The alanyl-tRNA synthetase AARS1 moonlights as a lactyltransferase to promote YAP signaling in gastric cancer.

Lactylation has been recently identified as a new type of posttranslational modification occurring widely on lysine residues of both histone and nonhistone proteins. The acetyltransferase p300 is thought to mediate protein lactylation, yet the cellular concentration of the proposed lactyl-donor, lactyl-coenzyme A, is about 1,000 times lower than that of acetyl-CoA, raising the question of whether p300 is a genuine lactyltransferase. Here, we report that alanyl-tRNA synthetase 1 (AARS1) moonlights as a bona fide lactyltransferase that directly uses lactate and ATP to catalyze protein lactylation. Among the candidate substrates, we focused on the Hippo pathway, which has a well-established role in tumorigenesis. Specifically, AARS1 was found to sense intracellular lactate and translocate into the nucleus to lactylate and activate the YAP-TEAD complex; and AARS1 itself was identified as a Hippo target gene that forms a positive-feedback loop with YAP-TEAD to promote gastric cancer (GC) cell proliferation. Consistently, the expression of AARS1 was found to be upregulated in GC, and elevated AARS1 expression was found to be associated with poor prognosis for patients with GC. Collectively, this work found AARS1 with lactyltransferase activity in vitro and in vivo and revealed how the metabolite lactate is translated into a signal of cell proliferation.

In Situ Growth of Conductive Metal-Organic Framework onto Cu2O for Highly Selective and Humidity-Independent Hydrogen Sulfide Detection in Food Quality Assessment.

The sensitivity of chemiresistive gas sensors based on metal oxide semiconductors (MOSs) has been inherently affected by ambient humidity because their reactive oxygen species are easily hydroxylated by water molecules, which significantly reduces the accuracy of the gas sensors in food quality assessment. Although conventional metal organic frameworks (MOFs) can serve as coatings for MOSs for humidity-independent gas detection, they have to operate at high working temperatures due to their low or nonconductivity, resulting in high power consumption, significant manufacturing inconvenience, and short-term stability due to the oxidation of MOFs. Here, the conductive and thickness-controlled CuHHTP (HHTP = 2,3,6,7,10,11-hexahydroxytriphenylene)-coated Cu2O are developed by combining in situ etching and layer-by-layer liquid-phase growth method, which achieves humidity-independent detection of H2S at room temperature. The response to H2S only decreases by 2.6% below 75% relative humidity (RH), showing a 9.6-fold improvement than the bare Cu2O sensor, which is ascribed to the fact that the CuHHTP layer hinders the adsorption of water molecules. Finally, a portable alarm system is developed to monitor food quality by tracking released H2S. Compared with gas chromatography method, their relative error is within 9.4%, indicating a great potential for food quality assessment.

Design and multilevel regulation of transition metal phosphides for efficient and industrial water electrolysis.

Renewable energy electrolysis of water to produce hydrogen is an effective measure to break the energy dilemma. However, achieving activity and stability at a high current density is still a key problem in water electrolyzers. Transition metal phosphides (TMPs), with high activity and relative inexpensiveness, have become excellent candidates for the production of highly pure green hydrogen for industrial applications. In this mini-review, multilevel regulation strategies including nanoscale control, surface composition and interface structure design of high-performance TMPs for hydrogen evolution are systematically summarized. On this basis, in order to achieve large-scale hydrogen production in industry, the hydrogen evolution performance and stability of TMPs at a high current density are also discussed. Peculiarly, the practical application and requirements in proton exchange membrane (PEM) or anion exchange membrane (AEM) electrolyzers can guide the advanced design of regulatory strategies of TMPs for green hydrogen production from renewable energy. Finally, the challenges and prospects in the future development trend of TMPs for efficient and industrial water electrolysis are given.

Elaborating the Crystal Water of Prussian Blue for Outstanding Performance of Sodium Ion Batteries.

