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Discovery of earth-abundant electrocatalysts to replace iridium for the oxygen evolution reaction (OER) in a proton exchange membrane water electrolyzer (PEMWE) represents a critical step in reducing the cost for green hydrogen production. We report a nanofibrous cobalt spinel catalyst codoped with lanthanum (La) and manganese (Mn) prepared from a zeolitic imidazolate framework embedded in electrospun polymer fiber. The catalyst demonstrated a low overpotential of 353 millivolts at 10 milliamperes per square centimeter and a low degradation for OER over 360 hours in acidic electrolyte. A PEMWE containing this catalyst at the anode demonstrated a current density of 2000 milliamperes per square centimeter at 2.47 volts (Nafion 115 membrane) or 4000 milliamperes per square centimeter at 3.00 volts (Nafion 212 membrane) and low degradation in an accelerated stress test.

A lithium-air battery based on lithium oxide (Li 2 O) formation can theoretically deliver an energy density that is comparable to that of gasoline. Lithium oxide formation involves a four-electron reaction that is more difficult to achieve than the one- and two-electron reaction processes that result in lithium superoxide (LiO 2 ) and lithium peroxide (Li 2 O 2 ), respectively. By using a composite polymer electrolyte based on Li 10 GeP 2 S 12 nanoparticles embedded in a modified polyethylene oxide polymer matrix, we found that Li 2 O is the main product in a room temperature solid-state lithium-air battery. The battery is rechargeable for 1000 cycles with a low polarization gap and can operate at high rates. The four-electron reaction is enabled by a mixed ion–electron-conducting discharge product and its interface with air.

Pt/SrTiO3 nanoparticle catalysts have been synthesized by surface organometallic chemistry in solution on a 5 g scale. Pt/SrTiO3 selectively and repeatedly upcycles isotactic polypropylene into uniform liquid products with Mn ∼ 200 Da.

Uranium mining and nuclear fuel production have led to significant U contamination. Past studies have focused on the bioreduction of soluble U(VI) to insoluble U(IV) as a remediation method. However, U(IV) is susceptible to reoxidation and remobilization when conditions change. Here, we demonstrate that a combination of adsorption and bioreduction of U(VI) in the presence of an organic ligand (siderophore desferrioxamine B, DFOB) and the Fe-rich clay mineral nontronite partially alleviated this problem. DFOB greatly facilitated U(VI) adsorption into the interlayer of nontronite as a stable U(VI)-DFOB complex. This complex was likely reduced by bioreduction intermediates such as the Fe(II)-DFOB complex and/or through electron transfer within a ternary Fe(II)-DFOB-U(VI) complex. Bioreduction with DFOB alone resulted in a mobile aqueous U(IV)-DFOB complex, but in the presence of both DFOB and nontronite U(IV) was sequestered into a solid. These results provide novel insights into the mechanisms of U(VI) bioreduction and the stability of U and have important implications for understanding U biogeochemistry in the environment and for developing a sustainable U remediation approach.

Advancements in many modern technologies rely on the continuous need for materials discovery. However, the design of synthesis routes leading to new and targeted solid-state materials requires understanding of reactivity patterns

Urinary tract obstruction is a common cause of renal failure in children and infants, and the pathophysiological mechanisms of obstructive nephropathy are largely unclear. It has been reported that m6A modulation is involved in renal injury. However, whether m6A RNA modulation is associated with obstructive nephropathy has not yet been reported. The aim of this study was to investigate the m6A epitranscriptome profiles in the kidneys of bilateral ureteral obstruction (BUO) in young rats.The total level of m6A in the kidneys was measured by liquid chromatography-tandem mass spectrometry. The mRNAs of related genes were detected by real-time PCR. Methylated RNA immunoprecipitation sequencing was performed to map the epitranscriptome-wide m6A profile.Global m6A levels were increased after BUO, and the mRNA expression levels of m6A methyltransferases and demethylases were significantly decreased in BUO group rat kidneys; the expression levels of EGFR and Brcal were significantly upregulated, while the mRNA expression levels of Notch1 were downregulated (P 0.05). A total of 154 genes associated with 163 m6A peaks were identified.The m6A epitranscriptome was significantly altered in BUO rat kidneys, which is potentially implicated in the pathophysiological processes of obstructive nephropathy.The m6A RNA modification was associated with the process of renal injury in ureteral obstructive nephropathy by participating in multiple dimensions. The dysregulation of m6A methyltransferases and demethylases may be related to the pathophysiological changes of BUO-induced obstructive nephropathy. The m6A RNA modulation of the genes EGFR, Brca1, and Notch1 that were related to the regulation of aquaporin2 might be the potential mechanism for the polyuresis after ureteral obstruction.

