serve pivotal roles in distributing reactant gases,collecting current,facilitating product water removal,and cooling the stack.Metal BPs,characterized by outstanding manufacturability,cost-effectiveness,higher power density,and mechanical strength,are emerging as viable alternatives to traditional graphite BPs.The foremost challenge for metal BPs lies in enhancing their corrosion resistance and conductivity under acidic conditions,necessitating the application of various coatings on their surfaces to ensure superior performance.This review summarizes and compares recent advancements in the research of eight distinct types of coatings for BPs in PEMFCs,including noble metal,carbide,ni-tride,and amorphous carbon(a-C)/metal compound composite coatings.The various challenges encountered in the manufacturing and fu-ture application of these coatings are also delineated.
基金financially supported by the National Key Research and Development Program of China (2020YFA0210900)the National Natural Science Foundation of China (21938001 and 21878344)+1 种基金Guangdong Provincial Key Research and Development Programme (2019B110206002)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program (2017BT01C102)。
文摘The selective aerobic oxidation of benzyl alcohol to benzaldehyde has attracted considerable attention because benzaldehyde is a high value-added product. The rate of this typical gas–liquid reaction is significantly affected by mass transfer. In this study, CoTPP-mediated(CoTPP: cobalt(II) mesotetraphenylporphyrin) selective benzyl alcohol oxidation with oxygen was conducted in a membrane microchannel(MMC) reactor and a bubble column(BC) reactor, respectively. We observed that 83% benzyl alcohol was converted within 6.5 min in the MMC reactor, but only less than 10% benzyl alcohol was converted in the BC reactor. Hydrodynamic characteristics and gas–liquid mass transfer performances were compared for the MMC and BC reactors. The MMC reactor was assumed to be a plug flow reactor,and the dimensionless variance was 0.29. Compared to the BC reactor, the gas–liquid mass transfer was intensified significantly in MMC reactor. It could be ascribed to the high gas holdup(2.9 times higher than that of BC reactor), liquid film mass transfer coefficient(8.2 times higher than that of BC reactor), and mass transfer coefficient per unit interfacial area(3.8 times higher than that of BC reactor). Moreover,the Hatta number for the MMC reactor reached up to 0.61, which was about 15 times higher than that of the BC reactor. The computational fluid dynamics calculations for mass fractions in both liquid and gas phases were consistent with the experimental data.
基金supported by the China Academy of Space Technology Innovation fund(2017ZY601026)。
文摘With the advantages of the multiple oxidation states and highly open crystal structures,vanadium-based composites have been considered as the promising cathode materials for aqueous zinc-ion batteries(ZIBs).However,the inherent inferior electrical conductivity,low specific surface area,and sluggish Zn^(2+)diffusion kinetics of the traditional vanadium-based oxides have greatly impeded their development.Herein,a novel hierarchical porous spindle-shaped Ag-V_(2)O_(5) with unique heterostructures was rationally designed via a simple MOF-assisted synthetic method and applied as stable cathode for aqueous ZIBs.The high specific surface area and hierarchically porous superstructures endowed Ag-V_(2)O_(5) with sufficient electrochemical active sites and shortened the diffusion pathways of Zn^(2+),which was beneficial to accelerate the reversible transport of Zn^(2+)and deliver a high specific capacity(426 mA h g^(-1) at 0.1 A g^(-1) and 96.5%capacity retention after 100 cycles).Meanwhile,the self-built-in electric fields at the heterointerface of Ag-V_(2)O_(5) electrode could strengthen the synergistic coupling interaction between Ag and V_(2)O_(5),which can effectively enhance the electric conductivity and maintain the structural integrity,resulting in superb rate capability(326.1 mA h g^(-1) at 5.0 A g^(-1))and remarkable cycling stability(89.7%capacity retention after 2000 cycles at 5.0 A g^(-1)).Moreover,the reversible Zn^(2+)storage mechanism was further investigated and elucidated by kinetics analysis and DFT calculations.
