A nickel-catalyzed C(sp^(2))–H alkynylation of unprotected α-substituted benzylamines is achieved by utilizing a transient directing group. The combination of a TDG with a nickel catalyst significantly improves the ...A nickel-catalyzed C(sp^(2))–H alkynylation of unprotected α-substituted benzylamines is achieved by utilizing a transient directing group. The combination of a TDG with a nickel catalyst significantly improves the reaction step and atom economy. It has been investigated that the 2,4,6-trimethylpyridine ligand was critical to achieve the optimized reactivity. This protocol provides a straightforward route for synthesizing the alkynylated free benzylamines, featuring good substrate compatibility and monoselectivity.展开更多
The transition metal-catalyzed C–H activation have been considered as increasingly useful approach for installing new functional groups onto organic small molecules due to their high step-and atom-economy,the abundan...The transition metal-catalyzed C–H activation have been considered as increasingly useful approach for installing new functional groups onto organic small molecules due to their high step-and atom-economy,the abundance of hydrocarbon compounds,and the potential for late-stage functionalization of complex organic molecules.The ortho-and meta-C-H activation and functionalization of aromatic compounds have been widely explored in recent years,however the distal para-C-H activation and functionalization has remained a significant challenge because of the difficulty in forming energetically favorable metallacyclic transition states.The utilization of appropriate directing groups or templates as well as the meticulous design of catalysts and ligands has proven to be effective in transition-metal-catalyzed remote para-C-H bonds activation and functionalization of aromatic compounds.This review aims to summarize the strategies for controlling para-selective C–H functionalization using the directing group,template engineering,and catalyst/ligand design under transition metals catalysis in recent years.展开更多
The directing mechanisms of liquid directing agents of zeolite Y and zeolite L were studied by means of light transmission, ultracentrifugation, NMR, XRD and “cross-exchange” experiments. It was discovered that not ...The directing mechanisms of liquid directing agents of zeolite Y and zeolite L were studied by means of light transmission, ultracentrifugation, NMR, XRD and “cross-exchange” experiments. It was discovered that not only microcfystals of zeolites, but also cage structures of zeolites play the directing role for crystallization of zeolites.展开更多
In this work,we show for the first time that high-silica zeolites(MFI,TON,MTT,and*MRE)could be synthesized from a combined strategy of both zeolite seeding and alcohol filling in the absence of organic structure-direc...In this work,we show for the first time that high-silica zeolites(MFI,TON,MTT,and*MRE)could be synthesized from a combined strategy of both zeolite seeding and alcohol filling in the absence of organic structure-directing agents(OSDAs).High-silica ZSM-5 zeolites with Si/Al ratios ranging from 38 to 240(TF-Al-ZSM-5)could be synthesized via this route.The key to the success of this technique was the employment of an aluminosilicate precursor with a fully 4-coordinated aluminum species as the initial source,wherein the rearrangement and condensation of the silicate species,rather than the aluminate species,occurred during zeolite crystallization.In addition,heteroatoms,such as Fe and B,could be incorporated into the zeolite frameworks.Catalytic tests for the methanol-to-propylene(MTP)reaction exhibited good catalytic performance for TF-Al-ZSM-5,which was comparable to that of the aluminosilicate ZSM-5 zeolite synthesized with OSDAs.Hence,this method offers viable opportunities for the industrial production and catalytic application of high-silica zeolites in the future.展开更多
Zeolite synthesis in contemporary chemical industries is predominantly conducted using organic structure‐directing agents(OSDAs),which are chronically hazardous to humans and the environment.It is a growing trend to ...Zeolite synthesis in contemporary chemical industries is predominantly conducted using organic structure‐directing agents(OSDAs),which are chronically hazardous to humans and the environment.It is a growing trend to develop an eco‐friendly and nuisanceless OSDA for zeolite synthesis.Herein,choline is employed as a non‐toxic and green OSDA to synthesize high silica Y zeolite with SiO2/Al2O3 ratios of 6.5–6.8.The prepared Y zeolite samples exhibited outstanding(hydro)thermal stability at ultrahigh temperature owing to the higher SiO2/Al2O3 ratio.The XRF,SEM,29Si‐NMR and 13Na+results suggested that choline plays a structure‐directing role in the synthesis of Y zeolite,while the feed molar fraction of Na+is a crucial determinant for the framework SiO2/Al2O3 ratio and the crystal morphology.展开更多
Zeolite FAU composites with a macro/meso-microporous hierarchical structure were hydrothermally synthesized using macro-mesoporous γ-Al_2O_3 monolith as the substrate by means of the liquid crystallization directing...Zeolite FAU composites with a macro/meso-microporous hierarchical structure were hydrothermally synthesized using macro-mesoporous γ-Al_2O_3 monolith as the substrate by means of the liquid crystallization directing agent(LCDA) induced method. No template was needed throughout the synthesis processes. The structure and porosity of zeolite composites were analyzed by means of X-ray powder diffraction(XRD), scanning electron microscopy(SEM) and N_2adsorption-desorption isotherms. The results showed that the supported zeolite composites with varied zeolitic crystalline phases and different morphologies can be obtained by adjusting the crystallization parameters, such as the crystallization temperature, the composition and the alkalinity of the precursor solution. The presence of LCDA was defined as a determinant for synthesizing the zeolite composites. The mechanisms for formation of the hierarchically porous FAU zeolite composites in the LCDA induced synthesis process were discussed. The resulting monolithic zeolite with a trimodal-porous hierarchical structure shows potential applicability where facile diffusion is required.展开更多
