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• A novel high-entropy electrocatalyst Ni 3 ZnC 0.7 @CoNiCuFe–NC has been fabricated. • Synergistic effect of multimetal, N, and C species improves catalytic activity. • This material exhibits outstanding catalytic performance for over water splitting. Due to unique electrical properties and high catalytic efficiency, transition metal nitrogen-codoped carbide (TM–N–C) has attracted tremendous interest as a multifunctional electrocatalyst for water splitting. Unlike traditional single-source modification, herein a novel pomegranate-like high-entropy (HE) electrocatalyst of Ni 3 ZnC 0.7 decorated with homogeneous multimetal (Fe, Co, Cu, and Ni) nitrogen-codoped carbon matrix (Ni 3 ZnC 0.7 @CoNiCuFe–NC) is reported. It can be implemented by the simple thermal annealing method of multimetal codoped zeolitic imidazolate framework (ZIF). Benefiting from the synergistic effects of plentiful TM–N–C species, template effect of ZIF and distinct nanoporous structure, HE electrocatalyst Ni 3 ZnC 0.7 @CoNiCuFe–NC exhibits outstanding electrocatalytic performance. When applied in strong alkaline electrolyte (1.0 M KOH), the overpotentials of Ni 3 ZnC 0.7 @CoNiCuFe–NC present as low as 202 and 97 mV for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) at 10 mA cm−2 current density. Surprisingly as a bifunctional electrode, it can achieve the low cell voltage of 1.53 V at 10 mA cm−2 current density for overall water splitting, which is comparable to conventional IrO 2 ||Pt/C electrode and superior to the recently reported analogous bifunctional catalysts. Thus, the work proposes the direction for the rational design of homogeneous distribution of TM–N–C material for water splitting in the green hydrogen energy industry. [ABSTRACT FROM AUTHOR]

In linguistics, the uncertainty of context due to polysemy is widespread, which attracts much attention. Quantum-inspired complex word embedding based on Hilbert space plays an important role in natural language processing (NLP), which fully leverages the similarity between quantum states and word tokens. A word containing multiple meanings could correspond to a single quantum particle which may exist in several possible states, and a sentence could be analogous to the quantum system where particles interfere with each other. Motivated by quantum-inspired complex word embedding, interpretable complex-valued word embedding (ICWE) is proposed to design two end-to-end quantum-inspired deep neural networks (ICWE-QNN and CICWE-QNN representing convolutional complex-valued neural network based on ICWE) for binary text classification. They have the proven feasibility and effectiveness in the application of NLP and can solve the problem of text information loss in CE-Mix [1] model caused by neglecting the important linguistic features of text, since linguistic feature extraction is presented in our model with deep learning algorithms, in which gated recurrent unit (GRU) extracts the sequence information of sentences, attention mechanism makes the model focus on important words in sentences and convolutional layer captures the local features of projected matrix. The model ICWE-QNN can avoid random combination of word tokens and CICWE-QNN fully considers textual features of the projected matrix. Experiments conducted on five benchmarking classification datasets demonstrate our proposed models have higher accuracy than the compared traditional models including CaptionRep BOW, DictRep BOW and Paragram-Phrase, and they also have great performance on F1-score. Eespecially, CICWE-QNN model has higher accuracy than the quantum-inspired model CE-Mix as well for four datasets including SST, SUBJ, CR and MPQA. It is a meaningful and effictive exploration to design quantum-inspired deep neural networks to promote the performance of text classification.

Rechargeable Zn–air batteries have received extensive attention due to their use of nontoxic materials, safety, and high energy density. However, the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) at the air electrode of Zn–air batteries both suffer from slow kinetics, limiting their commercialization development. Herein, we prepared Co, N, and S co-doped hollow carbon nanoboxes (Co–N/S-CNBs) rich in topological defects using polyphenylene sulfide (PPS) as a sulfur-rich carbon source. Critically, by utilizing the self-propagating high-temperature synthesis (SHS), PPS can avoid melting, while simultaneously enabling the catalyst to take on a unique hollow structure. Additional post-treatment to introduce Co and N atoms as active centers further increases the defect sites and microporous structures of the catalyst. Under alkaline electrolytes, the Co–N/S-CNBs enabled Zn–air batteries to exhibit excellent bifunctional catalytic activity for both ORR and OER, surpassing commercial catalysts. Chemical analysis showed that the cracking loss of small molecules from PPS during pyrolysis is the main reason for the formation of topological defects, where the defect sites act as active centers to enhance the catalytic performance. Overall, this work provides new insights into the mechanism of how defects are formed in such a catalyst, as well as shows how a high-performance bifunctional electrocatalyst can be utilized for practical Zn–air batteries.