基金supported by the National Key R&D Program of China (2022YFC3004701)the National Natural Science Foundation of China (52274242,51904293)+1 种基金the Natural Science Foundation of Jiangsu Province (BK20190627)the China Postdoctoral Science Foundation (2019M661998).
文摘In the process of green and smart mine construction under the context of carbon neutrality,China's coal safety situation has been continuously improved in recent years.In order to recognize the development of coal production in China and prepare for future monitoring and prevention of safety incidents,this study mainly elaborated on the basic situation of coal resources and national mining accidents over the past five years(2017-2021),from four dimensions(accident level,type,region,and time),and then proposed the preventive measures based on accident statistical laws.The results show that the storage of coal resources has obvious geographic characteristics,mainly concentrated in the Midwest,with coal resources in Shanxi and Shaanxi accounting for about 49.4%.The proportion of coal consumption has dropped from 70.2%to 56%between 2011 and 2021,but still accounts for more than half of the all.Meanwhile,the accident-prone areas are positively correlated with the amount of coal production.Among different levels of coal mine accidents,general accidents had the highest number of accidents and deaths,with 692 accidents and 783 deaths,accounting for 87.6%and 54.64%respectively.The frequency of roof,gas,and transportation accidents is relatively high,and the number of single fatalities caused by gas accidents is the largest,about 4.18.In terms of geographical distribution of accidents,the safety situation in Shanxi Province is the most severe.From the time distribution of coal mine accidents,the accidents mainly occurred in July and August,and rarely occurred in February and December.Finally,the"4+4"safety management model is proposed,combining the statistical results with coal production in China.Based on the existing health and safety management systems,the manage-ments are divided into four sub-categories,and more specific measures are suggested.
基金the National Natural Science Foundation of China(22208065)Guangxi Natural Science Foundation(2022GXNSFBA035483,2020GXNSFDA297007)+1 种基金Opening Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2021K009,2020K002)Special funding for‘Guangxi Bagui Scholars’.
文摘Photocatalytic CO_(2)reduction to valuable product exhibit promising prospect for solving the energy crisis and the greenhouse effect.Herein,Co-Ti_(3)C_(2)T_(x)/g-C_(3)N_(4)(Co-TC/CN)composite with enhanced photocatalytic performance for converting CO_(2)to CO and CH_(4)was constructed by electrostatic self-assembly method.The close contact interface between Co-Ti_(3)C_(2)T_(x)and g-C_(3)N_(4)nanosheets can be used as fast transport channels of photogenerated electrons and effectively promote the separation of photogenerated electrons and holes,and the interface between the Co and Ti_(3)C_(2)T_(x)might be the active sites for CO_(2)adsorption and activation.The optimized Co-Ti_(3)C_(2)T_(x)/g-C_(3)N_(4)composite exhibited the highest photocatalytic performance with the CO and CH_(4)production of 55.04 μmol·g^(-1)and 2.29 μmol·g^(-1),respectively,which were 7.5 times and 5.8 times than those of g-C_(3)N_(4).Furthermore,the stability of g-C_(3)N_(4)was improved after coupling with Co-Ti_(3)C_(2)T_(x).
基金the financial supports that are from the National Natural Science Foundation of China (21921006, U22A20414 and 21938007)the Natural Science Foundation of Jiangsu Province (BK20220002)the open project of the State Key Laboratory of China (KL21-04 and D2021FK055)。
文摘The synthesis of a continuous IMF zeolite membrane was fabricated on tubular substrates by seeded growth for the first time. The straight channels of IMF zeolite with diameters of 0.53–0.59 nm are distinguishable for p-xylene from o-xylene molecules. Pure IMF-phase high-silica IM-5 zeolite seeds with uniform and fine crystal size were fabricated by a new sonication-assisted aging process. The seeds were coated on the support by dipcoating and induced the formation of continuous membrane. Separation performance in p-/o-xylene mixture was investigated at various temperature and pressure. The typical IM-5zeolite membrane had p-/o-xylene separation factor of 3.7. Our results suggest that IM-5 zeolite is a potentially good membrane material for the separation of xylene mixtures.