Reported herein is the first example of heterogeneous palladium catalyzed C(sp^(3))-H bonds arylation by a transient-ligand-directed strategy.Using supported palladium(metallic state) na nopariticles as catalyst,a wid...Reported herein is the first example of heterogeneous palladium catalyzed C(sp^(3))-H bonds arylation by a transient-ligand-directed strategy.Using supported palladium(metallic state) na nopariticles as catalyst,a wide range of aryl iodides undergo the coupling with various o-methylbenzaldehyde derivatives to assemble a library of highly selective and functionalized o-benzylbenzaldehydes.The stability of the catalyst was easily recovered four runs without significant loss of activity.The XPS analysis of the catalyst before and after reaction indicated that the reaction might be carried out by a catalytic cycle starting with Pd~0.展开更多
Silicoaluminophosphates SAPO-11 molecular sieves with small particle size and hierarchical pores were synthesized using the directing agent method.The effect of crystallization time on the particle structure,morpholog...Silicoaluminophosphates SAPO-11 molecular sieves with small particle size and hierarchical pores were synthesized using the directing agent method.The effect of crystallization time on the particle structure,morphology,pore structure properties,and acid properties of SAPO-11 molecular sieves were investigated.Unlike the SAPO-11 molecular sieves synthesized with the conventional method,the results of XRD,SEM,BET and NH3-TPD analyses showed that the SAPO-11 molecular sieves synthesized by the directing agent method in a shorter crystallization time exhibited fine and uniform morphology.By increasing the crystallization time,the particle size of SAPO-11 molecular sieve was significantly reduced,and the mesoporous structure(intercrystalline pores)was formed.Furthermore,the external specific surface area and the total specific surface area reached 81.7 m^2/g and 192.0 m^2/g,respectively,which effectively reduced the pore mass transfer resistance and significantly increased the number of acid sites.The results of n-dodecane hydroisomerization revealed that the Pt/SAPO-11 prepared with the novel method exhibited higher catalytic activity and better hydroisomerization selectivity than that synthesized by the conventional hydrothermal method.Thus,the small particle molecular sieve showed a promising industrial application prospect to be used as catalyst support.展开更多
In this review, we highlight the recent development in Ru（II）-catalyzed C-H activations under redox neutral conditions. After a brief introduction of the C-H activations with oxidizing direct group by different tran...In this review, we highlight the recent development in Ru（II）-catalyzed C-H activations under redox neutral conditions. After a brief introduction of the C-H activations with oxidizing direct group by different transition metal catalysts, the examples with Ru（ll） catalyst were classified and introduced according to different internal oxidants used in the system. The features of each methodology will be highlighted and the plausible reaction mechanism will be presented if available.展开更多
Article 1 These regulations are formulated according to the rules of the State Law on foreign investment and the requirements of industrial policies to direct foreign investment, ensuring that it adapts to the program...Article 1 These regulations are formulated according to the rules of the State Law on foreign investment and the requirements of industrial policies to direct foreign investment, ensuring that it adapts to the programmes of China’s national economy and social development and protecting the legal rights and interests of investors.展开更多
High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental sta...High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental stability,ideal outdoor readability,and low energy consumption.However,the limited intrinsic structure of inorganic materials has presented a significant challenge in achieving precise patterning/pixelation at the micron scale.Here,we successfully developed the direct photolithography for WOx nanoparticles based on in situ photo-induced ligand exchange.This strategy enabled us to achieve ultra-high resolution efficiently(line width<4μm,the best resolution for reported inorganic electrochromic materials).Additionally,the resulting device exhibited impressive electrochromic performance,such as fast response(<1 s at 0 V),high coloration efficiency(119.5 cm^(2) C^(−1)),good optical modulation(55.9%),and durability(>3600 cycles),as well as promising applications in electronic logos,pixelated displays,flexible electronics,etc.The success and advancements presented here are expected to inspire and accelerate research and development(R&D)in high-resolution non-emissive displays and other ultra-fine micro-electronics.展开更多
Garlic planting requires a single seed with a scaly bud upward and vertically.In this study,an automatic garlic seed directing device was designed for auxiliary garlic seeding by utilizing a seed placed funnel,a corre...Garlic planting requires a single seed with a scaly bud upward and vertically.In this study,an automatic garlic seed directing device was designed for auxiliary garlic seeding by utilizing a seed placed funnel,a correcting mechanism,and an automatic control system.Three factors influenced device performance:characteristics of garlic seeds,limited notch diameter of the seed placed funnel,and funnel taper of the seed placed funnel.The most optimal structural parameters of the seed placed funnel were determined via theoretical analysis.The research samples of Lanling and Jinxiang garlic were divided into three groups according to their respective sizes.3D design software(Solidworks)was used to simulate the above three factors and analyze their rules of action.The obtained simulation results demonstrated that the suitable range of funnel taper and limited notch diameter of seed placed funnel for the three groups of seed were from 40°to 60°and 6-8 mm,respectively.The bench test showed that when the funnel taper was 60°and the limited notch diameter was 10 mm,the success rates of the three groups’seeds in terms of scaly bud directing were 89.8%,91.6%and 96.6%respectively,which satisfied the agricultural requirements of garlic planting.Accordingly,the corresponding results may promote the study and improvement of garlic intelligent planting equipment.展开更多
