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学者姓名:于岩
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Herein, a versatile amorphous-to-crystalline transformation (ACT) strategy is described, to furnish various metals (Cu, Co, Ni, Cs, and Y) based atomically dispersed catalysts (ADCs) on thin holey 2D Al2O3. This approach, which involves adjusting reactant stoichiometry, enables the continuous modulation of particle size of ADCs at an atomical level, giving the ultrafine products as single atom, cluster, or nanoparticle catalysts. This synthesis method allows a straightforward analysis and comparison of the reactivity of the ADCs catalysts based on the dispersion of the active metal. In the case of Cu, the cluster catalyst 0.2-Cu/Al2O3 outperforms the single atom catalyst 0.1-Cu/Al2O3 and the nanoparticle catalyst 0.3-Cu/Al2O3 in the oxidation of refractory organic molecules, thanks to its superior electron transport and surface adsorption properties. These findings are well supported by the Density functional theory (DFT) calculations. Additionally, this method facilitates the preparation of atomic clusters with a very small size of 0.5-1 nm, composed of just a few atoms, as exemplified by Ni-based ADCs. The developed synthesis enriches the library of ADCs and demonstrates the potential of amorphous-to-crystalline transformation in creating advanced ultrasmall functional materials.
Keyword :
amorphous-to-crystalline transformation amorphous-to-crystalline transformation atomically dispersed catalysts atomically dispersed catalysts cluster, precise size tailoring cluster, precise size tailoring single atom single atom
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GB/T 7714 | Wang, Yaping , Zhang, Tingshi , Huang, Xinlian et al. Amorphous-to-Crystalline Transformation for Tunable Synthesis of Single Atom, Cluster, and Nanoparticle Catalysts: Dispersion of Metal Elements (Cu, Co, Ni, Y, Cs) on Holey 2D Ultra-Thin Al2O3 Nanosheets [J]. | SMALL METHODS , 2025 . |
MLA | Wang, Yaping et al. "Amorphous-to-Crystalline Transformation for Tunable Synthesis of Single Atom, Cluster, and Nanoparticle Catalysts: Dispersion of Metal Elements (Cu, Co, Ni, Y, Cs) on Holey 2D Ultra-Thin Al2O3 Nanosheets" . | SMALL METHODS (2025) . |
APA | Wang, Yaping , Zhang, Tingshi , Huang, Xinlian , Zeng, Yurong , Wei, Siyuan , Zhuang, Zanyong et al. Amorphous-to-Crystalline Transformation for Tunable Synthesis of Single Atom, Cluster, and Nanoparticle Catalysts: Dispersion of Metal Elements (Cu, Co, Ni, Y, Cs) on Holey 2D Ultra-Thin Al2O3 Nanosheets . | SMALL METHODS , 2025 . |
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Herein, we report a hydrogen-bonded supramolecular hybrid composed of a cobaloxime complex and a covalent organic framework (COF) that achieves photocatalytic overall water splitting. The designed COF features ternary units and dual linkages, which induce asymmetric linkers. Upon photoexcitation, this asymmetry facilitates directed electron transfer and spatially separated redox sites, resulting in a long-lived charge-separated state. Consequently, the COF, hydrogen-bonded with cobaloxime as a hydrogen (H2) production cocatalyst, enables visible-light photocatalytic overall water splitting, simultaneously producing H2 and hydrogen peroxide (H2O2), outperforming the COFs with symmetric linker structures. This strategy of asymmetric structural design offers new insights for the design of photocatalysts with suppressed charge recombination for photocatalysis.
Keyword :
Asymmetric structure Asymmetric structure Covalent organic framework Covalent organic framework Overall water splitting Overall water splitting Photocatalysis Photocatalysis Single site Single site
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GB/T 7714 | Yu, Mingfei , Huang, Junhan , Niu, Qing et al. Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
MLA | Yu, Mingfei et al. "Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2025) . |
APA | Yu, Mingfei , Huang, Junhan , Niu, Qing , Li, Liuyi , Yu, Yan , Bi, Jinhong . Asymmetric Structural Design in Cobaloxime-Integrated Covalent Organic Frameworks to Facilitate Photocatalytic Overall Water Splitting . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 . |
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Halide solid electrolytes receive much attention due to their electrochemical properties, such as high ionic conductivity, oxidative stability, and ease of preparation. In this work, a bromide solid electrolyte LiBiBr4, exhibiting ease of processing and high ionic conductivity, is designed for the first time and investigated through a comparative investigation with monoclinic LiAlCl4 and LiAlBr4 for the migration path. The processing pressure for LiBiBr4 with annealing at 120 degrees C is less than one-tenth that of other chloride electrolytes (approximate to 5 MPa). Computational analyses unveil crucial mechanistic insights into the three migration mechanisms and the factors that influence them within the monoclinic structure. The distribution and distance of non-Li polyhedrons to the migration pathways are pivotal for the migration. The strategic positioning of the Bi polyhedron in LiBiBr4 is far from the Li+ pathway. The unique leap migration within the LiBiBr4 has a lower energy barrier and facilitates an interconnected migration that forms a 3D interstice network. This interconnected leap migration network within LiBiBr4 constitutes a Z-type interstice leap migration along the ab-axis. Thus, the LiBiBr4 obtains a high ionic conductivity of 0.19 mS cm(-1) with the 0.349 eV low activation energy. This discovery and research methods provide significant impetus and support for the development of halogen-based electrolytes.
