Control-Etched Ti3C2Tx MXene Nanosheets for a Low-Voltage-Operating Flexible Memristor for Efficient Neuromorphic Computation.

Hardware neural networks with mechanical flexibility are promising next-generation computing systems for smart wearable electronics. Overcoming the challenge of developing a fully synaptic plastic network, we demonstrate a low-operating-voltage PET/ITO/p-MXene/Ag flexible memristor device by controlling the etching of aluminum metal ions in Ti3C2Tx MXene. The presence of a small fraction of Al ions in partially etched MXene (p-Ti3C2Tx) significantly suppresses the operating voltage to 1 V compared to 7 V from fully Al etched MXene (f-Ti3C2Tx)-based devices. Former devices exhibit excellent non-volatile data storage properties, with a robust ∼103 ON/OFF ratio, high endurance of ∼104 cycles, multilevel resistance states, and long data retention measured up to ∼106 s. High mechanical stability up to ∼73° bending angle and environmental robustness are confirmed with consistent switching characteristics under increasing temperature and humid conditions. Furthermore, a p-Ti3C2Tx MXene memristor is employed to mimic the biological synapse by measuring the learning-forgetting pattern for ∼104 cycles as potentiation and depression. Spike time-dependent plasticity (STDP) based on Hebb's Learning rules is also successfully demonstrated. Moreover, a remarkable accuracy of ∼95% in recognizing modified patterns from the National Institute of Standards and Technology (MNIST) data set with just 29 training epochs is achieved in simulation. Ultimately, our findings underscore the potential of MXene-based flexible memristor devices as versatile components for data storage and neuromorphic computing.

Trimetallic Oxide Foam as an Efficient Catalyst for Fixation of CO2 into Oxazolidinone: An Experimental and Theoretical Approach.

The excess anthropogenic CO2 depletion via the catalytic approach to produce valuable chemicals is an industrially challenging, demanding, and encouraging strategy for CO2 fixation. Herein, we demonstrate a selective one-pot strategy for CO2 fixation into "oxazolidinone" by employing stable porous trimetallic oxide foam (PTOF) as a new catalyst. The PTOF catalyst was synthesized by a solution combustion method using transition metals Cu, Co, and Ni and systematically characterized by X-ray diffraction (XRD), thermogravimetric analysis (TGA), field emission scanning electron microscopy (FE-SEM), high-resolution transmission electron microscopy (HR-TEM), N2 sorption, temperature-programmed desorption (TPD), and X-ray photoelectron spectroscopy (XPS) analysis. Due to the distinctive synthesis method and unique combination of metal oxides and their percentage, the PTOF catalyst displayed highly interconnected porous channels along with uniformly distributed active sites on its surface. Well ahead, the PTOF catalyst was screened for the fixation of CO2 into oxazolidinone. The screened and optimized reaction parameters revealed that the PTOF catalyst showed highly efficient and selective activity with 100% conversion of aniline along with 96% selectivity and yield toward the oxazolidinone product at mild and solvent-free reaction conditions. The superiority of the catalytic performance could be due to the presence of surface active sites and acid-base cooperative synergistic properties of the mixed metal oxides. A doubly synergistic plausible reaction mechanism was proposed for the oxazolidinone synthesis experimentally with the support of DFT calculations along with bond lengths, bond angles, and binding energies. In addition, stepwise intermediate formations with the free energy profile were also proposed. Also, the PTOF catalyst displayed good tolerance toward substituted aromatic amines and terminal epoxides for the fixation of CO2 into oxazolidinones. Very interestingly, the PTOF catalyst could be significantly reused for up to 15 consecutive cycles with stable activity and retention in physicochemical properties.

REcovery and SURvival of patients with moderate to severe acute REspiratory distress syndrome (ARDS) due to COVID-19: a multicenter, single-arm, Phase IV itolizumab Trial: RESURRECT.

