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Proton-exchange membrane fuel cells (PEMFCs) and water electrolysis (PEMWE) are rapidly developing hydrogen energy conversion devices. Catalyst layers and membranes have been studied extensively and reviewed. However, few studies have compared gas diffusion layers (GDLs) in PEMWE and PEMFC. This review compares the differences and similarities between the GDLs of PEMWE and PEMFC in terms of their material and mass transport characteristics. First, the GDL materials are selected based on their working conditions. Carbon materials are prone to rapid corrosion because of the high anode potential of PEMWEs. Consequently, metal materials have emerged as the primary choice for GDLs. Second, the mutual counter-reactions of the two devices result in differences in mass transport limitations. In particular, water flooding and the effects of bubbles are major drawbacks of PEMFCs and PEMWE, respectively; well-designed structures can solve these problems. Imaging techniques and simulations can provide a better understanding of the effects of materials and structures on mass transfer. Finally, it is anticipated that this review will assist research on GDLs of PEMWE and PEMFC.
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Proton exchange membranes (PEMs) are subject to mechanical degradation, such as microcracks and pinhole formation, under real-world fuel cell operating conditions, which leads to great issues in terms of device death and safety concerns. Therefore, PEMs with self-healing features are imperative but have rarely been used for proton exchange membrane fuel cells (PEMFCs). Here, a dimensionally stable and self-healing PEM is developed by tuning the hydrogen bond and dipole-dipole interactions between the mature perfluorinated sulfonic acid (PFSA) and a self-healing copolymer, which is specifically synthesized with hexafluorobutyl acrylate (HFBA) and acrylic acid (AA). This hexafluorobutyl acrylate-acrylic acid copolymer (HFBA-co-AA) is suggested as the key to improving the self-healing efficiency of the blended PFSA/HFBA-co-AA membrane. This PFSA/HFBA-co-AA membrane can recover 43.6% of the original tensile strength within only 20 min at 80 °C. This study may pave an avenue toward the development of reliable and durable PEM for fuel cells.
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The limited yield of H2 production has posed a significant challenge in contemporary research. To address this issue, researchers have turned to the application of surface plasmon resonance (SPR) materials in photocatalytic H2 generation. SPR, arising from collective electron oscillations, enhances light absorption and facilitates efficient separation and transfer of electron-hole pairs in semiconductor systems, thereby boosting photocatalytic H2 production efficiency. However, existing reviews predominantly focus on SPR noble metals, neglecting non-noble metals and SPR semiconductors. In this review, we begin by elucidating five different SPR mechanisms, covering hot electron injection, electric field enhancement, light scattering, plasmon-induced resonant energy transfer, and photo-thermionic effect, by which SPR enhances photocatalytic activity. Subsequently, a comprehensive overview follows, detailing the application of SPR materials-metals, non-noble metals, and SPR semiconductors-in photocatalytic H2 production. Additionally, a personal perspective is offered on developing highly efficient SPR-based photocatalysis systems for solar-to-H2 conversion in the future. This review aims to guide the development of next-gen SPR-based materials for advancing solar-to-fuel conversion.
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Recently, coupling the conventional low Pt-group-metal (low-PGM, LP) and emerging PGM-free (PF) moiety to form a composite LP/PF catalyst is proposed to be an advanced strategy to improve the intrinsic activity and stability of oxygen reduction reaction (ORR) catalysts. Milestones in terms of ORR mass activity are created by this type of catalyst. However, the specific synergy between LP and PF moieties has not been well elucidated. Herein, two model catalysts are synthesized, i.e., atomically dispersed Co/N/C supporting Pt single atoms (Co/N/C@Pt-SAs) and PtCo nanoparticles (Co/N/C@PtCo-NPs). Interestingly, the Co/N/C@PtCo-NPs catalyst presents higher ORR mass activity prior to Co/N/C@Pt-SAs. This is theoretically due to the dual "built-in electric field" in Co/N/C@PtCo-NPs: one electric field with a direction from Pt to Co in NPs and another from Pt to Co/N/C; that is, Pt gains higher electron density in Co/N/C@PtCo-NPs than that in Co/N/C@Pt-SAs, thus forming an asymmetric electron cloud, and regulating the adsorption and activation of oxygen-containing species. In addition, the existence of Co significantly decreases the average valence state of PtCo NPs, indicating a stronger affinity between PtCo NPs and Co/N/C substrate, to account for the enhanced stability.
