Publications by authors named "Daliang Zhang"

Prussian blue analogs (PBAs), as a classical kind of microporous materials, have attracted substantial interests considering their well-defined framework structures, unique physicochemical properties and low cost. However, PBAs typically adopt cubic structure that features small pore size and low specific surface area, which greatly limits their practical applications in various fields ranging from gas adsorption/separation to energy conversion/storage and biomedical treatments. Here we report the facile and general synthesis of unconventional hexagonal open PBA structures.

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Recently, halide perovskites have been recognized for their thermochromic characteristics, showing significant potential in information encryption applications. However, the limited luminescence color gamut hinders the encryption of complex multicolor information. Herein, for the first time, multicolor thermochromic perovskites with luminescence covering the entire visible spectrum have been designed.

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Article Synopsis
  • The synthesis of high-quality single-crystal covalent organic frameworks (COFs) is challenging, especially in controlling their shapes; this study presents a simple method to achieve desired morphologies using triptycene derivatives and varying aniline amounts.
  • A series of COF single crystals with different aspect ratios and defined facets were successfully synthesized and characterized through various analytical techniques, confirming their structural quality.
  • The research highlights the importance of aniline as a modulator in crystal growth and shows that the aspect ratio of these crystals affects their adsorption properties, linking COF morphology to functional performance.
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  • The study challenges the conventional understanding of covalent organic frameworks (COFs) by revealing two distinct pore types in a widely studied imine-based COF through real-space imaging.
  • Real-space imaging led to a reconsideration of the structural model, emphasizing differences in pore configurations and the presence of previously unidentified defects.
  • This research underscores the complexity of COF structures and the necessity for advanced characterization methods to accurately assess their properties and potential applications.
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The Li/Mn ordered structure of lithium-rich (LR) cathodes leads to the heterogeneous LiMnO and LiTMO components, readily triggering structural degeneration and performance degradation in long-term cycling. However, the lack of guiding principles for promoting cation disorder within the transition metal (TM) layers has posed a persistent challenge in designing homogeneous layered LR cathodes. Herein, the (Li + Mn) content in the TM layer as a criterion for the design of cation-disordered layered LR cathodes is proposed.

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Copper (Cu) nanomaterials are a unique kind of electrocatalysts for high-value multi-carbon production in carbon dioxide reduction reaction (CORR), which holds enormous potential in attaining carbon neutrality. However, phase engineering of Cu nanomaterials remains challenging, especially for the construction of unconventional phase Cu-based asymmetric heteronanostructures. Here the site-selective growth of Cu on unusual phase gold (Au) nanorods, obtaining three kinds of heterophase fcc-2H-fcc Au-Cu heteronanostructures is reported.

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Creating structural defects in a controlled manner within metal-organic frameworks (MOFs) poses a significant challenge for synthesis, and concurrently, identifying the types and distributions of these defects is also a formidable task for characterization. In this study, we demonstrate that by employing 2-sulfonylterephthalic acid as the ligand for synthesizing Zr (or Hf)-based MOFs, a crystal phase transformation from the common topology to the rare topology can be easily facilitated using a straightforward mixed-solvent strategy. The phase, characterized by an extensively open framework, can be considered a derivative of the phase, generated through the introduction of missing-cluster defects.

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The Yangtze River Delta urban agglomeration (YRDUA) is China's most representative region with remarkable economic development vitality. The purpose of this study is to provide valuable data analysis to actively respond to the population aging in China. We mainly focus on the spatial and temporal evolution of population aging in YRDUA from 2000 to 2020 using city-level population data.

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Although metal-organic frameworks (MOFs) have attracted more attention for the electrocatalytic CO reduction reaction (CORR), obtaining multicarbon products with a high Faradaic efficiency (FE) remains challenging, especially under neutral conditions. Here, we report the controlled synthesis of stable Cu(I) 5-mercapto-1-methyltetrazole framework (Cu-MMT) nanostructures with different facets by rationally modulating the reaction solvents. Significantly, Cu-MMT nanostructures with (001) facets are acquired using isopropanol as a solvent, which favor multicarbon production with an FE of 73.

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Environmentally friendly tin (Sn) perovskites have received considerable attention due to their great potential for replacing their toxic lead counterparts in applications of photovoltaics and light-emitting diodes (LEDs). However, the device performance of Sn perovskites lags far behind that of lead perovskites, and the highest reported external quantum efficiencies of near-infrared Sn perovskite LEDs are below 10%. The poor performance stems mainly from the numerous defects within Sn perovskite crystallites and grain boundaries, leading to serious non-radiative recombination.

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Article Synopsis
  • The research focuses on creating efficient mixed matrix membranes (MMMs) using metal-organic frameworks (MOFs) that are uniformly dispersed and highly loaded, addressing key challenges in their application.
  • A new method is introduced to synthesize oriented CuBDC/poly(m-phenylenediamine) (CuBDC/PmPD) MMMs at the air-solution interface, utilizing the dual function of metal ions for even MOF distribution.
  • The resulting MMM demonstrates strong separation capabilities for ion sieving and seawater desalination, thanks to its structural integrity and interconnected channels formed by the oriented MOF distribution, paving the way for advanced membrane technologies.
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Electron modulation presents a captivating approach to fabricate efficient electrocatalysts for the oxygen evolution reaction (OER), yet it remains a challenging undertaking. In this study, an effective strategy is proposed to regulate the electronic structure of metal-organic frameworks (MOFs) by the construction of MOF-on-MOF heterogeneous architectures. As a representative heterogeneous architectures, MOF-74 on MOF-274 hybrids are in situ prepared on 3D metal substrates (NiFe alloy foam (NFF)) via a two-step self-assembly method, resulting in MOF-(74 + 274)@NFF.