High pressure induces dramatic changes and novel phenomena in condensed volatiles

Immunotherapies have revolutionized cancer treatment modalities; however, predicting clinical response accurately and reliably remains challenging. Neoantigen load is considered as a fundamental genetic determinant of therapeutic response. However, only a few predicted neoantigens are highly immunogenic, with little focus on intratumor heterogeneity (ITH) in the neoantigen landscape and its link with different features in the tumor microenvironment. To address this issue, we comprehensively characterized neoantigens arising from nonsynonymous mutations and gene fusions in lung cancer and melanoma. We developed a composite NEO2IS to characterize interplays between cancer and CD8+ T-cell populations. NEO2IS improved prediction accuracy of patient responses to immune-checkpoint blockades (ICBs). We found that TCR repertoire diversity was consistent with the neoantigen heterogeneity under evolutionary selections. Our defined neoantigen ITH score (NEOITHS) reflected infiltration degree of CD8+ T lymphocytes with different differentiation states and manifested the impact of negative selection pressure on CD8+ T-cell lineage heterogeneity or tumor ecosystem plasticity. We classified tumors into distinct immune subtypes and examined how neoantigen-T cells interactions affected disease progression and treatment response. Overall, our integrated framework helps profile neoantigen patterns that elicit T-cell immunoreactivity, enhance the understanding of evolving tumor-immune interplays and improve prediction of ICBs efficacy.

Background Presently, there is no consensus regarding the optimal serum uric acid (SUA) concentration for pediatric patients. Adenoid and tonsillar hypertrophy is considered to be closely associated with pediatric metabolic syndrome and cardiovascular risk and is a common condition in children admitted to the hospital. Therefore, we aimed to evaluate the relationship between SUA and dyslipidemia and propose a reference range for SUA concentration that is associated with a healthy lipid profile in hospitalized children with adenoid and tonsillar hypertrophy. Methods Preoperative data from 4922 children admitted for elective adenoidectomy and/or tonsillectomy surgery due to adenoid and tonsillar hypertrophy were collected. SUA concentrations were scaled to standard deviation (SD), and SUA deviations were expressed as SD from the mean SUA of children without dyslipidemia. Results The mean SUA concentration of the participants was 4.27 ± 1.01 mg/dL, and the prevalence of hyperuricemia was 1.6% when it was defined using an SUA of ≥ 7.0 mg/dL. Participants with dyslipidemia (856, 17.4%) had a higher prevalence of hyperuricemia (3.4% vs. 1.2%, P P 1 SD above the mean value of the participants with ortholiposis. Conclusions SUA was independently associated with dyslipidemia in children with adenoid and tonsillar hypertrophy, and an SUA

The development of general strategies for the electronic tuning of a catalyst’s active site is an ongoing challenge in heterogeneous catalysis. To this end, herein we describe the application of Li-ion battery cathode and anode materials as redox non-innocent catalyst supports that can be continuously modulated as a function of lithium intercalation. A zero-valent nickel complex was oxidatively grafted onto the surface of lithium manganese oxide (LixMn2O4) to yield isolated Ni(II) occupying the vacant interstitial octahedral site in the Li diffusion channel on the surface and subsurface of the spinel structure (Ni/LixMn2O4). The activity of Ni/LixMn2O4 for olefin hydrogenation, as a representative probe reaction, was found to increase monotonically as a function of support reductive lithiation. Simulation of Ni/LixMn2O4 reveals the dramatic impact of surface redox states on the viability of the homolytic oxidative addition mechanism for H2 activation. Catalyst control through support lithiation was extended to an organotantalum complex on LixTiO2, demonstrating the generality of this phenomenon.

Atomically-dispersed Pd species supported on MnO2 synthesized by the chemisorption of Pd(tricyclohexylphosphine)2 catalyze the low temperature (295–323 K) oxidation of CO to CO2.

The coronavirus disease of 2019 pandemic has catalyzed the rapid development of mRNA vaccines, whereas, how to optimize the mRNA sequence of exogenous gene such as severe acute respiratory syndrome coronavirus 2 spike to fit human cells remains a critical challenge. A new algorithm, iDRO (integrated deep-learning-based mRNA optimization), is developed to optimize multiple components of mRNA sequences based on given amino acid sequences of target protein. Considering the biological constraints, we divided iDRO into two steps: open reading frame (ORF) optimization and 5′ untranslated region (UTR) and 3′UTR generation. In ORF optimization, BiLSTM-CRF (bidirectional long-short-term memory with conditional random field) is employed to determine the codon for each amino acid. In UTR generation, RNA-Bart (bidirectional auto-regressive transformer) is proposed to output the corresponding UTR. The results show that the optimized sequences of exogenous genes acquired the pattern of human endogenous gene sequence. In experimental validation, the mRNA sequence optimized by our method, compared with conventional method, shows higher protein expression. To the best of our knowledge, this is the first study by introducing deep-learning methods to integrated mRNA sequence optimization, and these results may contribute to the development of mRNA therapeutics.