Prussian blue (PB) is one of the main cathode materials with industrial prospects for the sodium ion battery. The structural stability of PB materials is directly associated with the presence of crystal water within the open 3D framework. However, there remains a lack of consensus regarding whether all forms of crystal water have detrimental effects on the structural stability of the PB materials. Currently, it is widely accepted that interstitial water is the stability troublemaker, whereas the role of coordination water remains elusive. In this work, the dynamic evolution of PB structures is investigated during the crystal water (in all forms) removal process through a variety of online monitoring techniques. It can be inferred that the PB-130 °C retains trace coordination water (1.3%) and original structural integrity, whereas PB-180 °C eliminates almost all of crystal water (∼12.1%, including both interstitial and coordinated water), but inevitably suffers from structural collapse. This is mainly because the coordinated water within the PB material plays a crucial role in maintaining structural stability via forming the -N≡C-FeLS-C≡N- conjugate bridge. Consequently, PB-130 °C with trace coordination water delivers superior reversible capacity (113.6 mAh g-1), high rate capability (charge to >80% capacity in 3 min), and long cycling stability (only 0.012% fading per cycle), demonstrating its promising prospect in practical applications.

NIR-II Excitable Water-Dispersible Two-Dimensional Conjugated Polymer Nanoplates for In Vivo Two-Photon Luminescence Bioimaging.

While two-dimensional conjugated polymers (2DCPs) have shown great promise in two-photon luminescence (TPL) bioimaging, 2DCP-based TPL imaging agents that can be excited in the second near-infrared window (NIR-II) have rarely been reported so far. Herein, we report two 2DCPs including 2DCP1 and 2DCP2, with octupolar olefin-linked structures for NIR-II-excited bioimaging. The 2DCPs are customized with the fully conjugated donor-acceptor (D-A) linkage and aggregation-induced emission (AIE) active building blocks, leading to good two-photon absorption into the NIR-II window with a 2PACS of ∼64.0 GM per choromophore for both 2DCPs. Moreover, 2DCP1 powders can be exfoliated into water-dispersible nanoplates with a Pluronic F-127 surfactant-assisted temperature-swing method, accompanied by both a drastic reduction of 2PACS throughout the range of 780-1080 nm and a sharp increase of photoluminescence quantum yield to 33.3%. The 2DCP1 nanoplates are subsequently proven to be capable of assisting in visualizing mouse brain vasculatures with a penetration depth of 421 µm and good contrast in vivo, albeit that only 19% of previous 2PACS at 1040 nm is preserved. This work not only provides important insights on how to construct NIR-II excitable 2DCPs for TPL bioimaging but also how to investigate the exfoliation-photophysical property correlation of 2DCPs, which should aid in future research on developing highly efficient TPL bioimaging agents.

Oxygen-deficient WO3-x spheres for electrochemical N2 oxidation to nitrate.

Nitrate synthesis via the electrochemical nitrogen oxidation reaction (e-NOR) is widely recognized as a potential alternative to the energy-intensive Ostwald process. However, electrocatalysts with strong N2 adsorption and activation abilities remain largely undeveloped due to kinetic hindrances caused by the high bond energy of NN. Here we designed a hollow WO3 sphere with an optimal concentration of oxygen vacancies and studied its e-NOR performance. The optimally synthesized oxygen-deficient WO3 (WO3-x) achieved a high nitrate yield of 311.15 µmol h-1gcat.-1 and a Faraday efficiency of 2.00 %, which is probably due to the presence of a moderate amount of oxygen vacancies on the WO3-x surface and the hollow spherical structure, which further improves the accessibility of the inner active surface. Our work could potentially stimulate research into transition metal oxide-based materials for e-NOR applications.

Quantitative Time-Resolved Visualization of Catalytic Degradation Reactions of Environmental Pollutants by Integrating Single-Drop Microextraction and Fluorescence Sensing.