BACKGROUND: Itolizumab, an anti-CD6 monoclonal antibody, down-regulates COVID-19-mediated inflammation and the acute effects of cytokine release syndrome. This study aimed to evaluate the safety and efficacy of itolizumab in hospitalized COVID-19 patients with PaO2/FiO2 ratio (PFR) ≤200 requiring oxygen therapy. RESEARCH DESIGN AND METHODS: This multicenter, single-arm, Phase 4 study enrolled 300 hospitalized adults with SARS-CoV-2 infection, PFR ≤200, oxygen saturation ≤94%, and ≥1 elevated inflammatory markers from 17 COVID-19 specific tertiary Indian hospitals. Patients received 1.6 mg/kg of itolizumab infusion, were assessed for 1 month, and followed-up to Day 90. Primary outcome measures included incidence of severe acute infusion-related reactions (IRRs) (≥Grade-3) and mortality rate at 1 month. RESULTS: Incidence of severe acute IRRs was 1.3% and mortality rate at 1 month was 6.7% (n = 20/300). Mortality rate at Day 90 was 8.0% (n = 24/300). By Day 7, most patients had stable/improved SpO2 without increasing FiO2 and by Day 30, 91.7% patients were off oxygen therapy. Overall, 63 and 10 patients, respectively, reported 123 and 11 treatment-emergent adverse events up to Days 30 and 90. No deaths were attributable to itolizumab. Patient-reported outcomes showed gradual and significant improvement for all five dimensions on EQ-5D-5L. CONCLUSION: Itolizumab demonstrated acceptable safety with a favorable prognosis in hospitalized COVID-19 patients. CLINICAL TRIAL REGISTRATION: CTRI/2020/09/027941 (Clinical Trials Registry of India).

Ferrocene anchored activated carbon as a versatile catalyst for the synthesis of 1,5-benzodiazepines via one-pot environmentally benign conditions.

1,5-Benzodiazepine is considered as one of the central moieties in the core unit of most drug molecules. Construction of such moieties with a new C-N bond under solvent-free and mild reaction conditions is challenging. Herein, we present a benign protocol for one pot synthesis of 1,5-benzodiazepine derivatives by using ferrocene (FC) supported activated carbon (AC) as a heterogeneous catalyst. The catalyst FC/AC was characterized by several analytical and spectroscopic techniques to reveal its physicochemical properties and for structural confirmation. The synthesized catalyst FC/AC was explored for its catalytic activity in the synthesis of 1,5-benzodiazepines through condensation of o-phenylenediamine (OPDA) and ketones (aromatic and aliphatic) under solvent-free conditions. The robust 10 wt% FC/AC catalyst demonstrated appreciable activity with 99% conversion of diamines and 91% selectivity towards the synthesis of the desired benzodiazepine derivatives under solvent-free conditions at 90 °C in 8 h. Additionally, several reaction parameters such as catalyst loading, reaction temperature, effect of reaction time and effect of different solvents on selectivity were also studied and discussed in-depth. To understand the scope of the reaction, several symmetrical and unsymmetrical ketones along with different substituted diamines were tested with the synthesized catalyst. All prepared reaction products were obtained in good to efficient yields and were isolated and identified as 1,5-benzodiazepines and no side products were observed. The obtained catalyst characterization data and the activity studies suggested that, the synergetic effect occurred due to the uniform dispersion of ferrocene over the AC surface with numerous acidic sites which triggered the reaction of diamine and ketone to form the corresponding benzodiazepine derivative and the same was illustrated in the plausible mechanism. Furthermore, the synthesized catalyst was tested for leaching and recyclability, and the results confirmed that catalyst can be used for up to six consecutive cycles without much loss in the catalytic activity and its morphology which makes the process sustainable and economical for scale-up production. The present method offered several advantages such as an ecofriendly method, excellent yields, sustainable catalytic transformation, easy work-up and isolation of products, and quick recovery of catalyst.

Carbon Transition-metal Oxide Electrodes: Understanding the Role of Surface Engineering for High Energy Density Supercapacitors.

