目的探究不同肉酱比对鹿肉酱中挥发性有机化合物(volatile organic compounds,VOCs)影响的差异性,并筛选不同肉酱比的关键性VOCs。方法利用电子鼻结合气相色谱-离子迁移谱法(gas chromatography-ion mobility spectrometry,GC-IMS)检测...目的探究不同肉酱比对鹿肉酱中挥发性有机化合物(volatile organic compounds,VOCs)影响的差异性,并筛选不同肉酱比的关键性VOCs。方法利用电子鼻结合气相色谱-离子迁移谱法(gas chromatography-ion mobility spectrometry,GC-IMS)检测不同肉酱比加工的鹿肉酱样品中的香气类别及VOCs成分,通过计算偏最小二乘法判别(partial least squares discriminant analysis,PLS-DA)和正交-偏最小二乘法判别(orthogonal partial least squares discriminant analysis,OPLS-DA)分析变量重要性因子(variable important for the projection,VIP),筛选可区分不同肉酱比的鹿肉酱样品中差异性影响最关键的变量敏感物质及VOCs(VIP>1)。结果电子鼻传感器S3、S7、S9和S10对应的氨类、芳香族、硫化物和萜烯类、芳香族、硫化氢类、烷烃类等敏感物质是不同肉酱比的鹿肉酱样品中最关键的挥发类特征性气味;利用GC-IMS共检测出82种主要VOCs,筛选出33种关键差异性特征VOCs(VIP>1),与电子鼻的关键特征性香气检测结果一致。结论基于电子鼻和GC-IMS的主要特征香气标志物的聚类分析能够有效、全面、客观地对不同肉酱比的鹿肉酱中关键挥发性性气味和VOCs进行区分和评价。展开更多
目的优化黑参甜米酒加工工艺,测定其挥发性成分。方法以黑参添加量、甜酒曲添加量、发酵时间、发酵温度进行单因素试验,通过正交试验确定最佳工艺。结果在黑参添加量为4%、甜酒曲添加量为2.0%、发酵温度30℃、发酵时间为72 h时的条件下...目的优化黑参甜米酒加工工艺,测定其挥发性成分。方法以黑参添加量、甜酒曲添加量、发酵时间、发酵温度进行单因素试验,通过正交试验确定最佳工艺。结果在黑参添加量为4%、甜酒曲添加量为2.0%、发酵温度30℃、发酵时间为72 h时的条件下感官评分最高,酒精度为15%vol,其理化指标及微生物指标符合相关标准。所得黑参甜米酒酒香浓郁并伴有黑参特有的香气,口感醇厚、色泽清亮。通过顶空-气相色谱-离子迁移谱法(headspace gas chromatography ion mobility spectrometry,HS-GC-IMS)分析,共鉴定出36个挥发性成分,其中成分明确的有29种,酸类6种、烃类2种、醇类6种、酯类4种、酚类1种、醛类7种、酮类3种。结论以黑参和糯米为原料制备黑参甜米酒,通过对黑参米酒加工工艺的优化,得到适宜的加工条件,通过HS-GC-IMS测定米酒中的挥发性成分,为新型米酒成分的分析提供参考,为米酒赋予黑参特有的保健功能。展开更多
Aqueous zinc-ion batteries(AZIBs) are promising candidates for the large-scale energy storage systems due to their high intrinsic safety,cost-effectiveness and environmental friendliness.However,issues such as dendrit...Aqueous zinc-ion batteries(AZIBs) are promising candidates for the large-scale energy storage systems due to their high intrinsic safety,cost-effectiveness and environmental friendliness.However,issues such as dendrite growth,hydrogen evolution reaction,and interfacial passivation occurring at the anode/electrolyte interface(AEI) have hindered their practical application.Constructing a stable AEI plays a key role in regulating zinc deposition and improving the cycle life of AZIBs.The fundamentals of AEI and the challenges faced by the Zn anode due to unstable interfaces are discussed.A comprehensive summary of electrolyte regulation strategies by electrolyte engineering to achieve a stable Zn anode is provided.The effectiveness evaluation techniques for stable AEI are also analyzed,including the interfacial chemistry and surface morphology evolution of the Zn anode.Finally,suggestions and perspectives for future research are offered about enabling a durable and stable AEI via electrolyte engineering,which may pave the way for developing high-performance AZIBs.展开更多
To obtain high-performance Zr-based ultra-high-temperature composites,Zr-based ultra-high-temperature gradient composites were prepared by changing the laying method of the infiltrant via reactive melt infiltration.Th...To obtain high-performance Zr-based ultra-high-temperature composites,Zr-based ultra-high-temperature gradient composites were prepared by changing the laying method of the infiltrant via reactive melt infiltration.The effects of different infiltrant laying methods on the microstructure and ablative properties of Zr-based ultrahigh-temperature gradient composites were investigated.The results showed that the gradient structure of the Zr-based ultrahigh-temperature gradient composites differed when the composition ratio of the infiltrant was changed.When the thicknesses of the Zr/Mo/Si layers were 6/4/12 mm and 8/2/12 mm,the SiMoZrC solid solution content in the samples increased and decreased along the infiltration direction,respectively.The gradient samples were ablated in an oxyacetylene flame at 3000°C for 40 s.The ablation resistance of the sample was the highest when the infiltrant was a powder and the thickness of the Zr/Mo/Si layer was 6/4/12 mm.展开更多