Transition-metal catalyzed C--H functionalization of benzaldehydes is of great interest in organic synthesis. Herein, we developed a transient directing group assisted amidation of benzaldehydes catalyzed by rhodium c...Transition-metal catalyzed C--H functionalization of benzaldehydes is of great interest in organic synthesis. Herein, we developed a transient directing group assisted amidation of benzaldehydes catalyzed by rhodium catalyst. With the employment of 10 mol% of 4-trifluoromethyl aniline, the in situ generated imine groups as the directing group efficiently enable this transformation. By using this protocol, a wide range of benzaldehydes were efficiently converted into the corresponding N-（2-formylphenyl）benzamides utilizing dioxazolones as the nitrogen source.展开更多
Dispatched by the Chinese government,a multidisciplinary team of 30 researchers collaborated with a team from Myanmar to conduct a 14-day on-site investigation.The work encompassed seismic intensity assessments,field ...Dispatched by the Chinese government,a multidisciplinary team of 30 researchers collaborated with a team from Myanmar to conduct a 14-day on-site investigation.The work encompassed seismic intensity assessments,field surveys,and loss evaluations.The paper focuses on the intensity distribution and structural damage characteristics of the 2025 M7.9 Myanmar earthquake,yielding the following key findings.(1)The seismogenic fault rupture propagated in a nearly N-S direction,with a surface rupture length of approximately 450 km.The seismic impact zone exhibited an elongated N-S distribution and a shorter E-W span,distributed like a belt around the seismogenic fault.(2)Within the seismic impact zones,existing buildings comprised five primary structural types,with timber(bamboo)structures constituting the largest proportion(≈80%in rural areas,≈50%in urban areas).The relatively low disaster losses and casualties were primarily attributable to the good seismic performance and low damage ratio of timber(bamboo)structures across varying intensity zones.(3)An anomalous zone of intensityⅨwas located at the boundary between intensityⅥandⅦregions in Nay Pyi Taw.Here,ridge topography combined with soft soil layers significantly amplified ground motion,exacerbating structural damage.(4)Directional effects of ground motion were observed,with the structural damage phenomena and peak ground acceleration(PGA)values in the N-S direction exceeding those in the E-W direction.This validates that the maximum PGA distribution of strike-slip fault earthquakes aligns with the fault strike.The research is expected to provide technical support for post-disaster reconstruction planning,site selection,and disaster mitigation strategies in Myanmar.展开更多
With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power ...With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.展开更多
Developing deep fragmented soft coalbed methane(CBM)can significantly enhance domestic natural gas supplies,reduce reliance on imported energy,and bolster national energy security.This manuscript provides a comprehens...Developing deep fragmented soft coalbed methane(CBM)can significantly enhance domestic natural gas supplies,reduce reliance on imported energy,and bolster national energy security.This manuscript provides a comprehensive review of commonly employed coalbed methane extraction technologies.It then delves into several critical issues in the current stage of CBM exploration and development in China,including the compatibility of existing technologies with CBM reservoirs,the characteristics and occurrence states of CBM reservoirs,critical desorption pressure,and gas generation mechanisms.Our research indicates that current CBM exploration and development technologies in China have reached an internationally advanced level,yet the industry is facing unprecedented challenges.Despite progress in low-permeability,high-value coal seams,significant breakthroughs have not been achieved in exploring other types of coal seams.For different coal reservoirs,integrated extraction technologies have been developed,such as surface pre-depressurisation and segmented hydraulic fracturing of coal seam roof strata.Additionally,techniques like large-scale volume fracturing in horizontal wells have been established,significantly enhancing reservoir stimulation effects and coalbed methane recovery rates.However,all of these technologies are fundamentally based on permeation.These technologies lack direct methods aimed at enhancing the diffusion rate of CBM,thereby failing to fully reflect the unique characteristics of CBM.Current CBM exploration and development theories and technologies are not universally applicable to all coal seams.They do not adequately account for the predominantly adsorbed state of CBM,and the complex and variable gas generation mechanisms further constrain CBM development in China.Finally,continuous exploration of new deep CBM exploration technologies is necessary.Integrating more effective reservoir stimulation technologies is essential to enhance technical adaptability concerning CBM reservoir characteristics,gas occurrence states,and gas generation mechanisms,ultimately achieving efficient CBM development.We conclude that while China possesses a substantial foundation of deep fractured CBM resources,industry development is constrained and requires continuous exploration of new CBM exploration and development technologies to utilize these resources effectively.展开更多
Large-scale deployment of carbon dioxide(CO_(2))removal technology is an essential step to cope with global warming and achieve carbon neutrality.Direct air capture(DAC)has recently received increasing attention given...Large-scale deployment of carbon dioxide(CO_(2))removal technology is an essential step to cope with global warming and achieve carbon neutrality.Direct air capture(DAC)has recently received increasing attention given the high flexibility to remove CO_(2)from discrete sources.Porous materials with adjustable pore characteristics are promising sorbents with low or no latent heat of vaporization.This review article has summarized the recent development of porous sorbents for DAC,with a focus of pore engineering strategy and adsorption mechanism.Physisorbents such as zeolites,porous carbons,metal-organic frameworks(MOFs),and amine-modified chemisorbents have been discussed and their challenges in practical application have been analyzed.At last,future directions have been proposed,and it is expected to inspire collaborations from chemistry,environment,material science and engineering communities.展开更多
