Precise and efficient wavefront control is essential for next-generation photonic systems.While metasurfaces provide a powerful platform,their implementation—particularly in the terahertz(THz)regime,which is vital fo...Precise and efficient wavefront control is essential for next-generation photonic systems.While metasurfaces provide a powerful platform,their implementation—particularly in the terahertz(THz)regime,which is vital for 6G communications,optical computing,and biomedical imaging—is often constrained by limited structural tunability,computationally intensive full-wave simulations,and complex fabrication processes.Here,we present a height–slope co-design strategy that enables the scalable 3D printing of high-performance,multifunctional metasurfaces.By introducing sidewall slope as an additional structural degree of freedom,the accessible design space is significantly expanded,enabling electromagnetic functionalities beyond those achievable with conventional width-or height-only modulation.A compact analytical model replaces brute-force parameter sweeps,accelerating the design process by over two orders of magnitude while maintaining high accuracy.Additionally,slope-assisted resonance tuning improves transmission efficiency,and integration with coating techniques enables broadband amplitude modulation and asymmetric transmission.The proposed strategy is experimentally validated through the design,fabrication,and characterization of a series of THz metasurfaces exhibiting enhanced beam control,mechanical stability,and spectral versatility.This geometric co-design approach provides a scalable and generalizable methodology for the rapid realization of multifunctional photonic components.展开更多
The selective hydrogenation of nitroaromatic compounds to produce phenylamines plays a crucial role in various industrial processes.Here,we introduce a Cu-MoO_(2)@C catalyst,which is synthesized by pyrolyzing a polyox...The selective hydrogenation of nitroaromatic compounds to produce phenylamines plays a crucial role in various industrial processes.Here,we introduce a Cu-MoO_(2)@C catalyst,which is synthesized by pyrolyzing a polyoxometalate-based metal-organic framework(POMOF),exhibiting remarkable catalytic efficiency in the selective hydrogenation of nitroaromatics.Specifically,nearly 100%conversion and 97%selectivity in hydrogenation of 4-nitrostyrene(4-NS)to 4-aminostyrene(4-AS)were achieved over the Cu-MoO_(2)@C catalyst under light irradiation.This promoted yield of 4-AS is ascribed to the plasmonic photothermal effect of Cu nanoparticles(NPs),which facilitate efficient photothermal conversion,as well as the strong electronic interactions at Cu/MoO_(2) interfaces,which facilitate the selective reduction of the N≡O bond while minimizing the reduction of the C≡C bond.Furthermore,the Cu-MoO_(2)@C catalyst demonstrates outstanding stability,maintaining high catalytic activity over eight cycles with minimal performance degradation.Its versatility was evidenced by the effective hydrogenation of a variety of nitroaromatic substrates containing different reducible functional groups.This study underscores the potential of Cu-MoO_(2)@C as an efficient,stable,and adaptable catalyst for the selective hydrogenation of nitroaromatic compounds,presenting a promising solution for industrial applications.展开更多
Metal-organic frameworks have emerged as promising electrode materials for metal-ion batteries due to their superior structural customizability.However,they face challenges such as poor reversibility and easy degradat...Metal-organic frameworks have emerged as promising electrode materials for metal-ion batteries due to their superior structural customizability.However,they face challenges such as poor reversibility and easy degradation during electrochemical redox processes.Here,we report the synthesis ofπ-d conjugated coordination polymers through NH_(3)-vapor-assisted self-polymerization of NiCl_(2)·6H_(2)O with 1,2,4,5-benzenetetramine tetrahydrochloride(namely,Ni-BTA).The synthesized Ni-BTA exhibits an open lattice structure that enhances the capacity for metal-ion diffusion,ensuring prolonged electrochemical cycling stability.Moreover,electrochemical characterizations reveal that Ni-BTA functions as a bifunctional material,serving as both cathode and anode materials for lithium-ion batteries(LIBs).After 1,000 cycles at 1.0 A g^(−1),the cathode and anode show high discharge capacities of 199.7 and 338.4 mAh g^(−1),respectively.Additionally,symmetrical all-organic batteries constructed with Ni-BTA exhibit a high specific capacity of 30.6 mAh g-1 and an ultrastable coulombic efficiency of approximately≈100%after 6,000 cycles at 1.0 A g^(−1).Furthermore,Ni-BTA exhibits versatility as a robust cathode for aluminum ion batteries(AIBs),delivering a discharge capacity of 18.7 mAh g^(−1) after 10,000 cycles at 1.0 A g^(−1).These findings highlight the potential of Ni-BTA as a versatile and durable electrode materials for both LIBs and AIBs.展开更多
基金National Natural Science Foundation of China(61875093)。
文摘Precise and efficient wavefront control is essential for next-generation photonic systems.While metasurfaces provide a powerful platform,their implementation—particularly in the terahertz(THz)regime,which is vital for 6G communications,optical computing,and biomedical imaging—is often constrained by limited structural tunability,computationally intensive full-wave simulations,and complex fabrication processes.Here,we present a height–slope co-design strategy that enables the scalable 3D printing of high-performance,multifunctional metasurfaces.By introducing sidewall slope as an additional structural degree of freedom,the accessible design space is significantly expanded,enabling electromagnetic functionalities beyond those achievable with conventional width-or height-only modulation.A compact analytical model replaces brute-force parameter sweeps,accelerating the design process by over two orders of magnitude while maintaining high accuracy.Additionally,slope-assisted resonance tuning improves transmission efficiency,and integration with coating techniques enables broadband amplitude modulation and asymmetric transmission.The proposed strategy is experimentally validated through the design,fabrication,and characterization of a series of THz metasurfaces exhibiting enhanced beam control,mechanical stability,and spectral versatility.This geometric co-design approach provides a scalable and generalizable methodology for the rapid realization of multifunctional photonic components.