Due to a series of exceptional properties,titanium and titanium alloys have received extensive attention in recent years.Different from other alloy systems,there are two allotropes and a sequence of metastable phases ...Due to a series of exceptional properties,titanium and titanium alloys have received extensive attention in recent years.Different from other alloy systems,there are two allotropes and a sequence of metastable phases in titanium alloys.By summarizing the recent investigations,the phase transformation processes corresponding to the common phases and also some less reported phases are reviewed.For the phase transformation only involvingαandβphases,it can be divided intoβ→αtransformation and a reverse transformation.The former one has been demonstrated from the orientation relationship betweenαandβphases and the regulation ofαmorphology.For the latter transformation,the role of the stress has been discussed.In terms of the metastable phases,the mechanisms of phase formation and their effects on microstructure and mechanical properties have been discussed.Finally,some suggestions about the development of titanium alloys have been proposed.展开更多
The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulati...The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulations of ethane dehydrogenation over Co@BEA zeolite at different temperatures.AIMD simulations showed that a sharp decrease in free energy barrier as temperature increased.Our analysis of the temperature dependence of activation free energies uncovered an unusual entropic effect accompanying the reaction.The unique spatial structures around the Co active site at different temperatures influenced both the extent of charge transfer in the transition state and the arrangement of 3d orbital energy levels.We provided explanations consistent with the principles of thermodynamics and statistical physics.The insights gained at the atomic level have offered a fresh interpretation of the intricate long-range interplay between local chemical reactions and extensive chemical environments.展开更多
Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2) reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.Howe...Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2) reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.However,photoreduction of CO_(2) by MHP remains a challenge because of the slow charge separation and transfer.Herein,a cobalt single-atom modified nitrogen-doped graphene(Co-NG)cocatalyst is prepared for enhanced photocatalytic CO_(2) reduction of bismuth-based MHP Cs_(3)Bi_(2)Br_(9).The optimal Cs_(3)Bi_(2)Br_(9)/Co-NG composite exhibits the CO production rate of 123.16μmol g^(-1)h^(-1),which is 17.3 times higher than that of Cs_(3)Bi_(2)Br_(9).Moreover,the Cs_(3)Bi_(2)Br_(9)/Co-NG composite photocatalyst exhibits nearly 100% CO selectivity as well as impressive long-term stability.Charge carrier dynamic characterizations such as Kelvin probe force microscopy(KPFM),single-particle PL microscope and transient absorption(TA)spectroscopy demonstrate the vital role of Co-NG cocatalyst in accelerating the transfer and separation of photogenerated charges and improving photocatalytic performance.The reaction mechanism has been demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy measurement.In addition,in situ X-ray photoelectron spectroscopy test and theoretical calculation reveal the reaction reactive sites and reaction energy barriers,demonstrating that the introduction of Co-NG promotes the formation of ^(*)COOH intermediate,providing sufficient evidence for the highly selective generation of CO.This work provides an effective single-atom-based cocatalyst modification strategy for photocatalytic CO_(2) reduction and is expected to shed light on other photocatalytic applications.展开更多
