Low-concentration acetone detection is of great importance for acetone sensor in the fields of environmental protection and noninvasive diagnosis.In this work,mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)n-p heterojunctions were...Low-concentration acetone detection is of great importance for acetone sensor in the fields of environmental protection and noninvasive diagnosis.In this work,mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)n-p heterojunctions were constructed for efficient improvement of low-concentration acetone gas sensing.The gas-sensing results indicated that the mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)composites with a significantly large specific surface area exhibited significantlyenhanced acetone gas-sensitive performance compared to pure Fe_(2)O_(3).The Fe_(2)O_(3)/Cr_(2)O_(3)composites demonstrated a high response,good selectivity and excellent stability over200 days to 10 ppm acetone at 220℃.And the theoretical detection limit was calculated to reach 0.285 ppm acetone.A feasible acetone sensing mechanism was proposed through electronic band structure and density functional theory.The improved low-concentration acetone sensing performance was due to the formed mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)n-p heterojunctions with a large specific surface area.The Fe_(2)O_(3)/Cr_(2)O_(3)composites showed excellent acetone gas-sensitive performance,which could be a promising candidate for developing low-concentration acetone sensing devices at low working temperatures.展开更多
Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NH...Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.展开更多
Obesity has become a global threat to health;however,the available drugs for treating obesity are limited.We investigated the anti-obesity effect of hydroxy-α-sanshool(HAS),an amide derived from the fruit of Zanthoxy...Obesity has become a global threat to health;however,the available drugs for treating obesity are limited.We investigated the anti-obesity effect of hydroxy-α-sanshool(HAS),an amide derived from the fruit of Zanthoxylum bungeanum,which promotes the management of obesity by triggering the browning of white adipose tissue(WAT)targeting the membrane receptor of transient receptor potential vanilloid 1(TRPV1).However,HAS easily undergoes configuration transformation and oxidative degradation.The short peptide CKGGRAKDC or adipose-targeting sequence(ATS)binds specifically to prohibitin on the surface of WAT cells and can be used as recognition assembly to enhance adipocyte targetability.Furthermore,mesoporous silica nanoparticles(MSNs)are widely used in drug delivery systems because of their large specific surface area and pore volume.Therefore,HAS-loaded adipose-targeted MSNs(MSNs-ATS)were developed to enhance the adipocyte targetability,safety,and efficacy of HAS,and tested on mature 3T3-L1 cells and obese mouse models.MSNs-ATS showed higher specificity for adipocyte targetability without obvious toxicity.HAS-loaded MSNs-ATS showed anti-obesity effects superior to those of HAS alone.In conclusion,we successfully developed adipocyte-targeted,HAS-loaded MSNs with good safety and anti-obesity effects.展开更多
Photocatalytic solar energy conversion to hydrogen is sustainable and attractive for addressing the global energy and environmental issue. Herein, a novel photocatalytic system (NiS/Ni3S4 cocatalysts modified mesoporo...Photocatalytic solar energy conversion to hydrogen is sustainable and attractive for addressing the global energy and environmental issue. Herein, a novel photocatalytic system (NiS/Ni3S4 cocatalysts modified mesoporous TiO2) with superior photocatalytic hydrogen evolution capability through the synergistic impact of NiS/Ni3S4 (NiSx) cocatalyst and efficient hole scavenger has been demonstrated. The photocatalytic hydrogen evolution of TiO2-NiSx hybrids with the different content of NiSx and upon different organic hole scavengers was both investigated. The hybrid of TiO2 decorated with 3%(mole ratio of Ni^2+) NiSx cocatalyst in methanol solution showed the optimal photocatalytic hydrogen evolution rate of 981.59 μmol h^-1 g^-1 which was about 20 times higher than that of bare mesoporous TiO2. Our results suggested that the boosted hydrogen production performance is attributed to both the improved photoinduced electrons migration between NiS and Ni3S4 in cocatalyst and the high hole captured efficiency by hole scavengers of methanol.展开更多
Background:PANoptosis has been identified as a robust inflammatory cell death pathway triggered upon host defense against invaded pathogens such as bacteria and viruses,however,pathogen-free tumor PANoptosis has not b...Background:PANoptosis has been identified as a robust inflammatory cell death pathway triggered upon host defense against invaded pathogens such as bacteria and viruses,however,pathogen-free tumor PANoptosis has not been achieved yet.Reactive oxygen and nitrogen species capable of inducing robust and diverse cell death pathways such as pyroptosis,apoptosis,and necroptosis are supposed to be the potential triggers for tumor PANoptosis by ultrasound(US)-controlled sono-piezodynamic therapy.Methods:S-nitrosothiols(SNO)-zinc peroxide(ZnO_(2))@cyclic dinucleotide(CDN)@mesoporous tetragonal barium titanate(mtBTO)nanoparticles(NZCB NPs)were synthesized by hydrothermal method with subsequent annealing,in situ growth,and finally surface functionalization.Scanning electron microscopy,transmission electron microscopy,X-ray diffraction,atomic force microscopy,Fourier transform infrared spectroscopy,and electron spin resonance were used for materials characterizations.Murine melanoma B16 cells are employed to investigate the in vitro US-initiated tumor PANoptosis by NZCB NPs.In vivo US-initiated tumor PANoptosis was investigated on B16 tumor-bearing C57BL/6J mice.Results:A“boiling-bubbling”strategy is developed to endow the piezoelectric BTO nanocatalysts,with mesoporous architecture,which enables the encapsulation of the immune-agonist CDN(9.4 wt%)to initiate innate immunity of the host.Then,SNO-functionalized ZnO_(2)was further employed to cap the mesoporous nanocatalysts,forming multifunctional piezocatalytic NZCB NPs.Under US irradiation,intracellular massive reactive oxygen and nitrogen species such as superoxide anion radicals,nitric oxide(NO),and peroxynitrite(ONOO-)could be produced from the piezoelectric NZCB NPs,which,synergized with CDN-triggered anti-tumoral immunity,lead to highly immunogenic tumor PANoptosis by NZCB NPs through the tumor microenvironment remodeling.Intratumoral injection of NZCB NPs leads to substantial tumor PANoptosis with immune potentiation,ultimately destroying the tumor xenografts effectively.Conclusion:The present work presents the mesostructure design of piezocatalytic nanomaterials and the crosstalk between oxidative stress and anti-tumor immunity within the tumor,facilitating promising tumor PANoptosis by nanocatalytic oxidation with high effectiveness and biocompatibility.展开更多