基金National Natural Science Foundation of China,Grant/Award Numbers:22209126,22279095Shccig-Qinling Program。
文摘The utilization of single atoms(SAs)as trifunctional electrocatalyst for nitro-gen reduction,oxygen reduction,and oxygen evolution reactions(NRR,ORR,and OER)is still a formidable challenge.Herein,we devise one-pot synthesized palladium SAs stabilized on nitrogen-doped carbon palladium SA electrocat-alyst(Pd-SA/NC)as efficient trifunctional electrocatalyst for NRR,ORR,and OER.Pd-SA/NC performs a robust catalytic activity toward NRR with faradaic efficiency of 22.5%at-0.25 V versus reversible hydrogen electrode(RHE),and the relative Pd utilization efficiency is enhanced by 17-fold than Pd-NP/NC.In addition,the half-wave potential reaches 0.876 V versus RHE,amounting to a 58-time higher mass activity than commercial Pt/C.Moreover,the overpotential at 10 mA cm-2 is as low as 287 mV for Pd-SA/NC,outperforming the commer-cial IrO2 by 360 times in turnover frequency at 1.6 V versus RHE.Accordingly,the assembled rechargeable zinc-air battery(ZAB)achieves a maximum power den-sity of 170 mW cm-2,boosted by 2.3 times than Pt/C–IrO2.Two constructed ZABs efficiently power the NRR-OER system to electrochemically generate ammonia implying its superior trifunctionality.
基金grants from the National Basic Research and Development Program of China(2009CB119200)the National Natural Science Foundation of China(31071683)
文摘Four strains of the Q biotype and one of the B biotype of the whitefly Bemisia tabaci collected from China were characterised for resistance to four neonicotinoid insecticides and pymetrozine.Q biotype strains showed moderate to strong resistance to imidacloprid,thiamethoxam and acetamiprid,but little or no cross-resistance to dinotefuron.Resistance to neonicotinoids was consistently associated with resistance to pymetrozine,despite the latter having a distinct(though unresolved)mode of action.The single B biotype strain proved largely susceptible to all the insecticides investigated.Resistance in the Q biotype strains was associated with over-expression of a cytochrome P450 monooxygenase gene,CYP6CM1,whose substrate specificity presumably accounts for the observed cross-resistance profiles.
基金This work was supported by the National Natural Science Foundation of China(21766001,21961160741)Guangxi Natural Science Foundation of China(2018GXNSFAA281342)+1 种基金the Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2018Z009)Special funding for"Guangxi Bagui Scholars".
文摘Magnetic starch microspheres(AAM-MSM)were synthesized via an inverse emulsion graft copolymerization by using mechanically activated cassava starch(MS)as a crude material,acrylic acid(AA)and acrylamide(AM)as graft copolymer monomers,and methyl methacrylate(MMA)as the dispersing agent and used as an adsorbent for the removal of Cd(Ⅱ)ions from aqueous solution.Fourier-transform infrared spectroscopy(FT-IR),X-ray photoelectron spectroscopy(XPS),scanning electron microscopy(SEM),and vibrating sample magnetometry(VSM)were used to characterize the AAM-MSM adsorbent.The results indicated that AA,AM,and MMA were grafted to the MS,and the Fe_(3)O_(4) nanoparticles were encapsulated in the AAM-MSM adsorbent microspheres.The adsorbent exhibited a smooth surface,uniform size,and good sphericity because of the addition of the MMA and provided more adsorption sites for the Cd(Ⅱ)ions.The maximum adsorption capacity of Cd(Ⅱ)on the AAM-MSM was 39.98 mg·g^(-1).The adsorbents were superparamagnetic,and the saturation magnetization was 16.7 A·m^(2)·kg^(-1).Additionally,the adsorption isotherms and kinetics of the adsorption process were further investigated.The process of Cd(Ⅱ)ions adsorbed onto the AAM-MSM could be described more favorably by the pseudo-second-order kinetic and Langmuir isothermal adsorption models,which suggested that the chemical reaction process dominated the adsorption process for the Cd(Ⅱ)and chemisorption was the rate-controlling step during the Cd(Ⅱ)removal process.
