Tandem reductive amination and deuteration over a phosphorus-modified iron center.

Deuterated amines are key building blocks for drug synthesis and the identification of metabolites of new pharmaceuticals, which drives the search for general, efficient, and widely applicable methods for the selective synthesis of such compounds. Here, we describe a multifunctional phosphorus-doped carbon-supported Fe catalyst with highly dispersed isolated metal sites that allow for tandem reductive amination-deuteration sequences. The optimal phosphorus-modified Fe-based catalyst shows excellent performance in terms of both reactivity and regioselectivity for a wide range of deuterated anilines, amines, bioactive complexes, and drugs (>50 examples).

A Synergistic Dual-Atom Sites Nanozyme Augments Immunogenic Cell Death for Efficient Immunotherapy.

Inducing immunogenic cell death (ICD) is a promising approach to elicit enduring antitumor immune responses. Hence, extensive efforts are being made to develop ICD inducers. Herein, a cascaded dual-atom nanozyme with Fe and Cu sites (FeCu-DA) as an efficient ICD inducer is presented.

Adsorption of neonicotinoid insecticides by mulch film-derived microplastics and their combined toxicity.

Mulch films allow for efficient crop production, yet their low recovery after use causes severe microplastics (MPs) pollution in agricultural soils. MPs in agricultural environments undergo complex ageing processes, which can alter their interactions with coexisting neonicotinoids and result in unpredictable ecological risks. Here, polyethylene (PE) and polybutylene adipate terephthalate (PBAT), typical mulch films, were chosen for the preparation of PE-MPs and PBAT-MPs.

Incoherence-to-coherence crossover observed in charge-density-wave material 1T-TiSe.

Analogous to the condensation of Cooper pairs in superconductors, the Bose-Einstein condensation (BEC) of electron-hole pairs in semiconductors and semimetals leads to an emergence of an exotic ground state - the excitonic insulator state. In this paper, we study the electronic structure of 1T-TiSe utilizing angle-resolved photoemission spectroscopy and alkali-metal deposition. Alkali-metal adatoms are deposited in-situ on the sample surface, doping the system with electrons.

Single-Atom Iridium Nanozyme-Based Persistent Luminescence Nanoparticles for Multimodal Imaging-Guided Combination Tumor Therapy.

Persistent luminescence nanoparticles (PLNPs) can achieve autofluorescence-free afterglow imaging, while near-infrared (NIR) emission realizes deep tissue imaging. Nanozymes integrate the merits of nanomaterials and enzyme-mimicking activities with simple preparation. Here PLNPs are prepared of ZnGaGeO:Cr with NIR emission at 700 nm.

Synthesis of Chlorophylls-Doped Guanine Crystals with High Reflection and Depolarization for Green Camouflage Coating.

Hyperspectral imaging technology can record the spatial and spectral information of the targets and significantly enhance the levels of military reconnaissance and target detection. It has scientific importance to mimic "homochromatic and homospectral" camouflage materials that have hyperspectral similarity with the green vegetation, one of the most common natural backgrounds. It is a big challenge to exquisitely simulate the spectral of green vegetation in visible and near-infrared windows because of the slight differences between the artificial green dyes and vegetation, the instability of chlorophylls, and the easy loss of hydroxide bands due to the loss of water from the camouflage materials.

Synergistically Modulating Conductive Filaments in Ion-Based Memristors for Enhanced Analog In-Memory Computing.

Memristors offer a promising solution to address the performance and energy challenges faced by conventional von Neumann computer systems. Yet, stochastic ion migration in conductive filament often leads to an undesired performance tradeoff between memory window, retention, and endurance. Herein, a robust memristor based on oxygen-rich SnO2 nanoflowers switching medium, enabled by seed-mediated wet chemistry, to overcome the ion migration issue for enhanced analog in-memory computing is reported.

Strategies Toward High Selectivity, Activity, and Stability of Single-Atom Catalysts.

Single-atom catalysts (SACs) hold immense promise in facilitating the rational use of metal resources and achieving atomic economy due to their exceptional atom-utilization efficiency and distinct characteristics. Despite the growing interest in SACs, only limited reviews have holistically summarized their advancements centering on performance metrics. In this review, first, a thorough overview on the research progress in SACs is presented from a performance perspective and the strategies, advancements, and intriguing approaches employed to enhance the critical attributes in SACs are discussed.