Introduction: Megalin plays an important role in proximal tubule uptake of filtered proteins. Downregulation and dysfunction of megalin were previously demonstrated in IgA nephropathy (IgAN); however, its relationship to IgAN progression remains unclear. Methods: We measured renal megalin mRNA and miR-148b, previously identified as a regulator of megalin, in a retrospective cohort of 417 IgAN patients at the time of biopsy, and evaluated their associations with chronic kidney disease (CKD) progression event, defined as end-stage renal disease or ≥40% decline in estimated glomerular filtration rate, using Cox proportional hazard models. Risk classification statistics were calculated for CKD progression. Results: During a median follow-up of 43 months, 121 (29.0%) patients reached the CKD progression event. Patients in the highest tertile of renal megalin mRNA had a lower risk for CKD progression than in the lowest tertile (hazard ratio (HR): 0.407, 95% confidence interval (CI) 0.231–0.719; p = 0.002). Log megalin mRNA was independent and negatively associated with CKD progression in IgAN (HR: 0.529, 95% CI 0.377–0.742; p < 0.001). The addition of renal megalin mRNA to a model with traditional risk factors improved risk prediction of disease progression (C statistic from 0.76 to 0.80; integrated discrimination index: 0.04 [95% CI: 0.02–0.07]). Moreover, patients in the highest tertile of renal miR-148b had a 2.3-fold higher risk for CKD progression compared with those in the lowest tertile. Conclusions: Lower renal megalin mRNA levels were associated with a greater risk of CKD progression in IgAN independent of clinical and pathological characteristics, suggesting that renal megalin could be an important prognostic factor for IgAN.

Nonenzymatic glucose biosensors based on electrospun porous La–Sr–Co–Ni–O nanofibers used for clinical, industrial, and environmental applications.

We investigated the magnetic effect of Mn2+ ions on an exciton of Mn-doped CsPbI3 quantum dots (QDs), where we looked for the signatures of an exciton magnetic polaron known to produce a large effective magnetic field in Mn-doped CdSe QDs. In contrast to Mn-doped CdSe QDs that can produce ∼100 T of magnetic field upon photoexcitation, manifested as a large change in the energy and relaxation dynamics of a bright exciton, Mn-doped CsPbI3 QDs exhibited little influence of a magnetic dopant on the behavior of a bright exciton. However, a μs-lived dark exciton in CsPbI3 QDs showed 40% faster decay in the presence of Mn2+, equivalent to the effect of ∼3 T of an external magnetic field. While further study is necessary to fully understand the origin of the large difference in the magneto-optic property of an exciton in two systems, we consider that the difference in antiferromagnetic coupling of the dopants is an important contributing factor.

Summary Recycling spent lithium-ion batteries plays a significant role in alleviating the shortage of raw materials and environmental problems. However, recycled materials are deemed inferior to commercial materials, preventing the industry from adopting recycled materials in new batteries. Here, we demonstrate that the recycled LiNi1/3Mn1/3Co1/3O2 has a superior rate and cycle performance, verified by various industry-level tests. Specifically, 1 Ah cells with the recycled LiNi1/3Mn1/3Co1/3O2 have the best cycle life result reported for recycled materials and enable 4,200 cycles and 11,600 cycles at 80% and 70% capacity retention, which is 33% and 53% better than the state-of-the-art, commercial LiNi1/3Mn1/3Co1/3O2. Meanwhile, its rate performance is 88.6% better than commercial powders at 5C. From experimental and modeling results, the unique microstructure of recycled materials enables superior electrochemical performance. The recycled material outperforms commercially available equivalent, providing a green and sustainable solution for spent lithium-ion batteries.

Enabling extreme fast charging (XFC, ≤10–15 min charging) requires a comprehensive understanding of its implications. While lithium plating is a key bottleneck for the anode, the full extent of limitations for the cathode are not well-understood, particularly in extended-cycle settings with well-defined battery designs and conditions. This article presents cycle-life implications of XFC on cathodes at multiple length scales, combining electrochemical analyses, degradation modeling, and post-test characterizations. The comprehensive test matrix includes 41 well-defined gr/NMC pouch cells under varied fast-charge rates (1–9C) and state-of-charges cycled up to 1000 times. Cathode issues remain minimal in early cycling, but begin to accelerate in later life, when distinct cracking is found and identified as a fatigue mechanism. The bulk structure of cathodes remains intact, but distinct particle surface reconstruction is observed; however, this shows less pronounced effect on cathode aging than does cracking.

