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Developing integrated non-noble metal electrocatalysts with mass activity comparable to noble metal is a significant challenge for overall water splitting. Herein, we constructed an integrated amorphous cobalt phosphoselenide (a-CoPSe) electrode via amorphization and dual anion-mediated strategy, achieving a significant improvement in the electrochemical active surface area (ECSA) and turnover frequency (TOF). The a-CoPSe offers large ECSA (65.9 m2 g−1) and high TOF values of 35.7 s−1 for hydrogen evolution reaction (HER) and 31.9 s−1 for oxygen evolution reaction (OER) at 300 mV. The mass activities of a-CoPSe are 890.4 A g−1 Co for HER at 300 mV and 677.4 A g−1 Co for OER at 250 mV, which are comparable to commercial Pt/C (10014.6 A g−1) and RuO 2 (232.6 A g−1). Theoretical calculation reveals amorphous cobalt with balanced charges regulated by phosphorus and selenium atoms simultaneously facilitate H 2 O* , H* , OH* and OOH* adsorption, which greatly promotes the HER and OER kinetics. [Display omitted] • The a-CoPSe with tunable charge density is prepared by electrodeposition method. • The a-CoPSe offers large ECSA, desirable TOF and excellent EIS during HER and OER. • The a-CoPSe exhibits superior mass activities of alkaline HER and OER. • The a-CoPSe has simultaneous optimized H2O, H, OH and OOH binding energies. [ABSTRACT FROM AUTHOR]

This work compares three catalysts with different spacing of silver-copper(Ⅰ) oxide nanoparticles. When the distance is too large, the CO spillover efficiency will be reduced, and when the distance is too small, non-optimal electronic structure inhibits C–C coupling. Moderate distance can optimize both the spillover and the electronic structure for an effective C–C coupling. [Display omitted] • The effect of catalysts with different silver-copper nanoparticle spacings on tandem-catalyzed CO 2 reduction is firstly investigated. • Appropriate distances can optimize both CO spillover at the silver site and *CO enrichment at the copper site to facilitate C–C coupling. • Faraday efficiency of C 2 products reached 70.7 % for AgCu 2 O S /C at −0.55 V (vs. RHE). • Characterization of intermediates in the reaction process by in situ ATR FT-IR spectroscopy and in situ Raman spectroscopy demonstrates the enhancement of CO spillover as well as C–C coupling. Using renewable electricity to drive the catalytic conversion of CO 2 into C 2 products is an effective measure to combat climate change and mitigate the greenhouse effect. Since electrochemical CO 2 reduction reaction involves multiple proton-electron transfer processes, the selectivity of products especially C 2+ products remain undesirable, because it is difficult to optimize both the CO spillover and the electronic structure for an effective C–C coupling. In this study, by adjusting the distance between silver and copper(Ⅰ) oxide nanoparticles, the CO spillover and the electronic structure of the relay catalyst are optimized simultaneously. Comparing with dissimilar distance, it is found that the relay catalyst with appropriate distance can obtains the best selectivity and activity of the C 2 products in this system, with a Faradaic efficiency of 70.7 % at − 0.55 V (vs. RHE), remarkably, maintaining above 55 % from − 0.35 to − 0.95 V (vs. RHE). In situ infrared/Raman spectroscopy is used to characterize the intermediates during the reaction, proving that the high efficiency of CO spillover and optimized electronic structure together promote C–C coupling, which improves the selectivity of C 2 products. [ABSTRACT FROM AUTHOR]

Hydrogen production from direct alkaline seawater electrolysis at large current density is a key technology for marine energy projects. However, catalyst poisoning due to insoluble precipitation is a key issue that should be addressed. In this work, we used Pt/CNT electrocatalysts modified with molecular metal chalcogenide complexes. During the direct electrolysis of alkaline seawater, the modified Pt/CNT electrocatalyst can effectively reduce the formation of insoluble precipitates on the cathode surface, which is conducive to the stable operation of the hydrogen evolution reaction. Theoretical simulations and in situ experiments both demonstrate that the modified Pt/CNT was affected by the coordination to form coordination compounds, which effectively prevented the formation of insoluble precipitates. The alkaline anion exchange membrane (AEM) electrolyzer with a modified Pt/CNT electrocatalyst exhibited an industrially required current density of 1.0 A cm−2 at 2.0 V and 60 °C, achieving long-term stability in excess of 600 h. [Display omitted] • Pt/CNT electrocatalysts modified with molecular metal chalcogenide complexes. • Modified Pt/CNT can effectively reduce the formation of insoluble precipitates on the cathode surface. • Direct electrolysis of alkaline seawater at high current densities, achieving long-term stability of over 600 h. [ABSTRACT FROM AUTHOR]

Abstract The changes of stress level for the ultra-high strength Al-Zn-Mg-Cu-Zr alloy were described by constitutive equation with considering lattice diffusion of aluminum, zinc, magnesium and copper. Zener–Hollomon (Z) parameter expression based on the constitutive equation with considering lattice diffusion was used to reflect the changes of microstructure. The critical stress σ c for the initiation of dynamic recrystallization (DRX) was introduced to calculate the Z parameter. Steady-state dislocation density ρ sat and critical dislocation density ρ c for the initiation of DRX decreased with the increase of deformation temperature. The dependence of diffusion activation energy Q on temperature and strain rate was given and the effects of deformation conditions on Q were discussed in detail. Microstructural evolution revealed that low angle boundaries (2–5°) created in the process of dynamic recovery (DRV) could convert into subgrain boundary, thus the original grains were divided into subgrains, and then subgrains transformed into DRX grains by the way of progressive rotation. When the Z value was high (ln Z > 30.9), DRV was the main softening mechanism. With the decrease of Z value, both of DRV and DRX played an important roles in softening effect, while with the further decrease of Z value (ln Z < 28.6), DRX became the main softening mechanism. Continuous dynamic recrystallization (CDRX) and discontinuous dynamic recrystallization (DDRX) operated together under the condition of lower Z value, but CDRX was confirmed as the dominant DRX mechanism. Highlights • The dislocation density under different deformation conditions was calculated. • The Z parameter based on the model with considering lattice diffusion was constructed. • The effects of deformation conditions on diffusion activation energy were discussed. • The effects of Z parameter on deformation mechanism were discussed in detail. [ABSTRACT FROM AUTHOR]

Due to the shortage of global freshwater resources and sufficient seawater resources, electrolysis of seawater has become a research hotspot. However, the presence of chloride ions in seawater greatly hinders the development of seawater electrolysis, therefore, constructing catalyst with high catalytic activity and stability against chloride corrosion is essential for seawater electrolysis. In this work, we synthesize F doped FeP and CoP nanosheets with P vacancies (F-FeCoP v @IF) by rapidly molten salt and gas-phase phosphorization strategy, which displays bifunctional activity for HER and OER in alkaline seawater. And the assembled F-FeCoP v @IF needs 1.94 V and 1.62 V to drive 1000 mA cm−2 for overall seawater splitting in alkaline seawater and simulated industrial seawater. And the F-FeCoP v @IF has outstanding long-term durability for over 100 h and nearly 100% FE. DFT calculations reveal that F-doping and P vacancies can synergistically modulate the electronic structure of FeCoP, which enable F-FeCoP v @IF serve as excellent bifunctional electrocatalyst. [Display omitted] • We synthesize F/Fe-CoP v @IF nanosheet by molten salt and gas-phase phosphorization. • F/Fe-CoP v @IF exhibits bifunctional electrocatalytic activity in alkaline seawater. • F/Fe-CoP v @IF needs 1.94 V to drive 1000 mA cm−2 for overall seawater splitting. • F-doping and P vacancy synergistically tune the electronic structure of Fe-CoP. [ABSTRACT FROM AUTHOR]