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The cathodic oxygen reduction reaction (ORR) has been continuously attracting worldwide interest due to the increasing popularity of proton exchange membrane (PEM) fuel cells. So far, various Pt-group metal (PGM) or PGM-free catalysts have been developed to facilitate the ORR. However, there is still a gap to achieve the expected goals as proposed by the U.S. Department of Energy (DoE). Recently, PGM-free@PGM hybrid catalysts, such as the M/N/C@PtM catalyst, have achieved the milestones of oxygen reduction, as reviewed in our recent work. It is, nevertheless, still challenging to unravel the underlying structure-property relationships. Here, by applying different Pt/Co ratios, a series of Co/N/C@PtxCo catalysts are synthesized. Interestingly, the ORR activity and stability are not linear with the Pt content, but show a volcano-like curve with increased Pt usage. This relationship has been deeply unraveled to be closely related to the contents of pyrrolic N, pyridinic N, and graphitized carbon in catalysts. This work provides guidelines to rationally design the coupled PGM-free@PGM catalysts toward the ORR by appropriate surface engineering.
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New anti-lung cancer therapies are urgently required to improve clinical outcomes. Since ganodermanontriol (GDNT) has been identified as a potential antineoplastic agent, its role in lung adenocarcinoma (LUAD) is investigated in this study. Concretely, lung cancer cells were treated with GDNT and/or mycophenolate mofetil (MMF), after which MTT assay, flow cytometry and Western blot were conducted. Following bioinformatics analysis, carboxylesterase 2 (CES2) was knocked down and rescue assays were carried out in vitro. Xenograft experiment was performed on mice, followed by drug administration, measurement of tumor growth and determination of CES2, IMPDH1 and IMPDH2 expressions. As a result, the viability of lung cancer cells was reduced by GDNT or MMF. GDNT enhanced the effects of MMF on suppressing viability, promoting apoptosis and inducing cell cycle arrest in lung cancer cells. GDNT up-regulated CES2 level, and strengthened the effects of MMF on down-regulating IMPDH1 and IMPDH2 levels in the cells. IMPDH1 and IMPDH2 were highly expressed in LUAD samples. CES2 was a potential target for GDNT. CES2 knockdown reversed the synergistic effect of GDNT and MMF against lung cancer in vitro. GDNT potentiated the role of MMF in inhibiting tumor growth and expressions of CES2 and IMPDH1/2 in lung cancer in vivo. Collectively, GDNT suppresses the progression of LUAD by activating CES2 to enhance the metabolism of MMF.
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Adenocarcinoma del Pulmón , Antineoplásicos , Lanosterol/análogos & derivados , Neoplasias Pulmonares , Humanos , Animales , Ratones , Ácido Micofenólico/farmacología , Antineoplásicos/farmacología , Adenocarcinoma del Pulmón/tratamiento farmacológico , Neoplasias Pulmonares/tratamiento farmacológico , CarboxilesterasaRESUMEN
BACKGROUND: Ferroptosis is a new form of nonapoptotic and iron-dependent type of cell death. Glutathione peroxidase-4 (GPX4) plays an essential role in anti-ferroptosis by reducing lipid peroxidation. Although acute myeloid leukemia (AML) cells, especially relapsed and refractory (R/R)-AML, present high GPX4 levels and enzyme activities, pharmacological inhibition of GPX4 alone has limited application in AML. Thus, whether inhibition of GPX4 combined with other therapeutic reagents has effective application in AML is largely unknown. METHODS: Lipid reactive oxygen species (ROS), malondialdehyde (MDA), and glutathione (GSH) assays were used to assess ferroptosis in AML cells treated with the hypomethylating agent (HMA) decitabine (DAC), ferroptosis-inducer (FIN) RAS-selective lethal 3 (RSL3), or their combination. Combination index (CI) analysis was used to assess the synergistic activity of DAC + RSL3 against AML cells. Finally, we evaluated the synergistic activity of DAC + RSL3 in murine AML and a human R/R-AML-xenografted NSG model in vivo. RESULTS: We first assessed GPX4 expression and found that GPX4 levels were higher in AML cells, especially those with MLL rearrangements, than in NCs. Knockdown of GPX4 by shRNA and indirect inhibition of GPX4 enzyme activity by RSL3 robustly induced ferroptosis in