Confinement effect is an effective method to enhance carbon dioxide(CO_(2))solubility.In this study,a hybrid sorbent of 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([Hmim][NTf_2])/mesoporous titanium ...Confinement effect is an effective method to enhance carbon dioxide(CO_(2))solubility.In this study,a hybrid sorbent of 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([Hmim][NTf_2])/mesoporous titanium dioxide(M-TiO_(2))/water(H_2O)was developed,and its confinement effect was regulated by changing the pore structure of M-TiO_(2).CO_(2) solubility in the hybrid sorbent was measured experimentally,and the thermodynamic properties including Henry's constant and desorption enthalpy were calculated.Furthermore,the confinement effect in the hybrid sorbent was quantified.Additionally,the hybrid sorbent was recycled with a multi-cycle experiment.The results showed that M-TiO_(2) calcined at 773.2 K(MT500)could lead to an efficient confinement effect.CO_(2) solubility in the hybrid sorbent increased by 49.8%compared to that of H_2O when the mass fraction of[Hmim][NTf_2]/MT500 was 5.0%(mass),where the contribution of confinement effect on Gibbs free energy occupied 5.2%.展开更多
As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 n...As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 nm)severely limits their application in scenarios such as macromolecular mass transfer and so on.In order to overcome this re-striction,mesoporous MOFs(meso-MOFs)with a larger aperture(2-50 nm)have attracted much attention due to their potential applications in biological macromolecular catalysis,energy storage and other fields.To date,how to accurately regulate its mesopore topology and pore ordering still faces important technical challenges.展开更多
Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,...Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.展开更多
Mesoporous framework supported metal nanoparticle catalyst represents a promising material platform for creating multiple active sites that drive tandem reactions. In this study, we demonstrate a novel catalyst design...Mesoporous framework supported metal nanoparticle catalyst represents a promising material platform for creating multiple active sites that drive tandem reactions. In this study, we demonstrate a novel catalyst design that involves the encapsulation of CuNi alloy nanoparticles within mesoporous silicon carbide nanofibers (mSiC_(f)) to achieve efficient tandem conversion of furfural (FFA) into 2-(isopropoxymethyl)furan (IPF). The unique one-dimensional (1D) mesoporous structure of mSiC_(f), coupled with abundant oxygen-containing groups, offers a favorable surface microenvironment for the stabilization of bimetallic CuNi active sites. Through carefully optimizing metal to acid sites, we have developed a catalyst containing a total mass ratio of 20 % Cu and Ni, which exhibits a remarkable performance with complete FFA conversion and 92 % IPF selectivity in 4 h. In-depth mechanistic investigations have revealed that the superior activity of this catalyst is attributed to a tandem reaction mechanism. Initially, FFA is hydrogenated at the dual metal active sites to produce furfuryl alcohol (FOL) as an intermediate, which is subsequently etherified at the acid sites with suitable species and strengths on the mSiC_(f) supports. Additionally, the robust 1D mSiC_(f) framework effectively protects the metal sites from agglomeration, resulting in excellent reusability of the catalyst. This study underscores the potential of mesoporous silicon carbide-supported bimetallic active sites for achieving enhanced tandem catalytic functionality.展开更多
Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted...Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted as ZnS(en)0.5)as a hard template.Inorganic–organic hybrid ZnS(en)0.5,Cd0.5Zn0.5S(en)x,and Cd0.5Zn0.5S nanosheets were sequentially fabricated,and their transformation processes were analyzed in detail.The fabricated Cd0.5Zn0.5S nanosheets exhibited high photocatalytic hydrogen evolution reaction activity in the presence of a sacrificial agent.The Cd0.5Zn0.5S nanosheets exhibited remarkably high H2 production activity of~1395μmol∙h^−1∙g^−1 in pure water with no co-catalyst,which is the highest value reported thus far for bare photocatalysts,to the best of our knowledge.The high activity of these nanosheets is attributed to their distinct nanostructure(e.g.,short transfer distance of photoinduced charge carriers,large number of unsaturated surface atoms,and large surface area).Moreover,ternary NiCo2S4 nanoparticles were employed to facilitate the charge separation and enhance the surface kinetics of H2 evolution.The H2 production rate reached~62.2 and~2436μmol∙h^−1∙g^−1 in triethanolamine and pure water,respectively,over the NiCo2S4/Cd0.5Zn0.5S heterojunctions.The result indicated that the Schottky junction was critical to the enhanced activity.The proposed method can be used for fabricating other highly efficient CdZnS-based photocatalysts for solar-energy conversion or other applications.展开更多
1.Introduction Magnesium oxide(MgO)has attracted considerable attention in recent years due to its economic viability,excellent biocompatibil-ity,chemical stability,and non-toxic,odorless nature[1,2].These inherent pr...1.Introduction Magnesium oxide(MgO)has attracted considerable attention in recent years due to its economic viability,excellent biocompatibil-ity,chemical stability,and non-toxic,odorless nature[1,2].These inherent properties position it as a promising candidate for various applications.展开更多