Novel catalysts of strongly coupled nickel-cobalt nitrides/carbon nanocage (NiCoN/C nanocages) with good water solubility and low cost are utilized to simultaneously catalytically reduce three nitrophenol isomers (2-NP, 3-NP and 4-NP) into corresponding aminophenol (2-AP, 3-AP and 4-AP) within nearly 5 min at room temperature. It is the first report that only one reagent (dopamine) can achieve fast discrimination of three nitrophenol isomers one by one. The reduced product of 3-NP (3-AP) can selectively form fluorescent substance with dopamine with maximum emission wavelength at 465 nm. The reduced product of 4-NP (4-AP) can selectively react with dopamine to form purple solution with absorption peak at 550 nm. It achieves fluorescent detection of 3-NP from 50 nM to 1.2 μM with the limit detections (LOD) of 17 nM for 3-NP, and colorimetric detection of 4-NP from 5 μM to 200 μM with LOD of 1.7 μM. It also realizes nitrophenol detection in tap water. When 0.30, 0.60, 1.00 μM 3-NP and 10, 50, 100 μM 4-NP are added to water samples, recoveries are 98.8–104.6% for 3-NP and 98.8–101.8% for 4-NP. [Display omitted] • Novel water-soluble catalysts of NiCoN/C nanocages to reduce nitrophenol into aminophenol. • Fast fluorescent and colorimetric discrimination of three nitrophenol isomers one by one using dopamine. • Fluorescent detection of 3-NP with LOD of 17 nM and colorimetric detection of 4-NP LOD of 1.7 μM. [ABSTRACT FROM AUTHOR]

Achieving acidic seawater hydrogen production under commercial current densities remains a challenge. We present here a novel strategy through strong metal-support interaction (SMSI) and Pt-p-block alloys (PtM@CNT, M = Ga, In, Pb, and Bi) to construct a stable electronic perturbation and achieve acidic seawater hydrogen evolution performance at commercial current densities for the first time. SMSI stabilizes electronic perturbation and promotes durability up to 360 h. The optimized Pt 61 Ga 39 @CNT exhibits an overpotential of 18 mV at 10 mA cm−2 in 0.5 M H 2 SO 4 and maintains 360 h stability at 500 mA cm−2 in acidic seawater. Density functional theory (DFT) calculation reveals that the optimized d -band center of Pt and ΔG H* increase the catalytic activity, and the higher vacancy formation energy enhances the durability. Overall, this discovery not only first achieves stable acidic seawater hydrogen production under commercial current densities, but also opens a new opportunity to explore catalytic applications of p-block alloys and SMSI stabilized electronic perturbation. [Display omitted] • A stable electronic perturbation was realized through SMSI and Pt-p-block alloys. • This catalyst achieved excellent hydrogen evolution from acidic seawater. • DFT provides evidence for stable electronic perturbation and promote effect. [ABSTRACT FROM AUTHOR]

The Ru, B co-doped cobalt phosphide electrocatalysts were prepared by in situ phase reconstruction method. Thanks to the unique structure and the electronic structure modulation caused by the heteroatom doping, the designed nanomaterials have good electrocatalytic performance in a wide pH range and exhibit good corrosion resistance. [Display omitted] • Electronic structure modulation of porous cobalt phosphide nanosheets through the introduction of Ru and B atoms. • The obtained electrocatalyst achieves excellent catalytic performances toward HER in wide pH range. • The electrolysis cell can be powered by sustainable energy sources, including solar and thermal energies. Developing efficient electrocatalysts to achieve sustainable hydrogen production from electrocatalytic water splitting remains a task of great significance and challenges. Atomic doping is of importance to enhance the performance of electrocatalysts by modulating the local microenvironmental of the designed nanomaterials. Herein, we have developed a porous CoP electrocatalyst with Ru and B atoms co-doping (Ru/B-CoP). Benefiting from the atomic doping and the unique multivacancy nanosheet structure, only 39 mV, 52 mV, and 87 mV are required to achieve 10 mA cm−2 for HER in 0.5 M H 2 SO 4 , 1 M KOH, and 1 M PBS, respectively, and also achieves excellent performance in seawater. It is shown that the introduction of Ru, B in CoP can successfully regulate the electronic structure of the samples and can provide enormous potential in the field of sustainable energy storage and conversion. [ABSTRACT FROM AUTHOR]

Seawater electrolysis is an efficient method for producing carbon-neutral hydrogen; however, it is hindered by high energy cost and chlorine evolution reaction. In this study, we report Ru, P dual-doped NiMoO 4 multichannel nanorods in-situ grown on nickel foam (Ru/P-NiMoO 4 @NF), which can achieve chlorine-free hydrogen production by coupling seawater splitting with thermodynamically favorable urea oxidation. The Ru/P-NiMoO 4 @NF exhibits bifunctional activity with working potentials of 0.23 V to deliver 3000 mA cm−2 for HER and 1.46 V to deliver 1000 mA cm−2 for UOR. The overall urea splitting system in the two-electrode electrolyzer require low voltage of 1.73 V to drive 500 mA cm−2, and demonstrate remarkable durability to keep above 100 mA cm−2 for 145 h. Density functional theory calculations reveal that dual-doping modulate the d -band center of catalyst, thus enhancing the adsorption of reactants and intermediates. This work provides information for designing catalysts for combing seawater splitting with urea purification. [Display omitted] • Ru/P dual-doped NiMoO 4 with multi-channel structure (Ru/P-NiMoO 4 @NF) is obtained. • Ru/P-NiMoO 4 @NF requires 1.73 V to drive 500 mA cm−2 for OUS in alkaline seawater. • Ru/P-NiMoO 4 @NF needs an overpotential of 232 mV to achieve − 3000 mA cm−2 for HER. • Ru/P-NiMoO 4 @NF can degrade urea from 300 to below 100 mg/ml at 150 mA cm−1 in 4 h. • Ru/P doping modulate the d -band center of NiMoO 4 to realize the enhanced activity. [ABSTRACT FROM AUTHOR]

In this work, the ultrathin (0.9 nm) of interstitial metallene with controlled vacancies are successfully prepared for the first time. The interstitial V Pd -PdH 0.41 metallene displays a unique nitrogen reduction (NRR) activity in Li 2 SO 4 solution. [Display omitted] • Ultrathin interstitial metallene with vacancies are obtained for the first time. • TOF of V Pd -PdH 0.41 is 14.97 times than Pd NSs without vacancies. • This catalyst has great stability during the continuous test for 100 h. • In situ Raman/ATR-SEIRAS/DFT display the synergy mechanism for NRR. It is of great significance to controlled synthesis of high activity, selectivity and durable electrocatalysts. In this work, for the first time, the ultrathin (0.9 nm) of interstitial metallene with controlled vacancies and lattice hydrogen atoms are successfully gained. With the optimal lattice hydrogen atoms and composition, the interstitial V Pd -PdH 0.41 metallene exhibits the great nitrogen reduction (NRR) activity in Li 2 SO 4 solution, among interstitial PdH x with different extent of vacancies, interstitial PdH 0.41 without vacancies and Pd nansheets. The density functional theory (DFT), in situ Raman and Attenuated total reflection surface-enhanced infrared absorption spectrum (ATR-SEIRAS) tests further display that the V Pd on the interstitial V Pd -PdH 0.41 metallene can urges the adsorption and arousal of N 2 , while lattice hydrogen atoms as active hydrogen source to follow an association mechanism rather than a dissociation mechanism, showing nice NRR performance at low overpotential. [ABSTRACT FROM AUTHOR]

Integrating thermodynamically favorable hydrazine oxidation reactions (HzOR) with seawater electrolysis will avoid chlorine evolution reaction (ClER) and realize decoupled hydrogen evolution. Herein, the self-supporting Ru-doped FeP 4 nanosheets (Ru-FeP 4 /IF) grown on iron foam are successfully constructed as bifunctional electrocatalysts to facilitate H 2 production and HzOR simultaneously. Benefiting from trace Ru doping tuning the size and chemisorption of FeP 4 , the as-prepared Ru-FeP 4 /IF requires low potential of 318.0 mV and 335.0 mV to drive 1000 mA cm−2 for HER and HzOR in alkaline seawater, respectively. Notably, only an ultralow voltage of 0.90 V is required to reach 1000 mA cm−2 with outstanding long-term stability and 100% Faradaic efficiency when Ru-FeP 4 /IF is assembled in a two-electrode cell for overall hydrazine splitting (OHzS). Density functional theory (DFT) calculations show that Ru-doped modulates electronic structure to optimize adsorption free energy of H* (ΔG H*) for HER and decrease dehydrogenation of *N 2 H 4 to *N 2 H 3 for HzOR on FeP 4. [Display omitted] • We achieved in-situ growth of Ru-doped FeP 4 nanosheets on iron foam. • Trace Ru doping tunes the size and chemisorption of FeP 4. • The Ru-FeP 4 /IF for OHzS requires voltage of 0.90 V to drive 1000 mA cm−2. • DFT calculations show that Ru doping reduces ΔG H* and promotes *N 2 H 4 to *N 2 H 3. [ABSTRACT FROM AUTHOR]

