Ultrafast and Durable Sodium-Ion Storage of Pseudocapacitive VN@C Hybrid Nanorods from Metal-Organic Framework.

Vanadium nitride (VN) is a promising electrode material for sodium-ion storage due to its multivalent states and high electrical conductivity. However, its electrochemical performance has not been fully explored and the storage mechanism remains to be clarified up to date. Here, the possibility of VN/carbon hybrid nanorods synthesized from a metal-organic framework for ultrafast and durable sodium-ion storage is demonstrated.

Corrigendum: Bispecific NK-cell engager targeting BCMA elicits stronger antitumor effects and produces less proinflammatory cytokines than T-cell engager.

[This corrects the article DOI: 10.3389/fimmu.2023.

Hundred-Fold Enhancement in the Anomalous Hall Effect Induced by Hydrogenation.

The anomalous Hall effect (AHE) is one of the most fascinating transport properties in condensed matter physics. However, the AHE magnitude, which mainly depends on net spin polarization and band topology, is generally small in oxides and thus limits potential applications. Here, we demonstrate a giant enhancement of AHE in a LaCoO-induced 5d itinerant ferromagnet SrIrO by hydrogenation.

Evaporative cooling and reaction of carbon dioxide clusters by low-energy electron attachment.

Anionic carbonate CO3- has been found in interstellar space and the Martian atmosphere, but its production mechanism is in debate so far. To mimic the irradiation-induced reactions on icy micrograins in the Martian atmosphere and the icy shell of interstellar dust, here we report a laboratory investigation on the dissociative electron attachments to the molecular clusters of CO2. We find that anionic species (CO2)n-1O- and (CO2)n- (n = 2, 3, 4) are produced in the concerted reaction and further stabilized by the evaporative cooling after the electron attachment.

Boosting Oxygen Reduction at Pt(111)|Proton Exchange Ionomer Interfaces through Tuning the Microenvironment Water Activity.

A proton exchange ionomer is one of the most important components in membrane electrode assemblies (MEAs) of polymer electrolyte membrane fuel cells (PEMFCs). It acts as both a proton conductor and a binder for nanocatalysts and carbon supports. The structure and the wetting conditions of the MEAs have a great impact on the microenvironment at the three-phase interphases in the MEAs, which can significantly influence the electrode kinetics such as the oxygen reduction reaction (ORR) at the cathode.

Selective CO Photoreduction Enabled by Water-stable Cu-based Metal-organic Framework Nanoribbons.

The goal of photocatalytic CO reduction system is to achieve near 100 % selectivity for the desirable product with reasonably high yield and stability. Here, two-dimensional metal-organic frameworks are constructed with abundant and uniform monometallic active sites, aiming to be an emerged platform for efficient and selective CO reduction. As an example, water-stable Cu-based metal-organic framework nanoribbons with coordinatively unsaturated single CuII sites are first fabricated, evidenced by X-ray diffraction patterns and X-ray absorption spectroscopy.

Selective Photoreduction of CO to CH Triggered by Metal-Vacancy Pair Sites.

Selectively achieving the photoreduction of carbon dioxide (CO) to methane (CH) remains a significant challenge, which primarily arises from the complexity of the protonation process. In this work, we designed metal-vacancy pair sites in defective metal oxide semiconductors, which anchor the reactive intermediates with a bridged linkage for the selective protonation to produce CH. As an example, oxygen-deficient NbO nanosheets are synthesized, in which the niobium-oxygen vacancy pair sites are demonstrated by X-ray photoelectron spectroscopy and electron paramagnetic resonance spectra.

The pH-Induced Increase of the Rate Constant for HER at Au(111) in Acid Revealed by Combining Experiments and Kinetic Simulation.

Origins of pH effects on the kinetics of electrocatalytic reactions involving the transfer of both protons and electrons, including the hydrogen evolution reaction (HER) considered in this study, are heatedly debated. By taking the HER at Au(111) in acid solutions of different pHs and ionic concentrations as the model systems, herein, we report how to derive the intrinsic kinetic parameters of such reactions and their pH dependence through the measurement of curves and the corresponding kinetic simulation based on the Frumkin-Butler-Volmer theory and the modified Poisson-Nernst-Planck equation. Our study reveals the following: (i) the same set of kinetic parameters, such as the standard activation Gibbs free energy, charge transfer coefficient, and Gibbs adsorption energy for H at Au(111), can simulate well all the curves measured in solutions with different pH and temperatures; (ii) on the reversible hydrogen electrode scale, the intrinsic rate constant increases with the increase of pH, which is in contrast with the decrease of the HER current with the increase of pH; and (iii) the ratio of the rate constants for HER at Au(111) in M HClO + (0.