Developing high-performance non-noble metal bifunctional oxygen reduction and evolution reaction electrocatalysts is a critical factor for the commercialization of rechargeable Zn–air batteries. Herein, Co/Co–N/Co–O rooted on reduced graphene oxide (rGO) hybrid boron and nitrogen codoped carbon (BCN) nanotube arrays (BCN/rGO-Co) is prepared by facile low-temperature precross-linking and high-temperature pyrolysis treatment. Benefit from the synergistic effect of its B/N codoping, Co/Co–N/Co–O bifunctional active sites, 3D hybrid porous structure of BCN nanotubes, and highly conductive rGO sheets. The obtained BCN/rGO-Co exhibits superior bifunctional oxygen catalytic activity with a positive ORR half-wave potential (0.85 V) and a low OER potential (1.61 V) at 10 mA cm–2. Additionally, the BCN/rGO-Co-based liquid Zn–air batteries displays a large peak power density of 157 mW cm–2, and a long charge/discharge cycle stability of 200 h, outdoing the commercial Pt/C+Ru/C catalyst.

The cleanup of oily wastewater and crude-oil spills is a global challenge. Traditional membrane materials are inefficient for oil/water separation under harsh conditions and limited by sorption speeds because of the high viscosity of crude oil. Herein, a kind of Graphene-wrapped polyphenylene sulfide fibrous membrane with superior chemical resistance and hydrophobicity for efficient oil/water separation and fast adsorption of crude oil all-weather is reported. The reduced graphene oxide (rGO)@polyphenylene sulfide (PPS) fibrous membrane can be applied in the various harsh conditions with Joule heating and solar heating. In addition, the oil(dichloromethane)/water separation flux of rGO@PPS reached 12 903 L m–2h–1, and the separation efficiency reached 99.99%. After 10 cycles, the rGO@PPS still performed high separation flux and filtration efficiency. More importantly, the rGO@PPS still retained its high conductivity, excellent filtration efficiency, and stable hydrophobicity after acid or alkali treatment. Moreover, the rGO@PPS can be heated by solar energy to absorb viscous crude oil during the day, while at night, the crude oil can be adsorbed by Joule heating. The time to adsorb crude oil can be reduced by 98.6% and 97.3% through Joule heating and solar heating, respectively. This all-weather utilization greatly increases the adsorption efficiency and effectively reduces energy consumption.

As cathode in the aqueous Zn ion battery, NaV6O15in the NaV6O15/V2O5can endow the battery with high rate performance and cycle stability, and heterojunction structure can provide vacancy for Zn2+storage and transport.

Hollow oxygen deficiency-enriched NiFe2O4@N/rGO serves as highly efficient bifunctional electrocatalysts for overall water splitting. The resultant NiFe2O4@N/rGO-800 exhibits excellent overall water splitting performance and good long-term stability.

In this paper, numerical investigation of hypersonic gas flow over two typical gap-cavity structures is carried out using all-speed preconditioned density-based solver. Such structures filled with porous seal in the gap are often present at the joint locations of control surfaces of the hypersonic vehicles. Single-domain approach is adopted to integrate the governing equations for both porous and fluid regions. The basic thermal invasion characteristic is first illustrated using the maze gap-cavity structure without sealing. Then, the influence of seal filling depth on the thermal invasion characteristic is investigated for the structure with sealing. Finally, a comparison of thermal invasion characteristics between maze and straight gap-cavity structures is performed to examine the influence of gap bending. Results show that the main source of hot airflow invading into the gap is from the millimeter scale gas layer within the boundary layer. And the invasion characteristic presents approximate stationary behavior. A primary vortex occurs in the gap adjacent to the leeward wall, which is ascribed to the impinging effect between the separate boundary flow and the windward wall. This effect is also the main driving force of thermal invasion. A treatment of filling the seal in certain depth inside the gap can significantly reduce the thermal load of seal and maintain an acceptable level of the invading mass flow rate. Additionally, it is found that the gap bending exerts a limited block effect on the thermal invasion without sealing, and this effect can be ignored with sealing. These results can provide a reference for optimizing the seal gap-cavity structure configuration.