Titanium dioxide (TiO 2) is widely used as a representative transition metal oxides (TMOs) catalyst for electrocatalytic nitrogen reduction reaction (NRR). However, the low stability, low selectivity, low ammonia (NH 3) yield and high overpotential of TiO 2 towards NRR strongly restricted its application in NRR. Here, we firstly add H to the lattice to synthesize a black TiO 2−x with oxygen vacancies (OVs) (B-TiO 1.8) for electrocatalytic NRR. After we optimized the amount of H and OVs, the NH 3 yield and stability can achieve 31.6 μg h−1 mg cat −1 and 100 h at − 0.1 V (vs. RHE), respectively, the faradaic efficiency (FE) can achieve 47.7% at 0 V (vs. RHE). In situ FTIR / ESR / XPS / TPD illustrate that OVs can promote the adsorption and activation of nitrogen (N 2), and lattice H can increase the number of OVs and stabilize them, suppress the hydrogen evolution reaction (HER) and promote the hydrogenation of N 2. [Display omitted] • TiO 2−x with lattice H is synthesized for the first time. • The lattice H can increase the number of OVs, stabilize the OVs. • The lattice H can suppress HER and promote hydrogenation of N 2 process. • In situ FTIR / ESR / XPS / TPD illustrate the synergistic promotion of lattice H and OVs in electrocatalytic NRR. [ABSTRACT FROM AUTHOR]

Powerful, efficient, and corrosion-resistant electrocatalysts are in need to achieve high-current-density neutral seawater hydrogen evolution. Here, a novel strategy through strong metal-support interaction (SMSI) and incorporation of Pt to construct PtNb-Nb 2 O 5 clusters @C was developed with stable high-current-density neutral seawater hydrogen evolution property for the first time. SMSI prevents agglomeration and corrosion of nanomaterials. Pt sites were proposed to play an anabranch role by binding H* to stabilize the Nb valence state and prevent water dissociation incapacitation. The optimized PtNb-Nb 2 O 5 @CC delivers low overpotentials of 440 mV (500 mA cm−2) and 570 mV (1000 mA cm−2) in neutral seawater and has 360 h excellent durability at 500 mA cm−2. In-situ Fourier transform infrared spectroscopy (FTIR), in-situ Raman spectroscopies and theoretical calculations supported the hydrogen evolution reaction (HER) mechanism. PtNb-Nb 2 O 5 heterogeneous interface provided more active sites for water dissociation. OH* adsorbed on Nb sites in stable Nb 2 O 5 , and H* adsorbed on Nb sites and desorbed as H 2 on Pt sites in stable PtNb. Overall, this work not only first achieves stable high-current-density neutral seawater hydrogen evolution property, but also opens a new opportunity to explore SMSI and incorporation of Pt to prevent agglomeration, corrosion, and water dissociation incapacitation for catalytic applications under high current densities. [Display omitted] • A novel strategy through strong metal-support interaction and incorporation of Pt was proposed. • This strategy can prevent agglomeration, corrosion and water dissociation incapacitation. • PtNb-Nb 2 O 5 clusters @C was synthesized by solvent-free microwave method. • Stable high-current-density neutral seawater hydrogen evolution property was achieved. • In-situ characterizations and theoretical calculations demonstrate the reaction mechanism. [ABSTRACT FROM AUTHOR]

A method through SMSI and heterostructure of Pd-M x C@CNT (M = W, Mo and Cr) to construct a stable Lewis acid-base pair was first proposed, showing good EOR activity, stability and C1 selectivity. The Pd-W 2 C@CNT nanomaterials exhibited the highest mass activity (13.9 A mg Pd −1) and C1 selectivity (74.15%). This work not only developed a stable Lewis acid-base pair for electrocatalysis, but the introduction of stable Lewis acid-base pair opened up new ideas for the design of other catalytic reaction catalysts. [Display omitted] • Synthesis of Pd-M x C@CNT material with stable Lewis acid-base pair. • Improving materials stability through stable Lewis acid-base pair and SMSI. • In alkaline EOR the C1 selectivity and mass activity reaches 74.15% and 13.9 A mg Pd −1, respectively. • After 20 000 s i- t test, there is still a mass activity of about 7.1 A mg Pd −1. • After 20 000 cycles of CV, it still retains 89.7% of the initial activity. Pd-based catalysts have been widely studied as electrocatalysts for ethanol oxidation reaction (EOR) because of their higher oxygenophilic properties. However, there are still some disadvantages such as low activity, poor stability and poor selectivity, which hinder the development of EOR. Herein, a method through strong metal-support interaction (SMSI) and heterostructure of Pd-M x C@CNT (M = W, Mo and Cr) to construct a stable Lewis acid-base pair is proposed. Pd-W 2 C@CNT nanomaterial showed the highest mass activity (13.9 A mg Pd −1), C1 selectivity (74.15%) and stability, better than Pd Black (3.5 A mg Pd −1, 7.2%) and Pd@CNT (4.1 A mg Pd −1, 7.6%). Ex situ and in situ electrochemical experiments reveal that the introduction of W 2 C became a stable electron donor for Pd, increasing the electron density of Pd atoms and forming a stable Lewis acidity Pd atoms to weaken the adsorption of intermediates. Reducing the electron density of W 2 C and forming a stable Lewis basicity W 2 C to provide sufficient OH adspecies for the reaction, thereby increasing the selectivity of the C1 pathway. Furthermore, the Pd-M x C@CNT synthesized by this method also exhibited excellent EOR activity, stability and C1 selectivity and glycerol oxidation reaction (GOR) performance. [ABSTRACT FROM AUTHOR]

The synthesis of intermetallic compounds with small size and defective structures is rigorous challenge. In this work, the small size (< 10 nm) of intermetallic PdM (M = Pb, Sn, In) with ordered vacancies (OVs) are successfully prepared by ultrafast and solvent-free microwave method for the first time. With the optimized vacancies, atomic arrangement and components, the intermetallic OVs-Pd 3 Pb-2 shows the best nitrogen reduction (NRR) performance among intermetallic OVs-PdM (M = Sn, In), intermetallic OVs-Pd 3 Pb with various degrees of vacancies, intermetallic Pd 3 Pb with vacancies-free, Pd 3 Pb/CNT and Pd/CNT in Li 2 SO 4 solution. In situ Raman spectroscopy, in situ attenuated total reflectance surface-enhanced infrared absorption spectroscopy (ATR-SEIRAS) technique and density functional theory (DFT) further demonstrate the synergy mechanism of good NRR activity at low overpotentials on OVs-Pd 3 Pb-2 catalysts. In this work, the small size (< 10 nm) of intermetallic PdM (M = Pb, Sn, In) with ordered vacancies (OVs) are gained for the first time. The intermetallic OVs-Pd 3 Pb-2 shows the outstanding electrocatalytic NRR performance. [Display omitted] • Ultrasmall intermetallic PdM with vacancies are gained for the first time. • This catalyst was prepared by solvent-free microwave method. • TOF of OVs-Pd 3 Pb-2 is 12.4 times than Pd 3 Pb without vacancies. • In situ Raman/ATR-SEIRAS/DFT demonstrate the synergy mechanism for NRR. [ABSTRACT FROM AUTHOR]