Current methods for evaluating catalytic degradation reactions of environmental pollutants primarily rely on chromatography that often suffers from intermittent analysis, a long turnaround period, and complex sample pretreatment. Herein, we propose a quantitative time-resolved visualization method to evaluate the progress of catalytic degradation reactions by integrating sample pretreatment [single-drop microextraction, (SDME)], fluorescence sensing, and a smartphone detection platform. The dechlorination reaction of chlorobenzene derivatives was first investigated to validate the feasibility of this approach, in which SDME plays a critical role in direct sample pretreatment, and inorganic CsPbBr3 perovskite encapsulated in a metal-organic framework (MOF-5) was utilized as the fluorescent chromogenic agent (FLCA) in SDME to realize fast in situ colorimetric detection via the color switching from green (CsPbBr3) to blue (chlorine lead bromide, inorganic CsPbCl3 perovskite). The smartphone, which can calculate the B/G value of FLCA, serves as a data output window for quantitative time-resolved visualization. Further, a [Eu(PMA)]n (PMA= pyromellitic acid) fluorescent probe was constructed to use as an FLCA for the in situ evaluation of cinnamaldehyde and p-nitrophenol catalytic reduction. This approach not only minimizes the utilization of organic solvents and achieves quantitively efficient time-resolved visualization but also provides a feasible method for in situ monitoring of the progress of catalytic degradation reactions.

Embedding oxophilic rare-earth single atom in platinum nanoclusters for efficient hydrogen electro-oxidation.

Designing Pt-based electrocatalysts with high catalytic activity and CO tolerance is challenging but extremely desirable for alkaline hydrogen oxidation reaction. Herein we report the design of a series of single-atom lanthanide (La, Ce, Pr, Nd, and Lu)-embedded ultrasmall Pt nanoclusters for efficient alkaline hydrogen electro-oxidation catalysis based on vapor filling and spatially confined reduction/growth of metal species. Mechanism studies reveal that oxophilic single-atom lanthanide species in Pt nanoclusters can serve as the Lewis acid site for selective OH- adsorption and regulate the binding strength of intermediates on Pt sites, which promotes the kinetics of hydrogen oxidation and CO oxidation by accelerating the combination of OH- and *H/*CO in kinetics and thermodynamics, endowing the electrocatalyst with up to 14.3-times higher mass activity than commercial Pt/C and enhanced CO tolerance. This work may shed light on the design of metal nanocluster-based electrocatalysts for energy conversion.

Rational Design of Highly Efficient PdIn-In2O3 Interfaces by a Capture-Alloying Strategy for Benzyl Alcohol Partial Oxidation.

Well-dispersed PdIn bimetallic alloy nanoparticles (1-4 nm) were immobilized on mesostructured silica by an in situ capture-alloying strategy, and PdIn-In2O3 interfaces were rationally constructed by changing the In2O3 loading and reduction temperature. The catalytic performance for benzyl alcohol partial oxidation was evaluated, and a catalytic synergy was observed. The Pd-rich PdIn-In2O3 interface is prone to be formed on the catalyst with a low In2O3 loading after being reduced at 300 °C. It was demonstrated that the Pd-rich PdIn-In2O3 interface was more active for benzyl alcohol partial oxidation than In-rich Pd2In3 species, which was likely to be formed at a high reduction temperature (400 °C). The high catalytic activity on the Pd-rich PdIn-In2O3 interface was attributed to the exposure of more Pd-enriched active sites, and an optimized PdIn-In2O3/Pd assemble ratio enhanced the oxygen transfer during partial oxidation. The density functional theory (DFT) calculation confirmed that the Pd-rich Pd3In1(111)-In2O3 interface facilitated the activation of oxygen molecules, resulting in high catalytic activity.

A Static Tin-Manganese Battery with 30000-Cycle Lifespan Based on Stabilized Mn3+/Mn2+ Redox Chemistry.

High-potential Mn3+/Mn2+ redox couple (>1.3 V vs SHE) in a static battery system is rarely reported due to the shuttle and disproportionation of Mn3+ in aqueous solutions. Herein, based on reversible stripping/plating of the Sn anode and stabilized Mn2+/Mn3+ redox couple in the cathode, an aqueous Sn-Mn full battery is established in acidic electrolytes. Sn anode exhibits high deposition efficiency, low polarization, and excellent stability in acidic electrolytes. With the help of H+ and a complexing agent, a reversible conversion between Mn2+ and Mn3+ ions takes place on the graphite surface. Pyrophosphate ligand is initially employed to form a protective layer through a complexation process with Sn4+ on the electrode surface, effectively preventing Mn3+ from disproportionation and hindering the uncontrollable diffusion of Mn3+ to electrolytes. Benefiting from the rational design, the full battery delivers satisfied electrochemical performance including a large capacity (0.45 mAh cm-2 at 5 mA cm-2), high discharge plateau voltage (>1.6 V), excellent rate capability (58% retention from 5 to 30 mA cm-2), and superior cycling stability (no decay after 30 000 cycles). The battery design strategy realizes a robustly stable Mn3+/Mn2+ redox reaction, which broadens research into ultrafast acidic battery systems.

