Spatial correlation of desorption events accelerates water exchange dynamics at Pt/water interfaces.

The altered solvation structures and dynamical properties of water molecules at the metal/water interfaces will affect the elementary step of an electrochemical process. Simulating the interfacial structure and dynamics with a realistic representation will provide us with a solid foundation to make a connection with experimental studies. To surmount the accuracy-efficiency tradeoff and provide dynamical insights, we use state-of-the-art machine learning molecular dynamics (MLMD) to study the water exchange dynamics, which are fundamental to adsorption/desorption and electrochemical reaction steps.

DNA lesion-gated dumbbell nanodevices enable on-demand activation of the cGAS-STING pathway for enhancing cancer immunotherapy.

Utilizing the cGAS-STING pathway to combat immune evasion is one of the most promising strategies for enhancing cancer immunotherapy. However, current techniques for activating the cGAS-STING pathway often face a dilemma, mainly due to the balance between efficacy and safety. Here, we develop a uracil base lesion-gated dumbbell DNA nanodevice (UBLE) that allows on-demand activation and termination of the cGAS-STING pathway in tumor cells, thereby enhancing cancer immunotherapy.

Population expansion from central plain to northern coastal China inferred from ancient human genomes.

The population history of the northern coastal Chinese is largely unknown due to the lack of ancient human genomes from the Neolithic to historical periods. In this study, we reported 14 newly generated ancient genomes from Linzi, one of China's densely populated and economically prosperous cities from the Zhou to Han Dynasties. The ancient samples in this study were dated to the Warring States period to the Eastern Han Dynasty (∼2,000 BP).

Enhancing the tribopositive characteristics of polyvinyl alcohol (PVA)-carbon composites by optimizing the PVA-carbon interaction with various carbon fillers.

Incorporating carbon-based fillers into triboelectric nanogenerators, TENGs, is a compelling strategy to enhance the power output. However, the lack of systematic studies comparing various carbon fillers and their impact on tribopositive contact layers necessitates further research. To address these concerns, various carbon fillers (including buckminsterfullerene (C), graphene oxide (GO), reduced graphene oxide (rGO), multi-wall carbon nanotube (MWCNT), and super activated carbon (SAC)) with distinct structural and electrical properties are mixed with polyvinyl alcohol, PVA, to form PVA-carbon composites and used as tribopositive layers in the contact-separation of TENGs.

Oxygen activation and transfer for catalytic wet-air oxidation of wastewater: a short review.

With the rapid growth of population and industrial production, wastewater pollution has become a major environmental issue. Wastewater pollution also poses a threat to water resources and human health. Catalytic wet-air oxidation (CWAO) is one of the most economical and environmentally friendly technologies, especially for the treatment of toxic and non-biodegradable pollutants in wastewater.

Time-resolved single-cell transcriptomic sequencing.

Cells experience continuous transformation under both physiological and pathological circumstances. Single-cell RNA sequencing (scRNA-seq) is competent in disclosing the disparities of cells; nevertheless, it poses challenges in linking the individual cell state at distinct time points. Although computational approaches based on scRNA-seq data have been put forward for trajectory analysis, the result is based on assumptions and fails to reflect the actual states.

Computational discovery of two-dimensional tetragonal group IV-V monolayers.

The two-dimensional (2D) hexagonal group IV-V family has attracted significant attention due to their unique properties and potential applications in electronics, spintronics, and photocatalysis. In this study, we report the discovery of a stable tetragonal allotrope, termed the Td4 phase, of 2D IV-V monolayers through a structural search utilizing an adaptive genetic algorithm. We investigate the geometric structures, structural stabilities, and band structures of the Td4-phase 2D IV-V monolayers (where IV = Si, Ge, Sn; V = P, As, Sb) based on the first-principles calculations.

Enhancing electrical conductivity in zirconium-doped SiC ceramics through synergistic effects of crystal structure and free carbon control.

Polymer-derived ceramics (PDCs) have risen to prominence for applications in electrochemical energy storage, electromagnetic absorbing, and sensing materials, among others. However, a multitude of critical properties in PDCs are still limited by their intrinsic poor electrical conductivity. Herein, novel vinyl and zirconium-modified polycarbosilane precursors with improved electrical conductivity were synthesized through a Grignard coupling reaction of vinyl magnesium chloride and zirconocene dichloride, followed by the insertion polymerization with dichlorodimethylsilane and sodium.