Rational control of the compositions, morphologies and sizes of electrocatalyst are the key factors for achieving high performance of electrocatalytic reactions. Herein, a newly ultrathin PtRuRhCoNi high-entropy alloy nanowires (HEA-NWs) (~1.6 nm) catalyst is designed. The PtRuRhCoNi NWs/C achieved high mass activity of 7.68 A mg−1 PtRuRh , ultrahigh C1 selectivity of 78% for ethanol oxidation reaction. For hydrogen evolution reaction, the PtRuRhCoNi NWs/C also reached high mass activity, turnover frequency (11.99 A mg−1 PtRuRh , 31.9 s−1, 0.5 M H 2 SO 4 and 8.07 A mg−1 PtRuRh , 26.7 s−1, 1 M KOH at −0.05 V vs. RHE) and stability. Theoretical calculations demonstrated that the excellent electroactivity of HEA is benefited by the self-complementary effect through strong orbital coupling, which maximized the electroactivity towards both oxidation and reduction and preferred binding of key intermediate. The design of pH-universal multifunctional catalyst by rational control of the compositions, morphologies and sizes strategy can facilitate the research of advanced catalysts. [Display omitted] • A newly ultrathin PtRuRhCoNi high-entropy alloy nanowires (~1.6 nm) catalyst is designed. • The PtRuRhCoNi NWs/C reaches 7.68 A mg−1 PtRuRh activity and 78% C1 selectivity for EOR. • The PtRuRhCoNi NWs/C achieves high mass activity, TOF and stability for HER in acidic and alkaline solutions. • DFT shows that the excellent electroactivity of HEA is benefited by the self-complementary effect through strong orbital coupling. [ABSTRACT FROM AUTHOR]

Preparation of low-cost, highly activity and stable bifunctional electrocatalysts for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) in acidic media has great challenges. Here, a series of M-Ru/RuO 2 @CNT (M = Mn, Cd, Cu) bifunctional catalysts were synthesized by doping and strong metal-support interaction (SMSI) strategies to improve the activity and stability of the catalysts. The experiment results show that the optimized Mn–Ru/RuO 2 @CNT catalyst with ultra-small particle size (2.5 nm) has the best catalytic performance, and the OER and HER tests at 10 mA cm−2 in 0.5 M H 2 SO 4 solution show excellent overpotentials of 177 mV and 30 mV respectively, which are better than most of the catalysts reported recently. In addition, current densities of 10 mA cm−2 and 100 mA cm−2 can be obtained at 1.43 V and 1.51 V when measuring water splitting and can last up to 100 h at a current density of 100 mA cm−2. And this is the first time to achieve the stability of acid water splitting of Ru-based catalyst under large current density. Density functional theory (DFT) calculations show that after manganese doping, the electronic structure is changed by charge redistribution between doped ions and ruthenium-based catalysts containing heterojunctions, and the binding energy of intermediates is optimized to improve the catalytic activity; the stability of the catalyst is improved by increasing the formation energy of ruthenium vacancy and preventing the formation of ruthenium vacancy. In this paper, bifunctional Mn–Ru/RuO 2 @CNT catalysts with a particle size of 2.5 nm were successfully prepared, and the long-time stability of Ru-based catalysts in acidic media at high current density was achieved for the first time by doping and strong metal-support interaction strategies. The excellent performance comes from the effective modulation of electrons between the manganese and ruthenium groups and the interaction between the metal particles and the support to produce the excellent performance. [Display omitted] • M-Ru/RuO 2 @CNT catalysts containing Ru/RuO 2 heterojunctions have been synthesized by doping and SMSI strategies. • Mn-Ru/RuO 2 @CNT shows the best HER, OER and overall water splitting (OWS) performance in acidic media. • DFT showed that doping reduces the dissolution of the active site and improves the catalyst performance. [ABSTRACT FROM AUTHOR]

Copper-based catalysts are widely used to adjust the activity and selectivity of CO 2 electroreduction reactions (CO 2 RR). In this article, we choose to use hollow mesoporous carbon spheres (HMCS) to confine and protect Cu clusters to achieve high C 2 selectivity. The electrocatalytic results show that when the amount of Cu clusters confined by HMCS reaches 20% (Cu/HMCS 5 -20%), the selectivity of C 2 products reach 88.7% at − 1.0 V vs. RHE. In situ Fourier transform infrared spectroscopy (FTIRS) shows that Cu clusters confined and protected by HMCS is beneficial to the conversion of *CO to *CHO, while the nanocavities formed by HMCS can effectively confine the in situ formed *CHO carbon intermediates, which facilitates the C-C bond coupling to form C 2 H 4 and C 2 H 5 OH. We proposes a method to improve the C 2 selectivity of CO 2 RR and reduce the amount of Cu in CO 2 RR by using the confinement effect of HMCS. A method is proposed to confine and protect Cu clusters in HMCS while forming a confinement effect nanocavity. The method proposed here to improve the C 2 selectivity of CO 2 RR using copper clusters confined by HMCSs not only protects the Cu clusters but also provides a confinement effect nanocavity that reduces the amount of Cu. [Display omitted] • Nanoconfinement engineering over hollow mesoporous carbon spheres. • Protecting the state of Cu clusters over hollow mesoporous carbon spheres. • Cu/HMCS 5 -20% has a C 2 Faraday efficiency as high as 88.7% for CO 2 RR. • Providing a confinement effect nanocavity that reduces the amount of Cu used. [ABSTRACT FROM AUTHOR]

HEPi/C hybrid nanosheets exhibit excellent HER performance in 0.5 M H 2 SO 4 solution, the overpotential of 40 mV at 10 mA cm−2 is lower than that of commercial Pt/C (η 10 = 48 mV), and has excellent catalytic stability. More interestingly, at an overpotential of 50 mV, the mass activity of the HEPi/C hybrid nanosheets is as high as 1.6 A mg−1 noble metal. [Display omitted] • The first synthesis of high-entropy phosphate/carbon (HEPi/C) hybrid nanosheets. • HEPi/C hybrid nanosheets can be prepared on a large scale. • HEPi/C hybrid nanosheets show excellent HER performance in acidic solutions. It is a huge challenge to develop acidic hydrogen evolution reaction (HER) non-platinum (Pt) catalysts with high activity and excellent stability. In this work, a two-step method was used to synthesize high-entropy phosphate/carbon (HEPi/C) hybrid nanosheets for the first time. First, high-entropy metal–organic framework (HE-MOF) nanosheets were synthesized by an entropy-driven mechanochemical method at room temperature, and then high-temperature phosphating is performed. HEPi/C hybrid nanosheets exhibit excellent HER performance in 0.5 M H 2 SO 4 solution, the overpotential of 40 mV at 10 mA cm−2 is lower than that of commercial Pt/C (η 10 = 48 mV), and has excellent catalytic stability. More interestingly, at an overpotential of 50 mV, the mass activity of the HEPi/C hybrid nanosheets is as high as 1.6 A mg−1 noble metal. This work provides an attractive non-Pt-based material for acidic HER, and also provides a new idea for designing highly efficient and stable hybrid materials composed of high-entropy materials and carbon for electrocatalytic applications. [ABSTRACT FROM AUTHOR]

It is an insurmountable challenge to synthesize carrier-supported ultra-small immiscible alloy catalyst with simple one-step method today. Here, we creatively report the first preparation of immiscible Ru-based alloys (RuRE-rGO NPs, RE=Gd, Er, Yb, La) with ~5 nm by solvent-free microwave reduction. Additionally, in alkaline electrocatalytic hydrogen evolution reaction (HER), RuGd-rGO NPs performed admirable (η = 12 mV at 10 mA cm−2, TOF=30.6 H 2 s−1 at 0.1 V), which also can be stable for 500 h even if it provides industry-related current density of 500 mA cm−2. Density functional theory further indicates that from initial to final state of the reaction, RuGd-rGO NPs have large exothermic energy (−1.34 eV), while the dissociation energy barrier of H 2 O is relatively low, causing the most likely occurrence of HER. This work provides sufficient space for the synthesis of ultra-small immiscible nano-alloy supported catalysts. The general-purpose ultra-small incompatible alloy RuRE-rGO NPs supported by carrier are synthesized by a one-step microwave reduction method with high yield and large-scale preparation, environmentally friendly, economical and low energy consumption, and exhibits excellent industrial-grade alkaline hydrogen evolution performance. [Display omitted] • The first synthesis of carrier-supported super-small incompatible alloy RuRE-rGO. • Solvent-free microwave reduction is simple, large-scale and environmentally friendly. • RuRE-rGO NPs have excellent electrocatalytic performance in alkaline HER. [ABSTRACT FROM AUTHOR]