基金financially supported by the National Natural Science Foundation of China(No.22162014)the Graduate Student Innovation Foundation of Jiangxi Province(No.YC2023-B110).
文摘The selective hydrogenation of nitroaromatic compounds to produce phenylamines plays a crucial role in various industrial processes.Here,we introduce a Cu-MoO_(2)@C catalyst,which is synthesized by pyrolyzing a polyoxometalate-based metal-organic framework(POMOF),exhibiting remarkable catalytic efficiency in the selective hydrogenation of nitroaromatics.Specifically,nearly 100%conversion and 97%selectivity in hydrogenation of 4-nitrostyrene(4-NS)to 4-aminostyrene(4-AS)were achieved over the Cu-MoO_(2)@C catalyst under light irradiation.This promoted yield of 4-AS is ascribed to the plasmonic photothermal effect of Cu nanoparticles(NPs),which facilitate efficient photothermal conversion,as well as the strong electronic interactions at Cu/MoO_(2) interfaces,which facilitate the selective reduction of the N≡O bond while minimizing the reduction of the C≡C bond.Furthermore,the Cu-MoO_(2)@C catalyst demonstrates outstanding stability,maintaining high catalytic activity over eight cycles with minimal performance degradation.Its versatility was evidenced by the effective hydrogenation of a variety of nitroaromatic substrates containing different reducible functional groups.This study underscores the potential of Cu-MoO_(2)@C as an efficient,stable,and adaptable catalyst for the selective hydrogenation of nitroaromatic compounds,presenting a promising solution for industrial applications.
基金support from the National Natural Science Foundation of China(Nos.U2267224 and 52076074)BRICS STI Framework Programme(No.52261145703)+4 种基金Higher Education Discipline Innovation Project(National 111 Project,No.B16016)the supports by Italy-Singapore Science and Technology Cooperation(Grant No.R23101R040)Singapore A*STAR SERC CRF Awardthe computing resources at the A*STAR Computational Resource CentreNational Supercomputer Centre,Singapore.
文摘Metal-organic frameworks have emerged as promising electrode materials for metal-ion batteries due to their superior structural customizability.However,they face challenges such as poor reversibility and easy degradation during electrochemical redox processes.Here,we report the synthesis ofπ-d conjugated coordination polymers through NH_(3)-vapor-assisted self-polymerization of NiCl_(2)·6H_(2)O with 1,2,4,5-benzenetetramine tetrahydrochloride(namely,Ni-BTA).The synthesized Ni-BTA exhibits an open lattice structure that enhances the capacity for metal-ion diffusion,ensuring prolonged electrochemical cycling stability.Moreover,electrochemical characterizations reveal that Ni-BTA functions as a bifunctional material,serving as both cathode and anode materials for lithium-ion batteries(LIBs).After 1,000 cycles at 1.0 A g^(−1),the cathode and anode show high discharge capacities of 199.7 and 338.4 mAh g^(−1),respectively.Additionally,symmetrical all-organic batteries constructed with Ni-BTA exhibit a high specific capacity of 30.6 mAh g-1 and an ultrastable coulombic efficiency of approximately≈100%after 6,000 cycles at 1.0 A g^(−1).Furthermore,Ni-BTA exhibits versatility as a robust cathode for aluminum ion batteries(AIBs),delivering a discharge capacity of 18.7 mAh g^(−1) after 10,000 cycles at 1.0 A g^(−1).These findings highlight the potential of Ni-BTA as a versatile and durable electrode materials for both LIBs and AIBs.