This study aimed to investigate the value of high-frequency ultrasound (HFUS) in differentiation of the seronegative rheumatoid arthritis (SNRA) and osteoarthritis (OA) and in the diagnosis of SNRA. 83 patients diagnosed with SNRA (SNRA group) and 40 diagnosed with OA (OA group) who received HFUS were retrospectively analyzed. The grayscale (GS) scores, power Doppler (PD) scores, and bone erosion (BE)scores were recorded, and added up to calculate the total scores of US variables. The correlations of the total scores of US variables with the 28-joint disease activity score (DAS28), erythrocyte sedimentation rate (ESR) and C-reactive protein (CRP) were analyzed. The diagnostic efficacy of the total scores of US variables for SNRA was assessed. In the SNRA group, the detection rate of abnormal US findings in the joints and tendons by GS and PD as well as BE was higher than those in the OA group. There were significant differences between the two groups in GS scores and PD scores of joints and tendons, and BE scores of joints (P P P > 0.05). Among different US variables, the diagnostic value of total PD scores of the joints was the highest for SNRA. HFUS could be used to differentiate SNRA from OA and make a diagnosis of SNRA based on joint and tendon synovial sheath assessment.

Few studies have reported the roles of the complement system in concomitant idiopathic membranous nephropathy and IgA nephropathy (IMN-IgAN). Complement factor B (CFB) is a crucial factor that involved in the alternative complement pathway. We aimed to evaluate the association between disease activity (eGFR, anti-PLA2R antibody levels and 24 h urinary protein excretion), progression and serum CFB levels of IMN-IgAN patients. In total, 39 IMN-IgAN patients (median follow-up, 46.6 months), 99 IMN patients and 92 IgAN patients participated in this study. The disease progression event was defined as end-stage renal disease (ESRD) or a 30% decline in estimated glomerular filtration rate (eGFR). The serum CFB concentration was measured by enzyme-linked immunosorbent assay. Serum CFB levels were lower in IMN-IgAN patients than in patients with IgAN only (P

Molten salts are promising reaction media candidates for the discovery of novel materials; however, they offer little control over oxidation state compared to aqueous solutions. Here, we demonstrated that when two hydroxides are mixed, their melts become fluxes with tunable solubility, which are surprisingly powerful solvents for ternary chalcogenides and offer effective paths for crystal growth to new compounds. We report that precise control of the oxidation state of Ni is achievable in mixed molten LiOH/KOH to grow single crystals of all known ternary K-Ni-S compounds. It is also possible to access several new phases, including a new polytope of β-K2Ni3S4, as well as low-valence KNi4S2 and K4Ni9S11. KNi4S2 is a two-dimensional low-valence nickel-rich sulfide, and β-K2Ni3S4 has a hexagonal lattice. Moreover, using KNi4S2 as a template, we obtained a new layered binary Ni2S by topotactic deintercalation of K. The new binary Ni2S has a van der Waals gap and can function as a new host layer for intercalation chemistry, as demonstrated by the intercalation of LiOH between its layers. The oxidation states of low-valence KNi4S2 and Ni2S were studied using X-ray absorption spectroscopy and X-ray photoelectron spectroscopy. Density functional theory calculations showed large antibonding interactions at the Fermi level for both KNi4S2 and Ni2S, corresponding to the flat-bands with large Ni-dx2-y2 character.