Keyword :
LiBiBr4 LiBiBr4 lithium Ion batteries lithium Ion batteries migration path migration path solid-state electrolyte solid-state electrolyte
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GB/T 7714 | Chao, Yu , Yang, Sisheng , Xu, Chenyuan et al. Z-Type Interstice Leap Migration Driving High Ionic Conductivity in Monoclinic LiBiBr4 Solid State Electrolyte [J]. | SMALL , 2025 , 21 (19) . |
MLA | Chao, Yu et al. "Z-Type Interstice Leap Migration Driving High Ionic Conductivity in Monoclinic LiBiBr4 Solid State Electrolyte" . | SMALL 21 . 19 (2025) . |
APA | Chao, Yu , Yang, Sisheng , Xu, Chenyuan , Li, Borong , Liu, Zheyuan , Fu, Xiaobin et al. Z-Type Interstice Leap Migration Driving High Ionic Conductivity in Monoclinic LiBiBr4 Solid State Electrolyte . | SMALL , 2025 , 21 (19) . |
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Single-atom catalysts (SACs) anchored on defective supports offer exceptional catalytic efficiency but face challenges in stabilizing isolated metal atoms and optimizing metal-support interactions. Here, a defect-driven strategy is reported to construct a 3D dendritic SAC comprising interwoven ultrathin TiO2 nanowires (NWs) with abundant oxygen vacancies (OVs) that stabilize atomically dispersed cobalt (Co) sites. Using hydrothermal synthesis followed by acid etching and calcination, Ti & horbar;Co & horbar;Ti motifs are engineered at OVs site. The 3D architecture provides multiscale porosity and charge transport, achieving syngas production rates of 28.4 mmol g(-1)h(-1) (CO) and 13.9 mmol g(-1)h(-1) (H-2) with a high turnover frequency (TOF) of 10.6 min(-1), surpassing many other state-of-the-art Co-based SACs. In situ Raman and electron paramagnetic resonance (EPR) analysis reveal OVs consumption during Co anchoring, while density functional theory (DFT) validates charge redistribution from Ti to Co, enabling efficient electron transfer and inducing strong electronic interactions that enhance CO2 adsorption and activation. The results highlight the interplay between atomic-scale coordination environments and macroscale architectural order in harnessing the catalytic potential of SACs and ultrathin 1D NWs.
Keyword :
CO2 photoreduction CO2 photoreduction defect engineering defect engineering oxygen vacancy oxygen vacancy single atom catalyst single atom catalyst ultrathin 1D nanowires ultrathin 1D nanowires
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GB/T 7714 | Yan, Jiawei , Lin, Yalan , Lin, Mingxiong et al. Defect-Driven Atomic Engineering: Oxygen Vacancy-Stabilized Co Single Atoms on Ordered Ultrathin TiO2 Nanowires for Efficient CO2-to-Syngas Photoreduction [J]. | SMALL , 2025 , 21 (22) . |
MLA | Yan, Jiawei et al. "Defect-Driven Atomic Engineering: Oxygen Vacancy-Stabilized Co Single Atoms on Ordered Ultrathin TiO2 Nanowires for Efficient CO2-to-Syngas Photoreduction" . | SMALL 21 . 22 (2025) . |
APA | Yan, Jiawei , Lin, Yalan , Lin, Mingxiong , Huang, Xinlian , Dong, Weilong , Huang, Haoyang et al. Defect-Driven Atomic Engineering: Oxygen Vacancy-Stabilized Co Single Atoms on Ordered Ultrathin TiO2 Nanowires for Efficient CO2-to-Syngas Photoreduction . | SMALL , 2025 , 21 (22) . |
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Traditional nanofiltration membranes allow high rejection of low molecular weight organic matter, yet suffer from a low flux and a high operation pressure, and they pose an environmental concern because they are made of petroleum-based polymers. Herein, a novel environmentally friendly filter membrane for ultrafast molecular separation has been developed using natural and artificial biomaterials as building units. Cellulose micron fibers, a natural biopolymer, serve as a stable substrate for the growth of hydroxyapatite (HAP) nanowire bunches, which are the main inorganic components of bones and teeth. The vertically aligned HAP nanowire bunches provide abundant nanoscale surfaces and confinement space for the attachment of dopamine and subsequently self-polymerization into polydopamine (PDA) sub-micron particles, which are a melanin-like bioactive polymer. On the one hand, the as-built micro-nano hierarchical configuration enables ultrahigh permeance (>6000 L m(-2) h(-1) bar(-1)) through the filter membrane at a low pressure (62 mbar). On the other hand, molecular dynamics simulations reveal that synergy between multiple molecular interactions of HAP and PDA contributes to the universal separation of different organic pollutants from water (i.e., cationic and anionic dyes and antibiotics) at a high removal rate of > 97 %. Overall, this work ingeniously uses biocompatible biomaterials to build a hierarchical filter membrane, thereby enabling ultrafast and efficient molecular separation.
