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Copper nanoclusters (CuNCs) are emerging electrochemiluminescence (ECL) emitters with unique molecule‐like electronic structures, high abundance, and low cost. However, the synthesis of CuNCs with high ECL efficiency and stability in a scalable manner remains challenging. Here, we report a facile gram‐scale approach for preparing self‐assembled CuNCs (CuNCsAssy) induced by ligands with exceptionally boosted anodic ECL and stability. Compared to the disordered aggregates that are inactive in ECL, the CuNCsAssy shows a record anodic ECL efficiency for CuNCs (10 %, wavelength‐corrected, relative to Ru(bpy)3Cl2/tripropylamine). Mechanism studies revealed the unusual dual functions of ligands in simultaneously facilitating electrochemical excitation and radiative transition. Moreover, the assembly addressed the limitation of poor stability of conventional CuNCs. As a proof of concept, an ECL biosensor for alkaline phosphatase detection was successfully constructed with an ultralow limit of detection of 8.1×10−6 U/L. [ABSTRACT FROM AUTHOR]

Nitric oxide (NO) exhibits both pro‐ and anti‐tumor effects. Therefore, real‐time in vivo imaging and quantification of tumor NO dynamics are essential for understanding the conflicting roles of NO played in pathophysiology. The current molecular probes, however, cannot provide high‐resolution imaging in deep tissues, making them unsuitable for these purposes. Herein, we designed a photoacoustic probe with an absorption maximum beyond 1000 nm for high spatial quantitative imaging of in vivo tumor NO dynamics. The probe exhibits remarkable sensitivity, selective ratiometric response behavior, and good tumor‐targeting abilities, facilitating ratiometric imaging of tumor NO throughout tumor progression in a micron‐resolution level. Using the probe as the imaging agent, we successfully quantified NO dynamics in tumor, liver and kidney. We have pinpointed an essential concentration threshold of around 80 nmol/cm3 for NO, which plays a crucial role in the "double‐edged‐sword" function of NO in tumors. Furthermore, we revealed a reciprocal relationship between the NO concentration in tumors and that in the liver, providing initial insights into the possible NO‐mediated communication between tumor and the liver. We believe that the probe will help resolve conflicting aspects of NO biology and guide the design of imaging agents for tumor diagnosis and anti‐cancer drug screening. [ABSTRACT FROM AUTHOR]

An aligned and laminated sulfur-absorbed mesoporous carbon/carbon nanotube (CNT) hybrid cathode has been developed for lithium-sulfur batteries with high performance. The mesoporous carbon acts as sulfur host and suppresses the diffusion of polysulfide, while the CNT network anchors the sulfur-absorbed mesoporous carbon particles, providing pathways for rapid electron transport, alleviating polysulfide migration and enabling a high flexibility. The resulting lithium-sulfur battery delivers a high capacity of 1226 mAh g−1 and achieves a capacity retention of 75 % after 100 cycles at 0.1 C. Moreover, a high capacity of nearly 900 mAh g−1 is obtained for 20 mg cm−2, which is the highest sulfur load to the best of our knowledge. More importantly, the aligned and laminated hybrid cathode endows the battery with high flexibility and its electrochemical performances are well maintained under bending and after being folded for 500 times. [ABSTRACT FROM AUTHOR]

A combination of ab initio calculations, circular dichroism, nuclear magnetic resonance, and X-ray photoelectron spectroscopy has shown that aluminum ions can induce the formation of backbone ring structures in a wide range of peptides, including neurodegenerative disease related motifs. These ring structures greatly destabilize the protein and result in irreversible denaturation. This behavior benefits from the ability of aluminum ions to form chemical bonds simultaneously with the amide nitrogen and carbonyl oxygen atoms on the peptide backbone. [ABSTRACT FROM AUTHOR]