To assess the efficacy of sacral neuromodulation (SNM) for neurogenic bladder (NB), guided by intraoperative three-dimensional imaging of sacral computed tomography (CT) and mobile C-arm fluoroscopy through video-urodynamics examination. We enrolled 52 patients with NB who underwent conservative treatment with poor results between September 2019 and June 2021 and prospectively underwent SNM guided by intraoperative three-dimensional imaging of sacral CT and mobile C-arm fluoroscopy. Video-urodynamics examination, voiding diary, quality of life questionnaire, overactive bladder symptom scale (OABSS) scoring, and bowel dysfunction exam were completed and recorded at baseline, at SNM testing, and at 6-month follow-up phases. Finally, we calculated the conversion rate from period I to period II, as well as the treatment efficiency and the occurrence of adverse events during the testing and follow-up phases. The testing phase of 52 NB patients was 18–60 days, with an average of (29.3 ± 8.0) days. Overall, 38 patients underwent SNM permanent electrode implantation, whose follow-up phase was 3–25 months, with an average of (11.9 ± 6.1) months. Compared with baseline, the voiding times, daily catheterization volume, quality of life score, OABSS score, bowel dysfunction score, maximum detrusor pressure before voiding, and residual urine volume decreased significantly in the testing phase. The daily voiding volume, functional bladder capacity, maximum urine flow rate, bladder compliance, and maximum cystometric capacity increased significantly in the testing phase. Besides, the voiding times, daily catheterization volume, quality of life score, OABSS score, bowel dysfunction score, maximum detrusor pressure before voiding, and residual urine volume decreased further from the testing to follow-up phase. Daily voiding volume, functional bladder capacity, maximum urine flow rate, bladder compliance, and maximum cystometric capacity increased further from testing to follow-up. At baseline, 10 ureteral units had vesicoureteral reflux (VUR), and 9 of them improved in the testing phase. Besides, there was 1 unit that further improved to no reflux during the follow-up phase. At baseline, 10 patients had detrusor overactivity (DO), and 8 of them improved in the testing phase. Besides, 1 patient’s symptoms further improved during the follow-up phase. At baseline, there were 35 patients with detrusor-bladder neck dyssynergia (DBND); 14 (40.0%) of them disappeared during the testing phase. Among 13 cases who had DBND in the testing phase, 6 (46.2%) disappeared during the follow-up phase. Of the 47 patients with detrusor-external sphincter dyssynergia (DESD) at baseline, 8 (17.0%) disappeared during the testing phase. Among 26 cases who had DESD in the testing phase, 6 (23.1%) disappeared during the follow-up phase. The effective rate of this study was 88.5% (46/52), and the conversion rate from phase I to phase II was 73.1% (38/52). Additionally, the efficacy in a short-term follow-up was stable. SNM guided by intraoperative three-dimensional imaging of sacral CT and mobile C-arm fluoroscopy is an effective and safe treatment option for NB in short time follow-up. It would be well improved in the bladder storage function, sphincter synergetic function and emptying efficiency by video-urodynamics examination in this study.Trial registration: Chinese Clinical Trial Registry. ChiCTR2100050290. Registered August 25 2021. http://www.chictr.org.cn/index.aspx.

PurposeTo establish a predictive model for upper urinary tract damage (UUTD) in children with neurogenic bladder (NB) and verify its efficacy.MethodsA retrospective study was conducted that consisted of a training cohort with 167 NB patients and a validation cohort with 100 NB children. The clinical data of the two groups were compared first, and then univariate and multivariate logistic regression analyses were performed on the training cohort to identify predictors and develop the nomogram. The accuracy and clinical usefulness of the nomogram were verified by receiver operating characteristic (ROC) curve, calibration curve and decision curve analyses.ResultsThere were no significant differences in other parameters between the training and validation cohorts except for age (all P > 0.05). Recurrent urinary tract infection, bladder compliance, detrusor leak point pressure, overactive bladder and clean intermittent catheterization were identified as predictors and assembled into the nomogram. The nomogram showed good discrimination with the area under the ROC curve (AUC) in the training cohort (0.806, 95% CI: 0.737–0.874) and validation cohort (0.831, 95% CI: 0.753–0.0.909). The calibration curve showed that the nomograms were well calibrated, with no significant difference between the predicted and observed probabilities. Decision curve analysis indicated that the nomogram has good clinical applicability.ConclusionThis study presents an effective nomogram incorporating five clinical characteristics that can be conveniently applied to assess NB children' risk of progressing to UUTD.

Isolated solid-state atomic defects with telecom optical transitions are ideal quantum photon emitters and spin qubits for applications in long-distance quantum communication networks. Prototypical telecom defects, such as erbium, suffer from poor photon emission rates, requiring photonic enhancement using resonant optical cavities. Moreover, many of the traditional hosts for erbium ions are not amenable to direct incorporation with existing integrated photonics platforms, limiting scalable fabrication of qubit-based devices. Here, we present a scalable approach toward CMOS-compatible telecom qubits by using erbium-doped titanium dioxide thin films grown atop silicon-on-insulator substrates. From this heterostructure, we have fabricated one-dimensional photonic crystal cavities demonstrating quality factors in excess of 5 × 10