Keyword :
Biomaterials Biomaterials Cellulose Cellulose Filter Membranes Filter Membranes Hydroxyapatite Nanowires Hydroxyapatite Nanowires Polydopamine Polydopamine
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GB/T 7714 | Wu, Linhan , Shi, Dehuan , Lin, Fuwang et al. Ultrafast molecular separation through all-biomaterial membranes with a hierarchical configuration and mechanism study [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 . |
MLA | Wu, Linhan et al. "Ultrafast molecular separation through all-biomaterial membranes with a hierarchical configuration and mechanism study" . | SEPARATION AND PURIFICATION TECHNOLOGY 361 (2025) . |
APA | Wu, Linhan , Shi, Dehuan , Lin, Fuwang , Chen, Fei-Fei , Yang, Chengkai , Yu, Yan . Ultrafast molecular separation through all-biomaterial membranes with a hierarchical configuration and mechanism study . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 361 . |
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The uncontrolled dendritic growth and severe side reactions significantly constrain zinc-ion batteries' further application. This study presents a novel micellar gel electrolyte, innovatively designed through hydrophobic association. The micellar gel electrolyte harmonizes macroscopic and microscopic properties through a rational hierarchical design. At the macroscopic level, the hydrophilic domains as water-absorbing nets and the hydrophobic domains as pillars are intricately interwoven. On the microscopic scale, the copolymerization resulted in a microphase-separated architecture, with hydrophilic and hydrophobic domains establishing distinct micro-regions within the gel matrix. The hydrophilic domains contribute to the stabilization of the hydrogen bond network through amide groups, while the abundant carbonyl groups optimize the solvation structure and migration pathways of Zn2+. The hydrophobic domains provide a robust supporting framework while simultaneously reducing H2O activity and thereby minimizing parasitic reactions. Thus, the enhanced interfacial stability forms a robust and flexible barrier against dendrite formation. The rational hierarchical gel composition and cross-linked network effectively direct Zn deposition preferentially along the (002) plane, ensuring a uniform and stable interface. The assembled Zn & Vert;MnO2 batteries show 80% capacity retention after 1200 cycles at 1C.
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GB/T 7714 | Chen, Zheming , Lin, Yushuang , Shi, Dehuan et al. Rational hierarchical micellar gel electrolytes with synergistic hydrophobic-hydrophilic integration for dendrite-free zinc-ion batteries [J]. | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (9) : 6709-6718 . |
MLA | Chen, Zheming et al. "Rational hierarchical micellar gel electrolytes with synergistic hydrophobic-hydrophilic integration for dendrite-free zinc-ion batteries" . | JOURNAL OF MATERIALS CHEMISTRY A 13 . 9 (2025) : 6709-6718 . |
APA | Chen, Zheming , Lin, Yushuang , Shi, Dehuan , Song, Kangwei , Luo, Jing , Qiu, Yanbin et al. Rational hierarchical micellar gel electrolytes with synergistic hydrophobic-hydrophilic integration for dendrite-free zinc-ion batteries . | JOURNAL OF MATERIALS CHEMISTRY A , 2025 , 13 (9) , 6709-6718 . |
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Here, we investigate PbSnS2, a wide band gap (1.13 eV) compound, as a promising thermoelectric material for power generation. Single crystal X-ray diffraction analysis reveals its 2D-layered structure, akin to the GeSe structure type, with Pb and Sn atoms sharing the same crystallographic site. The polycrystalline PbSnS2 exhibits an intrinsically ultralow lattice thermal conductivity (kappa(lat)) of 0.37 W m(-1) K-1 at 573 K. However, the low carrier concentration (n) leads to suboptimal electrical conductivity (sigma), capping the ZT value at 0.1. Accordingly, the halogen elements (Cl, Br, and I) are employed as the n-type dopants to improve the n. The DFT results indicate a significant weakening of Pb/Sn & horbar;S bonds upon halogen-doping, contributing to the observed reduction in kappa(lat). Our analysis indicates the activation of multiconduction band transport driven by halogen substitution. The PbSnS1.96Br0.04 has a high power factor of five times that of intrinsic PbSnS2. Halogen-doping weakens the Pb/Sn & horbar;S bonds and enhances the phonon scattering, leading to an ultralow kappa(lat) of 0.29 W m(-1) K-1 at 873 K for PbSnS1.96Br0.04. Consequently, PbSnS1.96Br0.04 achieved a maximum ZT value of 0.82 at 873 K.