Porous FeF3/MWCNTs composite cathode promoting high performance aluminum storage.

Rechargeable aluminum-ion batteries (RAIBs) attract great attention for stationary energy storage, but there remains a lack of suitable cathode materials for them. Here, a porous iron fluoride/multi wall carbon nanotube (FeF3/MWCNTs) composite as a cathode for RAIBs shows high discharge capacity (180 mA h g-1) and good rate performance, while MWCNTs play crucial roles in improving conductivity and cycle stability. Various characterizations elucidate its conversion-type mechanism, in particular, the Fe3+/Fe2+ conversion exhibits a high operating potential of 1.75 V and discharge capacity of 123 mA h g-1, which is very promising for practical applications.

Ultrafast and Long-Cycle Stable Aluminum Polyphenylene Batteries.

Rechargeable aluminum-ion batteries (RAIBs) are highly sought after due to the extremely high resource reserves and theoretical capacity (2980 mA h/g) of metal aluminum. However, the lack of ideal cathode materials restricts its practical advancement. Here, we report a conductive polymer, polyphenylene, which is produced by the polymerization of molecular benzene as a cathode material for RAIBs with an excellent electrochemical performance. In electrochemical redox, polyphenylene is oxidized and loses electrons to form radical cations [C6H4]3n+ and intercalates with [AlCl4]- anion to achieve electrical neutrality and realize electrochemical energy storage. The stable structure of polyphenylene makes its discharge specific capacity reach 92 mA h/g at 100 mA/g; the discharge plateau is about 1.4 V and exhibits an excellent rate performance and long cycle stability. Under the super high current density of 10 A/g (∼85 C), the charging can be completed in 25 s, and the capacities have almost no decay after 30,000 cycles. Aluminum polyphenylene batteries have the potential to be used as low-cost, easy-to-process, lightweight, and high-capacity superfast rechargeable batteries for large-scale stationary power storage.

A core-shelled Sb@C nanorod cathode with a graphene aerogel interlayer for high-capacity aluminum ion batteries.

Rechargeable aluminum-ion batteries, RAIBs, as a prime candidate for next-generation batteries, have attracted much attention due to their extremely high anode capacity and good safety. However, the lack of matching high-capacity cathode materials and reasonable design limit their practical development. Herein, core-shelled Sb@C nanorods are prepared by polymer coating and thermal reduction as a metal-based cathode for RAIBs. The carbon shell and graphene aerogel interlayer effectively block the diffusion and shuttling of charging products, thus exhibiting excellent electrochemical performance. This Al-Sb battery delivers an initial discharge capacity of 656 mA h g-1 at 100 mA g-1, a stable discharge voltage of 0.9 V, and excellent cycling stability maintained at 306 mA h g-1 after 500 cycles at 1 A g-1. Serial characterizations are used to monitor the structural changes of Sb in reversible reactions and to determine the configuration of the charged products, showing that the product exists in the form of [SbCl4]+ cations, that is, a five-electron transfer reaction occurs with a very high theoretical capacity (1100 mA h g-1). This study sheds light on the energy storage mechanism of a metallic Sb cathode in RAIBs, and provides new insights into the study of high-capacity cathodes and the rational design of battery structures.

MoO3 Nanorods Decorated by PbMoO4 Nanoparticles for Enhanced Trimethylamine Sensing Performances at Low Working Temperature.