AML cells. To reduce the dose of RSL3 and avoid side effects, low doses of DAC (0.5 µM) and RSL3 (0.05 µM) synergistically facilitate ferroptosis by inhibiting the AMP-activated protein kinase (AMPK)-SLC7A11-GPX4 axis. Knockdown of AMPK by shRNA enhanced ferroptosis, and overexpression of SLC7A11 and GPX4 rescued DAC + RSL3-induced anti-leukemogenesis. Mechanistically, DAC increased the expression of MAGEA6 by reducing MAGEA6 promoter hypermethylation. Overexpression of MAGEA6 induced the degradation of AMPK, suggesting that DAC inhibits the AMPK-SLC7A11-GPX4 axis by increasing MAGEA6 expression. In addition, DAC + RSL3 synergistically reduced leukemic burden and extended overall survival compared with either DAC or RSL3 treatment in the MLL-AF9-transformed murine model. Finally, DAC + RSL3 synergistically reduced viability in untreated and R/R-AML cells and extended overall survival in two R/R-AML-xenografted NSG mouse models. CONCLUSIONS: Our study first identify vulnerability to ferroptosis by regulating MAGEA6-AMPK-SLC7A11-GPX4 signaling pathway. Combined treatment with HMAs and FINs provides a potential therapeutic choice for AML patients, especially for R/R-AML.
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BACKGROUND: Automatic recognition of cough sounds shows promise in the diagnosis of respiratory conditions. This study investigated the diagnostic value of cough sounds in elderly patients with lower respiratory tract infection (LRTI). METHODS: We selected 83 elderly patients with suspected LRTI who sought medical advice at our hospital from January 2022 to September 2022, and grouped them into the infected and uninfected categories, according to their clinical traits. The cough sound of each subject was recorded and features were extracted using the Mel Frequency Cepstrum Coefficient. Four cough sound indexes, including the length of light or heavy cough time (T1), frequency of sound, decibels full scale (dBFs) and total length of cough time (T0) were compared between the two groups. The diagnostic efficacy of each index was analyzed using the receiver operating characteristic (ROC) curve. RESULTS: 22 patients were diagnosed with LRTI in the infected group including 15 males and 7 females, 13 were in the LRTI-free uninfected group, including 7 males and 6 females. Cough sound indexes were higher in the infected group compared with the uninfected group at T1 (p = 0.127), frequency of sound (p = 0.894), dBFs (p = 0.532) and T0 (p = 0.854). ROC curve analysis showed that the area under the curve (AUC) values of the above four indexes and the combined indexes for LRTI diagnosis were 0.680, 0.503, 0.577, 0.486 and 0.696, respectively. CONCLUSIONS: Cough sounds are correlated with LRTI. However, due to the small sample size of this study, the current results do not find that automatic recognition of cough has obvious diagnostic value, but its diagnostic potential in elderly patients with LRTI cannot be denied.
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Inteligencia Artificial , Infecciones del Sistema Respiratorio , Masculino , Femenino , Humanos , Anciano , Infecciones del Sistema Respiratorio/diagnóstico , Tos/diagnóstico , Curva ROCRESUMEN
Cancer is one of the greatest dangers to human wellbeing and survival. A key barrier to effective cancer therapy is development of resistance to anticancer medications. In cancer cells, the AAA+ ATPase family member thyroid hormone receptor interactor 13 (TRIP13) is key in promoting treatment resistance. Nonetheless, knowledge of the molecular processes underlying TRIP13based resistance to anticancer therapies is lacking. The present study evaluated the function of TRIP13 expression in anticancer drug resistance and potential methods to overcome this resistance. Additionally, the underlying mechanisms by which TRIP13 promotes resistance to anticancer drugs were explored, including induction of mitotic checkpoint complex surveillance system malfunction, promotion of DNA repair, the enhancement of autophagy and the prevention of immunological clearance. The effects of combination treatment, which include a TRIP13 inhibitor in addition to other inhibitors, were discussed. The present study evaluated the literature on TRIP13 as a possible target and its association with anticancer drug resistance, which may facilitate improvements in current anticancer therapeutic options.