A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate t...A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate that spent LiFePO_(4)/C cathode materials with good performance can be regenerated by roasting at 650℃ for 11 h with the addition ofLi_(2)CO_(3),FePO_(4),V_(2)O_(5),and glucose.V_(2)O_(5) is added to improve the cycle performance of regenerated cathode materials.Glucose is used to revitalize the carbon layers on the surface of spent LiFePO_(4)/C particles for improving their conductivity.The regenerated V-doped LiFePO_(4)/C shows an excellent electrochemical performance with the discharge specific capacity of 161.36 mA·h/g at 0.2C,under which the capacity retention is 97.85%after 100 cycles.展开更多
The Janus fabrics designed for personal moisture/thermal regulation have garnered significant attention for their potential to enhance human comfort.However,the development of smart and dynamic fabrics capable of mana...The Janus fabrics designed for personal moisture/thermal regulation have garnered significant attention for their potential to enhance human comfort.However,the development of smart and dynamic fabrics capable of managing personal moisture/thermal comfort in response to changing external environments remains a challenge.Herein,a smart cellulose-based Janus fabric was designed to dynamically manage personal moisture/heat.The cotton fabric was grafted with N-isopropylacrylamide to construct a temperature-stimulated transport channel.Subsequently,hydrophobic ethyl cellulose and hydrophilic cellulose nanofiber were sprayed on the bottom and top sides of the fabric to obtain wettability gradient.The fabric exhibits anti-gravity directional liquid transportation from hydrophobic side to hydrophilic side,and can dynamically and continuously control the transportation time in a wide range of 3–66 s as the temperature increases from 10 to 40℃.This smart fabric can quickly dissipate heat at high temperatures,while at low temperatures,it can slow down the heat dissipation rate and prevent the human from becoming too cold.In addition,the fabric has UV shielding and photodynamic antibacterial properties through depositing graphitic carbon nitride nanosheets on the hydrophilic side.This smart fabric offers an innovative approach to maximizing personal comfort in environments with significant temperature variations.展开更多
The layer-by-layer deposition strategy of additive manufacturing makes it ideal to fabricate dissimilar alloy components with varying functionality,which has promising application potential in a large number of indust...The layer-by-layer deposition strategy of additive manufacturing makes it ideal to fabricate dissimilar alloy components with varying functionality,which has promising application potential in a large number of industrial areas.In this study,two components composed of ERCuAl-A2 aluminum bronze(CuAl9)and Inconel 718 nickel-based superalloy were fabricated with different deposition orders by wire-arc directed energy deposition.Subject to changes in heat input and thermophysical properties of the substrate,the transition region of the deposited Cu-Ni component with the bottom half of CuAl9 and the top half of Inconel 718 is narrow and serrated.This region features a laminated intermetallic compound layer due to the convection and rapid cooling in the molten pool.In contrast,the Ni-Cu component deposited in the opposite order exhibits a 2 mm gradient transition zone.Within this region,a large number of diverse precipitates were found as well as regional variations in grain size due to the multi-layer partial remelting.Both two components show strong bonds and their tensile specimens tested along the vertical direction always fracture at the softer CuAl9 side.Excellent tensile properties along the horizontal direction were obtained for Cu-Ni(Ultimate tensile strength:573 MPa,yield stress:302 MPa,elongation:22%),while those of Ni-Cu are much lower due to the existence of the solidification cracks in the transition zone.The results from this study provide a reference for the additive manufacturing of Cu/Ni dissimilar alloy components,as well as their microstructure and mechanical properties control.展开更多
基金supported financially by the Excellent Going Abroad Expert's Training Program in Hebei Province (No. 201940)the Hebei Natural Science Foundation of China (No. H2020208030)the S & T Program of Hebei (No. 22567607H) for financial support。
文摘A nickel-catalyzed C(sp^(2))–H alkynylation of unprotected α-substituted benzylamines is achieved by utilizing a transient directing group. The combination of a TDG with a nickel catalyst significantly improves the reaction step and atom economy. It has been investigated that the 2,4,6-trimethylpyridine ligand was critical to achieve the optimized reactivity. This protocol provides a straightforward route for synthesizing the alkynylated free benzylamines, featuring good substrate compatibility and monoselectivity.
基金support from the National Natural Science Foundation of China(No.21901206)Postdoctoral Science Foundation of China(No.2022M712589)+2 种基金General Key R&D Projects in Shaanxi Province(No.2023-YBGY-321)Natural Science Foundation of Chongqing(No.CSTB2022NSCQ-MSX0826)National&Local Joint Engineering Research Center for mineral Salt Deep Utilization,Huaiyin Institute of Technology(No.SF202407)for financial support。
文摘The transition metal-catalyzed C–H activation have been considered as increasingly useful approach for installing new functional groups onto organic small molecules due to their high step-and atom-economy,the abundance of hydrocarbon compounds,and the potential for late-stage functionalization of complex organic molecules.The ortho-and meta-C-H activation and functionalization of aromatic compounds have been widely explored in recent years,however the distal para-C-H activation and functionalization has remained a significant challenge because of the difficulty in forming energetically favorable metallacyclic transition states.The utilization of appropriate directing groups or templates as well as the meticulous design of catalysts and ligands has proven to be effective in transition-metal-catalyzed remote para-C-H bonds activation and functionalization of aromatic compounds.This review aims to summarize the strategies for controlling para-selective C–H functionalization using the directing group,template engineering,and catalyst/ligand design under transition metals catalysis in recent years.