Supercapacitors store electrical energy by ion adsorption at the interface of the electrode-electrolyte (electric double layer capacitance, EDLC) or through faradaic process involving direct transfer of electrons via oxidation/reduction reactions at one electrode to the other (pseudocapacitance). The present minireview describes the recent developments and progress of carbon-transition metal oxides (C-TMO) hybrid materials that show great promise as an efficient electrode towards supercapacitors among various material types. The review describes the synthetic methods and electrode preparation techniques along with the changes in the physical and chemical properties of each component in the hybrid materials. The critical factors in deriving both EDLC and pseudocapacitance storage mechanisms are also identified in the hope of pointing to the successful hybrid design principles. For example, a robust carbon-metal oxide interaction was identified as most important in facilitating the charge transfer process and activating high energy storage mechanism, and thus methodologies to establish a strong carbon-metal oxide contact are discussed. Finally, this article concludes with suggestions for the future development of the fabrication of high-performance C-TMO hybrid supercapacitor electrodes.

Topotactic Transformations in an Icosahedral Nanocrystal to Form Efficient Water-Splitting Catalysts.

Designing high-performance, precious-metal-based, and economic electrocatalysts remains an important challenge in proton exchange membrane (PEM) electrolyzers. Here, a highly active and durable bifunctional electrocatalyst for PEM electrolyzers based on a rattle-like catalyst comprising a Ni/Ru-doped Pt core and a Pt/Ni-doped RuO2 frame shell, which is topotactically transformed from an icosahedral Pt/Ni/Ru nanocrystal, is reported. The RuO2 -based frame shell with its highly reactive surfaces leads to a very high activity for the oxygen evolution reaction (OER) in acidic media, reaching a current density of 10 mA cm-2 at an overpotential of 239 mV, which surpasses those of previously reported catalysts. The Pt dopant in the RuO2 shell enables a sustained OER activity even after a 2000 cycles of an accelerated durability test. The Pt-based core catalyzes the hydrogen evolution reaction with an excellent mass activity. A two-electrode cell employing Pt/RuO2 as the electrode catalyst demonstrates very high activity and durability, outperforming the previously reported cell performances.

Ferric phosphide carbon nanocomposites emerging as highly active electrocatalysts for the hydrogen evolution reaction.

Rational design and synthesis of efficient hydrogen evolution reaction (HER) electrocatalysts from Earth-abundant elements are essential for the development of economical water-splitting processes. This Frontier article will highlight the recent development and advances in designing ferric phosphide (FeP) based electrode materials for the HER.

Recent advances in electrocatalysts toward the oxygen reduction reaction: the case of PtNi octahedra.

Designing highly efficient and durable electrocatalysts for the oxygen reduction reaction (ORR), the key step for the operation of polymer electrolyte membrane fuel cells (PEMFCs), is of a pivotal importance for advancing PEMFC technology. Since the most significant progress has been made on Pt3Ni(111) alloy surfaces, nanoscale PtNi alloy octahedra enclosed by (111) facets have emerged as promising electrocatalysts toward the ORR. However, because their practical uses have been hampered by the cost, sluggish reaction kinetics, and poor durability, recent advances have engendered a wide variety of structure-, size-, and composition-controlled bimetallic PtNi octahedra. Herein, we therefore review the important recent developments of PtNi octahedral electrocatalysts point by point to give an overview of the most promising strategies. Specifically, the present review article focuses on the synthetic methods for the PtNi octahedra, the core-shell and multi-metallic strategies for performance improvement, and their structure-, size-, and composition-control-based ORR activity. By considering the results achieved in this field, a prospect for this alloy nanocatalysts system for future sustainable energy applications is also proposed.

Urine to highly porous heteroatom-doped carbons for supercapacitor: A value added journey for human waste.

