查看更多>>摘要：Development of heterogeneous molecular photocatalysts for promising light-driven hydrogen evolution reaction(HER)is highly de-manding but still challenging.Here,we report the blue-greenish emitting dinuclear metal-organic halides as photocatalyst by incor-porating site-specific single copper(Ⅰ)atoms that exhibit an efficient carbon-negative H2 production.Interestingly,the electronic prop-erties,including the spin and charge density of central Cu(Ⅰ)active site,can be triggered by substituent modulation in metal-organic halides,which greatly affect the exciton dissociation kinetics and thus the HER reactivity.The optimized spin density in these hetero-geneous photocatalysts drastically boosts the hydrogen production rate from 1250 to 3130 pmol·g-1·h-1.Our molecular strategy pro-vides a platform that rationally facilitates electronic modulation of copper(Ⅰ)atoms,tunes the macroscopic optoelectronic properties of photocatalystsand boosts carbon-negative HER activity,extending the boundaries of conventional molecular-based photocatalysts.
查看更多>>摘要：Amorphous nanomaterials are metastable nanomaterials which only have short-range order within a few neighboring atoms,based on the local chemical bondings.Dif-ferent from crystalline materials,the amorphous nanomaterials lack of long-range order exhibit many intriguing and unique structu ral features,such as abundant active sites,structural flexibility,intrinsic isotropy and fast ionic transport.However,due to the unco nven-tional structural complexity,the systematic study and understanding of amorphous nanomaterials are still in the early stage.In this review,we will describe our journey to the synthesis,characterization and applications of amorphous nanomaterials,including catalysis,energy storage,optics and mechanics.
查看更多>>摘要：Graphene nanoribbons(GNRs),which can be considered as a special type of conjugated polymers,are quasi-one-dimensional gra-phene cutouts with an opened band gap,revealing great potential as functional materials in optoelectronic,spintronic,and ener-gy-related applications.An effective strategy to modulate the properties of GNRs is doping heteroatoms into the n-skeleton.Thanks to the bottom-up synthetic approach,a number of heteroatom-doped GNRs with precise structures have been reported,exhibiting in-triguing properties.Nevertheless,a comprehensive summary of the progress of this field has remained elusive.In this review,we summarize the history and advances in bottom-up synthesized heteroatom-doped GNRs,including their synthetic routes,electronic properties,and promising applications.We hope to establish the reliable structure-property relationship,and provide guidance for the molecular design of heteroatom-doped GNRs in the future.
查看更多>>摘要：With rational designability,versatile tunability,and quantum coherence,molecular electron spin qubits could offer new opportuni-ties for quantum information science,enabling simplified implementation of quantum algorithms and chemical-specific quantum sensing.The development of these transformative technologies relies on coherent addressing of single molecular electron spin qubits with high initialization,manipulation,and readout fidelities.This is unfeasible to conventional electron spin resonance spec-troscopy,which is widely used for coherent addressing of ensemble electron spins,due to its low initialization efficiency and readout sensitivity.Taking advantage of single spin detectability of single-molecule spectroscopy,scanning tunneling microscopy,atomic force microscopy,and quantum metrology,several strategies have been developed to empower electron spin resonance spectros-copy with single qubit addressability.In this Emerging Topic,we introduce principles and technical implementation of strategies for coherent addressing of single molecular electron spin qubits,discuss their potential applicability in quantum technologies,and point out their challenges in terms of scalability,molecular design,and/or decoherence suppression.We discuss future directions to over-come these challenges and to improve single qubit addressing technologies,which will facilitate the advancement of molecular quantum information science.
查看更多>>摘要：Advanced functionalization-decorated porous organic polymers(POPs)are emerging as a prominent research focus,spanning from their construction to applications in gas storage and separation,catalysis,energy storage,electrochemistry,and other areas.Further-more,the inherent organic nature,tailored pore structures,and adjustable chemical components of POPs offer a versatile platform for the incorporation of various metal active sites.Meticulously designed molecular building blocks can serve as organic ligands uniformly distributed throughout POPs,leading to the effective isolation of inorganic metal active sites at the molecular level.In this manner,POPs containing active metal centers bridge the gap between organic and inorganic scaffolds.This review aims to provide an overview of recent research progress on metal-decorated POPs,focusing on strategies for incorporating metal active sites into POPs and their applications in adsorption,separation,catalysis,and photoelectrochemistry.Finally,current challenges and future prospects are dis-cussed for further research.
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