Ethylene Methoxycarbonylation over Heterogeneous Pt/MoS Single-Atom Catalyst: Metal-Support Concerted Catalysis.

Ethylene methoxycarbonylation (EMC) to methyl propanoate (MP) is an industrially important reaction and commercially uses a homogeneous Pd-phosphine organometallic complex as the catalyst and corrosive strong acid as the promoter. In this work, we develop a Pt/MoS heterogeneous single-atom catalyst (SAC) which exhibits high activity, selectivity, and good recyclability for EMC reaction without need of any liquid acid. The production rate of MP achieves 0.

Effects of microplastics on litter decomposition in wetland soil.

Microplastics (MPs) may interfere with the primary ecological processes of soil, which has become a growing global environmental issue. In terrestrial ecosystems, litter decomposition is the main process of nutrient cycling, particularly for carbon (C) and nitrogen (N). However, how microplastic pollution could alter wetland litter decomposition has barely been investigated.

AlO-Stabilized Pt Nanozymes: Peroxidase Mimetics and Application in Glucose Detection.

As promising alternatives for natural enzymes, much attention has been paid to nanozymes. And our recent study showed that the medium acid sites on the support are the active sites for the adsorption and oxidation of the substrate. Thus, in this work, due to the abundance of medium acid sites, AlO was chosen as the support to prepare Pt/AlO nanozymes.

Locally Ordered Single-Atom Catalysts for Electrocatalysis.

Single-atom catalysts manifest nearly 100 % atom utilization efficiency, well-defined active sites, and high selectivity. However, their practical applications are hindered by a low atom loading density, uncontrollable location, and ambiguous interaction with the support, thereby posing challenges to maximizing their electrocatalytic performance. To address these limitations, the ability to arrange randomly dispersed single atoms into locally ordered single-atom catalysts (LO-SACs) substantially influences the electronic effect between reactive sites and the support, the synergistic interaction among neighboring single atoms, the bonding energy of intermediates with reactive sites and the complexity of the mechanism.

Technology and Integration Roadmap for Optoelectronic Memristor.

Optoelectronic memristors (OMs) have emerged as a promising optoelectronic Neuromorphic computing paradigm, opening up new opportunities for neurosynaptic devices and optoelectronic systems. These OMs possess a range of desirable features including minimal crosstalk, high bandwidth, low power consumption, zero latency, and the ability to replicate crucial neurological functions such as vision and optical memory. By incorporating large-scale parallel synaptic structures, OMs are anticipated to greatly enhance high-performance and low-power in-memory computing, effectively overcoming the limitations of the von Neumann bottleneck.

Atomic Insights into Synergistic Nitroarene Hydrogenation over Nanodiamond-Supported Pt -Fe Dual-Single-Atom Catalyst.

Fundamental understanding of the synergistic effect of bimetallic catalysts is of extreme significance in heterogeneous catalysis, but a great challenge lies in the precise construction of uniform dual-metal sites. Here, we develop a novel method for constructing Pt -Fe /ND dual-single-atom catalyst, by anchoring Pt single atoms on Fe -N sites decorating a nanodiamond (ND) surface. Using this catalyst, the synergy of nitroarenes selective hydrogenation is revealed.

Biomimetic Synthesis of Organic Molecular-Doped Fluorescent Guanine Crystals with Pearlescence.

Biomimetic synthesis of guanine crystals has been focused on in the last years. However, multi-functional guanine crystals occluded with fluorescent molecules have not been realized in the laboratory. Here, the controllable synthesis of guanine crystal microplatelets with fluorescence and pearlescence was achieved for the first time by incorporating Nile red (NR) or fluorescein isothiocyanate (FITC) molecules into guanine crystals.

A Manganese-Based Metal-Organic Framework as a Cold-Adapted Nanozyme.

The development of cold-adapted enzymes with high efficiency and good stability is an advanced strategy to overcome the limitations of catalytic medicine in low and cryogenic temperatures. In this work, inspired by natural enzymes, a novel cold-adapted nanozyme based on a manganese-based nanosized metal-organic framework (nMnBTC) is designed and synthesized. The nMnBTC as an oxidase mimetic not only exhibits excellent activity at 0 °C, but also presents almost no observable activity loss as the temperature is increased to 45 °C.