In this study, we aimed to investigate the therapeutic effect of miR-21 in the treatment of spinal cord injury (SCI) as well as its underlying molecular mechanisms. Real-time PCR and western blot were performed to measure the expression of miR-21, PTEN, and PDCD4 in SCI rats. Locomotion recovery assessment, Nissl staining, IHC assay, and TUNEL assay were utilized to observe the therapeutic effect of miR-21 in the treatment of SCI. Bioinformatics analysis and luciferase assay were conducted to establish the signaling pathway of miR-21, PTEN, and PDCD4. The regulatory relationships between miR-21 and PTEN/PDCD4 were further validated by real-time PCR, western blot, MTT assay, and flow cytometry. Compared with sham-operated rats, SCI rats showed decreased expression of miR-21 along with increased expression of PTEN/PDCD4. Exosomes were equally distributed in MSCs transfected with miR-21, PTEN siRNA, or scramble controls. The exosomes isolated from the supernatant of cultured MSCs could improve the functional recovery of SCI rats by reducing SCI-induced neuron loss. In addition, miR-21 was shown to inhibit the expression of PTEN/PDCD4 and suppress neuron cell death. Moreover, PTEN and PDCD4 were validated as virtual targets of miR-21. In addition, the miR-21/PTEN/PDCD4 signaling pathway was shown to enhance cell viability and suppress cell death in vivo. The exosomes collected from the supernatant of transfected MSCs contained miR-21, which could improve the functional recovery of SCI rats and suppress cell death both in vivo and in vitro via the miR-21/PTEN/PDCD4 signaling pathway.

(CF3C6H4)2SnO, (CH3C6H4)2SnO and Ph2SnO were successfully synthesized for the transesterification of DMC with BPA. The products of mono-methylcarbonate-ended-BPA (MmC(1)) and two-methylcarbonate-ended-BPA (DmC(1)) were selectively synthesized over them. The catalysts were characterized by FT-IR, TG and XPS. When Ph2SnO was used as the catalyst at 170 °C, the BPA conversion reached to 28.60% and the transesterification selectivity reached to 98.35%. As for (CF3C6H4)2SnO, BPA conversion and transesterification selectivity declined to 12.48% and 64.74%, respectively. The BPA conversion increased to 42.83%, but the transesterification selectivity declined to 44.55% over (CF3C6H4)2SnO. Notability, the higher transesterification selectivity of Ph2SnO was due to its lowest electron binding energy of Sn4+. More importantly, the DMC adsorption, activation and decomposition process over (CF3C6H4)2SnO, (CH3C6H4)2SnO and Ph2SnO were characterized by TG–MS and in situ DRIFT techniques, which provided more information about the mechanism of transesterification and methylation.

A green, environmentally friendly, and nontoxic method was developed to synthesize carboxylic anhydrides (NCAs) from γ-benzyl-l-glutamate (BLG) and dimethyl carbonate (DMC) though two steps: synthesis of N-methoxycarbonyl-γ-benzyl-l-glutamate intermediate (NOM-BLG) and cyclization. The highest yields of NOM-BLG (up to 83.7%) and NCA-BLG (up to 66.7%) were obtained. Most importantly, the use of DMC will open an innovative door to synthesize NCAs.

Polyphenylene sulfide (PPS) membranes were fabricated via a thermally induced phase separation method using mixed diluent of epsilon-caprolactam (CPL) and diphenyl sulfone (DPS). The effect of changing the CPL/DPS weight ratio on the structure and properties of prepared PPS membranes were investigated. The morphologies and performances of obtained PPS membranes were characterized by scanning electron microscopy, static water contact angles, mechanical strength, porosity, permeability and salt rejection rate. The characterized results showed that the morphologies of PPS membrane changed from cellular, bi-continuous to spherulitic structure with the increase of CPL/DPS mass ratio. PPS membranes exhibited the excellent stability and high salt rejection ratio in VMD experiments. The largest permeate flux stabilized at 10.63 L/(m2·h1) and the highest salt rejection remained above 98.9% after operating for 10 h.