Mesoporous Ni-Al composite oxide(MNA)with excellent textural and surface properties was prepared using a facile calcination-induced metal heteroatom doping approach and was evaluated as support of Pt-based catalyst fo...Mesoporous Ni-Al composite oxide(MNA)with excellent textural and surface properties was prepared using a facile calcination-induced metal heteroatom doping approach and was evaluated as support of Pt-based catalyst for methylcyclohexane dehydrogenation at a low temperature.The homogeneous incorporation of Ni atoms into the mesoporous framework of alumina and the formation of surface Ni-O-Al bonds benefit the generation of surface coordinated unsaturated aluminum species,which play a crucial role in highly homogenously dispersing Pt active sites in a form of single-atom clusters.Consequently,the resultant catalyst Pt/MNA displayed significantly improved catalytic performance.For example,at 300℃,catalyst Pt/MNA demonstrated a notable catalytic activity with a maximum hydrogen evolution rate of 3057 mmol/gPt/min,even after a long-time reaction up to 100 h or regeneration,which is inspiringly superior to the state-of-the-art supported Ptbased catalysts.The obviously boosted catalytic reactivity of catalyst Pt/MNA can be attributed to the excellent structural and textural properties,the remarkably raised Pt utilization efficiency,and the synergic catalytic effect derived from the interface electron transfer from support MNA to metallic Pt active sites.Our results provided a rational design strategy for the development of promising Pt-based catalyst for methylcyclohexane dehydrogenation,which is vital in the utilization of methylcyclohexane-toluene system for hydrogen storage.展开更多
MXene has attracted great attention due to its high conductivity,large specific surface area and tunable surface functional groups.However,MXene(e.g.,Ti_(3)C_(2))nanosheets tend to stack and mainly offer in-plane site...MXene has attracted great attention due to its high conductivity,large specific surface area and tunable surface functional groups.However,MXene(e.g.,Ti_(3)C_(2))nanosheets tend to stack and mainly offer in-plane sites,showing limited capability in improving the oxygen reduction reaction(ORR)performance of iron phthalocyanine(FePc).In this study,mesoporous Ti_(3)C_(2)(Meso-Ti_(3)C_(2))loaded FePc(FePc/Meso-Ti_(3)C_(2))catalysts were prepared by a simple ultrasonic liquid-phase compounding strategy.Meso-Ti_(3)C_(2)possesses abundant mesopores and edge sites,which optimize the coordination environment and the electronic structure of the FeN4 center in FePc.This optimization improves the mass transfer and the accessibility of the active sites,synergistically enhancing the ORR performance of FePc.As a result,FePc/Meso-Ti_(3)C_(2)shows excellent ORR activity and stability under alkaline conditions with a half-wave potential of 0.914 V against the reversible hydrogen electrode(RHE)and a Tafel slope of 57.2 mV/dec.Furthermore,the zinc-air battery assembled with FePc/Meso-Ti_(3)C_(2)delivers a peak power density of 183.1 mW/cm^(2)and a good long-term discharge stability,exceeding those of FePc/Ti_(3)C_(2)and commercial 20%Pt/C catalysts(20%Pt by mass).展开更多
Nanostructured transition metal oxides,employed as anode materials for lithium-ion batteries,exhibit a higher capacity than the theoretical capacity based on the conversion reaction.To date,the reasons behind this phe...Nanostructured transition metal oxides,employed as anode materials for lithium-ion batteries,exhibit a higher capacity than the theoretical capacity based on the conversion reaction.To date,the reasons behind this phenomenon are unclear.For the one-step evolution of anode material for lithium-ion batteries,it is essential to understand the lithium storage reaction mechanism of the anode material.Herein,we provide a detailed report on the lithium storage and release mechanism of MnO2,using synchrotron-based X-ray techniques.X-ray diffraction and X-ray absorption spectroscopy results indicate that during the first discharge,MnO2 is reduced in the order of MnO2→LixMnO2(1<X<2)→MnO→Mn metal,followed by a reversible reaction between Mn metal and Mn3O4.Furthermore,soft X-ray absorption spectroscopy results indicate that additional reversible formation-decomposition of the electrolyte-derived surface layer occurs and contributes to the reversible capacity of MnO2 after the first discharge.These findings contribute to further understanding of the reaction mechanism and additional lithium storage of MnO2 and suggest practical strategies for developing high energy density anode materials for next-generation Li batteries.展开更多
To clarify the preparation mechanisms of uorinated ordered mesoporous carbon materials (FOMCs), the dissipative par- ticle dynamics method was used to simulate the self-assembly process of the amphiphilic triblock pol...To clarify the preparation mechanisms of uorinated ordered mesoporous carbon materials (FOMCs), the dissipative par- ticle dynamics method was used to simulate the self-assembly process of the amphiphilic triblock poly(ethylene oxide)- poly(propylene oxide)-poly(ethylene oxide) copolymer Pluronic F127 in the aqueous system. The self-assembly mechanisms in aqueous phase and the formation mechanisms of micropores and mesopores were investigated. It was found that the mesoporous structure of the FOMCs was formed by the hydrophobic segments of F127, while the pore wall was formed by both the hydrophilic segments and the carbon precursor in the system. The microporous structure on the pore wall was con- structed by the carbon source in the hydrophilic segments’ spaces after the template was removed. Our ndings could provide understanding and knowledge for the synthesis of mesoporous carbon by the self-assembly method on the mesoscopic scale.展开更多
Structrue and pore characteristics of the mesoporous silica synthesized in acid medium were studied by means of XRD, HRTEM, BET, FT-IR, DSC-TGA, and the reaction mechanism was also investigated deeply. The results sho...Structrue and pore characteristics of the mesoporous silica synthesized in acid medium were studied by means of XRD, HRTEM, BET, FT-IR, DSC-TGA, and the reaction mechanism was also investigated deeply. The results show that mesopores in the sample possess hexagonal arrays obviously, whereas the structure of silica matrix is amorphous. The results also show that the acting mode of silica and CTMA+ inside the mesopores was chemical bonding force. The structure of mesoporous silica was mainly dependent on the aggregational condition of micelle of CTMA+ as well as their liquid-crystallized status. In addition, condensation and dehydration of silicate radicals were accompanied in the process of calcination, which resulted in the mesoporous structure ordered in local range and the pore sizes largening.展开更多
To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li me...To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.展开更多