Precise adjustment of the electronic structure of conductive MOFs load materials plays an important role in the design of electrocatalysts. In this paper, a hydrogen evolution catalyst in the full pH range was prepared by using a rapid microwave method to partially carbonize conductive MOFs materials and quickly anchoring small metal Ru nanoparticles on them. [Display omitted] • Ru@p-Co 3 HHTP 2 is quickly prepared by a microwave solid-phase pyrolysis method. • Partial carbonization and SMSI in microwave improves stability and reactivity. • This catalyst has excellent hydrogen evolution performance in the full pH range. • DFT calculations and experiments revealed the synergy between Ru and p-Co 3 HHTP 2. Conductive metal organic frameworks (MOFs) have limited their long-term development in the actual electrocatalytic test process due to their low activity and poor stability. Here, for the first time, ultra-small Ru nanoparticles supported by a novel conductive MOF material (Co 3 HHTP 2) were synthesized simply and quickly (60 s) using only a household microwave oven. In this process, the conductive MOF is partially carbonized, strong metal carrier interaction (SMSI) is generated, and Ru nanoparticles are firmly attached to the carrier to form Ru@p-Co 3 HHTP 2. The Ru@p-Co 3 HHTP 2 -3.2% catalyst has excellent hydrogen evolution performance in the full pH range. Density functional theory calculations (DFT) result shows that the partial carbonization of the conductive MOF and the presence of SMSI promote the charge transfer at the interface between Ru nanoparticles and Co 3 HHTP 2 , which not only synergistically accelerates the water dissociation step and reduces the hydrogen adsorption energy, but also enhances the stability of the catalyst. [ABSTRACT FROM AUTHOR]

Energy dissipation during the motion of droplet in the microfluidic system depends on the adhesion behaviors between droplet and the micro-channel. However, the "quasi-dynamic" droplet/soft substrate interfacial behaviors during wetting, stretching and separation has not got enough attention. In this paper, the adhesion behaviors between droplet and polydimethylsiloxane (PDMS) film were studied by an adhesion test device and the role of substrate deformation in the adhesion behaviors has been discussed. Results showed that the droplet/PDMS film adhesion force consisted of a snap-in force, a maximum force and a pull-off force. The snap-in force increased with increasing of the elastic modulus of the PDMS film. However, the maximum force and the pull-off force decreased as the elastic modulus of the PDMS film enhanced. Moreover, the snap-in force, the maximum force and the pull-off force increased with increasing of droplet volume and retracting velocity. It is indicated that the interactional behaviors between droplet and soft PDMS during wetting, stretching and separation were closely associated with the adhesion parameters and the elastic modulus of the PDMS film. The findings are helpful to optimizing the mechanical properties of the PDMS micro-channel in the microfluidic system and can further enrich the liquid/solid interfacial adhesion theory. [Display omitted] [ABSTRACT FROM AUTHOR]

[Display omitted] • The incorporation of sulfur and fluorine atoms decreases polyimide mechanical properties. • The wear resistance of FPI and SPI is lower than PI. • The interaction potential energies of SPI and FPI are larger than that of PI due to the polarization of F and S. • The friction and wear almost becomes terrible with the temperature increasing. In order to explore the friction and wear mechanisms of polyimide with metal, this work addressed the tribological properties of the polyimide with different molecular structures in a wide temperature range. It was found that the incorporation of fluorine and sulfur atoms into polyimide had a significant effect on their mechanical and tribological properties. Generally, the wear rates of FPI and SPI are much higher than PI, and FPI displays the worst friction coefficient. To deeper reveal the fundamental reasons, the FTIR, XPS, EDS, SEM characterizations were carried out combined with molecular dynamic simulation. The calculation results from the Molecular Dynamics model between PI and Fe showed that the interaction potential energy of SPI and FPI was larger than that of PI due to the polarization of F and S. Judged from the structures of transfer film, SPI and FPI was easily adhered on the surface of counterpart, even chemical reaction. The XPS analysis further confirmed the possibility of tribo-chemical reactions between SPI/FPI and Fe. This study will provide the theoretical guidance for other polymer molecular design and its tribological research. [ABSTRACT FROM AUTHOR]

Driven by doped Pt atom, the prepared Pt-FeP/C hollow nanorod catalysts successfully solve the rebarbative kinetic problem of insufficient proton-feeding in the NRR process, and the highest NH 3 yield value of 10.22 μg h−1 cm–2 among multitudinous Fe-based catalysts at a low potential of -0.05 V (vs. RHE) is achieved. [Display omitted] • Through an etching and in-situ carbonating process, we have fabricated the FeP-based nanomaterial for NRR for the first time. • The Pt-FeP/C nanorod presents high NH3 productivity of 10.22 μg h−1 cm−2 at −0.05 V (vs. RHE) with ultra-high lifespan. • The DFT calculation and ATR-SEIRAS results verify the reaction path and protons-feeding kinetic process. Following the guidance of nitrogenase, the natural iron-based catalysts with remarkably high activity in nitrogen reduction reaction (NRR) may be a talent option to develop artificial molecular mimics. However, the electrochemical NRR process of iron-based catalysts still suffers from the high overpotential, poor lifespan, and slow reaction kinetics of the hydrogenation process. Through a controllable etching and in-situ carbonating process, a Pt-doped FeP/C hollow nanorod catalysts was fabricated. Driven by the doped Pt atom, the catalyst solves the key kinetic problem about insufficient proton feeding in the process of nitrogen reduction, and actively transfers protons to intermediates of the hydrogenation steps in NRR. Moreover, the as-prepared catalyst presents the highest NH 3 yield value of 10.22 μg h−1 cm−2 among multitudinous Fe based catalysts at lower potential of −0.05 V (vs. RHE) with an excellent Faraday efficiency (FE) of 15.3 %, which is higher than FeP/C without the Pt-driven proton-feeding effect, and the cathodic current density presents no significant change within 50 h. In addition, the density functional theory (DFT) and Attenuated total reflection surface-enhanced infrared absorption spectrum (ATR-SEIRAS) results verify the reaction path and protons-feeding kinetic process. [ABSTRACT FROM AUTHOR]

Fluid-solid interfacial friction and adhesion behaviors play critical roles in microfluidic control systems. In this paper, the responses of fluid-solid interfacial friction force and adhesion force to voltage were studied under electrowetting conditions. Results showed that the fluid-solid interfacial friction force increased two orders of magnitude by voltage in the electrowetting transition region. The responses of friction force and adhesion force to the voltage were almost instantaneous on the time scale. It is indicated that the friction force and adhesion force can be manipulated over a wide range in real-time by voltage. The findings are helpful to provide a method for manipulating the fluid-solid interfacial friction force and adhesion force in real-time using voltage. • The fluid-solid interfacial friction force increased two orders of magnitude by applied voltage. • The fluid-solid interfacial adhesion force increased from 30 μN to 250 μN under applied voltage. • Fluid-solid interfacial friction and adhesion force can be manipulated over a wide range in real-time by voltage. [ABSTRACT FROM AUTHOR]

PdPb nanosponges exhibit the high activity and selectivity for nitrogen reduction reaction electrocatalysis in 0.1 M HCl solution and the NH 3 yield reached 25.68 μg mg−1 cat h−1 (5.14 μg cm−2 h−1) at 0.05 V vs. RHE, corresponding Faraday efficiency was 5.79 %. At the −0.05 V vs. RHE, the NH 3 yield reached the maximum, 37.68 μg mg−1 cat h−1 (7.54 μg cm−2 h−1). • The PdPb nanosponges catalyst material was synthesized for the first time and used for the NRR reaction. • After introducing Pb metal to Pd nanosponges, the NH3 yield reached 25.68 μg mg−1 cat h−1 at 0.05 V vs. RHE (FE 5.79%). • DFT shows that the Pb in PdPb nanosponges can promote the adsorption of N 2 , inhibit *H adsorption. • This strategy can also be applied to other materials such as RuO 2 mamomaterials. Electrochemical N 2 reduction reaction (NRR) under milder conditions has become more and more promising and attractive due to its simplicity, high energy conversion efficiency and no need for expensive agents. But the designed electrocatalysts at ambient conditions are insufficient in activity and Faraday efficiency (FE). Among these electrocatalysts, Pd-based materials are promising NRR electrocatalysts ascribed to they have nitrogen reduction activity at a low overpotential. However, poorly NH 3 yields and FEs of Pd-based nanomaterials are still significant problems. Herein we report PdPb nanosponges that perform effectively electroreduction of N 2 to NH 3 under ambient conditions. It was found Pb element can inhibit the hydrogen evolution reaction (HER) of Pd and enhance NRR performance. According to our experiment, in 0.1 M HCl, the NH 3 yield of PdPb/C was 25.68 μg mg−1 cat h−1 (5.14 μg cm−2 h−1) at 0.05 V vs. RHE, and corresponding FE was 5.79 %, which is one of the most active materials at 0.05 V vs. RHE among the currently reported literature. Further reducing the voltage to more negative (−0.05 V vs. RHE), the NH 3 yield increased to the highest value, 37.68 μg mg−1 cat h−1 (7.54 μg cm−2 h−1), 8 times better than Pd/C (4.8 μg mg−1 cat h−1). Moreover, this catalyst also shows a great stability after 10 h. Besides that, density functional theory (DFT) also corresponds to the experimental results. The introduction of Pb can effectively reduce *H adsorption, inhibit HER, decrease the *NNH generation free energy of NRR process and improve NRR activity. Surprisingly, our ideas can also be extended to other materials such as RuO 2. It provides an excellent channel for the rational design of high-efficiency NRR electrocatalysts at ambient conditions in the future. [ABSTRACT FROM AUTHOR]