Efficient Interfacial Sites between Metallic and Oxidized Cobalt for Propene Hydroformylation.

Currently, the hydroformylation of short olefins is operated almost exclusively by using Rh catalysts. Considering the high cost and scarcity of rhodium resources, it is important to develop non-noble metal catalysts toward hydroformylation. Herein, we report an efficient cobalt-based catalyst rich in interfacial sites between metallic and oxidized cobalt species for the hydroformylation of short olefin, propene, under a moderate syngas pressure.

Leveraging Interlayer Interaction in M-N-C Catalysts for Enhanced Activity in Oxygen Reduction Reactions.

Atomically dispersed metal-nitrogen-carbon (M-N-C) materials are deemed promising catalysts for the oxygen reduction reaction (ORR) in fuel cells. Yet the multilayer nature of M-N-C has been largely neglected in computational analysis. To bridge the gap, we conducted a first-principles investigation using bilayer M-N-C models (TMN/G-TMN/G, TM = Mn, Fe, Co, Ni, Cu, G = graphene, , = 3 or 4), where the TMs on the top serves as the active center.

Efficient Large DNA Fragment Knock-in by Long dsDNA with 3'-Overhangs Mediated CRISPR Knock-in (LOCK) in Mammalian Cells.

An efficient and precise genome-editing approach is in high demand in any molecular biology or cell biology laboratory worldwide. However, despite a recent rapid progress in the toolbox tailored for precise genome-editing, including the base editors and prime editors, there is still a need for a cost-effective knock-in (KI) approach amenable for long donor DNA cargos with high efficiency. By harnessing the high-efficient double-strand break (DSB) repair pathway of microhomology-mediated end joining, we previously showed that a specially designed 3'-overhang double-strand DNA (odsDNA) donor harboring 50-nt homology arm (HA) allows high-efficient exogenous DNA KI when combined with CRISPR-Cas9 technology.

Data-Driven Discovery of a Covalent Organic Framework Heterojunction as Efficient Photocatalysts for Overall Solar Water Splitting.

Searching for highly efficient visible-light photocatalysts is a high-cost and time-consuming process in the water splitting field. The integration of data-driven screening based on the database and density functional theory calculations represents a promising approach. In this study, we first present a topologically assembled single-layer covalent organic framework (COF) that is used to build a COF heterojunction database via AA stacking.

Optimized full CO photoreduction process by defective spinel atomic layers.

The impact of defects on the carbon dioxide (CO) photoreduction property is sometimes contradictory. Herein, we employ two-dimensional materials, possessing high-density and high-uniformity active sites, as ideal models to thoroughly investigate the influence of defects on three main processes during CO photoreduction. As an example, oxygen-deficient ZnGaO atomic layers are successfully fabricated, verified by the electron spin resonance spectra, X-ray photoelectron spectroscopy spectra and X-ray absorption near edge structure spectra.

Directly imaging excited state-resolved transient structures of water induced by valence and inner-shell ionisation.

Real-time imaging of transient structure of the electronic excited state is fundamentally critical to understand and control ultrafast molecular dynamics. The ejection of electrons from the inner-shell and valence level can lead to the population of different excited states, which trigger manifold ultrafast relaxation processes, however, the accurate imaging of such electronic state-dependent structural evolutions is still lacking. Here, by developing the laser-induced electron recollision-assisted Coulomb explosion imaging approach and molecular dynamics simulations, snapshots of the vibrational wave-packets of the excited (A) and ground states (X) of DO are captured simultaneously with sub-10 picometre and few-femtosecond precision.

Fundamentals and Challenges of Engineering Charge Polarized Active Sites for CO Photoreduction toward C Products.