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The susceptibility to moisture of metal-organic frameworks (MOFs) is a critical bottleneck for their wider practical application. Constructing core-shell composites has been postulated as an effective strategy for enhancing moisture resistance, but for fragile MOFs this has rarely been accomplished. We report herein, for the first time, the construction of a customized hydrophobic porous shell, NTU-COF, on the particularly fragile MOF-5 by a "Plug-Socket Anchoring" strategy.

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Structural and compositional inhomogeneity is common in zeolites and considerably affects their properties. Thickness-limited lateral resolution, lack of depth resolution, and electron dose-constrained focusing limit local structural studies of zeolites in conventional transmission electron microscopy (TEM). We demonstrate that a multislice ptychography method based on four-dimensional scanning TEM (4D-STEM) data can overcome these limitations.

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Although isomerism is a typical and significant phenomenon in organic chemistry, it is rarely found in covalent organic framework (COF) materials. Herein, for the first time, we report a controllable synthesis of topological isomers in three-dimensional COFs via a distinctive tetrahedral building unit under different solvents. Based on this strategy, both isomers with a or net (termed JUC-620 and JUC-621) have been obtained, and their structures are determined by combining powder X-ray diffraction and transmission electron microscopy.

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Constructing active heterointerfaces is powerful to enhance the electrochemical performances of transition metal dichalcogenides, but the interface density regulation remains a huge challenge. Herein, MoO /MoS heterogeneous nanorods are encapsulated in nitrogen and sulfur co-doped carbon matrix (MoO /MoS @NSC) by controllable sulfidation. MoO and MoS are coupled intimately at atomic level, forming the MoO /MoS heterointerfaces with different distribution density.

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Benefiting from their unique structural merits, three-dimensional (3D) large-pore COF materials demonstrate high surface areas and interconnected large channels, which makes these materials promising in practical applications. Unfortunately, functionalization strategies and application research are still absent in these structures. To this end, a series of functional 3D -topologized COFs are designed based on porphyrin or metalloporphyrin moieties, named JUC-640-M (M = Co, Ni, or H).

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Many quantum magnetic materials suffer from structural imperfections. The effects of structural disorder on bulk properties are difficult to assess systematically from a chemical perspective due to the complexities of chemical synthesis. The recently reported S = 1/2 kagome lattice antiferromagnet, (CHNH)NaTiF, , with highly symmetric kagome layers and disordered interlayer methylammonium cations, shows no magnetic ordering down to 0.

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Article Synopsis
  • - The development of a novel polyimide covalent organic framework (PI-COF) provides a new type of electrode material for rechargeable devices, showcasing intrinsic redox reactions by altering electroactive site charge states.
  • - A water-assisted synthetic method was used to enhance the reaction rate and successfully created a highly crystalline PI-COF with a unique dual active center structure, yielding significant porosity and surface area (2669 m²/g).
  • - As a lithium-ion battery cathode, the COF combined with carbon nanotubes achieved impressive performance, delivering an initial charge capacity of 233 mAh/g and maintaining 80 mAh/g after 1800 cycles, even at high current densities.
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The capture of radioactive I vapor from nuclear waste under industrial operating conditions remains a challenging task, as the practical industrial conditions of high temperature (≥150 °C) and low I concentration (∼150 ppmv) are unfavorable for I adsorption. We report a novel guanidinium-based covalent organic framework (COF), termed TGDM, which can efficiently capture I under industrial operating conditions. At 150 °C and 150 ppmv I, TGDM exhibits an I uptake of ∼30 wt %, which is significantly higher than that of the industrial silver-based adsorbents such as Ag@MOR (17 wt %) currently used in the nuclear fuel reprocessing industry.

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With the development of ultralow-dose (scanning) transmission electron microscopy ((S)TEM) techniques, atomic-resolution imaging of highly sensitive nanomaterials has recently become possible. However, applying these techniques to the study of sensitive bulk materials remains challenging due to the lack of suitable specimen preparation methods. We report that cryogenic focused ion beam (cryo-FIB) can provide a solution to this challenge.

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Thermoelectric materials are typically highly degenerate semiconductors, which require high carrier concentration. However, the efficiency of conventional doping by replacing host atoms with alien ones is restricted by solubility limit, and, more unfavorably, such a doping method is likely to cause strong charge-carrier scattering at ambient temperature, leading to deteriorated electrical performance. Here, an unconventional doping strategy is proposed, where a small trace of alien atoms is used to stabilize cation vacancies in Cu SbSe  by compositing with CuAlSe , in which the cation vacancies rather than the alien atoms provide a high density of holes.

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Background: Patient Perceived Value (PPV) provides a valuable perspective to explain why the government reforms on health system in terms of functional medical treatment performance improvement did not decrease the crowded waiting line or increased patient satisfaction in China.

Methods: Questionnaires comprising seven constructs were sent to patients from seven highly recognized hospitals in Zhejiang Province of China. It was collected via face-by-face in a twelve-month period (2019), and 2586 valid data were collected for SPSS statistic accordingly.

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Objective: Magnetic resonance imaging (MRI) is gradually replacing computed tomography (CT) in the examination of bones and joints. The accurate and automatic segmentation of the bone structure in the MRI of the shoulder joint is essential for the measurement and diagnosis of bone injuries and diseases. The existing bone segmentation algorithms cannot achieve automatic segmentation without any prior knowledge, and their versatility and accuracy are relatively low.

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Traditional electrolysis of water produces hydrogen with a purity of ∼98%. Using ion transport membranes to prevent the migration of oxygen (O) from the anode to the cathode, the purity of H can be increased to ∼99.8%, but it still cannot fulfill the requirement for use in fuel cells (>99.

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