Laser powder bed fusion AlSi10Mg exhibits severe mechanical anisotropy, which hinders its applications in industrial field. In the present work, we investigated the mechanisms of anisotropy in the light of phase stress partition, using traditional crystal plasticity and mechanism-based strain gradient crystal plasticity models. Two representative volume elements of the Al-Si cellular structures, corresponding to 35℃ and 200℃ build platform temperatures, were built to assess the influences of Al matrix strength and strain gradient on phase stress partition and anisotropy. In addition, the maximum principal stress distribution of the Si-rich network was probed, based on which the potential damage sites and densities were evaluated. The results show that the anisotropic strength and damage both originate from the elongated Si-rich network. According to the comparison between the 35℃ and 200℃ materials, an increase in Al phase strength can change the phase stress partition and effectively mitigate the anisotropy degree. Moreover, it is revealed that the strain gradient tends to alleviate anisotropy and delay damage evolution. The findings of this work can pave the way to developing high-performance LPBF Al alloys with lower degrees of anisotropy.

To investigate the mechanical behavior of the microlayered metallic thin films (MMMFs) at elevated temperature, an enhanced discrete-continuous model (DCM), which couples rather than superposes the two-dimensional climb/glide-enabled discrete dislocation dynamics (2D-DDD) with the linearly elastic finite element method (FEM), is developed in this study. In the present coupling scheme, two especial treatments are made. One is to solve how the plastic strain captured by the DDD module is transferred properly to the FEM module as an eigen-strain; the other is to answer how the stress field computationally obtained by the FEM module is transferred accurately to the DDD module to drive those discrete dislocations moving correctly. With these two especial treatments, the interactions between adjacent dislocations and between dislocation pile-ups and inter-phase boundaries (IBs), which are crucial to the strengthening effect in MMMFs, are carefully taken into account. After verified by comparing the computationally predicted results with the theoretical solutions for a dislocation residing in a homogeneous material and nearby a bi-material interface, this 2D-DDD/FEM coupling scheme is used to model the tensile mechanical behaviors of MMMFs at elevated temperature. The strengthening mechanism of MMMFs and the layer thickness effect are studied in detail, with special attentions to the influence of dislocation climb on them. [ABSTRACT FROM AUTHOR]

As important structural materials widely used in aerospace and automotive industries, aluminum alloys are perfect candidates for development of laser metal additive manufacturing (AM). Amongst AM aluminum alloys, laser powder bed fusion (LPBF) AlSi10Mg has received substantial attention due to its good printability and relatively low cost. Great efforts have been devoted to seek optimum process parameters that can enhance mechanical performance. However, a large scattering of material properties arises from the literature data, especially for the as built state, thus casting a shadow over further development of LPBF Al alloys. This review article aims to summarize the recent progresses on the characterization of microstructure, assessment of strengthening and damage mechanisms, evaluation of fracture and fatigue resistance, and attempts to build a primary comprehensive link between mechanical performance and microstructure for the as built state. Following the analysis of the state of the art, the review will finally provide an outlook on additional efforts needed to quantify the microstructure-property relation, based on which maximizing the potential of mechanical performance through optimizing microstructure may be achieved.

Abstract: To model the deformation of single crystal nickel based superalloys (SCNBS) with low stacking fault energy (SFE), three-dimensional discrete dislocation dynamics (3D-DDD) is extended by incorporating dislocation dissociation mechanism. The present 3D-DDD simulations show that, consistent with the existing TEM observation, the leading partial can enter the matrix channel efficiently while the trailing partial can hardly glide into it when the dislocation dissociation is taken into account. To determine whether the dislocation dissociation can occur or not, a critical percolation stress (CPS) based criterion is suggested. According to this CPS criterion, for SCNBS there exists a critical matrix channel width. When the channel width is lower than this critical value, the dislocation tends to dissociate into an extended configuration and vice versa. To clarify the influence of dislocation dissociation on CPS, the classical Orowan formula is improved by incorporating the SFE. Moreover, the present 3D-DDD simulations also show that the yielding stress of SCNBSs with low SFE may be overestimated up to 30% if the dislocation dissociation is ignored. With dislocation dissociation being considered, the size effect due to the width of γ matrix channel and the length of γ′ precipitates on the stress–strain responses of SCNBS can be enhanced remarkably. In addition, due to the strong constraint effect by the two-phase microstructure in SCNBS, the configuration of formed junctions is quite different from that in single phase crystals such as Cu. The present results not only provide clear understanding of the two-phase microstructure levelled microplastic mechanisms in SCNBSs with low SFE, but also help to develop new continuum-levelled constitutive laws for SCNBSs. [Copyright &y& Elsevier]