基金Department of Envirenmental Medicine, Bethune University of Medical Sciences
文摘The directing mechanisms of liquid directing agents of zeolite Y and zeolite L were studied by means of light transmission, ultracentrifugation, NMR, XRD and “cross-exchange” experiments. It was discovered that not only microcfystals of zeolites, but also cage structures of zeolites play the directing role for crystallization of zeolites.
文摘In this work,we show for the first time that high-silica zeolites(MFI,TON,MTT,and*MRE)could be synthesized from a combined strategy of both zeolite seeding and alcohol filling in the absence of organic structure-directing agents(OSDAs).High-silica ZSM-5 zeolites with Si/Al ratios ranging from 38 to 240(TF-Al-ZSM-5)could be synthesized via this route.The key to the success of this technique was the employment of an aluminosilicate precursor with a fully 4-coordinated aluminum species as the initial source,wherein the rearrangement and condensation of the silicate species,rather than the aluminate species,occurred during zeolite crystallization.In addition,heteroatoms,such as Fe and B,could be incorporated into the zeolite frameworks.Catalytic tests for the methanol-to-propylene(MTP)reaction exhibited good catalytic performance for TF-Al-ZSM-5,which was comparable to that of the aluminosilicate ZSM-5 zeolite synthesized with OSDAs.Hence,this method offers viable opportunities for the industrial production and catalytic application of high-silica zeolites in the future.
基金supported by the National Natural Science Foundation of China(Grant No.21802136)~~
文摘Zeolite synthesis in contemporary chemical industries is predominantly conducted using organic structure‐directing agents(OSDAs),which are chronically hazardous to humans and the environment.It is a growing trend to develop an eco‐friendly and nuisanceless OSDA for zeolite synthesis.Herein,choline is employed as a non‐toxic and green OSDA to synthesize high silica Y zeolite with SiO2/Al2O3 ratios of 6.5–6.8.The prepared Y zeolite samples exhibited outstanding(hydro)thermal stability at ultrahigh temperature owing to the higher SiO2/Al2O3 ratio.The XRF,SEM,29Si‐NMR and 13Na+results suggested that choline plays a structure‐directing role in the synthesis of Y zeolite,while the feed molar fraction of Na+is a crucial determinant for the framework SiO2/Al2O3 ratio and the crystal morphology.
基金the financial support from the National Natural Science Foundation of China(No.20973022 and No.11472048)the State Key Laboratory of Catalytic Materials and Reaction Engineering(RIPP,SINOPEC)(Serial No.33600000-14-ZC0607-0006)
文摘Zeolite FAU composites with a macro/meso-microporous hierarchical structure were hydrothermally synthesized using macro-mesoporous γ-Al_2O_3 monolith as the substrate by means of the liquid crystallization directing agent(LCDA) induced method. No template was needed throughout the synthesis processes. The structure and porosity of zeolite composites were analyzed by means of X-ray powder diffraction(XRD), scanning electron microscopy(SEM) and N_2adsorption-desorption isotherms. The results showed that the supported zeolite composites with varied zeolitic crystalline phases and different morphologies can be obtained by adjusting the crystallization parameters, such as the crystallization temperature, the composition and the alkalinity of the precursor solution. The presence of LCDA was defined as a determinant for synthesizing the zeolite composites. The mechanisms for formation of the hierarchically porous FAU zeolite composites in the LCDA induced synthesis process were discussed. The resulting monolithic zeolite with a trimodal-porous hierarchical structure shows potential applicability where facile diffusion is required.
基金financially supported by the National Natural Science Foundation of China(No.21861030)the Program for Young Talents of Science and Technology in Universities of Inner Mongolia Autonomous Region(No.NJYT-17-A22)。
文摘Reported herein is the first example of heterogeneous palladium catalyzed C(sp^(3))-H bonds arylation by a transient-ligand-directed strategy.Using supported palladium(metallic state) na nopariticles as catalyst,a wide range of aryl iodides undergo the coupling with various o-methylbenzaldehyde derivatives to assemble a library of highly selective and functionalized o-benzylbenzaldehydes.The stability of the catalyst was easily recovered four runs without significant loss of activity.The XPS analysis of the catalyst before and after reaction indicated that the reaction might be carried out by a catalytic cycle starting with Pd~0.
基金We thank the National Natural Science Fund of China(2016-Z0030)Natural Science Foundation of Liaoning Province(L2017 LQN008,L2019014).