The gas sensing performance of metal oxides is limited by the lack of conductivity and sensing activity. Inducing the release of more electrons and activating more chemisorbed oxygen ions to participate in the gas sensing reaction can effectively overcome this limitation. The development of a PbMoO4/MoO3 heterostructure prepared by the addition of Pb2+ ions with MoO3 nanorods is reported for highly sensitive and selective trimethylamine (TMA) detection. The response of the PbMoO4/MoO3 sensor (33.2) to 10 ppm TMA is improved 3-fold compared to the MoO3 sensor (10.7), and the working temperature is reduced from 170 to 133 °C. The enhanced gas sensing performance and mechanism of PbMoO4/MoO3 were demonstrated using the energy band diagram and X-ray photoelectron spectroscopy (XPS) analysis. It is mainly attributed to the following promotion: (1) the induction of Pb2+ ions increases the electron density around the Mo element, enabling the decorated MoO3 to release electrons easily; (2) the formed PbMoO4/MoO3 heterojunction endows a high degree of electron transfer at the interface; (3) the formation of the potential barrier causes the device resistance to decrease significantly upon TMA exposure. Finally, the practicability of the sensor was verified by detecting TMA released from Carassius auratus and shrimp to reflect their freshness.

Surfactant-Modulated a Highly Sensitive Fluorescent Probe of Fully Conjugated Covalent Organic Nanosheets for Detecting Copper Ions in Aqueous Solution.

Efficient detection of aqueous copper ions is of high significance for environmental and human health, since copper is involved in potent redox activity in physiological and pathological processes. Covalent organic frameworks (COFs) have shown advantages in efficient capturing and detecting of copper ions due to their large surface area, robust chemical stability, and high sensitivity, but most of them are hydrophobic, leading to the limitation in sensing copper ions in aqueous media. Herein, the design and synthesis of an sp2 -carbon conjugated COF (sp2 -TPE-COF) are reported with surfactant-assisted water dispersion for detecting traces of copper ions based on the photo-induced electron transfer (PET) mechanism. Importantly, the olefin-linked conjugated backbone of sp2 -TPE-COF works as a signal amplified transducer for metal ion sensing. Notably, it is found that a surfactant-assisted strategy can greatly enhance COF's dispersion in aqueous solution and finely modulate their sensitivity with a significantly improved KSV to 15.15 × 104 m-1 in SDBS (sodium dodecyl benzene sulfonate) solution, the value of which is larger than that of a majority of COF/MOF based sensors for copper ions. This research demonstrates the promise of surfactant modulated fully π-conjugated COFs for sensing applications.

Cu2O induced Au nanochains for highly sensitive dual-mode detection of hydrogen sulfide.

Colorimetric and chemoresistive gas sensing methods have aroused great interest in H2S monitoring due to their unique merits of naked-eye readout, and highly sensitive and rapid detection. However, combining these two methods for gas detection, especially utilizing one material as their common sensing material is a grand challenge because they are inconsistent in sensing mechanism. Taking advantage of the strong chemical affinity of Cu2O for H2S and the excellent performance of localized surface plasmon resonance (LSPR) of Au nanoparticles (NPs) in the visible regions and its ability as a noble metal to enhance gas sensing property, the Cu2O-Au nanochains (NCs) were prepared for dual-mode detection of H2S gas. The Cu2O-Au chemoresistive gas sensor shows a 5-fold higher response than Cu2O sensor at room temperature with a low detection limit of 10 ppb. Such good performance is attributed to the spillover effect and catalytic activity of Au NPs, and the enhanced H2S adsorption after Au loading as revealed by density functional theory calculation. Test strips containing Cu2O-Au produced for gaseous H2S detection show superior color gradient changes (blue, yellow, and brown). Finally, the practicability of the method was validated by real-time monitoring H2S released from cell culture.

Atomic-precision Pt6 nanoclusters for enhanced hydrogen electro-oxidation.

The discord between the insufficient abundance and the excellent electrocatalytic activity of Pt urgently requires its atomic-level engineering for minimal Pt dosage yet maximized electrocatalytic performance. Here we report the design of ultrasmall triphenylphosphine-stabilized Pt6 nanoclusters for electrocatalytic hydrogen oxidation reaction in alkaline solution. Benefiting from the self-optimized ligand effect and atomic-precision structure, the nanocluster electrocatalyst demonstrates a high mass activity, a high stability, and outperforms both Pt single atoms and Pt nanoparticle analogues, uncovering an unexpected size optimization principle for designing Pt electrocatalysts. Moreover, the nanocluster electrocatalyst delivers a high CO-tolerant ability that conventional Pt/C catalyst lacks. Theoretical calculations confirm that the enhanced electrocatalytic performance is attributable to the bifold effects of the triphenylphosphine ligand, which can not only tune the formation of atomically precise platinum nanoclusters, but also shift the d-band center of Pt atoms for favorable adsorption kinetics of *H, *OH, and CO.