Entropy in catalyst dynamics under confinement.

Entropy during the dynamic structural evolution of catalysts has a non-trivial influence on chemical reactions. Confinement significantly affects the catalyst dynamics and thus impacts the reactivity. However, a full understanding has not been clearly established.

Water at electrode-electrolyte interfaces: combining HOD vibrational spectra with -molecular dynamics simulations.

We have undertaken a vibrational study of the structure of interfacial water and its potential dependence using HO : DO mixtures to explore the O-H and O-D stretching modes of HOD as well as the bending modes of HOD and HO. Due to the symmetry reduction, some of the complexity characteristic of the vibrational spectrum of water is removed in HOD. Coupled with potential-dependent simulations of the gold-water interface, this has enabled a deeper insight into the hydrogen-bond network of interfacial water and into how it is affected by the applied potential.

Synthesis and crystallization of a carboxylate functionalized -heterocyclic carbene-based Au cluster with strong photo-luminescence.

Here we report the synthesis and crystallization of a -COOH-capped -heterocyclic carbene (NHC)-protected Au cluster. The single-crystal structure of the -COOH-capped NHC-Au cluster reveals a classic icosahedral core with one Au atom in its center. The icosahedral core is surrounded by five NHC ligands with pseudo C5 symmetry and exposed carboxyls in a pentagonal antiprism fashion.

Achievement of a giant electromechanical conversion coefficient in a molecule-based ferroelectric.

Molecule-based ferroelectrics are promising candidates for flexible self-powered power supplies (, piezoelectric generators (PEGs)). Although the large electromechanical conversion coefficients ( × ) of piezoelectrics are key to enhancing the performance of PEGs in their nonresonant states, it remains a great challenge to obtain molecule-based piezoelectrics with large × . Here, we report a molecule-based ferroelectric [(CH)NCHCHCl][GaBr] (1) that exhibits the largest piezoelectric coefficient (∼454 pC N) and electromechanical conversion coefficient (4953.

Vesicular neurotransmitters exocytosis monitored by amperometry: theoretical quantitative links between experimental current spikes shapes and intravesicular structures.

Single cell amperometry has proven to be a powerful and well-established method for characterizing single vesicular exocytotic events elicited at the level of excitable cells under various experimental conditions. Nevertheless, most of the reported characteristics are descriptive, being mostly concerned with the morphological characteristics of the recorded current spikes (maximum current intensities, released charge, rise and fall times, ) which are certainly important but do not provide sufficient kinetic information on exocytotic mechanisms due to lack of quantitative models. Here, continuing our previous efforts to provide rigorous models rationalizing the kinetic structures of frequently encountered spike types (spikes with unique exponential decay tails and kiss-and-run events), we describe a new theoretical approach enabling a quantitative kinetic modeling of all types of exocytotic events giving rise to current spikes exhibiting exponential decay tails.

Ribosomal translation of fluorinated non-canonical amino acids for biologically active fluorinated macrocyclic peptides.

Fluorination has emerged as a promising strategy in medicinal chemistry to improve the pharmacological profiles of drug candidates. Similarly, incorporating fluorinated non-canonical amino acids into macrocyclic peptides expands chemical diversity and enhances their pharmacological properties, from improved metabolic stability to enhanced cell permeability and target interactions. However, only a limited number of fluorinated non-canonical amino acids, which are canonical amino acid analogs, have been incorporated into macrocyclic peptides by ribosomes for construction and target-based screening of fluorinated macrocyclic peptides.

Step-induced double-row pattern of interfacial water on rutile TiO(110) under electrochemical conditions.

Metal oxides are promising (photo)electrocatalysts for sustainable energy technologies due to their good activity and abundant resources. Their applications such as photocatalytic water splitting predominantly involve aqueous interfaces under electrochemical conditions, but probing oxide-water interfaces is proven to be extremely challenging. Here, we present an electrochemical scanning tunneling microscopy (EC-STM) study on the rutile TiO(110)-water interface, and by tuning surface redox chemistry with careful potential control we are able to obtain high quality images of interfacial structures with atomic details.

Automation and machine learning augmented by large language models in a catalysis study.

Recent advancements in artificial intelligence and automation are transforming catalyst discovery and design from traditional trial-and-error manual mode into intelligent, high-throughput digital methodologies. This transformation is driven by four key components, including high-throughput information extraction, automated robotic experimentation, real-time feedback for iterative optimization, and interpretable machine learning for generating new knowledge. These innovations have given rise to the development of self-driving labs and significantly accelerated materials research.