文摘Cation substitution in spinel cobaltites(e.g.,ACo2O4,in which A=Mn,Fe,Co,Ni,Cu,or Zn)is a promising strategy to precisely modulate their electronic structure/properties and thus improve the corresponding electrochemical performance for water splitting.However,the fundamental principles and mechanisms are not fully understood.This research aims to systematically investigate the effects of cation substitution in spinel cobaltites derived from mixed-metal-organic frameworks on the oxygen evolution reaction(OER).Among the obtained ACo2O4 catalysts,FeCo2O4 showed excellent OER performance with a current density of 10 mA·cm^-2 at an overpotential of 164 mV in alkaline media.Both theoretical calculations and experimental results demonstrate that the Fe substitution in the crystal lattice of ACo2O4 can significantly accelerate charge transfer,thereby achieving enhanced electrochemical properties.The crystal field of spinel ACo2O4,which determines the valence states of cations A,is identified as the key factor to dictate the OER performance of these spinel cobaltites.
基金the financial support from the National Key R&D Program of China(No.2017YFB0306504)National Natural Science Foundation of China(No.22008094,22178154 and 21878133)+2 种基金Chinese Postdoctoral Science Foundation(No.2019M651743,2020M671364 and 2020M673039)Natural Science Foundation of Jiangsu Province(No.BK20190852)Natural Science Foundation for Jiangsu Colleges and Universities(No.19KJB530005)
文摘A metal-free N-hydroxyphthalimide/hexagonal boron nitride(NHPI/h-BN)catalytic system was developed for deep oxidative desulfurization(ODS)of fuel oils.Detailed experiments find that the heterogenization process of loading NHPI on h-BN not only benefits to the dispersion and utilization of NHPI,but also can significantly promote the catalytic performance.By employing NHPI/h-BN as the catalyst,azodiisobutyronitrile(AIBN)as the metal-free initiator,a 95%conversion of dibenzothiophene(DBT)can be acquired under the reaction conditions of 120°C and atmospheric pressure with molecular oxygen(O_(2))as oxidant.Moreover,the heterogenization is convenient for the regeneration of the catalyst with>94%DBT conversion after being recycled seven times.Characterizations illustrate that the promoted catalytic activity along with the regenerability originate from the interactions between NHPI and h-BN.The catalytic mechanism study shows that molecular oxygen is readily activated by the NHPI/h-BN to form a superoxide radical(O_(2)^(·-)),which oxidize DBT to DBTO2 for desulfurization.
基金financially supported by the National Key Research and Development Program of China (2020YFA0210900)the National Natural Science Foundation of China (No. 21938001 and 21878344)Research and Innovation Team Construction Project of Guangdong University of Petrochemical Technology
文摘Propylene molecule owns two active sites,the direct epoxidation of propylene by dioxygen is still a challenge due to the limitation of selectivity.In this work,the direct liquid-phase propylene aerobic epoxidation protocol by chloride manganese meso-tetraphenylporphyrin(MnTPPCl)was developed.The conversion of propylene was 12.7%,and the selectivity towards PO(propylene oxide)reached up to 80.5%.The formation of PO was attributed to the mechanism via high-valent Mn species,which was confirmed by means of in situ UV–vis spectrum.