By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variationa...By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variational Zn-salen ligands RZn and NADH(reduced nicotinamide adenine dinucleotide)mimic modified tridentate ligands with square-planar Pd ions.UV-Vis and luminescence spectra experiments reveal that different anions could selec-tively interact with different sites of Zn-salen modified metal-organic cages to achieve the structural regulation of cage compound,by using the differentiated host-guest electrostatic interactions of counter ions with metal-organic hosts.Compared to other anions,the presence of chloride ions caused the most significant fluorescence emission enhancement of Pd‑R(Zn),meanwhile,the UV-Vis absorption band attributed to the salen aromatic backbone showed an absorption decrease,and the metal-to-ligand induced peak displayed a blue shift effect.Circular dichro-ism and ^(1)H NMR spectra further demonstrate that the introduction of chloride anions is beneficial to keeping a more rigid scaffold.展开更多
A 499.8 MHz SOLEIL-type superconducting cavity was simulated and designed for the first time in this paper.The higher-order mode(HOM)properties of the cavity were investigated.Two kinds of coaxial HOM couplers were de...A 499.8 MHz SOLEIL-type superconducting cavity was simulated and designed for the first time in this paper.The higher-order mode(HOM)properties of the cavity were investigated.Two kinds of coaxial HOM couplers were designed.Using 4 L-type and 4 T-type HOM couplers,the longitudinal impedance and the transverse impedances were suppressed to below 3 kΩand 30 kΩ/m,respectivly.The HOM damping requirements of Hefei Advanced Light Facility(HALF)were satisfied.This paper conducted an in-depth study on the radio frequency(RF)design,multipacting optimization,and thermal analysis of these coaxial couplers.Simulation results indicated that under operating acceleration voltage,the optimized couplers does not exhibit multiplicating or thermal breakdown phenomena.The cavity has the potential to reach a higher acceleration gradient.展开更多
Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species for...Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species formed on Au sites diffuses to the Ti sites to form the Ti-hydroperoxo intermedi-ates and contributes to the formation of propylene oxide(PO).In principle,thermal treatment will significantly affect the chemical and physical structures of Ti-containing materials.Consequently,the synergy between tailored Ti sites with different surface properties and Au sites is highly expected to enhance the catalytic performance for the reaction.Herein,we systematically studied the intrinsic effects of different microenvironments around Ti sites on the PO adsorption/desorption and conversion,and then effectively improved the catalytic performance by tailoring the number of surface hydroxyl groups.The Ti^(Ⅵ) material with fewer hydroxyls stimulates a remarkable enhancement in PO selectivity and H_(2) efficiency compared to the Ti^(Ⅵ) material that possessed more hydroxyls,offering a 7-fold and 4-fold increase,respectively.As expected,the Ti^(Ⅵ+Ⅳ) and Ti^(Ⅳ) materials also exhibit a similar phenomenon to the Ti^(Ⅵ) materials through the same thermal treatment,which strongly supports that the Ti sites microenvironment is an important factor in suppressing PO con-version and enhancing catalytic performance.These insights could provide guidance for the rational preparation and optimization of Ti-containing materials synergizing with Au catalysts for propylene epoxidation.展开更多
The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficien...The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2) conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2) electrolysis.It commences with an overview of the latest advancements in acidic CO_(2) electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2) electrolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2) electrolysis are suggested.展开更多
Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilita...Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer,but the precise ordered alignment is limited due to the non-covalentπ-stacking of COF layers,accordingly hindering out-of-plane transfer kinetics.Herein,we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO_(2) microsphere.Compared to the achiral COF analogues,the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration,thereby affording superior photocatalytic performance in hydrogen evolution from water splitting.Taking the simplest ketoenamine-linked chiral COF as a shell of SiO_(2) particle,the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g^(-1)h^(-1)along with the apparent quantum efficiency of 14.31% at 475 nm.Furthermore,the composite photocatalysts could be fabricated into a film device,displaying a remarkable photocatalytic performance of 178.0 mmol m^(-2)h^(-1)for hydrogen evolution.Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties.展开更多
文摘目的探究不同肉酱比对鹿肉酱中挥发性有机化合物(volatile organic compounds,VOCs)影响的差异性,并筛选不同肉酱比的关键性VOCs。方法利用电子鼻结合气相色谱-离子迁移谱法(gas chromatography-ion mobility spectrometry,GC-IMS)检测不同肉酱比加工的鹿肉酱样品中的香气类别及VOCs成分,通过计算偏最小二乘法判别(partial least squares discriminant analysis,PLS-DA)和正交-偏最小二乘法判别(orthogonal partial least squares discriminant analysis,OPLS-DA)分析变量重要性因子(variable important for the projection,VIP),筛选可区分不同肉酱比的鹿肉酱样品中差异性影响最关键的变量敏感物质及VOCs(VIP>1)。结果电子鼻传感器S3、S7、S9和S10对应的氨类、芳香族、硫化物和萜烯类、芳香族、硫化氢类、烷烃类等敏感物质是不同肉酱比的鹿肉酱样品中最关键的挥发类特征性气味;利用GC-IMS共检测出82种主要VOCs,筛选出33种关键差异性特征VOCs(VIP>1),与电子鼻的关键特征性香气检测结果一致。结论基于电子鼻和GC-IMS的主要特征香气标志物的聚类分析能够有效、全面、客观地对不同肉酱比的鹿肉酱中关键挥发性性气味和VOCs进行区分和评价。
文摘目的优化黑参甜米酒加工工艺,测定其挥发性成分。方法以黑参添加量、甜酒曲添加量、发酵时间、发酵温度进行单因素试验,通过正交试验确定最佳工艺。结果在黑参添加量为4%、甜酒曲添加量为2.0%、发酵温度30℃、发酵时间为72 h时的条件下感官评分最高,酒精度为15%vol,其理化指标及微生物指标符合相关标准。所得黑参甜米酒酒香浓郁并伴有黑参特有的香气,口感醇厚、色泽清亮。通过顶空-气相色谱-离子迁移谱法(headspace gas chromatography ion mobility spectrometry,HS-GC-IMS)分析,共鉴定出36个挥发性成分,其中成分明确的有29种,酸类6种、烃类2种、醇类6种、酯类4种、酚类1种、醛类7种、酮类3种。结论以黑参和糯米为原料制备黑参甜米酒,通过对黑参米酒加工工艺的优化,得到适宜的加工条件,通过HS-GC-IMS测定米酒中的挥发性成分,为新型米酒成分的分析提供参考,为米酒赋予黑参特有的保健功能。
基金financially supported by the National Natural Science Foundation of China (No. 52377222)the Natural Science Foundation of Hunan Province, China (Nos. 2023JJ20064, 2023JJ40759)。
文摘Aqueous zinc-ion batteries(AZIBs) are promising candidates for the large-scale energy storage systems due to their high intrinsic safety,cost-effectiveness and environmental friendliness.However,issues such as dendrite growth,hydrogen evolution reaction,and interfacial passivation occurring at the anode/electrolyte interface(AEI) have hindered their practical application.Constructing a stable AEI plays a key role in regulating zinc deposition and improving the cycle life of AZIBs.The fundamentals of AEI and the challenges faced by the Zn anode due to unstable interfaces are discussed.A comprehensive summary of electrolyte regulation strategies by electrolyte engineering to achieve a stable Zn anode is provided.The effectiveness evaluation techniques for stable AEI are also analyzed,including the interfacial chemistry and surface morphology evolution of the Zn anode.Finally,suggestions and perspectives for future research are offered about enabling a durable and stable AEI via electrolyte engineering,which may pave the way for developing high-performance AZIBs.
基金supported by the National Natural Science Foundation of China(No.U19A2099)the Open Fund for Hubei Provincial Key Laboratory of Advanced Aerospace Power Technology,China(No.DLJJ2103007)the Hunan Graduate Research Innovation Project,China(No.CX20220097)。
文摘To obtain high-performance Zr-based ultra-high-temperature composites,Zr-based ultra-high-temperature gradient composites were prepared by changing the laying method of the infiltrant via reactive melt infiltration.The effects of different infiltrant laying methods on the microstructure and ablative properties of Zr-based ultrahigh-temperature gradient composites were investigated.The results showed that the gradient structure of the Zr-based ultrahigh-temperature gradient composites differed when the composition ratio of the infiltrant was changed.When the thicknesses of the Zr/Mo/Si layers were 6/4/12 mm and 8/2/12 mm,the SiMoZrC solid solution content in the samples increased and decreased along the infiltration direction,respectively.The gradient samples were ablated in an oxyacetylene flame at 3000°C for 40 s.The ablation resistance of the sample was the highest when the infiltrant was a powder and the thickness of the Zr/Mo/Si layer was 6/4/12 mm.