The mesoporous hydroxyapatite （HA） was synthesized by hydrothermal method utilizing cationic surfactant cetyltrimethylammonium bromide （CTAB） as template. The crystalline phase, morphology and porous structure wer...The mesoporous hydroxyapatite （HA） was synthesized by hydrothermal method utilizing cationic surfactant cetyltrimethylammonium bromide （CTAB） as template. The crystalline phase, morphology and porous structure were characterized respectively by different detecting techniques. The results reveal that the particles are highly crystalline hydroxyapatite phase. The surfactant has little influence on the morphology of the crystals, but affects the porous structure obviously. The sample without CTAB has a low surface area not exceeding 33 m^2/g, and no distinct pores can be observed by TEM. While the samples obtained with the surfactant get better parameters. Numerous open-ended pores centered at 2-7 nm spread unequally on the surface of the hydroxyapatite nanorods. The N2 adsorption-desorption experiments show type IV isotherms with distinct hysteresis loops, illustrating the presence of mesoporous structure. When the mole ratio of CTAB to HA is 1：2, the sample has the largest surface area of 97.1 m^2/g and pore volume of 0.466 cm^3/g.展开更多
A series of functional,tungsten-containing mesoporous silica materials（W-SiO2） have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and m...A series of functional,tungsten-containing mesoporous silica materials（W-SiO2） have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and metal source respectively.These materials were then characterized through X-ray diffraction（XRD）,transmission electron microscopy（TEM）,Raman spectroscopy,Fourier transform infrared spectra（FTIR）,diffuse reflectance spectra（DRS）,and N2 adsorption-desorption,which were found to contain tungsten species that were effectively dispersed throughout the structure.The as-prepared materials W-SiO2 were also found to possess a mesoporous structure.The pore diameters of the respective sample W-SiO2-20 determined from the TEM images ranged from 2 to 4 nm,which was close to the average pore size determined from the nitrogen desorption isotherm（2.9 nm）.The materials were evaluated as catalysts for the heterogeneous oxidative desulfurization of dibenzothiophene（DBT）,which is able to achieve deep desulfurization within 40 min under the optimal conditions（Catalyst（W-SiO2-20）= 0.01 g,temperature = 60℃,oxidant（H2O2）= 20 μL）.For the removal of different organic sulfur compounds within oil,the ability of the catalyst（W-SiO2-20） under the same conditions to remove sulfur compounds decreased in the order：4,6-dimethyldibenzothiophene Dibenzothiophene Benzothiophene 1-dodecanethiol.Additionally,they did not require organic solvents as an extractant in the heterogeneous oxidative desulfurization process.After seven separate catalytic cycles,the desulfurization efficiency was still as high as 90.3%.From the gas chromatography-mass spectrometer analysis,DBT was entirely oxidized to its corresponding sulfone DBTO2 after reaction.A mechanism for the heterogeneous desulfurization reaction was proposed.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.62374154 and12374128)the National Key R&D Program of China(Nos.2022YFB3903200 and 2022YFB3903203)
文摘Low-concentration acetone detection is of great importance for acetone sensor in the fields of environmental protection and noninvasive diagnosis.In this work,mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)n-p heterojunctions were constructed for efficient improvement of low-concentration acetone gas sensing.The gas-sensing results indicated that the mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)composites with a significantly large specific surface area exhibited significantlyenhanced acetone gas-sensitive performance compared to pure Fe_(2)O_(3).The Fe_(2)O_(3)/Cr_(2)O_(3)composites demonstrated a high response,good selectivity and excellent stability over200 days to 10 ppm acetone at 220℃.And the theoretical detection limit was calculated to reach 0.285 ppm acetone.A feasible acetone sensing mechanism was proposed through electronic band structure and density functional theory.The improved low-concentration acetone sensing performance was due to the formed mesoporous Fe_(2)O_(3)/Cr_(2)O_(3)n-p heterojunctions with a large specific surface area.The Fe_(2)O_(3)/Cr_(2)O_(3)composites showed excellent acetone gas-sensitive performance,which could be a promising candidate for developing low-concentration acetone sensing devices at low working temperatures.
基金supported by the National Natural Science Foundation of China(NSFC)(Nos.22278092,22078116 and 22222805)Guangdong Provincial Key Research and Development Program(No.2020B1111380002)+2 种基金Science and Technology Research Project of Guangzhou(Nos.2023A03J0034,2023A04J0077 and 202102020467)State Key Laboratory of Pulp and Paper Engineering(No.202313)Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(No.202255464).
文摘Developing high-capacity carbon-based anode materials is crucial for enhancing the performance of lithium-ion batteries(LIBs).In this study,we presented a nitrogen-doped lignin mesoporous carbon/nickel/nickel oxide(NHMC/Ni/NiO)nanocomposite for developing high-capacity LIBs anode materials through carbonization and selective etching strategies.The synthesized NMHC/Ni/NiO-0.33 composite exhibited a highly regular microstructure with well-dispersed Ni/NiO particles.The composite had a surface area of 408 m^(2)·g^(−1),a mesopore ratio of 75.0%,and a pyridine–nitrogen ratio of 58.9%.The introduction of nitrogen atoms reduced the disordered structure of lignin mesoporous carbon and enhanced its electrical conductivity,thus improving the lithium storage capabilities of the composite.Following 100 cycles at a current density of 0.2 A·g^(−1),the composite demonstrated enhanced Coulomb efficiency and rate performance,achieving a specific discharge capacity of 1230.9 mAh·g^(−1).At a high-current density of 1 A·g^(−1),the composite exhibited an excellent specific discharge capacity of 714.6 mAh·g^(−1).This study presents an innovative method for synthesizing high-performance anode materials of LIBs.
基金supported by the Natural Science Foundation of Sichuan Province(No.2022NSFSC0720)Research Center for the Development of the Comprehensive Health Industry and Rural Revitalization of Sichuan TCM(No.DJKYB202306)State Administration of Traditional Chinese Medicine of Sichuan Province of China(No.2020HJZX001).