基金supported by National Natural Science Foundation of China(21868002 and 21961160741)the Natural Science Foundation of Guangxi Province(2018GXNSFAA281206,2020GXNSFGA297001,2020GXNSFAA297044)+2 种基金Dean Project of Guangxi Key Laboratory of Petrochemical Resource Processing and Process Intensification Technology(2021Z010)Specific research project of Guangxi for research bases and talents(AD18126005)special funding for‘Guangxi Bagui Scholars’,Guangxi scholarship fund for the middle-aged backbone teachers。
文摘Adsorptive recovery of valuable components from industrial wastewater is highly desirable for avoiding resource wastage but remains a challenge.Herein,we develop an efficient continuous adsorption process for recovering aromatic compounds in wastewater from styrene monomer and propylene oxide coproduction(SMPO)plant.Based on our insight into the potential of bio-based porous materials for adsorption application,starch-graft-polystyrene(SPS)and aryl-modifiedβ-cyclodextrin(ACD)were prepared,and novel hypercrosslinked porous polymers combined SPS with ACD(HSPS-ACDs)were synthesized through external crosslinking approach.In a binary-component system,the best-performing one HSPS-ACD(H)with high ACD content and large specific surface area possessed superior capacities for the representative aromatic compounds,acetophenone(AP,2.81 mmol·g^(-1))and 1-phenylethanol(1-PE,1.35 mmol·g^(-1))compared with the previously reported materials.Further,the adsorption properties of aromatic compounds on HSPS-ACD(H)were investigated in batch mode.For practical application,continuous adsorption experiments were conducted in a HSPS-ACD(H)-packed fixed bed,where the target aromatic components in wastewater were effectively retained and further released by elution.Besides showing the reversible adsorption and efficient enrichment effect,the HSPS-ACD(H)-packed fixed bed also maintained great stability in multiple cycles.Moreover,quantum chemical calculations were performed to elucidate the potential mechanism of adsorption of AP and 1-PE onto HSPS-ACD(H).
基金Financial support for this study was kindly provided by the National Natural Science Foundation Project of China(No.51804246,No.52174202)Natural Science Foundation of Xinjiang Province(No.2019D01C057)the Youth Talent Promotion Program of Shaanxi University Association for Science and Technology(No.20200425).
文摘Temperature variation and gas generation at diferent depths and positions in the coal combustion process were studied to determine the propagation and evolution of high temperature regions in the process of coal spontaneous combustion.This study selected coal samples from Mengcun,Shaanxi Province,People’s Republic of China,and developed a semi-enclosed experimental system(furnace)for simulating coal combustion.The thermal mass loss of coal samples under various heating rates(5,10,and 15℃/min)was analyzed through thermogravimetric analysis,and the dynamic characteristics of the coal samples were analyzed;the reliability of the semi-enclosed experimental system was verifed through the equal proportional method of fuzzy response.The results reveal that the high-temperature zone is distributed nonlinearly from the middle to the front end of the furnace,and the temperatures of points in this zone decreased gradually as the layer depth increased.The apparent activation energy of the coal samples during combustion frst increased and then decreased as the conversion degree increased.Furthermore,the proportion of mass loss and the mass loss rate in the coal samples observed in the thermogravimetric experiment is consistent with that observed in the frst and second stages of the experiment conducted using the semi-enclosed system.The research fndings can provide a theoretical basis for the prevention and control of hightemperature zones in coal combustion.
文摘The underground brine resource along the coast of Laizhou Bay is the world’s rare shallow underground brine resource,which occurs in the Laizhou city in the east,and extends to the coastal area of the Binzhou city in
基金supported by Intramural Foundation from Wenzhou Medical College
文摘Four naturally rare 5,6,7-trimethoxy-2,3-cis-dihydroflavonols (3-6) and two 5,6,7-trimethoxy-2,3-trans-dihydroflavonols (7-8) were designed and synthesized. Their antioxidative properties were evaluated by way of examining their scavenging capacities towards DPPH and O2^*- free radicals, as well as by measuring their inhibitory ability against LPO. Both the 2,3-trans and the 2,3- cis conformers exhibited certain quenching abilities to DPPH and O2^*- radicals, while most of the synthetic dihydroflavonols demonstrated remarkable inhibition to LPO.
基金support from the National Natural Science Foundation of China(No.U21A2093)Natural Science Foundation of Shaanxi Province(No.2022JM-260)Fundamental Research Funds for the Central Universities(No.G2022KY05109).This work is also financially supported by the Polymer Electromagnetic Functional Materials Innovation Team of Shaanxi Sanqin Scholars.We would like to thank Zhang San from Shiyanjia Lab(www.shiyanjia.com)for the VSM analysis.