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Antineoplásicos , Proteínas de Ciclo Celular , Humanos , Proteínas de Ciclo Celular/genética , Antineoplásicos/farmacología , Antineoplásicos/uso terapéutico , ATPasas Asociadas con Actividades Celulares Diversas/metabolismoRESUMEN
Molecular ferroelectric materials are widely applied in piezoelectric converters, non-volatile memorizers, and photovoltaic devices due to their advantages of adjustable structure, lightweight, easy processing, and environmental friendliness. However, designing multifunctional molecular ferroelectrics with excellent properties has always been a great challenge. Herein, a multiaxial molecular ferroelectric is successfully designed by modifying the quasi-spherical cation dabco with CuBr2 to obtain halogenated [Bretdabco]CuBr4 (Bretdabco = N-bromoethyl-N'-diazabicyclo [2.2.2]octane), which crystallizes in polar point groups (C6). Typical ferroelectric behaviors featured by the P-E hysteresis loop and switched ferroelectric domain are exhibited. Notably, the molecular ferroelectric shows a high TC of 460 K, which is rare in the field and could greatly expand the application range of this material. In addition, the band gap is adjustable through the regulation of halogen. Both the UV absorption spectra and theoretical calculations indicate that the molecular ferroelectrics belong to a direct band gap (2.14 eV) semiconductor. This tunable and narrow band gap semiconductor molecular ferroelectric material with high TC can be utilized more effectively in the study of optoelectronics and sensors, including piezoelectric energy harvesters. This research may provide a promising approach for the development of multiaxial molecular ferroelectrics with a tiny band gap and high TC.
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Lithium-sulfur (Li-S) batteries have high theoretical energy density but low sulfur utilization due to the inherent insulating nature of sulfur and the shuttle effect of polysulfides. Herein, the CO2-activation carbon paper was prepared by poly(p-phenylenebenzobisoxazole) (PBO) nanofiber and was first applied as an interlayer for efficiently alleviating the shuttle effect of polysulfides in Li-S batteries. This interlayer exhibits good flexibility and strength with rich -CâO and -COOH functional groups on the three-dimensional porous structure, which improves chemical adsorption on Li2Sx species and ion rapid diffusion via interconnected diffusion channels and thus enhances the electrochemical kinetics. The initial specific capacity is 1367.4 mAh g-1 and remains 999.8 mAh g-1 after 200 cycles at 0.2C and 780.1 mAh g-1 at 5C, and the Coulombic efficiency is high, up to 99.8%, which is much better than that for the carbon paper without CO2 activation. The highly conductive flexible PBO carbon paper may bring breakthroughs in performance and thus lead to more practical applications of Li-S batteries.
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Background: This study is a retrospective study. The purpose of this study is to construct and validate an early warning model of lung cancer through machine learning. Methods: The CDKN2A gene expression profile and clinical information were downloaded from The Cancer Genome Atlas (TCGA) database and divided into a tumor group and a normal group (n = 57). The top 5 somatic mutation-related genes were extracted from 567 somatic mutation data downloaded from TCGA database using random forest algorithm. Cox proportional hazard model and nomogram were constructed combining CDKN2A, 5 somatic mutation-related genes, gender, and smoking index. Patients were divided into high-risk and low-risk groups according to risk score. The predictability of the model in the prognosis of lung cancer was estimated by Kaplan-Meier survival analysis and receiver operating characteristics curve. Results: We constructed a prognostic model consisting of 5 somatic mutation-related genes (sphingosine 1-phosphate receptor 1 [S1PR1], dedicator of cytokinesis 7 [DOCK7], DEAD-box helicase 4 [DDX4], laminin subunit beta 3 [LAMB3], and importin 5 [IPO5]), cyclin-dependent kinase inhibitor 2A (CDKN2A), gender, and smoking indicators. The high-risk group had a lower overall survival rate compared to the low-risk group (hazard ratio = 2.14, P = 0 .0323). The area under the curve predicted for 3-year, 5-year, and 10-year survival rates are 0.609, 0.673, and 0.698, respectively. The accuracy, sensitivity, and specificity of the model for predicting the 10-year survival rate of lung cancer are 76.19%, 56.71%, and 86.23%. Conclusion: The lung cancer early warning model and nomogram may provide an essential reference for patients with lung cancer management in the clinic.