Structural Insights into the Phosphorylation-Enhanced Deubiquitinating Activity of UCHL3 and Ubiquitin Chain Cleavage Preference Analysis.

Ubiquitin C-terminal hydrolase-L3 (UCHL3), an important member of the ubiquitin C-terminal hydrolase family, is involved in DNA repair and cancer development. UCHL3 can cleave only complexes of monoubiquitin and its conjugates, such as Ub-AMC, His, or small ubiquitin-like modifier, but not polyubiquitin chains. Phosphorylation of Ser75 promotes the cleavage activity of UCHL3 toward poly-ubiquitin chains in vivo, but biochemical evidence in vitro is still lacking.

Highly Selective Hydrogenation of CO to Ethanol via Designed Bifunctional Ir-InO Single-Atom Catalyst.

Recently, CO hydrogenation for the controlled growth of the carbon chain to produce high-value C or C products has attracted great interest, where achieving high selectivity for a specific product remains a challenge, especially for ethanol. Herein, we have designed a bifunctional Ir-InO single-atom catalyst, integrating two active catalytic centers by anchoring the monatomic Ir onto the InO carrier. This Ir-InO single-atom catalyst is efficient for the hydrogenation of CO in liquid, yielding a high selectivity for ethanol (>99%) with an excellent initial turnover frequency (481 h).

Structural Regulation of Magnetic Polymer Microsphere@Ionic Liquids with an Intermediate Protective Layer and Application as Core-Shell-Shell Catalysts with High Stability and Activity.

A novel ionic liquid immobilized on a magnetic polymer microsphere catalyst is reported in this paper. The obtained core-shell-shell catalyst consisted of magnetic nanoparticles (MNPs) as the core, catalytic inert St-co-DVB as the intermediate protective layer, and cross-linked polyaryl imidazole ionic liquids as the active catalytic layer located at the outermost [Im[OH]/MNPs@P(St-DVB)@P(VBC-DVB)]. This catalyst exhibited a high ion-exchange rate (64.

High-Density and Thermally Stable Palladium Single-Atom Catalysts for Chemoselective Hydrogenations.

Single-atom catalysts (SACs) have shown superior activity and/or selectivity for many energy- and environment-related reactions, but their stability at high site density and under reducing atmosphere remains unresolved. Herein, we elucidate the intrinsic driving force of a Pd single atom with high site density (up to 5 wt %) under reducing atmosphere, and its unique catalytic performance for hydrogenation reactions. In situ experiments and calculations reveal that Pd atoms tend to migrate into the surface vacancy-enriched MoC surface during the carburization process by transferring oxide crystals to carbide crystals, leading to the surface enrichment of atomic Pd instead of formation of particles.

Strong Metal-Support Interactions between Pt Single Atoms and TiO.

Strong metal-support interaction (SMSI) has gained great attention in the field of heterogeneous catalysis. However, whether single-atom catalysts can exhibit SMSI remains unknown. Here, we demonstrate that SMSI can occur on TiO -supported Pt single atoms but at a much higher reduction temperature than that for Pt nanoparticles (NPs).

Photo-thermo Catalytic Oxidation over a TiO -WO -Supported Platinum Catalyst.

Photo-thermo catalysis, which integrates photocatalysis on semiconductors with thermocatalysis on supported nonplasmonic metals, has emerged as an attractive approach to improve catalytic performance. However, an understanding of the mechanisms in operation is missing from both the thermo- and photocatalytic perspectives. Deep insights into photo-thermo catalysis are achieved via the catalytic oxidation of propane (C H ) over a Pt/TiO -WO catalyst that severely suffers from oxygen poisoning at high O /C H ratios.

Strong metal-support interaction promoted scalable production of thermally stable single-atom catalysts.

Single-atom catalysts (SACs) have demonstrated superior catalytic performance in numerous heterogeneous reactions. However, producing thermally stable SACs, especially in a simple and scalable way, remains a formidable challenge. Here, we report the synthesis of Ru SACs from commercial RuO powders by physical mixing of sub-micron RuO aggregates with a MgAlFeO spinel.