Obtaining functionalized carbonaceous materials, with well-developed pores and doped heteroatoms, from waste precursors using environmentally friendly processes has always been of great interest. Herein, a simple template-free approach is devised to obtain porous and heteroatom-doped carbon, by using the most abundant human waste, "urine". Removal of inherent mineral salts from the urine carbon (URC) makes it to possess large quantity of pores. Synergetic effect of the heteroatom doping and surface properties of the URC is exploited by carrying out energy storage application for the first time. Suitable heteroatom content and porous structure can enhance the pseudo-capacitance and electric double layer capacitance, eventually generating superior capacitance from the URC. The optimal carbon electrode obtained particularly at 900 °C (URC-900) possesses high BET surface area (1040.5 m2g-1), good conductivity, and efficient heteroatom doping of N, S, and P, illustrating high specific capacitance of 166 Fg-1 at 0.5 Ag-1 for three-electrode system in inorganic electrolyte. Moreover, the URC-900 delivers outstanding cycling stability with only 1.7% capacitance decay over 5,000 cycles at 5 Ag-1. Present work suggests an economical approach based on easily available raw waste material, which can be utilized for large-scale production of new age multi-functional carbon nanomaterials for various energy applications.

Nanostructured materials on 3D nickel foam as electrocatalysts for water splitting.

Highly efficient and low-cost electrocatalysts are essential for water spitting via electrolysis in an economically viable fashion. However, the best catalytic performance is found with noble metal-based electrocatalysts, which presents a formidable obstacle for the commercial success of electrolytic water splitting-based H2 production due to their relatively high cost and scarcity. Therefore, the development of alternative inexpensive earth-abundant electrode materials with excellent electrocatalytic properties is of great urgency. In general, efficient electrocatalysts must possess several key characteristics such as low overpotential, good electrocatalytic activity, high stability, and low production costs. Direct synthesis of nanostructured catalysts on a conducting substrate may potentially improve the performance of the resultant electrocatalysts because of their high catalytic surface areas and the synergistic effect between the electrocatalyst and the conductive substrate. In this regard, three dimensional (3D) nickel foams have been advantageously utilized as electrode substrates as they offer a large active surface area and a highly conductive continuous porous 3D network. In this review, we discuss the most recent developments in nanostructured materials directly synthesized on 3D nickel foam as potential electrode candidates for electrochemical water electrolysis, namely, the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER). We also provide perspectives and outlooks for catalysts grown directly on 3D conducting substrates for future sustainable energy technologies.

Quality of life in acne vulgaris: Relationship to clinical severity and demographic data.

BACKGROUND: Acne vulgaris is known to impair many aspects of quality of life. However, the correlation of this impairment with clinical severity remains equivocal despite various school, community and hospital-based studies. AIM: A hospital-based study was undertaken to measure the impairment of quality of life of patients of acne vulgaris and correlate it with the severity of lesions. METHODS: This was a cross-sectional, questionnaire-based study in a cohort of 100 patients of acne vulgaris attending the outpatient department of our referral hospital. A physician measured the severity of lesions using the global acne grading system, and patients assessed quality of life by completing a questionnaire (Cardiff acne disability index). A correlation of these two was done; some additional correlations were brought out through demographic data collected from the patients. RESULTS: There was no correlation between the severity of acne vulgaris and an impaired quality of life. Patients who consumed alcohol and/or smoked cigarettes were found to have an impaired quality of life. While the severity of acne progressively lessened in older patients, the impact on quality of life increased. LIMITATIONS: The sample size was small and there was a lack of guaranteed reliability on the self-reported quality of life. CONCLUSION: The severity of acne vulgaris does not correlate with impairment in quality of life.

Outcomes of Short Segment Posterior Instrumentation in Unstable Thoracolumbar Fractures.