Keyword :
Halogen-doping Halogen-doping PbSnS2 PbSnS2 Single crystal Single crystal Thermoelectricity Thermoelectricity Ultralow thermal conductivity Ultralow thermal conductivity
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GB/T 7714 | Chen, Zixuan , Ming, Hongwei , Li, Zhi et al. Ultralow Thermal Conductivity in Halogen-Doped PbSnS2 with Optimized Thermoelectric Properties [J]. | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (21) . |
MLA | Chen, Zixuan et al. "Ultralow Thermal Conductivity in Halogen-Doped PbSnS2 with Optimized Thermoelectric Properties" . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION 64 . 21 (2025) . |
APA | Chen, Zixuan , Ming, Hongwei , Li, Zhi , Girard, Steven N. , Morris, Collin D. , Guo, Weiping et al. Ultralow Thermal Conductivity in Halogen-Doped PbSnS2 with Optimized Thermoelectric Properties . | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION , 2025 , 64 (21) . |
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Low-dimensional materials with charge density waves (CDW) are attractive for their potential to exhibit superconductivity and nontrivial topological electronic features. Here we report the two-dimensional (2D) chalcogenide, BaSbTe2S which acts as a new platform hosting these phenomena. The crystal structure of BaSbTe2S is composed of alternating atomically thin Te square-net layers and double rock-salt type [(SbTeS)2]2- slabs separated with Ba2+ atoms. Due to the electronic instability of the Te square net, an incommensurately modulated structure is triggered and confirmed by both single-crystal X-ray diffraction, electron diffraction, and the presence of an energy bandgap in this compound. Our first-principles electronic structure analysis and investigation of structural dynamical instability suggest that the Te network plays a dominant role in its origin. The incommensurate structure is refined with a modulation vector of q = 0.351(1)b* using an orthorhombic cell of a = 4.4696(5) & Aring;, b = 4.4680(5) & Aring;, and c = 15.999(2) & Aring; under superspace group Pmm2(0 beta 0)000 at 293 K. The modulation vector q varies as a function of both occupancy of Te in the square net and temperature, indicating the CDW order can be modulated by local distortions. The CDW can be suppressed by pressure, leading to the emergence of superconductivity with a T c up to 7.5 K at 13.6 GPa, suggesting a competition between the CDW order and superconductivity. Furthermore, electrical transport under the magnetic field reveals the existence of compensated high mobility electron- and hole-bands near the Fermi surface (mu similar to 600-3500 cm2V-1s-1), suggesting Dirac-like band dispersion.