文摘Silicoaluminophosphates SAPO-11 molecular sieves with small particle size and hierarchical pores were synthesized using the directing agent method.The effect of crystallization time on the particle structure,morphology,pore structure properties,and acid properties of SAPO-11 molecular sieves were investigated.Unlike the SAPO-11 molecular sieves synthesized with the conventional method,the results of XRD,SEM,BET and NH3-TPD analyses showed that the SAPO-11 molecular sieves synthesized by the directing agent method in a shorter crystallization time exhibited fine and uniform morphology.By increasing the crystallization time,the particle size of SAPO-11 molecular sieve was significantly reduced,and the mesoporous structure(intercrystalline pores)was formed.Furthermore,the external specific surface area and the total specific surface area reached 81.7 m^2/g and 192.0 m^2/g,respectively,which effectively reduced the pore mass transfer resistance and significantly increased the number of acid sites.The results of n-dodecane hydroisomerization revealed that the Pt/SAPO-11 prepared with the novel method exhibited higher catalytic activity and better hydroisomerization selectivity than that synthesized by the conventional hydrothermal method.Thus,the small particle molecular sieve showed a promising industrial application prospect to be used as catalyst support.
基金the NSFC(Nos.21372178 and 21572163)for financial supportsupported by the Scientific Innovation Program for College Students of Zhejiang Province(No. 2016R426061)
文摘In this review, we highlight the recent development in Ru（II）-catalyzed C-H activations under redox neutral conditions. After a brief introduction of the C-H activations with oxidizing direct group by different transition metal catalysts, the examples with Ru（ll） catalyst were classified and introduced according to different internal oxidants used in the system. The features of each methodology will be highlighted and the plausible reaction mechanism will be presented if available.
文摘Article 1 These regulations are formulated according to the rules of the State Law on foreign investment and the requirements of industrial policies to direct foreign investment, ensuring that it adapts to the programmes of China’s national economy and social development and protecting the legal rights and interests of investors.
基金supported by the National Key R&D Program of China(2022YFB3606501,2022YFB3602902)the Key projects of National Natural Science Foundation of China(62234004)+8 种基金the National Natural Science Foundation of China(U23A2092)Pioneer and Leading Goose R&D Program of Zhejiang(2024C01191,2024C01092)Innovation and Entrepreneurship Team of Zhejiang Province(2021R01003)Ningbo Key Technologies R&D Program(2022Z085),Ningbo 3315 Programme(2020A-01-B)YONGJIANG Talent Introduction Programme(2021A-038-B,2021A-159-G)“Innovation Yongjiang 2035”Key R&D Programme(2024Z146)Ningbo JiangBei District public welfare science and technology project(2022C07)the China National Postdoctoral Program for Innovative Talents(grant no.BX20240391)the China Postdoctoral Science Foundation(grant no.2023M743623).
文摘High-resolution non-emissive displays based on electrochromic tungsten oxides(WOx)are crucial for future near-eye virtual/augmented reality interactions,given their impressive attributes such as high environmental stability,ideal outdoor readability,and low energy consumption.However,the limited intrinsic structure of inorganic materials has presented a significant challenge in achieving precise patterning/pixelation at the micron scale.Here,we successfully developed the direct photolithography for WOx nanoparticles based on in situ photo-induced ligand exchange.This strategy enabled us to achieve ultra-high resolution efficiently(line width<4μm,the best resolution for reported inorganic electrochromic materials).Additionally,the resulting device exhibited impressive electrochromic performance,such as fast response(<1 s at 0 V),high coloration efficiency(119.5 cm^(2) C^(−1)),good optical modulation(55.9%),and durability(>3600 cycles),as well as promising applications in electronic logos,pixelated displays,flexible electronics,etc.The success and advancements presented here are expected to inspire and accelerate research and development(R&D)in high-resolution non-emissive displays and other ultra-fine micro-electronics.
基金Shandong Major Science and Technology Innovation Projects(2018CXGC0203)National Special Vegetable Industry Technology System Project(CARS-24-D-01)Shandong Agricultural University“Double-first-class”Collaborative Innovation Team of Horticultural Machinery Equipment(SYL2017XTTD07).
文摘Garlic planting requires a single seed with a scaly bud upward and vertically.In this study,an automatic garlic seed directing device was designed for auxiliary garlic seeding by utilizing a seed placed funnel,a correcting mechanism,and an automatic control system.Three factors influenced device performance:characteristics of garlic seeds,limited notch diameter of the seed placed funnel,and funnel taper of the seed placed funnel.The most optimal structural parameters of the seed placed funnel were determined via theoretical analysis.The research samples of Lanling and Jinxiang garlic were divided into three groups according to their respective sizes.3D design software(Solidworks)was used to simulate the above three factors and analyze their rules of action.The obtained simulation results demonstrated that the suitable range of funnel taper and limited notch diameter of seed placed funnel for the three groups of seed were from 40°to 60°and 6-8 mm,respectively.The bench test showed that when the funnel taper was 60°and the limited notch diameter was 10 mm,the success rates of the three groups’seeds in terms of scaly bud directing were 89.8%,91.6%and 96.6%respectively,which satisfied the agricultural requirements of garlic planting.Accordingly,the corresponding results may promote the study and improvement of garlic intelligent planting equipment.
基金Acknowledgement We thank National Basic Research Program of China （973 Program） （No. 2015CB856600）, the National Natural Science Foundation of China （Nos. 21632001, 21772002）, National Young Topnotch Talent Support Program, and Peking University Health Science Center （No. BMU20160541） for financial support of this work. We thank Bencong Zhu in this group for reproducing the results of 3b and 4f.