In patients with detrusor overactivity with impaired contractility (DOIC), it is difficult to relieve abnormal lower urinary tract symptoms during both storage and voiding using sacral neuromodulation (SNM) with constant frequency stimulation (CFS). We sought to evaluate the efficacy and safety of SNM using variable frequency stimulation (VFS) in patients with DOIC by comparing it with outcomes of SNM with CFS.Between September 2020 and May 2021, we prospectively enrolled 20 patients with DOIC, confirmed on urodynamic examination, and administered SNM with VFS. The patients were followed up and required to maintain voiding diaries and record scale scores of overactive bladder symptoms, psychology and quality of life, uroflowmetry, ultrasonic postvoid residual urine, and adverse events at baseline and during the CFS and VFS phases.The average testing phase was 26.3 ± 4.1 days. Compared with baseline values, overactive bladder symptom, psychologic health questionnaire, and quality of life scores, in addition to voiding frequency, urgency incontinence frequency, daily catheterization volume of voiding diary, and ultrasonic postvoid residual (PVR) decreased significantly during both the CFS and VFS phases (p 0.05). The average voided volume, functional bladder capacity, and maximum urine flow rate significantly increased during the CFS and VFS phases (p 0.05). In the VFS phase, voiding frequency, urgency incontinence frequency, daily catheterization volume of voiding diary, and ultrasonic PVR further decreased (p 0.05), whereas functional bladder capacity, maximum urine flow rate, quality of life score, overactive bladder symptom score, and psychologic health questionnaire score further improved compared with results obtained in the CFS phase (p 0.05). In the VFS phase, the success rate of further improvement of symptoms was 85.0%, and no new complications were noted.SNM that converts CFS into VFS may be an effective treatment option for patients with DOIC, exhibiting no increase in adverse events.

LiCoO

Hierarchical domain structures associated with oxygen octahedra tilting patterns were observed in lead-free (Bi

While lithium, manganese-rich (LMR) layered oxide cathode materials offer high energy density (>900 Wh kg-1) and low cost, LMR is susceptible to continuous capacity and voltage decay from the oxygen migration and side reaction with aqueous electrolyte at high voltage. Herein, the integration of Na/F co-doping (CD) and AlF3 coating on LMR is achieved without the need of complex atomic layer deposition. Akin to pristine and CD samples, CD with 1 wt % AlF3 (CD-1.0 wt %) shows excellent electrochemical performance with the capacity and voltage retentions of 93 and 91% after 150 cycles at 0.5C, respectively, and increased ionic conductivity. Spectroscopic analysis indicates that the coating mainly influences the Co distribution, where Co is enriched on the surface, and partial diffusion of Al3+ ions toward the bulk, leading to a slight change of transition-metal (TM) valence states at the nanometer scale and the formation of a stable Lix(CoAl)Oy phase. Post-cycling analysis reveals that CD-1.0 wt % can alleviate the formation of rock-salt structure and Mn dissolution. Besides, little to no metal segregation is detected for the cycled CD-1.0 wt % sample. This finding presents the first instance to apply co-doping and AlF3 coating as a new strategy to enhance the structural homogeneity and takes another step toward their commercial viability.

Flame-spray-pyrolysis (FSP) is a robust and scalable process to synthesize particles at the commodity-scale. FSP has been used to produce the precursor powders which were converted to the layered structure (R3m phase) by a postannealing step in making nickel-rich cathode materials (NCMs). Theoretically, the high flame temperature (normally >1500 K) in FSP can provide adequate energy for the phase conversion from rock-salt to layered structures and potentially enables one-step synthesis. However, the high flame temperature is a critical issue to cause lithium loss and structural degradation, preventing the formation of the layered phase. In this work, guided by the gaseous nucleation theory, we implemented several FSP processes with different solution recipes. The layered phase concentration in the as-burned products can be increased with the solution enthalpies. By adding a rapid quench step to suppress the lithium loss and phase degradation, the layered phase can be further increased. This work contributes new ideas to innovating process regarding the process efficiency and throughput of manufacturing cathode materials at a large scale.

Conventional phase diagram generation involves experimentation to provide an initial estimate of the set of thermodynamically accessible phases and their boundaries, followed by use of phenomenological models to interpolate between the available experimental data points and extrapolate to experimentally inaccessible regions. Such an approach, combined with high throughput first-principles calculations and data-mining techniques, has led to exhaustive thermodynamic databases (e.g. compatible with the CALPHAD method), albeit focused on the reduced set of phases observed at distinct thermodynamic equilibria. In contrast, materials during their synthesis, operation, or processing, may not reach their thermodynamic equilibrium state but, instead, remain trapped in a local (metastable) free energy minimum, which may exhibit desirable properties. Here, we introduce an automated workflow that integrates first-principles physics and atomistic simulations with machine learning (ML), and high-performance computing to allow rapid exploration of the metastable phases to construct “metastable” phase diagrams for materials far-from-equilibrium. Using carbon as a prototypical system, we demonstrate automated metastable phase diagram construction to map hundreds of metastable states ranging from near equilibrium to far-from-equilibrium (400 meV/atom). We incorporate the free energy calculations into a neural-network-based learning of the equations of state that allows for efficient construction of metastable phase diagrams. We use the metastable phase diagram and identify domains of relative stability and synthesizability of metastable materials. High temperature high pressure experiments using a diamond anvil cell on graphite sample coupled with high-resolution transmission electron microscopy (HRTEM) confirm our metastable phase predictions. In particular, we identify the previously ambiguous structure of n-diamond as a cubic-analog of diaphite-like lonsdaelite phase.