The hot deformation behavior of Al-Mg-Si alloy is studied based on diffusion mechanism. The quantity of low angle grain boundaries increases rapidly, accompanied by the formation of subgrains and recrystallization grains with the increase of strain. Dynamic recovery (DRV) and continuous dynamic recrystallization (CDRX) are the main softening mechanisms, of which the DRV is dominant. The kinetics of dynamic recrystallization (DRX) represented by Avrami relationship shows that the DRX volume fraction increases with increasing strain. Physical-based diffusion constitutive model is established to demonstrate the flow behavior of the alloy. The relationship between diffusion activation energy and deformation condition is analyzed, and the dependence of creep exponent on temperature and strain is discussed. The result shows that the model describes the flow stress accurately. Lattice diffusion is the main diffusion mechanism during hot deformation. The variation of creep exponent can be reflected by dislocation density when the deformation mechanism is controlled by dislocation motion. Dynamic precipitation and the impediment of dislocation motion can lead to high value of creep exponent of the alloy. Unlabelled Image • Three types of physical-based diffusion models are established to demonstrate the flow behavior of the alloy. • The main diffusion mechanism during hot deformation is determined by constitutive analyses. • The relationships between creep exponent, diffusion activation energy and deformation condition are discussed. • The microstructure evolution and the dynamic softening mechanisms are investigated during hot deformation. [ABSTRACT FROM AUTHOR]

Achieving rapid anodic oxygen evolution reaction (OER) kinetics and improving the stability of the corresponding ruthenium (Ru)-based catalysts is a current priority for the realisation of industrial water splitting. However, the activity and stability of O 2 evolution in electrocatalysis are largely inhibited by the insufficient adsorption of the reactant H 2 O and too strong adsorption of the intermediate OOH*, as well as by the dissolution of the active site due to excessive oxidation. To solve this challenge, herein, we developed a regulatory strategy combining lanthanide oxides and metal oxidative reconfiguration. The introduction of Eu 2 O 3 effectively promotes the adsorption of H 2 O, optimizes the adsorption energy of OOH*, and reduces the reaction energy barrier of acidic OER process. And the metal oxidation remodeling process exposed more active sites and prevented the peroxidation process. The optimized Ru/Eu 2 O 3 @CNT catalyst showed the highest catalytic activity and stability in acidic OER. Its mass activity was 1219.1 A g Ru -1 and the TOF value reached 4.4 s -1 at 1.48 V. Additionally, Ru/Eu 2 O 3 @CNT after oxidative reconstruction demonstrates the industrially needed current density of 1.0 A cm -2 at 1.71 V in PEM electrolyser, achieving stability in excess of 200 h., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

The sluggish kinetics and inherent instability over the Ru/RuO 2 clusters are still enormous challenges in proton exchange membrane (PEM) water electrolyzer. Herein, we innovatively report synergistic modulation of dynamic electron modification and strong metal-support interaction (SMSI) to activate and stabilize bifunctional fluorine doped Ru/RuO 2 clusters anchored on carbon nanotube (CNT), thus achieving efficient and stable acidic overall water splitting. Theoretical and experimental studies found that surface metal-fluorine modification layer could dynamically regulate the interfacial electronic environment to stabilize and activate multiple active Ru species; and the SMSI between Ru/RuO 2 cluster and CNT maintains stable electronic environment for dynamic electron modification and avoids migrating or shedding of active species in acidic environment. Therefore, the PEM electrolyzer assembled with optimal F 5.5 -Ru/RuO 2 @CNT can operate stably for 100 h at a high current density of 100 mA cm -2 , which is the first time that bifunctional Ru-based nanocatalysts applied to PEM device at a high current density., Competing Interests: Declaration of competing interest The authors declare that they have no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (Copyright © 2024 Elsevier Inc. All rights reserved.)

Glycerol electrooxidation reaction (GOR) to produce value-added chemicals, such as formic acid, could make more efficient use of abundant glycerol and meet future demand for formic acid as a fuel for direct or indirect formic acid fuel cells. Non-noble metal Cu-based catalysts have great potential in electro-reforming glycerol to formic acid. However, the high activity, selectivity and stability of Cu based catalysts in GOR cannot be achieved simultaneously. Here, we used ozone-assisted electrocatalyst to convert glycerol to formic acid under alkaline conditions, the onset potential was reduced by 60 mV, the Faraday efficiency (FE) reached 95 %. The catalyst has excellent stability within 300 h at the current density of 10 mA cm -2 . The electron spin resonance proved that ozone produced superoxide anion during the GOR. In situ Raman spectroscopy, electrochemical studies showed that glycerol can be activated with ozone in GOR, and the C-C bond can be broken to reduce the polymerization of glycerol on the catalyst surface, so as to produce more formic acid at a lower voltage. Moreover, the removal of dissolved O 3 from water can be up to 100 % after 30 minutes of GOR reaction at a solubility of 50 mg L -1 as measured by UV-VIS spectrophotometry., (© 2024 Wiley-VCH GmbH.)

The synthesis of nitrate by the electrochemical N 2 oxidation reaction (NOR) is currently one of the most promising routes. However, the traditional generation of nitrate depends on the oxidation reaction between N 2 and H 2 O (or ·OH), which involves complex reaction steps and intermediates, showing strong competition from oxygen evolution reaction (OER). Here, an effective NOR method is proposed to directly oxidize N 2 by using O 3 as a reactive oxygen source to reduce the reaction step. Electrochemical tests demonstrate that the nitrate yield of Pd-Mn 3 O 4 /CNT electrocatalyst reaches the milligram level, which is the highest yield reported so far for electrocatalytic NOR. Quantitative characterization is employed to establish a comprehensive set of benchmarks to confirm the intrinsic nature of nitrogen activation and test the O 3 -mediated reaction mechanism. Density functional theory (DFT) calculations show that the heterostructure Pd-Mn 3 O 4 leads to a strong adsorption preference for N 2 and O 3 , which greatly reduces the activation energy barrier for N 2 . This accelerates the synthesis of nitrate based on the direct formation mechanism, which reduces energy barriers and the reaction steps, thus increasing the performance of electrocatalytic nitrate production. The techno-economic analysis underscores the promising feasibility and sustainable economic value of the presented method., (© 2024 Wiley‐VCH GmbH.)

High entropy materials offer almost unlimited catalytic possibilities due to their variable composition, unique structure, and excellent electrocatalytic performance. However, due to the strong tendency of nanoparticles to coarsen and agglomerate, it is still a challenge to synthesize nanoparticles using simple methods to precisely control the morphology and size of the nanoparticles in large quantities, and their large-scale application is limited by high costs and low yields. Herein, a series of high-entropy oxides (HEOs) nanoparticles with high-density and ultrasmall size (<5 nm) loaded on carbon nanosheets with large quantities are prepared by Joule-heating treatment of gel precursors in a short period of time (≈60 s). Among them, the prepared (FeCoNiRuMn) 3 O 4-x catalyst shows the best electrocatalytic activity for oxygen evolution reaction, with low overpotentials (230 mV @10 mA cm -2 , 270 mV @100 mA cm -2 ), small Tafel slope (39.4 mV dec -1 ), and excellent stability without significant decay at 100 mA cm -2 after 100 h. The excellent performance of (FeCoNiRuMn) 3 O 4-x can be attributed to the synergistic effect of multiple elements and the inherent structural stability of high entropy systems. This study provides a more comprehensive design idea for the preparation of efficient and stable high entropy catalysts., (© 2024 Wiley‐VCH GmbH.)