ConspectusGlobal warming and climatic deterioration are partly caused by carbon dioxide (CO) emission. Given this, CO reduction into valuable carbonaceous fuels is a win-win route to simultaneously alleviate the greenhouse effect and the energy crisis, where CO reduction into hydrocarbon fuels by solar energy may be a potential strategy. Up to now, most of the current photocatalysts photoconvert CO to C products.

Dissociation dynamics of anionic carbon monoxide in dark states.

A resonant system consisting of an excess electron and a closed-shell atom or molecule, as a temporary negative ion, is usually in doublet-spin states that are analogous to bright states of photoexcitation of the neutral. However, anionic higher-spin states, noted as dark states, are scarcely accessed. Here, we report the dissociation dynamics of CO- in dark quartet resonant states that are formed by electron attachments to electronically excited CO (a3Π).

Bispecific NK-cell engager targeting BCMA elicits stronger antitumor effects and produces less proinflammatory cytokines than T-cell engager.

Bispecific antibodies have attracted more attention in recent years for the treatment of tumors, in which most of them target CD3, which mediates the killing of tumor cells by T cells. However, T-cell engager may cause serious side effects, including neurotoxicity and cytokine release syndrome. More safe treatments are still needed to address unmet medical needs, and NK cell-based immunotherapy is a safer and more effective way to treat tumors.

Strongly anisotropic ultrafast dynamic behavior of GaTe dominated by the tilted and flat bands.

The anisotropic transport properties of gallium telluride (GaTe) have been reported by several experiments, giving rise to many debates recently. The anisotropic electronic band structure of GaTe shows the extreme difference between the flat band and tilted band in two distinct directions,Γ¯-X¯andΓ¯-Y¯, and which we called as the mixed flat-tilted band (MFTB). Focusing on such two directions, the relaxation of photo-generated carriers has been studied using the non-adiabatic molecular dynamics (NAMD) method to investigate the anisotropic behavior of ultrafast dynamics.

The electrostatic effect and its role in promoting electrocatalytic reactions by specifically adsorbed anions.

The adsorption of anions and its impact on electrocatalytic reactions are fundamental topics in electrocatalysis. Previous studies revealed that adsorbed anions display an overall poisoning effect in most cases. However, for a few reactions such as the hydrogen evolution reaction (HER), oxidation of small organic molecules (SOMs), and reduction of CO and O, some specifically adsorbed anions can promote their reaction kinetics under certain conditions.

Selective CO -to-C H Photoconversion Enabled by Oxygen-Mediated Triatomic Sites in Partially Oxidized Bimetallic Sulfide.

Selective CO photoreduction into C fuels under mild conditions suffers from low product yield and poor selectivity owing to the kinetic challenge of C-C coupling. Here, triatomic sites are introduced into bimetallic sulfide to promote C-C coupling for selectively forming C products. As an example, FeCoS atomic layers with different oxidation degrees are first synthesized, demonstrated by X-ray photoelectron spectroscopy and X-ray absorption near edge spectroscopy spectra.

Construction of a Chiral β-Fluoroamine by Asymmetric Mannich Reaction of 2-Fluoroindanone with Pyrazolinone Ketimines.

The asymmetric Mannich reaction of 2-fluoroindanone with ketimine was developed under the catalysis of a kind of chiral copper complex, affording a chiral tetrahedral center containing fluorine. A series of β-fluoroamine derivatives can be obtained in excellent yields (73-94%) with high diastereoselectivities (>99:1 dr) and enantioselectivities (89-99%). The possible transition state was supported by density functional theory calculation.

Boosting Ferroptosis Therapy with Iridium Single-Atom Nanocatalyst in Ultralow Metal Content.

Nanocatalysts are promising tumor therapeutics due to their ability to induce reactive oxygen species in the tumor microenvironment. Although increasing metal loading can improve catalytic activity, the quandary of high metal content versus potential systemic biotoxicity remains challenging. Here, a fully exposed active site strategy by site-specific anchoring of single iridium (Ir) atoms on the outer surface of a nitrogen-doped carbon composite (Ir single-atom catalyst (SAC)) is reported to achieve remarkable catalytic performance at ultralow metal content (≈0.

Micro-alkaline environment enables CO electroreduction to multicarbons.

Improving the efficiency towards multicarbons of electrocatalytic CO2 reduction is desirable but challenging. In this perspective, researchers reported the design of micro-alkaline environment could benefit this issue.