Reticular Synthesis of 3D Metal Cluster-Based COFs With Record High-Connectivity for Efficient Photocatalytic HO Synthesis.

The assembly of metal clusters with organic building units by covalent bonds to form metal cluster-based covalent-organic frameworks (MCCOFs) material is a novel strategy in reticular synthesis. However, only 2, 3, and 6 connectivity of MCCOFs have been achieved in reported structures. Developing a higher connectivity remains a great challenge in the MCCOFs due to the difficulties in introducing multiple connecting nodes to the metal cluster.

An in-situ assembled cobweb-like adhesive with high processability.

Low temperature tolerant adhesive with high flexibility and adhesion strength is highly desired yet challenging owing to the presence of obvious volume shrinkage, increased brittleness, and reduced transmission of mechanical stress at low temperature. Inspired by the cobweb, we hereby develop a kind of flexible adhesive that can be used at low temperature by in-situ polymerization of disulfide bond-based polymer with polyoxometalate. This low-temperature tolerant adhesive presents high flexibility and adhesion strength, good processability and reversible adhesion ability, a wide tolerable temperature range (i.

Modulating Adsorption Kinetics in a 3D-Interconnected Nanocavity Framework with Narrow Apertures for Enhanced Propylene Separation.

The energy-intensive distillation currently used for CH/CH separation─challenged by their small boiling point difference─could be improved via adsorption. However, most porous materials face a trade-off among CH adsorption capacity, selectivity, and kinetics. Herein, we report the synthesis and characterization of a novel metal-organic framework, denoted NiPzBim, constructed from a weak Lewis-base pyrazole-based ligand PzBim and the weak Lewis-acid Ni, featuring 3D pore structures with nanocavities (∼1 nm) connected by very narrow apertures (∼5 Å).

Charge-Transport Divergence in Ultrastable Heterometal-Oxo Clusters Exerting Significant Effect on Photoreactivity.

The transfer path of photogenerated charges greatly affects the final photocatalytic performance, but this important fact has not been clearly demonstrated experimentally. Here, we construct an ultrastable crystalline catalytic system including three heterometal-oxo clusters, BiM-TBC4A (M = group IVB metal-Ti/Zr/Hf), which include cubic metal-oxo cluster core with eight Bi atoms at the vertices, one M atom at the body center, and six M atoms above the cubic face centers. It is worth noted that the change of group IVB elements in BiM-TBC4A can specifically modulate the LUMO-HOMO orbitals to distribute on different active metal atoms.

Dual Chern Insulators with Electronic and Magnonic Edge States in Two-Dimensional Ferromagnets.

Chern insulator (CI) exhibits rich physics with great interest in both theory and experiment. Here, we focus on the honeycomb and kagome ferromagnets and demonstrate that coupling the nontrivial electronic and magnonic bands allows for the dual CIs, where the quantum anomalous Hall effect and its bosonic analogue, i.e.

Floquet Quantum Anomalous Hall Effect with Tunable and High Chern Numbers in Two-Dimensional Antiferromagnet KMnBi.

The quantum anomalous Hall effect (QAHE) holds significant fundamental and technological importance in low-dissipation spintronics. We employ a tight-binding model and first-principles calculations to illustrate that Floquet engineering offers a fertile playground to realize high-Chern-number QAHE in two-dimensional (2D) antiferromagnets. Via tuning of light frequency, we put forward an abundant topological phase map, i.

Competition propels, rather than limits, the success of low-affinity B cells in the germinal center response.

The germinal center (GC) sets an environment where antigen-specific B cells are compelled to continuously increase their affinity to compete for the antigen and obtain Tfh help for survival and propagation. Previous studies indicated that low-affinity B cells are disadvantaged in the presence of high-affinity ones, suggesting that competition may lead to the elimination of low-affinity B cells and their descendants. However, using a multivalent virus-mimicking antigen, our study demonstrates that low-affinity B cells not only successfully participate in GC responses alongside high-affinity B cells but also undergo accelerated affinity maturation under the more stringent competition.

A Stable Polyoxovanadate-based Metal-organic Framework Containing Dual Catalytic Sites for Efficient Synthesis of p-benzoquinones.