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Neoplasias Pulmonares , Humanos , Estudios Retrospectivos , Neoplasias Pulmonares/patología , Pronóstico , Aprendizaje Automático , Modelos de Riesgos Proporcionales , beta CarioferinasRESUMEN
Currently, the development of high-performance protonic ceramic cells (PCCs) is limited by the scarcity of efficient mixed protonic-electronic conducting oxides that can act as air electrodes to satisfy the high protonic conductivity of electrolytes. Despite the extensive research efforts in the past decades, the development of mixed protonic-electronic conducting oxides still remains in a trial-and-error process, which is extremely time consuming and high cost. Herein, based on the data acquired from the published literature, the machine-learning (ML) method is introduced to accelerate the discovery of efficient mixed protonic-electronic conducting oxides. Accordingly, the hydrated proton concentration (HPC) of 3200 oxides is predicted to evaluate the proton conduction that is essential for enhancing the electrochemical performances of PCCs. Subsequently, feature importance for HPC is evaluated to establish a guideline for rapid and accurate design and development of high-efficiency mixed protonic-electronic conducting oxides. Thereafter, screened (La0.7 Ca0.3 )(Co0.8 Ni0.2 )O3 (LCCN7382) is prepared, and the experimental HPC adequately corresponds with the predicted results. Moreover, the PCC with LCCN7382 exhibits satisfactory electrochemical performances in electrolysis and fuel cell modes. In addition to the development of a promising air electrode for PCC, this study establishes a new avenue for ML-based development of mixed protonic-electronic conducting oxides.
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Through precise and ingenious molecular modification, we successfully obtained a multiaxial ferroelectric, [FEtDabco]ZnI3 (N-fluoroethyl-N'-ZnI3-1,4-diazabicyclo[2.2.2]octonium), with a record high Tc (540 K) among molecular ferroelectrics, which is promising for application under extreme thermal conditions.
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Layered double hydroxides (LDHs) with decent oxygen evolution reaction (OER) activity have been extensively studied in the fields of energy storage and conversion. However, their poor conductivity, ease of agglomeration, and low intrinsic activity limit their practical application. To date, improvement of the intrinsic activity and stability of NiFe-LDHs through the introduction of heteroatoms or its combination with other conductive substrates to enhance their water-splitting performance has drawn increasing attention. In this study, vertically interlaced ternary phosphatised nickel/iron hybrids grown on the surface of titanium carbide flakes (NiFeP/MXene) were successfully synthesised through a hydrothermal reaction and phosphating calcination process. The optimised NiFeP/MXene exhibited a low overpotential of 286 mV at 10 mA cm-2 and a Tafel slope of 35 mV dec-1 for the OER, which exceeded the performance of several existing NiFe-based catalysts. NiFeP/MXene was further used as a water-splitting anode in an alkaline electrolyte, exhibiting a cell voltage of only 1.61 V to achieve a current density of 10 mA cm-2. Density functional theory (DFT) calculations revealed that the combination of MXene acting as a conductive substrate and the phosphating process can effectively tune the electronic structure and density of the electrocatalyst surface to promote the energy level of the d-band centre, resulting in an enhanced OER performance. This study provides a valuable guideline for designing high-performance MXene-supported NiFe-based OER catalysts.
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While proton exchange membrane fuel cells (PEMFCs) continue to expand into commercial markets, there is still pressure to decrease cost. One of the largest opportunities to reducing cost is to reduce the amount of platinum-group metal (PGM) catalysts used in the electrodes (particularly the cathode). Over the past decade, exciting advances in the Fe/N/C family of PGM-free oxygen reduction reaction (ORR) catalysts has provided great optimism that not only can PGMs at the cathode be reduced but possibly be completely eliminated. In fact, in September 2017, Ballard Power Systems announced the commercialization of the world's first PEMFC product to utilize a PGM-free catalyst at the cathode (FCgen-micro (non-precious-metal catalyst, NPMC)). However, for these catalysts to be used in more demanding applications, an improved understanding and new design approaches for PGM-free catalyst layers will be required. Herein, some of the latest research on both modeling and experimental studies in the field of PGM-free catalyst layer research are discussed. In addition, a short discussion on Ballard's new NPMC is provided.