文摘Obesity has become a global threat to health;however,the available drugs for treating obesity are limited.We investigated the anti-obesity effect of hydroxy-α-sanshool(HAS),an amide derived from the fruit of Zanthoxylum bungeanum,which promotes the management of obesity by triggering the browning of white adipose tissue(WAT)targeting the membrane receptor of transient receptor potential vanilloid 1(TRPV1).However,HAS easily undergoes configuration transformation and oxidative degradation.The short peptide CKGGRAKDC or adipose-targeting sequence(ATS)binds specifically to prohibitin on the surface of WAT cells and can be used as recognition assembly to enhance adipocyte targetability.Furthermore,mesoporous silica nanoparticles(MSNs)are widely used in drug delivery systems because of their large specific surface area and pore volume.Therefore,HAS-loaded adipose-targeted MSNs(MSNs-ATS)were developed to enhance the adipocyte targetability,safety,and efficacy of HAS,and tested on mature 3T3-L1 cells and obese mouse models.MSNs-ATS showed higher specificity for adipocyte targetability without obvious toxicity.HAS-loaded MSNs-ATS showed anti-obesity effects superior to those of HAS alone.In conclusion,we successfully developed adipocyte-targeted,HAS-loaded MSNs with good safety and anti-obesity effects.
基金the National Natural Science Foundation of China(21501137)the Hubei Natural Science Foundation for financial support(2018CFB680)Support from the Australian Research Council(ARC)through ARC Discovery projects(DP130102699,DP 130102274,DP160102627)
文摘Photocatalytic solar energy conversion to hydrogen is sustainable and attractive for addressing the global energy and environmental issue. Herein, a novel photocatalytic system (NiS/Ni3S4 cocatalysts modified mesoporous TiO2) with superior photocatalytic hydrogen evolution capability through the synergistic impact of NiS/Ni3S4 (NiSx) cocatalyst and efficient hole scavenger has been demonstrated. The photocatalytic hydrogen evolution of TiO2-NiSx hybrids with the different content of NiSx and upon different organic hole scavengers was both investigated. The hybrid of TiO2 decorated with 3%(mole ratio of Ni^2+) NiSx cocatalyst in methanol solution showed the optimal photocatalytic hydrogen evolution rate of 981.59 μmol h^-1 g^-1 which was about 20 times higher than that of bare mesoporous TiO2. Our results suggested that the boosted hydrogen production performance is attributed to both the improved photoinduced electrons migration between NiS and Ni3S4 in cocatalyst and the high hole captured efficiency by hole scavengers of methanol.
基金supported by the Shanghai Rising-Star Program(23QA1407600,23QA1409500)the National Natural Science Foundation of China(82272135,82372121)the National Natural Science Foundation of Shanghai(22ZR1448200).
文摘Background:PANoptosis has been identified as a robust inflammatory cell death pathway triggered upon host defense against invaded pathogens such as bacteria and viruses,however,pathogen-free tumor PANoptosis has not been achieved yet.Reactive oxygen and nitrogen species capable of inducing robust and diverse cell death pathways such as pyroptosis,apoptosis,and necroptosis are supposed to be the potential triggers for tumor PANoptosis by ultrasound(US)-controlled sono-piezodynamic therapy.Methods:S-nitrosothiols(SNO)-zinc peroxide(ZnO_(2))@cyclic dinucleotide(CDN)@mesoporous tetragonal barium titanate(mtBTO)nanoparticles(NZCB NPs)were synthesized by hydrothermal method with subsequent annealing,in situ growth,and finally surface functionalization.Scanning electron microscopy,transmission electron microscopy,X-ray diffraction,atomic force microscopy,Fourier transform infrared spectroscopy,and electron spin resonance were used for materials characterizations.Murine melanoma B16 cells are employed to investigate the in vitro US-initiated tumor PANoptosis by NZCB NPs.In vivo US-initiated tumor PANoptosis was investigated on B16 tumor-bearing C57BL/6J mice.Results:A“boiling-bubbling”strategy is developed to endow the piezoelectric BTO nanocatalysts,with mesoporous architecture,which enables the encapsulation of the immune-agonist CDN(9.4 wt%)to initiate innate immunity of the host.Then,SNO-functionalized ZnO_(2)was further employed to cap the mesoporous nanocatalysts,forming multifunctional piezocatalytic NZCB NPs.Under US irradiation,intracellular massive reactive oxygen and nitrogen species such as superoxide anion radicals,nitric oxide(NO),and peroxynitrite(ONOO-)could be produced from the piezoelectric NZCB NPs,which,synergized with CDN-triggered anti-tumoral immunity,lead to highly immunogenic tumor PANoptosis by NZCB NPs through the tumor microenvironment remodeling.Intratumoral injection of NZCB NPs leads to substantial tumor PANoptosis with immune potentiation,ultimately destroying the tumor xenografts effectively.Conclusion:The present work presents the mesostructure design of piezocatalytic nanomaterials and the crosstalk between oxidative stress and anti-tumor immunity within the tumor,facilitating promising tumor PANoptosis by nanocatalytic oxidation with high effectiveness and biocompatibility.
基金the National Natural Science Foundation of China(22108115,22478415,and 21978134)Natural Science Foundation of Jiangsu Province(BK20241744)。
文摘Confinement effect is an effective method to enhance carbon dioxide(CO_(2))solubility.In this study,a hybrid sorbent of 1-hexyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([Hmim][NTf_2])/mesoporous titanium dioxide(M-TiO_(2))/water(H_2O)was developed,and its confinement effect was regulated by changing the pore structure of M-TiO_(2).CO_(2) solubility in the hybrid sorbent was measured experimentally,and the thermodynamic properties including Henry's constant and desorption enthalpy were calculated.Furthermore,the confinement effect in the hybrid sorbent was quantified.Additionally,the hybrid sorbent was recycled with a multi-cycle experiment.The results showed that M-TiO_(2) calcined at 773.2 K(MT500)could lead to an efficient confinement effect.CO_(2) solubility in the hybrid sorbent increased by 49.8%compared to that of H_2O when the mass fraction of[Hmim][NTf_2]/MT500 was 5.0%(mass),where the contribution of confinement effect on Gibbs free energy occupied 5.2%.