Non-alcoholic fatty liver disease (NAFLD) is increasingly recognized for its global prevalence and potential progression to more severe liver diseases such as non-alcoholic steatohepatitis (NASH). The gut microbiota plays a pivotal role in the pathogenesis of NAFLD, yet the detailed characteristics and ecological alterations of gut microbial communities during the progression from non-alcoholic fatty liver (NAFL) to NASH remain poorly understood. Methods: In this study, we conducted a comparative analysis of gut microbiota composition in individuals with NAFL and NASH to elucidate differences and characteristics. We utilized 16S rRNA sequencing to compare the intestinal gut microbiota among a healthy control group (65 cases), NAFL group (64 cases), and NASH group (53 cases). Random forest machine learning and database validation methods were employed to analyze the data. Results: Our findings indicate a significant decrease in the diversity of intestinal flora during the progression of NAFLD ( p  < 0.05). At the phylum level, high abundances of Bacteroidetes and Fusobacteria were observed in both NAFL and NASH patients, whereas Firmicutes were less abundant. At the genus level, a significant decrease in Prevotella expression was seen in the NAFL group (AUC 0.738), whereas an increase in the combination of Megamonas and Fusobacterium was noted in the NASH group (AUC 0.769). Furthermore, KEGG pathway analysis highlighted significant disturbances in various types of glucose metabolism pathways in the NASH group compared to the NAFL group, as well as notably compromised flavonoid and flavonol biosynthesis functions. The study uncovers distinct microbiota characteristics and microecological changes within the gut during the transition from NAFL to NASH, providing insights that could facilitate the discovery of novel biomarkers and therapeutic targets for NAFLD., Competing Interests: The authors declare that the research was conducted in the absence of any commercial or financial relationships that could be construed as a potential conflict of interest., (Copyright © 2024 Huang, Lyu, Xie, Li, Xing, Han, Lai, Ma, Zou, Zeng, Xu, Gao, Luo, Bolund, Tong and Fengping.)

The present work investigated the effect of destabilization time on the mechanical properties and microstructure evolution of high chromium cast iron, and scanning electron microscopy and electron probe microanalysis techniques were employed. The results show that the hardness of hypoeutectic high chromium cast iron is related to the size and volume fraction of secondary carbides precipitated from the matrix. The hardness of the alloy continues to rise due to the continuous increase of the volume fraction of the secondary carbide at the initial stage of destabilization. The alloy reaches its peak hardness value at 950 °C and 1000 °C for 1 hour holding time. The solid solubility of carbon and alloying elements in the matrix increases as the holding time extends, resulting in a large number of carbides redissolved into the matrix, making the hardness of the alloy decrease; the hardness of the alloy at 14 h is less than that at 10 min. Under 1050 °C, the size and density of the secondary carbide increase significantly; extending the holding time will lead to the continuous reduction of the carbide rod that provides strength, thus, the hardness curve shows a downward trend., Competing Interests: The authors declare no known competing financial interests or personal relationships that could have appeared to influence the work reported in this paper., (This journal is © The Royal Society of Chemistry.)

Developing highly active and stable acidic hydrogen evolution catalysts is of great significance and challenge for the long-term operation of commercial proton exchange membrane (PEM) electrolyzers. In this work, coplanar ultrathin nanosheets composed of rich-Frank partial dislocations (FPDs) are first synthesized. Ir nanoparticles and carbon (Dr-Ir/C NSs) use a nonequilibrium high-temperature thermal shock method (>1200 °C) and KBr template-assisted techniques. Dr-Ir/C NSs exhibit excellent hydrogen evolution reaction (HER) performance with a remarkably high mass activity of 6.64 A mg -1 at 50 mV, which is among the best Ir-based catalysts.In addition, Dr-Ir/C NSs are able to operate stably at 1.0 A cm -2 for 200 h as a cathode in a PEM electrolyser, and the original coplanar ultrathin nanosheets structure are maintained after the test, demonstrating excellent stability against stacking and agglomeration. Geometrical phase analysis and theoretical calculations show that the FPDs produce a 4% compressive strain in the Dr-Ir/C NSs, and the compressive strain weaken the adsorption of H* by Ir, thus increasing the intrinsic activity of the catalyst., (© 2023 Wiley-VCH GmbH.)

Under the high current density, the excessive strong adsorption of H* intermediates and H 2 accumulation the catalysts are the major obstacle to the industrial application of hydrogen evolation reaction (HER) catalysts. Herein, through experimental exploration, it is found that the superaerophobic Nitrogen (N)-doped carbon material can promote the rapid release of H 2 and provide H* desorption site for the hydrogen spillover process, which makes it have great potential as the catalysts support for hydrogen spillover. Based on this discovery, this work develops the hydrogen spillover catalyst with electron-rich Pt sites loaded on N-doped carbon nanocage (N-CNC) with adjustable work function. Through a series of comprehensive electrochemical tests, the existence of hydrogen spillover effort has been proved. Moreover, the in situ tests showed that pyrrolic-N can activate adjacent carbon sites as the desorption sites for hydrogen spillover. The Pt@N-1-CNC with the minimum work function difference (ΔΦ) between Pt NPs and support shows superior hydrogen evolution performance, only needs overpotential of 12.2 mV to reach current density of 10 mA cm -2 , outstanding turnover frequency (TOF) (44.7 s -1 @100 mV) and superior durability under the 360 h durability tests at current density of 50 mA cm -2 ., (© 2023 Wiley-VCH GmbH.)

Recently, hydrogen spillover based binary (HSBB) catalysts have received widespread attention due to the sufficiently utilized reaction sites. However, the specific regulation mechanism of spillover intensity is still unclear. Herein, we have fabricated oxygen vacancies enriched Ru/NiMoO 4-x to investigate the internal relationship between electron supply and mechanism of hydrogen spillover enhancement. The DFT calculations cooperate with in situ Raman spectrum to uncover that the H* spillover from NiMoO 4-x to Ru. Meanwhile, oxygen vacancies weakened the electron supply from Ru to NiMoO 4-x , which contributes to dilute the resistance of built-in electric field (BEF) for hydrogen spillover. In addition, the higher ion concentration in electrolyte will promote the H* adsorption step obviously, which is demonstrated by in situ EIS tests. As a result, the Ru/NiMoO 4-x exhibits a low overpotential of 206 mV at 3.0 A cm -2 , a small Tafel slope of 28.8 mV dec -1 , and an excellent durability of 550 h at the current density of 0.5 A cm -2 for HER in 1.0 M KOH seawater., (© 2023 Wiley-VCH GmbH.)

Complete ethanol oxidation reaction (EOR) in C1 pathway with 12 transferred electrons is highly desirable yet challenging in direct ethanol fuel cells. Herein, PtRh jagged nanowires synthesized via a simple wet-chemical approach exhibit exceptional EOR mass activity of 1.63 A mgPt -1 and specific activity of 4.07 mA cm -2 , 3.62-fold and 4.28-folds increments relative to Pt/C, respectively. High proportions of 69.33% and 73.42% of initial activity are also retained after chronoamperometric test (80 000 s) and 1500 consecutive potential cycles, respectively. More importantly, it is found that PtRh jagged nanowires possess superb anti-CO poisoning capability. Combining X-ray absorption spectroscopy, X-ray photoelectron spectroscopy as well as density functional theory calculations unveil that the remarkable catalytic activity and CO tolerance stem from both the Rh-induced electronic effect and geometric effect (manifested by shortened Pt─Pt bond length and shrinkage of lattice constants), which facilitates EOR catalysis in C1 pathway and improves reaction kinetics by reducing energy barriers of rate-determining steps (such as *CO → *COOH). The C1 pathway efficiency of PtRh jagged nanowires is further verified by the high intensity of CO 2 relative to CH 3 COOH/CH 3 CHO in infrared reflection absorption spectroscopy., (© 2023 Wiley-VCH GmbH.)