文摘Multiple hetero-interfaces would strengthen interfacial polarization and boost electromagnetic wave absorption,but still remain the formidable challenges in decreasing filler loadings.Herein,sandwich NC@Co/NC@MnO_(2)composites with hollow cavity,multiple hetero-interfaces,and hierarchical structures have been fabricated via the cooperative processes of self-sacrifice strategy and sequential hydrothermal reaction.In the sandwich composites,middle magnetic components(Co/NC)are wrapped by inner N-doped carbon(NC)matrix and outer hierarchical MnO_(2)nanosheets.Importantly,hollow engineering of sandwich composites with multiple hetero-interfaces greatly facilitates the enhancement of absorption bandwidth without sacrificing the absorption intensity.The maximum reflection loss of sandwich NC@Co/NC@MnO_(2)composites reaches-44.8 dB at 2.5 mm and the effective bandwidths is achieved as wide as 9.6 GHz at 2.3 mm.These results provide us a new insight into preparing efficient electromagnetic wave absorbers by interface engineering and hollow construction.
基金supported by the Hainan Province Science and Technology Special Fund(No.ZDYF2022SHFZ094)National Natural Science Foundation of China(No.22166016)+1 种基金Hainan Provincial Key Research and Development Program(No.ZDYF2020222)the open-ended fund of Key Laboratory of Agro-Forestry Environmental Processes and Ecological Regulation of Hainan Province(No.AFEPER202205).
文摘Establishing an effective charge transfer mechanism in carbon nitride(g-C_(3)N_(4))to enhance its photocatalytic activity remains a limiting nuisance.Herein,the combination design of a single Cu atom with hollow g-C_(3)N_(4)nanospheres(Cu-N_(3)structure)has been proven to offer significant opportunities for this crucial challenge.Moreover,this structure endows two pathways for charge transfer in the reaction,namely,the N atoms in the three-dimensional planar structure are only bonded with a single Cu atom,and charge transfer occurs between the plane and the layered structure due to the bending of the interlayered g-C_(3)N_(4)hollow nanospheres.Notably,Cu-N_(3)and hollow nanosphere structures have been certified to greatly enhance the efficiency of photogenerated carrier separation and transfer between the layers and planes by ultrafast spectral analysis.As a result,this catalyst possesses unparalleled photocatalytic efficiency.Specifically,the hydrogen production rate up to 2040μmol h^(−1) g^(−1),which is 51 times that of pure C_(3)N_(4)under visible light conditions.The photocatalytic degradation performance of tetracycline and oxidation performance of benzene is also expressed,with a degradation rate of 100%,a conversion of 97.3%and a selectivity of 99.9%.This work focuses on the structure-activity relationship to provide the possibilities for the development of potential photocatalytic materials.
基金supported by the National Key Research and Development Program Nanotechnology Specific Project(2020YFA0210900)the Science and Technology Key Project of Guangdong Province,China(2020B010188002)+5 种基金Guangdong Natural Science Funds for Distinguished Young Scholar(2022B1515020035)Guangdong Provincial Key R&D Program(2019B110206002)the National Natural Science Foundation of China(22078371,21938001,21961160741)the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(2017BT01C102)the Natural Science Foundation of Guangdong Province(2020A1515011141)the Science and Technology Project of Guangzhou City,China(202102020461)。
文摘Single-atom catalysts(SACs)are considered the best candidates for olefin hydroformylation due to their combined advantages of homogeneous and heterogeneous catalysts.Unlike conventional organo-phosphine modification,Rh SAC is modified by introducing Ca,resulting in a significant increase in activity(maximum~5.7-fold)and stability.Furthermore,a volcano curve between Ca addition ratio and catalytic activity is found.Introducing Ca significantly increases activity by decreasing the energy barrier,but excessive Ca decreases activity due to hindering substrate adsorption and reaction.