基金support from the National Natural Science Foundation of China(22088101,21733003,22365021,22305132)the Inner Mongolia Autonomous Region“Grassland Talents”Project(2024098)+3 种基金the Inner Mongolia Natural Science Foundation Youth Fund(2023QN02014)The Local Talent Project of Inner Mongolia(12000-15042222)the Basic Research Expenses Supported under 45 Years Old of Inner Mongolia(10000-23112101/036)the“Young Academic Talents”Program of Inner Mongolia University 23600-5233706.
文摘As a class of crystalline porous materials,metal-organic frameworks(MOFs)have shown unique advantages in the fields of catalysis,gas storage and separation,but their inherent microporous structure(pore diameter<2 nm)severely limits their application in scenarios such as macromolecular mass transfer and so on.In order to overcome this re-striction,mesoporous MOFs(meso-MOFs)with a larger aperture(2-50 nm)have attracted much attention due to their potential applications in biological macromolecular catalysis,energy storage and other fields.To date,how to accurately regulate its mesopore topology and pore ordering still faces important technical challenges.
基金supported by National Natural Science Foundation of China(52376104,52201158)Joint Funds of the National Natural Science Foundation of China(U20A20302)+3 种基金Innovative group projects in Hebei Province(E2021202006)the project of Science and Technology in the Universities of Hebei Province(JZX2023006)Natural Science Foundation of Hebei Province(C202202003)Hebei University of Technology Cross-disciplinary(XKJC-2024001)。
文摘Hierarchical lignin-derived ordered mesoporous carbon(HOMC)was significant for advanced supercapacitors.However,achieving controllable fabrication and optimizing electrochemical behavior were challenging.In this work,an eco-friendly HOMC was synthesized using lignin as carbon precursors and Zn^(2+)as cross-linking and pore-forming agents,followed by KHCO_(3)activation,eliminating the need for toxic phenolic resins and acid treatments for metal removal.Machine learning technology,specifically an Artificial Neural Network(ANN model,was utilized to assist the experimental design and prediction.The ANN model suggested an ideal hierarchical structure and optimized oxygen level,achieved through the adjustment of Zn^(2+)additive concentration,carbonization temperature,and subsequent KHCO_(3)activation to maximize capacitance.The HOMC electrode,with a micropore-to-mesopore ratio(S_(micro)/S_(meso))of 1.01 and an oxygen content of 8.81 at%,acquired a specific capacitance of 362 F·g^(-1)at 0.5 A·g^(-1)in 6 mol·L^(-1)KOH electrolyte.The assembled HOMC//HOMC supercapacitor could afford a high energy density of 33.38 Wh·kg^(-1)with a corresponding specific power density of 300 W·kg^(-1)in TEATFB PC electrolyte.Meanwhile,the long-term cycle stability of 94.33%was achieved after 20,000 cycles.This work provides an ANN assisted strategy for the synthesis of HOMC,highlighting its potential to valorize biomass and agricultural waste in sustainable energy storag solutions.
基金Supported by Research Foundation of Overseas Chinese Affairs Office,the State Council,P.R.China,and FujianProvincial Science and Technology Creation Foundation for Young Researchers(No.2 0 0 1J0 2 3)
文摘Sieve effect, complexation, ionic exchange, electrostatic interaction, hydrogen bonding, hydrophobic interaction, and molecular recognition based on molecular imprinting are comprehensively discussed.
基金supported by the National Natu-ral Science Foundation of China(Nos.52225204,52173233,and 52202085)the Innovation Program of Shanghai Municipal Edu-cation Commission(No.2021-01-07-00-03-E00109)+4 种基金Natural Sci-ence Foundation of Shanghai(No.23ZR1479200)the Shanghai Sci-entific and Technological Innovation Project(No.24520712800)“Shuguang Program”Supported by the Shanghai Education Devel-opment Foundation and Shanghai Municipal Education Commis-sion(No.20SG33)the Fundamental Research Funds for the Central Universities(No.2232024Y-01)the DHU Distinguished Young Professor Program(Nos.LZA2022001and LZB2023002).
文摘Mesoporous framework supported metal nanoparticle catalyst represents a promising material platform for creating multiple active sites that drive tandem reactions. In this study, we demonstrate a novel catalyst design that involves the encapsulation of CuNi alloy nanoparticles within mesoporous silicon carbide nanofibers (mSiC_(f)) to achieve efficient tandem conversion of furfural (FFA) into 2-(isopropoxymethyl)furan (IPF). The unique one-dimensional (1D) mesoporous structure of mSiC_(f), coupled with abundant oxygen-containing groups, offers a favorable surface microenvironment for the stabilization of bimetallic CuNi active sites. Through carefully optimizing metal to acid sites, we have developed a catalyst containing a total mass ratio of 20 % Cu and Ni, which exhibits a remarkable performance with complete FFA conversion and 92 % IPF selectivity in 4 h. In-depth mechanistic investigations have revealed that the superior activity of this catalyst is attributed to a tandem reaction mechanism. Initially, FFA is hydrogenated at the dual metal active sites to produce furfuryl alcohol (FOL) as an intermediate, which is subsequently etherified at the acid sites with suitable species and strengths on the mSiC_(f) supports. Additionally, the robust 1D mSiC_(f) framework effectively protects the metal sites from agglomeration, resulting in excellent reusability of the catalyst. This study underscores the potential of mesoporous silicon carbide-supported bimetallic active sites for achieving enhanced tandem catalytic functionality.