Solid‐state Li‐O2 batteries possess the ability to deliver high energy density with enhanced safety. However, designing a highly functional solid‐state air electrode is the main bottleneck for its further development. Herein, we adopt a hybrid electronic and ionic conductor to build solid‐state air electrode that makes the transition of Li‐O2 battery electrochemical mechanism from a three‐phase process to a two‐phase process. The solid‐state Li‐O2 battery with this hybrid conductor solid‐state air electrode shows decreased interfacial resistance and enhanced reaction kinetics. The Coulombic efficiency of Li‐O2 battery is also significantly improved, benefiting from the good contact between discharge products and electrode materials. In situ environmental transmission electron microscopy under oxygen was used to illustrate the reversible deposition and decomposition of discharge products on the surface of this hybrid conductor, visually verifying the two‐phase reaction. [ABSTRACT FROM AUTHOR]

Understanding evolution of antibiotic resistance is vital for containing its global spread. Yet our ability to in situ track highly heterogeneous and dynamic evolution is very limited. Here, we present a new single‐cell approach integrating D2O‐labeled Raman spectroscopy, advanced multivariate analysis, and genotypic profiling to in situ track physiological evolution trajectory toward resistance. Physiological diversification of individual cells from isogenic population with cyclic ampicillin treatment is captured. Advanced multivariate analysis of spectral changes classifies all individual cells into four subsets of sensitive, intrinsic tolerant, evolved tolerant and resistant. Remarkably, their dynamic shifts with evolution are depicted and spectral markers of each state are identified. Genotypic analysis validates the phenotypic shift and provides insights into the underlying genetic basis. The new platform advances rapid phenotyping resistance evolution and guides evolution control. [ABSTRACT FROM AUTHOR]

Modulating the electronic structure of atomically dispersed active sites is promising to boost catalytic activity but is challenging to achieve. Here we show a cooperative Ni single‐atom‐on‐nanoparticle catalyst (NiSA/NP) prepared via direct solid‐state pyrolysis, where Ni nanoparticles donate electrons to Ni(i)−N−C sites via a network of carbon nanotubes, achieving a high CO current density of 346 mA cm−2 at −0.5 V vs RHE in an alkaline flow cell. When coupled with a NiFe‐based anode in a zero‐gap membrane electrolyzer, the catalyst delivers an industrially relevant CO current density of 310 mA cm−2 at a low cell voltage of −2.3 V, corresponding to an overall energy efficiency of 57 %. The superior CO2 electroreduction performance is attributed to the enhanced adsorption of key intermediate COOH* on the electron‐rich Ni single atoms, as well as a high density of active sites. [ABSTRACT FROM AUTHOR]

Li‐ and Mn‐rich layered oxides are among the most promising cathode materials for Li‐ion batteries with high theoretical energy density. Its practical application is, however, hampered by the capacity and voltage fade after long cycling. Herein, a finite difference method for near‐edge structure (FDMNES) code was combined with in situ X‐ray absorption spectroscopy (XAS) and transmission electron microscopy/electron energy loss spectroscopy (TEM/EELS) to investigate the evolution of transition metals (TMs) in fresh and heavily cycled electrodes. Theoretical modeling reveals a recurring partially reversible LiMn2O4‐like sub‐nanodomain formation/dissolution process during each charge/discharge, which accumulates gradually and accounts for the Mn phase transition. From the modeling of spectra and maps of the valence state over large regions of the cathodes, it was found that the phase change is size‐dependent. After prolonged cycling, the TMs displayed different levels of inactivity. [ABSTRACT FROM AUTHOR]

It is of vital importance to capture lanthanides (nuclear fission products) from waste solutions for radionuclide remediation owing to their hazards. The effective separation of lanthanides are achieved by an acid/base‐stable and radiation‐resistant vanadate, namely, [Me2NH2]V3O7 (1). It exhibits high adsorption capacities for lanthanides (qmEu=161.4 mg g−1; qmSm=139.2 mg g−1). And high adsorption capacities are maintained over a pH range of 2.0–6.9 (qmEu=75.1 mg g−1 at low pH of 2.5). It displays high selectivity for Eu3+ (simulant of An3+) against a large excess of interfering ions. It can efficiently separate Eu3+ and Cs+ (or Sr2+) with the highest separation factor SFEu/Cs of 156 (SFEu/Sr of 134) to date. The adsorption mechanism is revealed by calculations and XPS, EXAFS, Raman, and elemental analyses. These merits combined with facile synthesis and convenient elution makes the title vanadate a promising lanthanide scavenger for environmental remediation. [ABSTRACT FROM AUTHOR]