文摘Transition-metal catalyzed C--H functionalization of benzaldehydes is of great interest in organic synthesis. Herein, we developed a transient directing group assisted amidation of benzaldehydes catalyzed by rhodium catalyst. With the employment of 10 mol% of 4-trifluoromethyl aniline, the in situ generated imine groups as the directing group efficiently enable this transformation. By using this protocol, a wide range of benzaldehydes were efficiently converted into the corresponding N-（2-formylphenyl）benzamides utilizing dioxazolones as the nitrogen source.
基金National Natural Science Foundation of China under Grant No.U2239252National Natural Science Foundation of China under Grant No.52279128Natural Science Foundation of Heilongjiang Province of China under Grant No.YQ2022E013。
文摘Dispatched by the Chinese government,a multidisciplinary team of 30 researchers collaborated with a team from Myanmar to conduct a 14-day on-site investigation.The work encompassed seismic intensity assessments,field surveys,and loss evaluations.The paper focuses on the intensity distribution and structural damage characteristics of the 2025 M7.9 Myanmar earthquake,yielding the following key findings.(1)The seismogenic fault rupture propagated in a nearly N-S direction,with a surface rupture length of approximately 450 km.The seismic impact zone exhibited an elongated N-S distribution and a shorter E-W span,distributed like a belt around the seismogenic fault.(2)Within the seismic impact zones,existing buildings comprised five primary structural types,with timber(bamboo)structures constituting the largest proportion(≈80%in rural areas,≈50%in urban areas).The relatively low disaster losses and casualties were primarily attributable to the good seismic performance and low damage ratio of timber(bamboo)structures across varying intensity zones.(3)An anomalous zone of intensityⅨwas located at the boundary between intensityⅥandⅦregions in Nay Pyi Taw.Here,ridge topography combined with soft soil layers significantly amplified ground motion,exacerbating structural damage.(4)Directional effects of ground motion were observed,with the structural damage phenomena and peak ground acceleration(PGA)values in the N-S direction exceeding those in the E-W direction.This validates that the maximum PGA distribution of strike-slip fault earthquakes aligns with the fault strike.The research is expected to provide technical support for post-disaster reconstruction planning,site selection,and disaster mitigation strategies in Myanmar.
基金financially supported by the National Key Research and Development Program of China(2023YFB3809300)。
文摘With the approaching of large-scale retirement of power lithium-ion batteries(LIBs),their urgent handling is required for environmental protection and resource reutilization.However,at present,substantial spent power batteries,especially for those high recovery value cathode materials,have not been greenly,sustainably,and efficiently recycled.Compared to the traditional recovery method for cathode materials with high energy consumption and severe secondary pollution,the direct repair regeneration,as a new type of short-process and efficient treatment methods,has attracted widespread attention.However,it still faces challenges in homogenization repair,electrochemical performance decline,and scaling-up production.To promote the direct regeneration technology development of failed NCM materials,herein we deeply discuss the failure mechanism of nickel-cobalt-manganese(NCM)ternary cathode materials,including element loss,Li/Ni mixing,phase transformation,structural defects,oxygen release,and surface degradation and reconstruction.Based on this,the detailed analysis and summary of the direct regeneration method embracing solid-phase sintering,eutectic salt assistance,solvothermal synthesis,sol-gel process,spray drying,and redox mediation are provided.Further,the upcycling strategy for regeneration materials,such as single-crystallization and high-nickelization,structural regulation,ion doping,and surface engineering,are discussed in deep.Finally,the challenges faced by the direct regeneration and corresponding countermeasures are pointed out.Undoubtedly,this review provides valuable guidance for the efficient and high-value recovery of failed cathode materials.
基金supported by the National Natural Science Foundation of China(52074045,52274074)the Science Fund for Distinguished Young Scholars of Chongqing(CSTB2022NSCQ-JQX0028).
文摘Developing deep fragmented soft coalbed methane(CBM)can significantly enhance domestic natural gas supplies,reduce reliance on imported energy,and bolster national energy security.This manuscript provides a comprehensive review of commonly employed coalbed methane extraction technologies.It then delves into several critical issues in the current stage of CBM exploration and development in China,including the compatibility of existing technologies with CBM reservoirs,the characteristics and occurrence states of CBM reservoirs,critical desorption pressure,and gas generation mechanisms.Our research indicates that current CBM exploration and development technologies in China have reached an internationally advanced level,yet the industry is facing unprecedented challenges.Despite progress in low-permeability,high-value coal seams,significant breakthroughs have not been achieved in exploring other types of coal seams.For different coal reservoirs,integrated extraction technologies have been developed,such as surface pre-depressurisation and segmented hydraulic fracturing of coal seam roof strata.Additionally,techniques like large-scale volume fracturing in horizontal wells have been established,significantly enhancing reservoir stimulation effects and coalbed methane recovery rates.However,all of these technologies are fundamentally based on permeation.These technologies lack direct methods aimed at enhancing the diffusion rate of CBM,thereby failing to fully reflect the unique characteristics of CBM.Current CBM exploration and development theories and technologies are not universally applicable to all coal seams.They do not adequately account for the predominantly adsorbed state of CBM,and the complex and variable gas generation mechanisms further constrain CBM development in China.Finally,continuous exploration of new deep CBM exploration technologies is necessary.Integrating more effective reservoir stimulation technologies is essential to enhance technical adaptability concerning CBM reservoir characteristics,gas occurrence states,and gas generation mechanisms,ultimately achieving efficient CBM development.We conclude that while China possesses a substantial foundation of deep fractured CBM resources,industry development is constrained and requires continuous exploration of new CBM exploration and development technologies to utilize these resources effectively.