INTRODUCTION: The spinal traumas are common and leading problem in orthopaedics practice. The individuals are at a risk of high energy trauma in modern era. Unstable thoracolumbar burst fractures are serious injuries of concern, if left untreated may result in marked morbidity and disability to the patient. Thoracolumbar is the second most common segment involved in the spinal cord following spinal injuries followed by cervical segment. The goal of treatment of any spinal injury is restoration of the patient to maximum possible function with disability free life. AIM: To analyse the outcomes of unstable thoracolumbar burst fractures stabilized with short segment posterior instrumentation with transpedicular screws. MATERIALS AND METHODS: This prospective interventional study consisted of 32 patients with unstable thoracolumbar burst fractures carried out at Department of Orthopaedics, New Civil Hospital, Surat during Jan 2014 to Dec 2015. We stabilized the patients with unstable thoracolumbar spinal fractures with short segment posterior instrumentation by using the intermediate screw option in the fractured vertebra level as a method of augmentation. Patients were evaluated for maintenance of spinal correction and neurological improvement after short segment posterior instrumentation in unstable thoracolumbar burst fractures. RESULTS: The mean age for males was 35.57 ± 11.62 years and for females was 33.56 ± 11.2 years. The most common vertebra involved in the study group was T12 (31.25%). In the study, about 66% patients had a fall from height as the mode of injury, whereas 34% injuries were due to road traffic accident. In the study group, the mean regional angle observed during pre-operative stages was 16.0°±5.1°. There was a statistically significant (p<0.05) difference between pre-op and post-operative regional angles as well as anterior wedge angles. There was a statistically significant difference (p<0.05) in the vertebral height between pre-operative and post-operative stages. CONCLUSION: Short segment posterior instrumentation is a very stable implant construct in maintenance of deformity correction and fracture reduction along with the added advantage of sparing of the motion segments.

A clinical and statistical survey of cutaneous changes in the first 120 hours of life.

BACKGROUND: The spectrum of dermatological manifestations during neonatal period varies from transient self-limiting conditions to serious dermatoses; the latter, fortunately few, are disproportionately stressful to the parents, who due to lack of specialized pediatric dermatology clinics frequently get tossed between a dermatologist and a pediatrician. OBJECTIVES: This study was formulated to record cutaneous changes over the first five postnatal days of life and to statistically correlate those changes occurring in ≥ 11 neonates with three (parity, associated illnesses, and mode of delivery) maternal and three (sex, birth weight, and gestational age) neonatal factors. METHODS: This descriptive, cross-sectional study at a tertiary care hospital entailed recording detailed dermatological examination of 300 neonates having some (physiological and/or pathological) cutaneous changes and their statistical evaluation using the Chi-square test and significance (P < 0.05) as above. RESULTS: Superficial cutaneous desquamation (SCD), Mongolian spots (MS), and erythema toxicum neonatorum (ETN) were the first three common changes among a total of 15 conditions observed overall; these three, as also milia and icterus, revealed statistical significance with both maternal as well as neonatal factors. Lanugo and napkin dermatitis (ND) were statistically significant with respect to two neonatal factors and cradle cap (CC), a single maternal factor. Gestational age was of statistical significance regarding five cutaneous changes, associated maternal illness during pregnancy regarding four, birth weight as well as parity regarding three each, and sex of the neonate as well as mode of delivery regarding two each. CONCLUSION: Despite observing a statistically significant correlation of eight cutaneous changes with three maternal and/or three neonatal factors, more extensive studies in neonatal dermatology are required for validation of these unique statistical correlations.

Dyshidrosiform pemphigoid with Parkinsonism in a nonagenarian Maharashtrian female.

Dyshidrosiform pemphigoid is a rare variant of bullous pemphigoid localized to the hands and feet whose characteristic subepidermal blisters develop as a result of binding of the IgG autoantibodies to intracellular plaque and extracellular face of the hemidesmosome recognizing a 230-kDa plakin molecule (BP230, BPAg1or BPAg1e) and a 180-kDa transmembrane protein. Neurodegenerative processes (viz., stroke, dementia, Parkinsonism, epilepsy, etc) uncover BPAg1-n, an alternatively spliced form of BPAg1-e that stabilizes the cytoskeleton of sensory neurons, generating autoantibodies that may subsequently lead to BP by cross-reacting with BPAg1-e. We present a patient with Parkinsonism who later developed blisters, erosions and crusts localized to the palms and soles, confirmed histopathologically as bullous pemphigoid. To the best of our knowledge, ours is the first case report from India wherein Parkinsonism-generated autoantibodies led to the development of dyshidrosiform pemphigoid due to their cross-reactivity with BPAg1-e.