文摘Two-dimensional mesoporous ultrathin Cd0.5Zn0.5S nanosheets with a thickness of~1.5 nm were fabricated using a multistep chemical transformation strategy involving inorganic–organic hybrid ZnS-ethylenediamine(denoted as ZnS(en)0.5)as a hard template.Inorganic–organic hybrid ZnS(en)0.5,Cd0.5Zn0.5S(en)x,and Cd0.5Zn0.5S nanosheets were sequentially fabricated,and their transformation processes were analyzed in detail.The fabricated Cd0.5Zn0.5S nanosheets exhibited high photocatalytic hydrogen evolution reaction activity in the presence of a sacrificial agent.The Cd0.5Zn0.5S nanosheets exhibited remarkably high H2 production activity of~1395μmol∙h^−1∙g^−1 in pure water with no co-catalyst,which is the highest value reported thus far for bare photocatalysts,to the best of our knowledge.The high activity of these nanosheets is attributed to their distinct nanostructure(e.g.,short transfer distance of photoinduced charge carriers,large number of unsaturated surface atoms,and large surface area).Moreover,ternary NiCo2S4 nanoparticles were employed to facilitate the charge separation and enhance the surface kinetics of H2 evolution.The H2 production rate reached~62.2 and~2436μmol∙h^−1∙g^−1 in triethanolamine and pure water,respectively,over the NiCo2S4/Cd0.5Zn0.5S heterojunctions.The result indicated that the Schottky junction was critical to the enhanced activity.The proposed method can be used for fabricating other highly efficient CdZnS-based photocatalysts for solar-energy conversion or other applications.
基金financially supported by the National Natural Science Foundation of China(11475041,U21A20323)Kunlun Talent Program of Qinghai Province,Qinghai Provincial Science and Technology Project(2024-QY-203)Sci-Tech Project of Qinghai Salt Lake Industry Co.,Ltd.(E141GH01).
文摘1.Introduction Magnesium oxide(MgO)has attracted considerable attention in recent years due to its economic viability,excellent biocompatibil-ity,chemical stability,and non-toxic,odorless nature[1,2].These inherent properties position it as a promising candidate for various applications.
基金supported by the National Natural Science Foundation of China(21975174 and 22378286)the Natural Science Foundation of Shanxi Province,China(202403021221036)+1 种基金the Funds for Central Government to Guide Local Science and Technology Development(YDZJSX2021A014)the Research Project Supported by Shanxi Scholarship Council of China(2024-036).
文摘Mesoporous Ni-Al composite oxide(MNA)with excellent textural and surface properties was prepared using a facile calcination-induced metal heteroatom doping approach and was evaluated as support of Pt-based catalyst for methylcyclohexane dehydrogenation at a low temperature.The homogeneous incorporation of Ni atoms into the mesoporous framework of alumina and the formation of surface Ni-O-Al bonds benefit the generation of surface coordinated unsaturated aluminum species,which play a crucial role in highly homogenously dispersing Pt active sites in a form of single-atom clusters.Consequently,the resultant catalyst Pt/MNA displayed significantly improved catalytic performance.For example,at 300℃,catalyst Pt/MNA demonstrated a notable catalytic activity with a maximum hydrogen evolution rate of 3057 mmol/gPt/min,even after a long-time reaction up to 100 h or regeneration,which is inspiringly superior to the state-of-the-art supported Ptbased catalysts.The obviously boosted catalytic reactivity of catalyst Pt/MNA can be attributed to the excellent structural and textural properties,the remarkably raised Pt utilization efficiency,and the synergic catalytic effect derived from the interface electron transfer from support MNA to metallic Pt active sites.Our results provided a rational design strategy for the development of promising Pt-based catalyst for methylcyclohexane dehydrogenation,which is vital in the utilization of methylcyclohexane-toluene system for hydrogen storage.
文摘MXene has attracted great attention due to its high conductivity,large specific surface area and tunable surface functional groups.However,MXene(e.g.,Ti_(3)C_(2))nanosheets tend to stack and mainly offer in-plane sites,showing limited capability in improving the oxygen reduction reaction(ORR)performance of iron phthalocyanine(FePc).In this study,mesoporous Ti_(3)C_(2)(Meso-Ti_(3)C_(2))loaded FePc(FePc/Meso-Ti_(3)C_(2))catalysts were prepared by a simple ultrasonic liquid-phase compounding strategy.Meso-Ti_(3)C_(2)possesses abundant mesopores and edge sites,which optimize the coordination environment and the electronic structure of the FeN4 center in FePc.This optimization improves the mass transfer and the accessibility of the active sites,synergistically enhancing the ORR performance of FePc.As a result,FePc/Meso-Ti_(3)C_(2)shows excellent ORR activity and stability under alkaline conditions with a half-wave potential of 0.914 V against the reversible hydrogen electrode(RHE)and a Tafel slope of 57.2 mV/dec.Furthermore,the zinc-air battery assembled with FePc/Meso-Ti_(3)C_(2)delivers a peak power density of 183.1 mW/cm^(2)and a good long-term discharge stability,exceeding those of FePc/Ti_(3)C_(2)and commercial 20%Pt/C catalysts(20%Pt by mass).
基金supported by the Samsung Reserach Funding & Incubation Center of Samsung Electronics under Project Number MA1401-52。
文摘Nanostructured transition metal oxides,employed as anode materials for lithium-ion batteries,exhibit a higher capacity than the theoretical capacity based on the conversion reaction.To date,the reasons behind this phenomenon are unclear.For the one-step evolution of anode material for lithium-ion batteries,it is essential to understand the lithium storage reaction mechanism of the anode material.Herein,we provide a detailed report on the lithium storage and release mechanism of MnO2,using synchrotron-based X-ray techniques.X-ray diffraction and X-ray absorption spectroscopy results indicate that during the first discharge,MnO2 is reduced in the order of MnO2→LixMnO2(1<X<2)→MnO→Mn metal,followed by a reversible reaction between Mn metal and Mn3O4.Furthermore,soft X-ray absorption spectroscopy results indicate that additional reversible formation-decomposition of the electrolyte-derived surface layer occurs and contributes to the reversible capacity of MnO2 after the first discharge.These findings contribute to further understanding of the reaction mechanism and additional lithium storage of MnO2 and suggest practical strategies for developing high energy density anode materials for next-generation Li batteries.