Polyphenylene sulfide (PPS) fiber products have been widely used for separation and filtration in harsh environments due to their excellent chemical resistance and relatively economical price. However, the poor temperature and weak oxidation resistance of PPS significantly shorten its service life under high temperature and strong oxidation environments. Herein, we report a type of oxidation-modified PPS (OPPS) fibers with excellent high temperature and oxidation resistance. This is achieved by oxidizing the thioether sulfide groups in PPS molecular chains into sulfoxide and sulfone groups and cross-linking the intermolecular chains. Both experiments and density functional theory (DFT) calculations indicate that hypochlorous acid (HClO) molecules can rapidly oxidize the PPS fiber surface. In addition, molecular dynamics (MD) simulations prove that there are strong hydrogen bonds and van der Waals interactions between HClO molecules and OPPS molecular chains, which promote the penetration of HClO molecules into the interior of the fiber to complete the layer-by-layer oxidation. The prepared OPPS-20 fibers exhibit excellent structural stability under high temperature and strong oxidant environments. Impressively, the OPPS-20 nonwoven filter still exhibits a high dust filtration efficiency of 99.95% after aging at 320 °C for 12 h, and the corresponding pressure drop is 24 Pa. In addition, the OPPS-20 nonwoven filter also maintains excellent filtration performance after aging in 60% HNO3solution for 12 h, and the filtration efficiency and pressure drop are 99.96% and 29 Pa, respectively. This work demonstrates that the novel OPPS fibers have excellent application prospects in the field of separation and filtration in harsh environments.

A two-dimensional discrete dislocation dynamics (DDD) technology by Giessen and Needleman (1995), which has been extended by integrating a dislocation-grain boundary interaction model, is used to computationally analyze the micro-cyclic plastic response of polycrystals containing micron-sized grains, with special attentions to significant influence of dislocation-penetrable grain boundaries (GBs) on the micro-plastic cyclic responses of polycrystals and underlying dislocation mechanism. Toward this end, a typical polycrystalline rectangular specimen under simple tension-compression loading is considered. Results show that, with the increase of cycle accumulative strain, continual dislocation accumulation and enhanced dislocation-dislocation interactions induce the cyclic hardening behavior; however, when a dynamic balance among dislocation nucleation, penetration through GB and dislocation annihilation is approximately established, cyclic stress gradually tends to saturate. In addition, other factors, including the grain size, cyclic strain amplitude and its history, also have considerable influences on the cyclic hardening and saturation.

The nanoindentation (NI) technique was employed to investigate the hydrogen effect on nanohardness near grain boundary (GB) of a polycrystalline nickel sample in the present work. An increase of nanohardness due to hydrogen segregation at GB was captured by nanoindentation experiments. With a newly developed GB hardening model, the observed hardening effect upon approaching GB in both H free and H charged polycrystalline Ni was explained. By combining the new GB hardening model with the model depicting dislocation transmission across GB, the hydrogen induced energy barrier enhancement was calculated, which can be used in multi-scale modeling of dislocation–GB interaction. The finding of this work is important for understanding hydrogen embrittlement mechanism of polycrystalline metals.

Nano-Twinned (NT) Cu under shock loading parallel to twin planes was investigated via nonequilibrium molecular dynamics (NEMD) simulations, with particular attention to the shock response and intrinsic deformation mechanism. During the shock compression process, a novel multi-stage phase transformation (MPT) scenario, i.e., from FCC phase to BCC phase and then to HCP phase, happens due to shock-enhanced twin boundary (TB) sliding. Both increasing the compressive strain caused by shock and decreasing the twin lamellae in the NT Cu can promote the MPT, with which the yield strength retains but the spallation strength increases. The critical shock pressure triggering the MPT depends exponentially on lamellae twin thickness (T). These new results have great potentials for improving the impact resistance of metals by tailoring their internal nanostructures.

Direct synthesis of diphenyl carbonate (DPC) from phenoxide, CO2and CCl4in one pot was realized with ZnCl2as catalyst. Trichloromethyl cation may act on potassium phenyl carbonate, which brings the carbonyl more easily attached on by the phenoxide. Onium salts promote the reaction greatly, especially with phenol and potassium carbonate instead of phenoxide as reactants. Moreover, the substituent on the aromatic ring has significant effects on the selectivity and yield of carbonate.