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Despite great progress in the development of nonprecious metal catalysts (NPMCs) over the past several decades, the performance and stability of these promising catalysts have not yet achieved commercial readiness for proton exchange membrane fuel cells (PEMFCs). Through rational design of the cathode catalyst layer (CCL), we demonstrate the highest reported performance for an NPMC-based membrane electrode assembly (MEA), achieving a peak power of 570 mW/cm2 under air. This record performance is achieved using a precommercial catalyst for which nearly all pores are <3 nm in diameter, challenging previous beliefs regarding the need for larger catalyst pores to achieve high current densities. This advance is achieved at industrially relevant scales (50 cm2 MEA) using a precommercial NPMC. In situ electrochemical analysis of the CCLs is also used to help gain insight into the degradation mechanism observed during galvanostatic testing. Overall, the performance of this NPMC-based MEA has achieved commercial readiness and will be introduced into an NPMC-based product for portable power applications.
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The in situ diazonium reduction reaction is a reliable and well-known approach for the surface modification of carbon materials for use in a range of applications, including in energy conversion, as chromatography supports, in sensors, etc. Here, this approach was used for the first time with mesoporous colloid-imprinted carbons (CICs), materials that contain ordered monodisperse pores (10-100 nm in diameter) and are inherently highly hydrophilic, using a common microporous carbon (Vulcan carbon (VC)), which is relatively more hydrophobic, for a comparison. The ultimate goal of this work was to modify the CIC wettability without altering its nanostructure and also to lower its susceptibility to oxidation, as required in fuel cell and battery electrodes, by the attachment of pentafluorophenyl (-PhF5) groups onto their surfaces. This was shown to be successful for the CIC, with the -PhF5 groups uniformly coating the inner pore walls at a surface coverage of ca. 90% and allowing full solution access to the mesopores, while the -PhF5 groups deposited only on the outer VC surface, likely blocking its micropores. Contact angle kinetics measurements showed enhanced hydrophobicity, as anticipated, for both the -PhF5 modified CIC and VC materials, even revealing superhydrophobicity at times for the CIC materials. In contrast, water vapor sorption and cyclic voltammetry suggested that the micropores remained hydrophilic, arising from the deposition of smaller N- and O-containing surface groups, caused by a side reaction during the in situ diazonium functionalization process.
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Exploring inexpensive and high-performance nonprecious metal catalysts (NPMCs) to replace the rare and expensive Pt-based catalyst for the oxygen reduction reaction (ORR) is crucial for future low-temperature fuel cell devices. Herein, we developed a new type of highly efficient 3D porous Fe/N/C electrocatalyst through a simple pyrolysis approach. Our systematic study revealed that the pyrolysis temperature, the surface area, and the Fe content in the catalysts largely affect the ORR performance of the Fe/N/C catalysts, and the optimized parameters have been identified. The optimized Fe/N/C catalyst, with an interconnected hollow and open structure, exhibits one of the highest ORR activity, stability and selectivity in both alkaline and acidic conditions. In 0.1 M KOH, compared to the commercial Pt/C catalyst, the 3D porous Fe/N/C catalyst exhibits â¼6 times better activity (e.g., 1.91 mA cm-2 for Fe/N/C vs 0.32 mA cm-2 for Pt/C, at 0.9 V) and excellent stability (e.g., no any decay for Fe/N/C vs 35 mV negative half-wave potential shift for Pt/C, after 10000 cycles test). In 0.5 M H2SO4, this catalyst also exhibits comparable activity and better stability comparing to Pt/C catalyst. More importantly, in both alkaline and acidic media (RRDE environment), the as-synthesized Fe/N/C catalyst shows much better stability and methanol tolerance than those of the state-of-the-art commercial Pt/C catalyst. All these make the 3D porous Fe/N/C nanostructure an excellent candidate for non-precious-metal ORR catalyst in metal-air batteries and fuel cells.
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An atomic-scale engineered octopod nanoframe architecture (OFA) consisting of 3D catalytic surfaces and beneficial high-index facets is developed via a facile one-pot synthesis method. Based on the reliable recipe and general method, various complex nanoframe architectures are developed. Specially, the PtCu OFAs exhibit exceptional activity and stability for the oxygen reduction reaction and can be easily scaled up to high-quality.