Wide-direct-band-gap monolayer carbon nitride CN: a potential metal-free photocatalyst for overall water splitting.

Two dimensional metal-free semiconductors with high work function have attracted extensive research interest in the field of photocatalytic water splitting. Herein, we have proposed a kind of highly stable monolayer carbon nitride CN with an anisotropic structure based on first principles density functional theory. The calculations of electronic structure properties, performed using the HSE06 functional, indicate that monolayer CN has a wide direct band gap of 2.

Selectivity descriptors of the catalytic -hexane cracking process over 10-membered ring zeolites.

Zeolite-mediated catalytic cracking of alkanes is pivotal in the petrochemical and refining industry, breaking down heavier hydrocarbon feedstocks into fuels and chemicals. Its relevance also extends to emerging technologies such as biomass and plastic valorization. Zeolite catalysts, with shape selectivity and selective adsorption capabilities, enhance efficiency and sustainability due to their well-defined network of pores, dimensionality, cages/cavities, and channels.

Updates on Hydrogen Value Chain: A Strategic Roadmap.

A strategic roadmap for noncarbonized fuels is a global priority, and the reduction of carbon dioxide emissions is a key focus of the Paris Agreement to mitigate the effects of rising temperatures. In this context, hydrogen is a promising noncarbonized fuel, but the pace of its implementation will depend on the engineering advancements made at each step of its value chain. To accelerate its adoption, various applications of hydrogen across industries, transport, power, and building sectors have been identified, where it can be used as a feedstock, fuel, or energy carrier and storage.

Harnessing the Power of Light: The Synergistic Effects of Crystalline Carbon Nitride and TiCT MXene in Photocatalytic Hydrogen Production.

Photocatalytic hydrogen evolution is an environmentally friendly means of energy generation. Although g-CN possesses fascinating features, its inherent shortcomings limit its photocatalytic applications. Therefore, modifying the intrinsic properties of g-CN and introducing cocatalysts are essential to ameliorate the photocatalytic efficiency.

Interfacial electronic state between hexagonal ZnO and cubic NiO.

The interface of two dissimilar materials gives rise to a myriad of interesting structural, magnetic, and electronic properties that may be utilized to produce novel materials with unique characteristics and functions. In particular, growing a cubic oxide film on top of a hexagonal oxide substrate results in such unique properties due to the conflict of their respective stabilization mechanisms within the interface layer. This study aims to elucidate the electronic properties of the interface between hexagonal ZnO and cubic NiO by analyzing the interface electronic states within epitaxial NiO films grown on ZnO substrates, expressed in the form of ultraviolet photoemission spectroscopy (UPS) for valence band structure and X-ray absorption spectroscopy (XAS) spectra for conduction band structure.

Investigation of emission plane control in GaInN/GaN multiple-quantum shells for efficient nanowire-based LEDs.

Significant attention has been directed toward core-shell GaInN/GaN multiple-quantum shell (MQS) nanowires (NWs) in the context of high-efficiency micro light-emitting diodes (micro-LEDs). These independent three-dimensional NWs offer the advantage of reducing the impact of sidewall etching regions. Furthermore, the emitting plane on the sidewalls demonstrates either nonpolar or semipolar orientation, while the dislocation density is exceptionally low.

Protocol for a comprehensive pipeline to study ancient human genomes.

Ancient genomics has revolutionized our understanding of human evolution and migration history in recent years. Here, we present a protocol to prepare samples for ancient genomics research. We describe steps for releasing DNA from human remains, DNA library construction, hybridization capture, quantification, and sequencing.

Two-dimensional radial-π-stacks in solution.

Highly organized π-aggregate architectures can strongly affect electronic couplings, leading to important photophysical behaviors. With the escalating interest in two-dimensional (2D) materials attributed to their exceptional electronic and optical characteristics, there is growing anticipation that 2D radial-π-stacks built upon radial π-conjugation nanorings, incorporating intra- and inter-ring electronic couplings within the confines of a 2D plane, will exhibit superior topological attributes and distinct properties. Despite their immense potential, the design and synthesis of 2D π-stacks have proven to be a formidable challenge due to the insufficient π-π interactions necessary for stable stacking.