基金financially supported by the National Natural Science Foundation of China(Nos.U23A20540,52371127)the Science and Technology Innovation Program of Hunan Province,China(No.2022RC3035)the Fundamental Research Funds for the Central Universities of Central South University,China(No.2024ZZTS0077)。
文摘Due to a series of exceptional properties,titanium and titanium alloys have received extensive attention in recent years.Different from other alloy systems,there are two allotropes and a sequence of metastable phases in titanium alloys.By summarizing the recent investigations,the phase transformation processes corresponding to the common phases and also some less reported phases are reviewed.For the phase transformation only involvingαandβphases,it can be divided intoβ→αtransformation and a reverse transformation.The former one has been demonstrated from the orientation relationship betweenαandβphases and the regulation ofαmorphology.For the latter transformation,the role of the stress has been discussed.In terms of the metastable phases,the mechanisms of phase formation and their effects on microstructure and mechanical properties have been discussed.Finally,some suggestions about the development of titanium alloys have been proposed.
文摘The C–H bond activation in alkane dehydrogenation reactions is a key step in determining the reaction rate.To understand the impact of entropy,we performed ab initio static and molecular dynamics free energy simulations of ethane dehydrogenation over Co@BEA zeolite at different temperatures.AIMD simulations showed that a sharp decrease in free energy barrier as temperature increased.Our analysis of the temperature dependence of activation free energies uncovered an unusual entropic effect accompanying the reaction.The unique spatial structures around the Co active site at different temperatures influenced both the extent of charge transfer in the transition state and the arrangement of 3d orbital energy levels.We provided explanations consistent with the principles of thermodynamics and statistical physics.The insights gained at the atomic level have offered a fresh interpretation of the intricate long-range interplay between local chemical reactions and extensive chemical environments.
文摘Metal halide perovskite(MHP)has become one of the most promising materials for photocatalytic CO_(2) reduction owing to the wide light absorption range,negative conduction band position and high reduction ability.However,photoreduction of CO_(2) by MHP remains a challenge because of the slow charge separation and transfer.Herein,a cobalt single-atom modified nitrogen-doped graphene(Co-NG)cocatalyst is prepared for enhanced photocatalytic CO_(2) reduction of bismuth-based MHP Cs_(3)Bi_(2)Br_(9).The optimal Cs_(3)Bi_(2)Br_(9)/Co-NG composite exhibits the CO production rate of 123.16μmol g^(-1)h^(-1),which is 17.3 times higher than that of Cs_(3)Bi_(2)Br_(9).Moreover,the Cs_(3)Bi_(2)Br_(9)/Co-NG composite photocatalyst exhibits nearly 100% CO selectivity as well as impressive long-term stability.Charge carrier dynamic characterizations such as Kelvin probe force microscopy(KPFM),single-particle PL microscope and transient absorption(TA)spectroscopy demonstrate the vital role of Co-NG cocatalyst in accelerating the transfer and separation of photogenerated charges and improving photocatalytic performance.The reaction mechanism has been demonstrated by in situ diffuse reflectance infrared Fourier-transform spectroscopy measurement.In addition,in situ X-ray photoelectron spectroscopy test and theoretical calculation reveal the reaction reactive sites and reaction energy barriers,demonstrating that the introduction of Co-NG promotes the formation of ^(*)COOH intermediate,providing sufficient evidence for the highly selective generation of CO.This work provides an effective single-atom-based cocatalyst modification strategy for photocatalytic CO_(2) reduction and is expected to shed light on other photocatalytic applications.
文摘By virtue of a 3∶1 complementary coordination strategy,a chiral heteroleptic metal-organic cage that con-tains divergent functional units,Pd‑R(Zn),was precisely constructed via self-assembly of monodentate variational Zn-salen ligands RZn and NADH(reduced nicotinamide adenine dinucleotide)mimic modified tridentate ligands with square-planar Pd ions.UV-Vis and luminescence spectra experiments reveal that different anions could selec-tively interact with different sites of Zn-salen modified metal-organic cages to achieve the structural regulation of cage compound,by using the differentiated host-guest electrostatic interactions of counter ions with metal-organic hosts.Compared to other anions,the presence of chloride ions caused the most significant fluorescence emission enhancement of Pd‑R(Zn),meanwhile,the UV-Vis absorption band attributed to the salen aromatic backbone showed an absorption decrease,and the metal-to-ligand induced peak displayed a blue shift effect.Circular dichro-ism and ^(1)H NMR spectra further demonstrate that the introduction of chloride anions is beneficial to keeping a more rigid scaffold.
基金supported by the Fundamental Research Funds for the Central Universities(WK2310000098).