To explore the value of ultrasound in the preoperative diagnosis of nonpalpable testis (NPT) in children. A retrospective study of 254 cases with NPT from May 2017 to December 2021. The preoperative ultrasound examination results were compared with the surgical exploration and pathological results. There were 254 cases (312 testes) NPT has got surgery in our centre. The surgical age were from 6 month to 12 years old, the median age was 2.33 years. There were 103 cases (136 testes) diagnosed as intra-abdominal testis (IAT) by preoperative ultrasound, and 80 cases (103 testes) of extra-abdominal testis (EAT), 71 cases (73 testes) of non-viable testis (NVT). There were 102 cases (135 testes) consistented as IAT by the diagnostic laparoscopy, the preoperative ultrasound’s coincidence of IAT was 99.02%. There were 80 cases (103 testes) consistented as EAT by the diagnostic laparoscopy, the preoperative ultrasound’s coincidence rate was100%. There were 62 cases (62 testes) consistented as NVT by the diagnostic laparoscopy, there were 9 cases (11 testes) misdiagnosed, the preoperative ultrasound’s coincidence rate was 84.9%. Ultrasound can provide valuable information for the preoperative diagnosis of children with nonpalpable testicles, and especially good at identifying the EAT and IAT with normal testicular morphology.

The limited durability of Pt electrocatalysis toward cathodic oxygen reduction reaction is a remaining challenge, yet crucial for the development of Proton Exchange Membrane Fuel Cell. Here, we present a robust catalyst consisted of ~ 3 nm PtCo core-shell nanoparticles supported by porous Graphene-Nitrogen nanofiber decorated with single-atomic Pt and Co, termed PtCo@Pt-Co-GNF. The approach uses polymer-fiber containing Polyacrylonitrile and Cobalt-Metal-Organic-Framework as precursors to the Graphene-Nitrogen template where Pt clusters are in-situ reduced for high temperature synthesis. In a fuel cell with a total Pt loading (anode + cathode) of 0.083 mg cm-2, the new catalyst delivers unprecedented mass activity of 2.48 A mgPt-1 at 0.9 ViR-free, and a high Pt utilization of 11.9 kW gPt-1 at 150 kPaabs initially. Operando X-ray absorption spectroscopies (XAS) of PtCo@Pt-Co-GNF show that the structures of Co moieties under working and ex-situ condition are different, and Co moieties are modified during oxygen reduction reaction. Density Functional Theory combined with Operando XAS unveils that the synergistic effect of atomic neighboring Pt-Co dual center facilitates the oxygen-intermediates-adsorption strengthened on Co moieties and weakened on Pt sites, eventually enhancing the catalytic activity. Theoretical simulation further manifests that the enhanced curvature of the carbon substrate lowers the reaction thermodynamic barrier favoring the formation of H2O rather than H2O2 over Co-N4. This result along with the high carbon graphitization and the strong interaction between PtCo and Co-N-C may likely be responsible for the drastically enhanced durability of the catalyst which underwent 60,000 Accelerated-Stress-Test cycles including 30,000 cycles in H2-Air cell and a continued 30,000 cycles in H2-O2 cell with no obvious structure and composition changes.

ObjectiveThe study aimed to investigate the diagnostic value of ultrasound in children’s transverse testicular ectopia (TTE).Materials and methodsWe retrospectively studies all TTE cases diagnosed in our hospital from January 2017 to December 2021. All cases were evaluated by ultrasound examination and compared to physical examination and diagnostic laparoscopy results.ResultsThis study included 14 TTE patients in total, with a median age was 1.08 years. In the 14 TTE, physical examination found 10 TTE cases, of which nine testes were located in the opposite scrotum, one testis was located in the opposite groin, and the other four testes were not observed by physical examination. All cases were diagnosed by preoperative ultrasound, and nine testes were located in the opposite scrotum, two testes were located in the opposite groin, and three testes were located next to the opposite iliac vessel in the abdominal cavity. Preoperative ultrasound showed the ectopic spermatic cord in six cases (6/14, 42.8%) and persistent Müllerian duct syndrome (PMDS) in one case (1/14, 7%). Diagnostic laparoscopy finally confirmed 14 cases of TTE, which was consistent with preoperative ultrasound, and the coincidence rate was 100% (14/14). Among the 14 cases of TTE, diagnostic laparoscopy showed that 12 cases had ectopic spermatic vessels and vas deferens (12/14, 85.7%), and six cases were associated with PMDS (6/14, 42.8%). When TTE was associated with the ectopic spermatic cord and PMDS, the diagnostic performance of diagnostic laparoscopy was better than that of preoperative ultrasound (P < 0.05). The testis volume of the affected side of TTE was less than that of the contralateral testis (P < 0.05).ConclusionUltrasonography is very helpful for the preoperative diagnosis of TTE in children, and it is suitable as a non-surgical method for locating ectopictestis. Preoperative assessment of the exact presence of PMDS is difficult and unclear. This may be related to factors such as pelvic developmental stages in infancy, examination techniques, and atypical imaging findings of PMDS.