A novel polyoxovanadate-based metal-organic framework (POV-MOF), [Cu(bix)]{VO} (V-Cu-MOF, bix=1,4-bis(imidazol-1-ylmethyl)benzene), has been successfully synthesized and characterized. The V-Cu-MOF demonstrates exceptional performance in the selective oxidation of 2,3,6-trimethylphenol to 2,3,5-trimethyl-1,4-benzoquinone within just 10 minutes under mild conditions using hydrogen peroxide as the oxidant. The V-Cu-MOF exhibits remarkable versatility, efficiently oxidizing various substituted phenols while maintaining high catalytic activity.

Quantum anomalous Hall effect in a nonmagnetic bismuth monolayer with a high Chern number.

The quantum anomalous Hall effect (QAHE) with a high Chern number hosts multiple dissipationless chiral edge channels, which is of fundamental interest and promising for applications in spintronics. However, QAHE is currently limited in two-dimensional (2D) ferromagnets with Chern number . Using a tight-binding model, we put forward that Floquet engineering offers a strategy to achieve QAHE in 2D nonmagnets, and, in contrast to generally reported QAHE in 2D ferromagnets, a high-Chern-number is obtained accompanied by the emergence of two chiral edge states.

Conjugated phthalocyanine-based framework as artificial SEI for over 400 Wh kg lithium-metal battery.

High-voltage lithium-metal batteries (HVLMBs) are appealing candidates for next-generation high-energy rechargeable batteries, but their practical applications are still limited by the severe capacity degradation, attributed to the poor interfacial stability and compatibility between the electrode and the electrolyte. In this work, a 2D conjugated phthalocyanine framework (CPF) containing single atoms (SAs) of cobalt (CoSAs-CPF) is developed as a novel artificial solid-electrolyte interphase (SEI) in which a large amount of charge is transferred to the CPF skeleton due to the Lewis acid activity of the Co metal sites and the strong electron-absorbing property of the cyano group (-CN), greatly enhancing the adsorption of the Li and regulating the Li distribution toward dendrite-free LMBs, which are superior to most of the reported SEI membranes. As a result, the Li||Li symmetrical cell with CoSAs-CPF-modified Li anodes (CoSAs-CPF@Li) exhibits a low polarization with an area capacity of 1.

3D Covalent Organic Frameworks with 16-Connectivity for Photocatalytic C(sp)-C(sp) Cross-Coupling.

The connectivity (valency) of building blocks for constructing 3D covalent organic frameworks (COFs) has long been limited to 4, 6, 8, and 12. Developing a higher connectivity remains a great challenge in the field of COF structural design. Herein, this work reports a hierarchical expansion strategy for making 16-connected building blocks to construct 3D COFs with sqc topology.

In situ Construction of Single-Atom Electronic Bridge on COF to Enhance Photocatalytic H Production.

Photocatalytic hydrogen production is one of the most valuable technologies in the future energy system. Here, we designed a metal-covalent organic frameworks (MCOFs) with both small-sized metal clusters and nitrogen-rich ligands, named COF-CuTG. Based on our design, small-sized metal clusters were selected to increase the density of active sites and shorten the distance of electron transport to active sites.

Insight into the Mechanism of CO Chemical Fixation into Epoxides by Windmill-Shaped Polyoxovanadate and -BuNX (X = Br, I).

Carbon dioxide (CO) coupled with epoxide to generate cyclic carbonate stands out in carbon neutrality due to its 100% atom utilization. In this work, the mechanism of CO cycloaddition with propylene oxide (PO) cocatalyzed by windmill-shaped polyoxovanadate, [(CNH)(CHO)VVO]·4CHOH (V-1), and -BuNX (X = Br, I) was thoroughly investigated using density functional theory (DFT) calculations. The ring-opening, CO-insertion, and ring-closing steps of the process were extensively studied.

Photochromic radical states in 3D covalent organic frameworks with zyg topology for enhanced photocatalysis.

Covalent-organic frameworks (COFs) with photoinduced donor-acceptor (D-A) radical pairs show enhanced photocatalytic activity in principle. However, achieving long-lived charge separation in COFs proves challenging due to the rapid charge recombination. Here, we develop a novel strategy by combining [6 + 4] nodes to construct -type 3D COFs, first reported in COF chemistry.