Polycyclic Aromatic Hydrocarbons as a New Class of Promising Cathode Materials for Aluminum-Ion Batteries.

As an emerging post-lithium battery technology, aluminum ion batteries (AIBs) have the advantages of large Al reserves and high safety, and have great potential to be applied to power grid energy storage. But current graphite cathode materials are limited in charge storage capacity due to the formation of stage-4 graphite-intercalated compounds (GICs) in the fully charged state. Herein, we propose a new type of cathode materials for AIBs, namely polycyclic aromatic hydrocarbons (PAHs), which resemble graphite in terms of the large conjugated π bond, but do not form GICs in the charge process. Quantum chemistry calculations show that PAHs can bind AlCl4 - through the interaction between the conjugated π bond in the PAHs and AlCl4 - , forming on-plane interactions. The theoretical specific capacity of PAHs is negatively correlated with the number of benzene rings in the PAHs. Then, under the guidance of theoretical calculations, anthracene, a three-ring PAH, was evaluated as a cathode material for AIBs. Electrochemical measurements show that anthracene has a high specific capacity of 157 mAh g-1 (at 100 mA g-1 ) and still maintains a specific capacity of 130 mAh g-1 after 800 cycles. This work provides a feasible "theory guides practice" research model for the development of energy storage materials, and also provides a new class of promising cathode materials for AIBs.

Fatigue Resistant Aerogel/Hydrogel Nanostructured Hybrid for Highly Sensitive and Ultrabroad Pressure Sensing.

Achieving high sensitivity over a broad pressure range remains a great challenge in designing piezoresistive pressure sensors due to the irreconcilable requirements in structural deformability against extremely high pressures and piezoresistive sensitivity to very low pressures. This work proposes a hybrid aerogel/hydrogel sensor by integrating a nanotube structured polypyrrole aerogel with a polyacrylamide (PAAm) hydrogel. The aerogel is composed of durable twined polypyrrole nanotubes fabricated through a sacrificial templating approach. Its electromechanical performance can be regulated by controlling the thickness of the tube shell. A thicker shell enhances the charge mobility between tube walls and thus expedites current responses, making it highly sensitive in detecting low pressure. Moreover, a nucleotide-doped PAAm hydrogel with a reversible noncovalent interaction network is harnessed as the flexible substrate to assemble the aerogel/hydrogel hybrid sensor and overcome sensing saturation under extreme pressures. This highly stretchable and self-healable hybrid polymer sensor exhibits linear response with high sensitivity (Smin  > 1.1 kPa-1 ), ultrabroad sensing range (0.12-≈400 kPa), and stable sensing performance over 10 000 cycles at the pressure of 150 kPa, making it an ideal sensing device to monitor pressures from human physiological signals to significant stress exerted by vehicles.

Compatibility between Activity and Selectivity in Catalytic Oxidation of Benzyl Alcohol with Au-Pd Nanoparticles through Redox Switching of SnOx.

A balance between catalytic activity and product selectivity remains a dilemma for the partial oxidation processes because the products are prone to be overoxidized. In this work, we report on the partial oxidation of benzyl alcohol using a modified catalyst consisting of nanosized Au-Pd particles (NPs) with tin oxide (SnOx) deposited on a mesoporous silica support. We found that the SnOx promotes the autogenous reduction of PdO to active Pd0 species on the Au-Pd NP catalyst (SnOx@AP-ox) before H2 reduction, which is due to the high oxophilicity of Sn. The presence of active Pd0 species and the enhancement of oxygen transfer by SnOx led to high catalytic activity. The benzaldehyde selectivity was enhanced with the increase of SnOx content on catalyst SnOx@AP-ox, which is ascribed to the modulated affinity of reactants and products on the catalyst surface through the redox switching of Sn species. After H2 reduction, SnOx was partially reduced and Au-Pd-Sn alloy was formed. The formation of Au-Pd-Sn alloy weakened both the catalytic synergy of Au-Pd alloy NPs and the adsorption of benzyl alcohol on the reduced catalyst, thus leading to low catalytic activity.