Dislocation dynamic simulations are intended as a tool to understand and predict the mechanical behavior of metallic materials, but its prediction has never been directly verified by experiments due to differences in specimen strain rate and size. In this work, a comprehensive experimental framework is proposed to attempt direct comparison between experiments and discrete dislocation dynamics (DDD) modelling. By integrating high-throughput sample fabrication and a customized testing apparatus, the sample size and strain rate typically employed in DDD simulations are explored experimentally. Constitutive properties such as stress-strain response are measured, and microstructural information is obtained from transmission electron microscopy (TEM) imaging, electron backscatter diffraction (EBSD), and TEM-based orientation mapping. Magnesium and copper were selected, as case studies, to demonstrate the newly developed experimental procedure. Measured stress-strain responses for Mg are consistent with those obtained with a miniaturized Hopkison bar experiments. By exploiting the validated workflow, the effect of strain rate on micropillar heterogeneous deformation and associated dislocation plasticity were revealed. The work establishes a methodology for the systematic study of not only metals but also other materials and structures at the microscale and high strain rates.

Ag-Doped MnFe2O4 catalyst (Ag/MnFe2O4) was synthesized by a simple sol–gel method followed by H2 reduction. Utilizing the localized surface plasmon resonance (LSPR) of Ag, ∼35-fold and ∼7-fold degr...

The generation of hydrogen in an environmentally benign way is highly essential to meet future energy demands. However, in the process of splitting water electrochemically, sluggish kinetics of the...

Current bottlenecks in cobalt (Co) supply have negatively impacted commercial battery production and inspired the development of cathode materials that are less reliant on Co. However, complete Co elimination is prevented by the lack of fundamental understanding of the impact of Co on cathode capacity and structural stability, as well as the lack of effective substitute components in practice. Here we investigate the roles of Co in purposely designed systems that include both Co-rich and Mn-substituted Co-free cathodes. Our results affirmed that Co plays an undeniable role in fast capacity and/or structural degradation, and found that Co is more destructive than Ni at high potentials, which offers unexpected but encouraging perspectives for Co reduction. Moreover, Mn substitution effectively alleviates the destructive effects of Co and enables a high potential functionality. With these fundamental discoveries, we demonstrated a series of LiNiαMnβXγO2 (X = single or multiple dopants) as a promising candidate for Co-free cathodes. Reduction on cobalt reliance is an urgent requirement in the development of sustainable cathode materials for Li-ion batteries. Here the authors analyse the roles of cobalt and its interplay with other ions in high-nickel layered oxides, and deduce a material formula for promising cobalt-free cathodes.

A superconducting interface Interfaces between materials can harbor quantum states that belong to neither of the materials. A classic example is the superconducting interface between two insulating oxides, LaAlO 3 and SrTiO 3 , with a critical temperature of around 200 millikelvin. Liu et al. observed superconductivity at a different interface—formed between KTaO 3 as a substrate and an overlayer of either EuO or LaAlO 3 —at a considerably higher temperature of about 2 kelvin. Transport measurements displayed anisotropy, which may indicate an unusual superconducting state. Science , this issue p. 716

It is of great research interest to understand the nanostructures contributing to the activity observed in the reduction of oxygen by non-platinum group metal (PGM) electrocatalysts in acidic media. Iron- and nitrogen-containing carbon networks are often the most studied structures, among which single-atom iron-coordinated nitrogen (FeNx) moieties have often been proposed to be the structures leading to the high activity in these non-PGM electrocatalysts. Iron nanoparticles embedded within a carbon support are also formed under certain conditions as a result of the synthetic processes in making non-PGM electrocatalysts. In this study, we present a study to understand the oxygen reduction reaction (ORR) activity of prepared iron- and nitrogen-containing non-PGM electrocatalysts obtained through the pyrolysis of metal-organic framework (MOF) precursors. We studied the structure-property relationship among nanostructures made from the MOF precursor ZIF-8 under different pyrolysis conditions. Density functional theory calculations were used to explain the effect of structural moieties on the ORR activity. Our results suggest that iron-coordinated C-N structures and iron nanoparticles act synergistically to catalyze the ORR.

A high density of gold (Au) nanoparticles has been observed on the surfaces of the coexisting opal nanospheres in kerogen-bearing shales from the Marcellus Formation. Our analyses of the Au nanopar...