基金financial support from the National Natural Science Foundation of China(Nos.22278011,22225803,22038001 and 22108007)Beijing Natural Science Foundation(No.Z230023)+1 种基金The Science&Technology Project of Beijing Municipal Education Committee(No.KZ201810005004)Beijing Nova Program(No.Z211100002121094)。
文摘Large-scale deployment of carbon dioxide(CO_(2))removal technology is an essential step to cope with global warming and achieve carbon neutrality.Direct air capture(DAC)has recently received increasing attention given the high flexibility to remove CO_(2)from discrete sources.Porous materials with adjustable pore characteristics are promising sorbents with low or no latent heat of vaporization.This review article has summarized the recent development of porous sorbents for DAC,with a focus of pore engineering strategy and adsorption mechanism.Physisorbents such as zeolites,porous carbons,metal-organic frameworks(MOFs),and amine-modified chemisorbents have been discussed and their challenges in practical application have been analyzed.At last,future directions have been proposed,and it is expected to inspire collaborations from chemistry,environment,material science and engineering communities.
基金National Natural Science Foundation of China(Nos.52174269,52374293)Science and Technology Innovation Program of Hunan Province,China(Nos.2024CK1009,2022RC1123)。
文摘A tunable oxidization and reduction strategy was proposed to directly regenerate spent LiFePO_(4)/C cathode materials by oxidizing excessive carbon powders with the addition of FePO_(4).Experimental results indicate that spent LiFePO_(4)/C cathode materials with good performance can be regenerated by roasting at 650℃ for 11 h with the addition ofLi_(2)CO_(3),FePO_(4),V_(2)O_(5),and glucose.V_(2)O_(5) is added to improve the cycle performance of regenerated cathode materials.Glucose is used to revitalize the carbon layers on the surface of spent LiFePO_(4)/C particles for improving their conductivity.The regenerated V-doped LiFePO_(4)/C shows an excellent electrochemical performance with the discharge specific capacity of 161.36 mA·h/g at 0.2C,under which the capacity retention is 97.85%after 100 cycles.
基金support of this work by National Key Research and Development Program of China(2019YFC19059003)the Natural Science Foundation of the Jiangsu Higher Education Institutions of China(23KJB430024)+1 种基金Jiangsu Funding Program for Excellent Postdoctoral Talent(2023ZB680)Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)are gratefully acknowledged.
文摘The Janus fabrics designed for personal moisture/thermal regulation have garnered significant attention for their potential to enhance human comfort.However,the development of smart and dynamic fabrics capable of managing personal moisture/thermal comfort in response to changing external environments remains a challenge.Herein,a smart cellulose-based Janus fabric was designed to dynamically manage personal moisture/heat.The cotton fabric was grafted with N-isopropylacrylamide to construct a temperature-stimulated transport channel.Subsequently,hydrophobic ethyl cellulose and hydrophilic cellulose nanofiber were sprayed on the bottom and top sides of the fabric to obtain wettability gradient.The fabric exhibits anti-gravity directional liquid transportation from hydrophobic side to hydrophilic side,and can dynamically and continuously control the transportation time in a wide range of 3–66 s as the temperature increases from 10 to 40℃.This smart fabric can quickly dissipate heat at high temperatures,while at low temperatures,it can slow down the heat dissipation rate and prevent the human from becoming too cold.In addition,the fabric has UV shielding and photodynamic antibacterial properties through depositing graphitic carbon nitride nanosheets on the hydrophilic side.This smart fabric offers an innovative approach to maximizing personal comfort in environments with significant temperature variations.
基金supported by the Key Research and Development Program of Shaanxi Province(2023-YBGY361)the National Natural Science Foundation of China(52275374 and 52205414)+1 种基金the Postdoctoral Fellowship Program of CPSF(GZC20232098)as well as the Xiaomi Foundation through Xiaomi Young Scholar Program。
文摘The layer-by-layer deposition strategy of additive manufacturing makes it ideal to fabricate dissimilar alloy components with varying functionality,which has promising application potential in a large number of industrial areas.In this study,two components composed of ERCuAl-A2 aluminum bronze(CuAl9)and Inconel 718 nickel-based superalloy were fabricated with different deposition orders by wire-arc directed energy deposition.Subject to changes in heat input and thermophysical properties of the substrate,the transition region of the deposited Cu-Ni component with the bottom half of CuAl9 and the top half of Inconel 718 is narrow and serrated.This region features a laminated intermetallic compound layer due to the convection and rapid cooling in the molten pool.In contrast,the Ni-Cu component deposited in the opposite order exhibits a 2 mm gradient transition zone.Within this region,a large number of diverse precipitates were found as well as regional variations in grain size due to the multi-layer partial remelting.Both two components show strong bonds and their tensile specimens tested along the vertical direction always fracture at the softer CuAl9 side.Excellent tensile properties along the horizontal direction were obtained for Cu-Ni(Ultimate tensile strength:573 MPa,yield stress:302 MPa,elongation:22%),while those of Ni-Cu are much lower due to the existence of the solidification cracks in the transition zone.The results from this study provide a reference for the additive manufacturing of Cu/Ni dissimilar alloy components,as well as their microstructure and mechanical properties control.