基金supported by the National Natural Science Foundation of China (No. 21104035)
文摘To clarify the preparation mechanisms of uorinated ordered mesoporous carbon materials (FOMCs), the dissipative par- ticle dynamics method was used to simulate the self-assembly process of the amphiphilic triblock poly(ethylene oxide)- poly(propylene oxide)-poly(ethylene oxide) copolymer Pluronic F127 in the aqueous system. The self-assembly mechanisms in aqueous phase and the formation mechanisms of micropores and mesopores were investigated. It was found that the mesoporous structure of the FOMCs was formed by the hydrophobic segments of F127, while the pore wall was formed by both the hydrophilic segments and the carbon precursor in the system. The microporous structure on the pore wall was con- structed by the carbon source in the hydrophilic segments’ spaces after the template was removed. Our ndings could provide understanding and knowledge for the synthesis of mesoporous carbon by the self-assembly method on the mesoscopic scale.
基金FundedbytheNationalNaturalScienceFoundationofChi na (5 0 2 72 0 4 8)andtheNaturalScienceFoundationofHubeiProv ince (2 0 0 1ABB0 76 )
文摘Structrue and pore characteristics of the mesoporous silica synthesized in acid medium were studied by means of XRD, HRTEM, BET, FT-IR, DSC-TGA, and the reaction mechanism was also investigated deeply. The results show that mesopores in the sample possess hexagonal arrays obviously, whereas the structure of silica matrix is amorphous. The results also show that the acting mode of silica and CTMA+ inside the mesopores was chemical bonding force. The structure of mesoporous silica was mainly dependent on the aggregational condition of micelle of CTMA+ as well as their liquid-crystallized status. In addition, condensation and dehydration of silicate radicals were accompanied in the process of calcination, which resulted in the mesoporous structure ordered in local range and the pore sizes largening.
基金Financial support from the National Natural Science Foundation of China (22075320)。
文摘To achieve high energy density in lithium batteries,the construction of lithium-ion/metal hybrid anodes is a promising strategy.In particular,because of the anisotropy of graphite,hybrid anode formed by graphite/Li metal has low transport kinetics and is easy to causes the growth of lithium dendrites and accumulation of dead Li,which seriously affects the cycle life of batteries and even causes safety problems.Here,by comparing graphite with two types of hard carbon,it was found that hybrid anode formed by hard carbon and lithium metal,possessing more disordered mesoporous structure and lithophilic groups,presents better performance.Results indicate that the mesoporous structure provides abundant active site and storage space for dead lithium.With the synergistic effect of this structure and lithophilic functional groups(–COOH),the reversibility of hard carbon/lithium metal hybrid anode is maintained,promoting uniform deposition of lithium metal and alleviating formation of lithium dendrites.The hybrid anode maintains a 99.5%Coulombic efficiency(CE)after 260 cycles at a specific capacity of 500 m Ah/g.This work provides new insights into the hybrid anodes formed by carbon-based materials and lithium metal with high specific energy and fast charging ability.
基金Projects(51102285,81170912)supported by the National Natural Science Foundation of ChinaProject supported by the Open Foundation of State Key Laboratory of Powder Metallurgy,China
文摘The mesoporous hydroxyapatite （HA） was synthesized by hydrothermal method utilizing cationic surfactant cetyltrimethylammonium bromide （CTAB） as template. The crystalline phase, morphology and porous structure were characterized respectively by different detecting techniques. The results reveal that the particles are highly crystalline hydroxyapatite phase. The surfactant has little influence on the morphology of the crystals, but affects the porous structure obviously. The sample without CTAB has a low surface area not exceeding 33 m^2/g, and no distinct pores can be observed by TEM. While the samples obtained with the surfactant get better parameters. Numerous open-ended pores centered at 2-7 nm spread unequally on the surface of the hydroxyapatite nanorods. The N2 adsorption-desorption experiments show type IV isotherms with distinct hysteresis loops, illustrating the presence of mesoporous structure. When the mole ratio of CTAB to HA is 1：2, the sample has the largest surface area of 97.1 m^2/g and pore volume of 0.466 cm^3/g.
基金supported by the National Nature Science Foundation of China(21276117,21376111,21406092)~~
文摘A series of functional,tungsten-containing mesoporous silica materials（W-SiO2） have been fabricated directly from an ionic liquid that contained imidazole and polyoxometalate,which acted as mesoporous template and metal source respectively.These materials were then characterized through X-ray diffraction（XRD）,transmission electron microscopy（TEM）,Raman spectroscopy,Fourier transform infrared spectra（FTIR）,diffuse reflectance spectra（DRS）,and N2 adsorption-desorption,which were found to contain tungsten species that were effectively dispersed throughout the structure.The as-prepared materials W-SiO2 were also found to possess a mesoporous structure.The pore diameters of the respective sample W-SiO2-20 determined from the TEM images ranged from 2 to 4 nm,which was close to the average pore size determined from the nitrogen desorption isotherm（2.9 nm）.The materials were evaluated as catalysts for the heterogeneous oxidative desulfurization of dibenzothiophene（DBT）,which is able to achieve deep desulfurization within 40 min under the optimal conditions（Catalyst（W-SiO2-20）= 0.01 g,temperature = 60℃,oxidant（H2O2）= 20 μL）.For the removal of different organic sulfur compounds within oil,the ability of the catalyst（W-SiO2-20） under the same conditions to remove sulfur compounds decreased in the order：4,6-dimethyldibenzothiophene Dibenzothiophene Benzothiophene 1-dodecanethiol.Additionally,they did not require organic solvents as an extractant in the heterogeneous oxidative desulfurization process.After seven separate catalytic cycles,the desulfurization efficiency was still as high as 90.3%.From the gas chromatography-mass spectrometer analysis,DBT was entirely oxidized to its corresponding sulfone DBTO2 after reaction.A mechanism for the heterogeneous desulfurization reaction was proposed.