Cube-like α-Fe2O3 supported on ordered multimodal porous carbon as high performance electrode material for supercapacitors.

Well-dispersed cube-like iron oxide (α-Fe2O3) nanoparticles (NPs) supported on ordered multimodal porous carbon (OMPC) are synthesized for the first time by a facile and efficient glycine-assisted hydrothermal route. The effect of OPMC support on growth and formation mechanism of the Fe2O3 NPs is discussed. OMPC as a supporting material plays a pivotal role of controlling the shape, size, and dispersion of the Fe2O3 NPs. As-synthesized α-Fe2O3/OMPC composites reveal significant improvement in the performance as electrode material for supercapacitors. Compared to the bare Fe2O3 and OMPC, the composite exhibits excellent cycling stability, rate capability, and enhanced specific capacitances of 294 F g(-1) at 1.5 A g(-1), which is twice that of OMPC (145 F g(-1)) and about four times higher than that of bare Fe2O3 (85 F g(-1)). The improved electrochemical performance of the composite can be attributed to the well-defined structure, high conductivity, and hierarchical porosity of OMPC as well as the unique α-Fe2O3 NPs with cube-like morphology well-anchored on the OMPC support, which makes the composite a promising candidate for supercapacitors.

Heteroatom-doped highly porous carbon from human urine.

Human urine, otherwise potentially polluting waste, is an universal unused resource in organic form disposed by the human body. We present for the first time "proof of concept" of a convenient, perhaps economically beneficial, and innovative template-free route to synthesize highly porous carbon containing heteroatoms such as N, S, Si, and P from human urine waste as a single precursor for carbon and multiple heteroatoms. High porosity is created through removal of inherently-present salt particles in as-prepared "Urine Carbon" (URC), and multiple heteroatoms are naturally doped into the carbon, making it unnecessary to employ troublesome expensive pore-generating templates as well as extra costly heteroatom-containing organic precursors. Additionally, isolation of rock salts is an extra bonus of present work. The technique is simple, but successful, offering naturally doped conductive hierarchical porous URC, which leads to superior electrocatalytic ORR activity comparable to state of the art Pt/C catalyst along with much improved durability and methanol tolerance, demonstrating that the URC can be a promising alternative to costly Pt-based electrocatalyst for ORR. The ORR activity can be addressed in terms of heteroatom doping, surface properties and electrical conductivity of the carbon framework.

Angiokeratoma circumscriptum in a young male.

A 20-year-old male presented with multiple eruptions on his right leg since birth; these bled and were painful on trivial trauma. Examination revealed dark brown, hyperkeratotic, indurated, verrucous linear plaques with irregular borders. Histopathological evidence of hyperkeratosis, acanthosis, and extensive vascular proliferation in papillary dermis confirmed clinical suspicion of angiokeratoma circumscriptum (AKC). Excision and skin grafting yielded a cosmetically favorable outcome. Angiokeratomas, first described by Mibeli in 1889, are a group of vascular ectasias involving the papillary dermis. Angiokeratomas are more common in males; however, AKC-the rarest of its five variants-exhibits a female preponderance (F:M:3:1). AKC is an extremely rare nevoid disorder, only 100 of its cases having been reported in the world literature until 2006. Herein, we have reported a typical case of AKC in a young male that was previously misdiagnosed, and the patient wrongly counseled about the likelihood of its spontaneous regression.

Familial myomatosis cutis et uteri, segmental type 2.

Reed's syndrome or familial myomatosis cutis et uteri, an autosomal dominant inherited condition with incomplete penetrance, is characterized by multiple cutaneous and uterine leiomyomas.[1] Uterine leiomyomas usually commence earlier compared to that in the general population and cutaneous leiomyomas may precede, follow or occur concurrently. Few patients may have associated renal cell carcinoma. Herein we report a case of a 50-year-old female with multiple, painful cutaneous leiomyomas and who had undergone hysterectomy owing to large uterine fibroids. Her 18-year-old daughter also has uterine fibroids.