文摘A 499.8 MHz SOLEIL-type superconducting cavity was simulated and designed for the first time in this paper.The higher-order mode(HOM)properties of the cavity were investigated.Two kinds of coaxial HOM couplers were designed.Using 4 L-type and 4 T-type HOM couplers,the longitudinal impedance and the transverse impedances were suppressed to below 3 kΩand 30 kΩ/m,respectivly.The HOM damping requirements of Hefei Advanced Light Facility(HALF)were satisfied.This paper conducted an in-depth study on the radio frequency(RF)design,multipacting optimization,and thermal analysis of these coaxial couplers.Simulation results indicated that under operating acceleration voltage,the optimized couplers does not exhibit multiplicating or thermal breakdown phenomena.The cavity has the potential to reach a higher acceleration gradient.
文摘Au sites supported on Ti-containing materials(Au/Ti-containing catalyst)are currently considered as a promising catalyst for the propylene epoxidation owing to the synergistic effect that hydrogen peroxide species formed on Au sites diffuses to the Ti sites to form the Ti-hydroperoxo intermedi-ates and contributes to the formation of propylene oxide(PO).In principle,thermal treatment will significantly affect the chemical and physical structures of Ti-containing materials.Consequently,the synergy between tailored Ti sites with different surface properties and Au sites is highly expected to enhance the catalytic performance for the reaction.Herein,we systematically studied the intrinsic effects of different microenvironments around Ti sites on the PO adsorption/desorption and conversion,and then effectively improved the catalytic performance by tailoring the number of surface hydroxyl groups.The Ti^(Ⅵ) material with fewer hydroxyls stimulates a remarkable enhancement in PO selectivity and H_(2) efficiency compared to the Ti^(Ⅵ) material that possessed more hydroxyls,offering a 7-fold and 4-fold increase,respectively.As expected,the Ti^(Ⅵ+Ⅳ) and Ti^(Ⅳ) materials also exhibit a similar phenomenon to the Ti^(Ⅵ) materials through the same thermal treatment,which strongly supports that the Ti sites microenvironment is an important factor in suppressing PO con-version and enhancing catalytic performance.These insights could provide guidance for the rational preparation and optimization of Ti-containing materials synergizing with Au catalysts for propylene epoxidation.
文摘The electrochemical reduction of CO_(2)(eCO_(2)R)under ambient conditions is crucial for reducing carbon emissions and achieving carbon neutrality.Despite progress with alkaline and neutral electrolytes,their efficiency is limited by(bi)carbonates formation.Acidic media have emerged as a solution,addressing the(bi)carbonates challenge but introducing the issue of the hydrogen evolu-tion reaction(HER),which reduces CO_(2) conversion efficiency in acidic environments.This review focuses on enhancing the selectivity of acidic CO_(2) electrolysis.It commences with an overview of the latest advancements in acidic CO_(2) electrolysis,focusing on product selectivity and electrocatalytic activity enhancements.It then delves into the critical factors shaping selectivity in acidic CO_(2) electrolysis,with a special emphasis on the influence of cations and catalyst design.Finally,the research challenges and personal perspectives of acidic CO_(2) electrolysis are suggested.
文摘Two-dimensional covalent organic frameworks(2D COFs)feature extendedπ-conjugation and ordered stacking sequence,showing great promise for high-performance photocatalysis.Periodic atomic frameworks of 2D COFs facilitate the in-plane photogenerated charge transfer,but the precise ordered alignment is limited due to the non-covalentπ-stacking of COF layers,accordingly hindering out-of-plane transfer kinetics.Herein,we address a chiral induction method to construct a parallelly superimposed stacking chiral COF ultrathin shell on the support of SiO_(2) microsphere.Compared to the achiral COF analogues,the chiral COF shell with the parallel AA-stacking structure is more conducive to enhance the built-in electric field and accumulates photogenerated electrons for the rapid migration,thereby affording superior photocatalytic performance in hydrogen evolution from water splitting.Taking the simplest ketoenamine-linked chiral COF as a shell of SiO_(2) particle,the resulting composite exhibits an impressive hydrogen evolution rate of 107.1 mmol g^(-1)h^(-1)along with the apparent quantum efficiency of 14.31% at 475 nm.Furthermore,the composite photocatalysts could be fabricated into a film device,displaying a remarkable photocatalytic performance of 178.0 mmol m^(-2)h^(-1)for hydrogen evolution.Our work underpins the surface engineering of organic photocatalysts and illustrates the significance of COF stacking structures in regulating electronic properties.