Exploring a simple, fast, solvent-free synthetic method for large-scale preparation of cheap, highly active electrocatalysts for industrial hydrogen evolution reaction is one of the most promising work today. In this work, a simple, fast and solvent-free microwave pyrolysis method is used to synthesize ultra-small (3.5 nm) Ru-Mo 2 C@CNT catalyst with heterogeneous structure and strong metal-support interaction in one step. The Ru-Mo 2 C@CNT catalyst only exhibits an overpotential of 15 mV at a current density of 10 mA cm -2 , and exhibits a large turnover frequency value up to 21.9 s -1 under an overpotential of 100 mV in 1.0 M KOH. In addition, this catalyst can reach high current densities of 500 mA cm -2 and 1000 mA cm -2 at low overpotentials of 56 mV and 78 mV respectively, and it displays high stability of 1000 h. This work provides a feasible way for the reasonable design of other large-scale production catalysts.

Despite its very high capacity (4200 mAh g -1 ), the widespread application of the silicon anode is still hampered by severe volume changes (up to 300%) during cycling, which results in electrical contact loss and thus dramatic capacity fading with poor cycle life. To address this challenge, 3D advanced Mxene/Si-based superstructures including MXene matrix, silicon, SiO x layer, and nitrogen-doped carbon (MXene/Si@SiO x @C) in a layer-by-layer manner were rationally designed and fabricated for boosting lithium-ion batteries (LIBs). The MXene/Si@SiO x @C anode takes the advantages of high Li + ion capacity offered by Si, mechanical stability by the synergistic effect of SiO x , MXene, and N-doped carbon coating, and excellent structural stability by forming a strong Ti-N bond among the layers. Such an interesting superstructure boosts the lithium storage performance (390 mAh g -1 with 99.9% Coulombic efficiency and 76.4% capacity retention after 1000 cycles at 10 C) and effectively suppresses electrode swelling only to 12% with no noticeable fracture or pulverization after long-term cycling. Furthermore, a soft package full LIB with MXene/Si@SiO x @C anode and Li[Ni 0.6 Co 0.2 Mn 0.2 ]O 2 (NCM622) cathode was demonstrated, which delivers a stable capacity of 171 mAh g -1 at 0.2 C, a promising energy density of 485 Wh kg -1 based on positive active material, as well as good cycling stability for 200 cycles even after bending. The present MXene/Si@SiO x @C becomes among the best Si-based anode materials for LIBs.

Inspired by natural photosynthesis, the design of new Z-scheme photocatalytic systems is very promising for boosting the photocatalytic performance of H 2 production and CO 2 reduction; however, until now, the direct synthesis of efficient Z-scheme photocatalysts remains a grand challenge. Herein, it is demonstrated that an interesting Z-scheme photocatalyst can be constructed by coupling In 2 O 3 and ZnIn 2 Se 4 semiconductors based on theoretical calculations. Experimentally, a class of ultrathin In 2 O 3 -ZnIn 2 Se 4 (denoted as In 2 O 3 -ZISe) spontaneous Z-scheme nanosheet photocatalysts for greatly enhancing photocatalytic H 2 production is made. Furthermore, Mo atoms are incorporated in the Z-scheme In 2 O 3 -ZISe nanosheet photocatalyst by forming the MoSe bond, confirmed by X-ray photoelectron spectroscopy, in which the formed MoSe 2 works as cocatalyst of the Z-scheme photocatalyst. As a consequence, such a unique structure of In 2 O 3 -ZISe-Mo makes it exhibit 21.7 and 232.6 times higher photocatalytic H 2 evolution activity than those of In 2 O 3 -ZnIn 2 Se 4 and In 2 O 3 nanosheets, respectively. Moreover, In 2 O 3 -ZISe-Mo is also very stable for photocatalytic H 2 production by showing almost no activity decay for 16 h test. Ultraviolet-visible diffuse reflectance spectra, photoluminescence spectroscopy, transient photocurrent spectra, and electrochemical impedance spectroscopy reveal that the enhanced photocatalytic performance of In 2 O 3 -ZISe-Mo is mainly attributed to its widened photoresponse range and effective carrier separation because of its special structure., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Objectives: Dopaminergic signaling in the basolateral amygdala (BLA) is important for emotion-related activity. However, little is known about the influence of dopamine (DA) on excitatory synaptic transmission of pyramidal neurons in BLA at early developmental stage. Here in this study, we observed the effect of DA on excitatory neurotransmission in the pyramidal cells of BLA in acute slices., Methods: Acute slices from amygdala of rats at the age of 14-16 days were prepared and maintained in vitro using standard method. Whole-cell patch clamp recordings were performed to examine the evoked excitatory postsynaptic current (eEPSC), spontaneous excitatory postsynaptic current (sEPSC) and miniature excitatory postsynaptic current (mEPSC). Drugs including DA and synaptic blockers were added in recording solution due to different experimental designs., Results: We found that bath application of DA at a concentration of 100 μM significantly inhibited the amplitude of evoked EPSC. However, the amplitude and frequency of mEPSC were not affected. We also found increased pair pulse facilitation after DA application, indicating DA inhibited excitatory neurotransmission through suppression of release probability at the pre-synaptic terminals. Importantly, DA was also effective in decreasing activity induced upregulation in sEPSCs. Moreover, the DA effects were not affected by either antagonist of dopamine 1 or dopamine 2-like receptors., Conclusion: We studied the effects of DA on excitatory neurotransmission and found that DA inhibited glutamatergic synaptic transmission via modulation of pre-synaptic release probability.

Opioids and the neuropeptide substance P (SP) modulate the expression of inflammatory cytokines and chemokines, which are under the control of nuclear factor kappaB (NF-kappaB). We investigated whether the neurokinin-1 receptor (SP receptor) pathway is biologically involved in morphine-mediated modulation of NF-kappaB promoter activation in a human neuronal cell line (NT2-N) that expresses both the mu-opioid receptor (MOR) and the SP receptor. Morphine significantly enhanced NF-kappaB promoter-directed luciferase activity in NT2-N neurons. DAMGO, a selective mu-opioid receptor agonist, also induced NF-kappaB promoter activation. The induced activation of NF-kappaB promoter by morphine or DAMGO was abolished not only by naltrexone (a opioid receptor antagonist) and CTAP (a selective, competitive mu-opioid receptor antagonist), but also by CP-96,345, a non-peptide SP receptor antagonist. Investigation of the mechanism responsible for morphine-induced activation of NF-kappaB promoter in NT2-N neurons demonstrated that morphine activates the SP promoter and induces SP expression in these cells. We also observed that SP activated NF-kappaB promoter and that CP-96,345 downregulated the expression of endogenous SP. Furthermore, dual immunofluorescent labeling revealed that there is co-expression of NK-1R and MOR in the processes of NT-2N neurons. These results suggest that morphine, by activating MOR, engages a positive feedback loop between NK-1R and SP. Activation of NK-1R could then impact NF-kappaB expression and therefore may be an important participant in the effect of morphine on immune responses in the central nervous system., (Copyright 2003 Wiley-Liss, Inc.)

Substance P (SP), the most extensively studied and potent member of the tachykinin family, is a major modulator of inflammation and immunomodulatory activities within the central and peripheral nervous systems. We have examined the gene expression of SP and its receptor in a human neuronal cell line (NT2-N). Using reverse transcribed polymerase chain reaction (RT-PCR), the four isoforms of preprotachykinin-A gene transcripts (alpha, beta, gamma, and delta) were detected in the NT2-N. We also identified the presence of mRNA for neurokinin-1 receptor (NK-1R), a primary receptor for SP, in the NT2-N cells. Concomitant with NT2 cell differentiation into neurons, SP and NK-1R mRNA expression increased consistently. Intracellular SP and cell membrane NK-1R immunoreactivity were all observed in NT2-N cells. Most importantly, we demonstrated that SP and NK-1R presented in NT2-N cells are functionally involved in the regulation of macrophage inflammatory protein 1 beta (MIP-1beta), an important beta-chemokine participating in the activation and directional migration of immune cells to sites of central nervous systems (CNS) inflammation. Thus, SP and its receptor may play an important role in modulation of neuronal functions related to regulation of immune activities within the CNS. The NT2-N cell line is well suited for in vitro investigations of the SP-NK-1R pathway in immune responses and inflammation in the CNS., (Copyright 2002 Wiley-Liss, Inc.)