A solvent-free processed low-temperature tolerant adhesive.

Ultra-low temperature resistant adhesive is highly desired yet scarce for material adhesion for the potential usage in Arctic/Antarctic or outer space exploration. Here we develop a solvent-free processed low-temperature tolerant adhesive with excellent adhesion strength and organic solvent stability, wide tolerable temperature range (i.e.

Floquet engineering of the orbital Hall effect and valleytronics in two-dimensional topological magnets.

We show that circularly polarized light is a versatile way to manipulate both the orbital Hall effect and band topology in two-dimensional ferromagnets. Employing the hexagonal lattice, we proposed that interactions between light and matter allow for the modulation of the valley polarization effect, and then band inversions, accompanied by the band gap closing and reopening processes, can be achieved subsequently at two valleys. Remarkably, the distribution of orbital angular momentum can be controlled by the band inversions, leading to the Floquet engineering of the orbital Hall effect, as well as the topological phase transition from a second-order topological insulator to a Chern insulator with in-plane magnetization, and then to a normal insulator.

Coupled Electronic and Magnonic Topological States in Two-Dimensional Ferromagnets.

Magnetic materials offer a fertile playground for fundamental physics discovery, with not only electronic but also magnonic topological states intensively explored. However, one natural material with both electronic and magnonic nontrivial topologies is still unknown. Here, we demonstrate the coexistence of first-order topological magnon insulators (TMIs) and electronic second-order topological insulators (SOTIs) in 2D honeycomb ferromagnets, giving rise to the nontrivial corner states being connected by the charge-free magnonic edge states.

Topology-Engineered Orbital Hall Effect in Two-Dimensional Ferromagnets.

Recent advances in the manipulation of the orbital angular momentum (OAM) within the paradigm of orbitronics presents a promising avenue for the design of future electronic devices. In this context, the recently observed orbital Hall effect (OHE) occupies a special place. Here, focusing on both the second-order topological and quantum anomalous Hall insulators in two-dimensional ferromagnets, we demonstrate that topological phase transitions present an efficient and straightforward way to engineer the OHE, where the OAM distribution can be controlled by the nature of the band inversion.

Coordinate-wise monotonic transformations enable privacy-preserving age estimation with 3D face point cloud.

The human face is a valuable biomarker of aging, but the collection and use of its image raise significant privacy concerns. Here we present an approach for facial data masking that preserves age-related features using coordinate-wise monotonic transformations. We first develop a deep learning model that estimates age directly from non-registered face point clouds with high accuracy and generalizability.

Screening TLR4 Binding Peptide from Venom Glands Based on Phage Display.

Toll-like receptor 4 (TLR4) is a crucial inflammatory signaling pathway that can serve as a potential treatment target for various disorders. A number of inhibitors have been developed for the TLR4 pathway, and although no inhibitors have been approved for clinical use, most have been screened against the TLR4-MD2 conformation. The venom gland is the organ of venomous snakes that secretes substances that are toxic to other animals.

Layer-coupled corner states in two-dimensional topological multiferroics.

The structural diversity and controllability in two-dimensional (2D) materials offers an intriguing platform for exploring a wide range of topological phenomena. The layer degree of freedom, as a novel technique for material manipulation, requires further investigation regarding its association with topological states. Here, using first-principles calculations and a tight-binding model, we propose a novel mechanism that couples the second-order topological corner states with the layer degree of freedom.

Bridging the Homogeneous and Heterogeneous Catalysis by Supramolecular Metal-Organic Cages with Varied Packing Modes.

Integrating the advantages of homogeneous and heterogeneous catalysis has proved to be an optimal strategy for developing catalytic systems with high efficiency, selectivity, and recoverability. Supramolecular metal-organic cages (MOCs), assembled by the coordination of metal ions with organic linkers into discrete molecules, have performed solvent processability due to their tunable packing modes, endowing them with the potential to act as homogeneous or heterogeneous catalysts in different solvent systems. Here, the design and synthesis of a series of stable {Cu} cluster-based tetrahedral MOCs with varied packing structures are reported.