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GB/T 7714 | Luo, Zhong-Zhen , Zhao, Hengdi , Cai, Weizhao et al. Charge Density Wave and Superconductivity in BaSbTe2S Heterolayer Crystal with 2D Te Square Nets [J]. | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (8) : 6753-6762 . |
MLA | Luo, Zhong-Zhen et al. "Charge Density Wave and Superconductivity in BaSbTe2S Heterolayer Crystal with 2D Te Square Nets" . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 147 . 8 (2025) : 6753-6762 . |
APA | Luo, Zhong-Zhen , Zhao, Hengdi , Cai, Weizhao , Shahabfar, Shima , Li, Juncen , Cai, Songting et al. Charge Density Wave and Superconductivity in BaSbTe2S Heterolayer Crystal with 2D Te Square Nets . | JOURNAL OF THE AMERICAN CHEMICAL SOCIETY , 2025 , 147 (8) , 6753-6762 . |
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In the quest to align with industrial benchmarks, a noteworthy gap remains in the field of electrochemical nitrogen fixation, particularly in achieving high Faradaic efficiency (FE) and yield. The electrocatalytic nitrogen fixation process faces considerable hurdles due to the difficulty in cleaving the highly stable NN triple bond. Additionally, the electrochemical pathway for nitrogen fixation is often compromised by the concurrent hydrogen evolution reaction (HER), which competes aggressively for electrons and active sites on the catalyst surface, thereby reducing the FE of nitrogen reduction reaction (NRR). To surmount these challenges, this study introduces an innovative bimetallic catalyst, CuGa2, synthesized through p-d orbital hybridization to selectively facilitate N2 electroreduction. This catalyst has demonstrated a remarkable NH3 yield of 9.82 mu g h-1 cm-2 and an associated FE of 38.25%. Our findings elucidate that the distinctive p-d hybridization interaction between Ga and Cu enhances NH3 selectivity by reducing the reaction energy barrier for hydrogenation and suppressing hydrogen evolution. This insight highlights the significance of p-d orbital hybridization in optimizing the electrocatalytic performance of CuGa2 for nitrogen fixation.
Keyword :
Bimetallic catalyst Bimetallic catalyst CuGa 2 alloy CuGa 2 alloy Electrochemical nitrogen fixation Electrochemical nitrogen fixation Liquid metals Liquid metals p -d orbital hybridization p -d orbital hybridization
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GB/T 7714 | Chen, Bin , Zheng, Chaoyang , Shi, Dehuan et al. p-d orbital hybridization induced by CuGa2 promotes selective N2 electroreduction [J]. | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2025 , 44 (1) . |
MLA | Chen, Bin et al. "p-d orbital hybridization induced by CuGa2 promotes selective N2 electroreduction" . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY 44 . 1 (2025) . |
APA | Chen, Bin , Zheng, Chaoyang , Shi, Dehuan , Huang, Yi , Deng, Renxia , Wei, Yang et al. p-d orbital hybridization induced by CuGa2 promotes selective N2 electroreduction . | CHINESE JOURNAL OF STRUCTURAL CHEMISTRY , 2025 , 44 (1) . |
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Conventional aqueous zinc-ion batteries (AZIBs) encounter challenges that compromise the reversibility and stability of the zinc anode. To mitigate these issues, this study proposes the incorporation of highly polar 1,2-propylene glycol (PG) as a co-solvent. PG's capacity to form hydrogen bonds with water molecules effectively reduces water activity and facilitates uniform Zn2+ deposition by establishing a negatively charged adsorption layer via PG molecules. By optimizing the water-to-PG ratio, a tailored electrolyte system was developed, and the electrochemical behavior of Zn2+ during the solvation-to-deposition process was systematically elucidated through experimental and theoretical analyses. The findings indicate that AZIBs incorporating 20 % PG achieve a cycle life of 2500 h at a current density of 1 mA cm- 2 and a capacity of 1 mA h cm- 2, underscoring the pivotal role of PG in stabilizing the zinc anode interface. The assembled Zn||VO2 full cells demonstrated exceptional performance in the 20 % PG electrolyte, sustaining 1100 stable cycles even at a high rate of 20C. Moreover, AZIBs with 20 % PG exhibited superior ionic conductivity at low temperatures, enabling Zn||Zn symmetric cells to operate stably for 2500 h at-20 degrees C. These results highlight the significant potential of 20 % PG in practical energy storage systems.
Keyword :
Adsorption modulation Adsorption modulation Aqueous zinc-ion batteries Aqueous zinc-ion batteries Dendrite-free Dendrite-free Electrolyte co-solvent Electrolyte co-solvent Solvation structure Solvation structure
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GB/T 7714 | Yi, Jinlan , Lin, Yushuang , Jiang, Yaming et al. Co-solvent electrolyte-induced interface engineering for enhanced stability in zinc-ion batteries [J]. | JOURNAL OF POWER SOURCES , 2025 , 629 . |
MLA | Yi, Jinlan et al. "Co-solvent electrolyte-induced interface engineering for enhanced stability in zinc-ion batteries" . | JOURNAL OF POWER SOURCES 629 (2025) . |
APA | Yi, Jinlan , Lin, Yushuang , Jiang, Yaming , Lu, Yusheng , Zheng, Xinyu , Zhong, Shenghong et al. Co-solvent electrolyte-induced interface engineering for enhanced stability in zinc-ion batteries . | JOURNAL OF POWER SOURCES , 2025 , 629 . |
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