A Janus heteroatom-doped carbon electrocatalyst for hydrazine oxidation
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PROVIDER: S-EPMC10084918 | biostudies-literature | 2022 Oct
REPOSITORIES: biostudies-literature
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Project description: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.
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Project description:Structural engineering is an effective methodology for the tailoring of the quantities of active sites in nanostructured materials for fuel cell applications. In the present study, Co nanoparticles were incorporated into the network of 3D nitrogen-doped carbon tubes (Co@NCNTs) that were obtained via the molten-salt synthetic approach at 800 °C. Morphological representation reveals that the Co@NCNTs are encompassed with Co nanoparticles on the surface of the mesoporous walls of the carbon nanotubes, which offers a significant active surface area for electrochemical reactions. The CoNPs/NCNTs-1 (treated with CaCl2) nanomaterial was used as a potential candidate for the electro-oxidation of hydrazine, which improved the response of hydrazine (~8.5 mA) in 1.0 M NaOH, as compared with CoNPs/NCNTs-2 (treated without CaCl2), NCNTs, and the unmodified GCE. Furthermore, the integration of Co helps to improve the conductivity and promote the lower onset electro-oxidation potential (-0.58 V) toward the hydrazine electro-oxidation reaction. In particular, the CoNPs/NCNTs-1 catalysts showed significant catalytic activity and stability performances i.e., the i-t curves showed notable stability when compared with their initial current responses, even after 10 days, which indicates the significant durability of the catalyst materials. This work could present a new approach for the design of efficient electrode materials, which can be used as a favorable candidate for the electro-oxidation of liquid fuels in fuel cell applications.
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Project description:Long cycle performance is a crucial requirement in energy storage devices. New formulations and/or improvement of "conventional" materials have been investigated in order to achieve this target. Here we explore the performance of a novel type of carbon nanospheres (CNSs) with three heteroatom co-doped (nitrogen, phosphorous and sulfur) and high specific surface area as anode materials for lithium ion batteries. The CNSs were obtained from carbonization of highly-crosslinked organo (phosphazene) nanospheres (OPZs) of 300 nm diameter. The OPZs were synthesized via a single and facile step of polycondensation reaction between hexachlorocyclotriphosphazene (HCCP) and 4,4'-sulphonyldiphenol (BPS). The X-ray Photoelectron Spectroscopy (XPS) analysis showed a high heteroatom-doping content in the structure of CNSs while the textural evaluation from the N₂ sorption isotherms revealed the presence of micro- and mesopores and a high specific surface area of 875 m²/g. The CNSs anode showed remarkable stability and coulombic efficiency in a long charge-discharge cycling up to 1000 cycles at 1C rate, delivering about 130 mA·h·g-1. This study represents a step toward smart engineering of inexpensive materials with practical applications for energy devices.
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Project description:The efficient electrocatalysts for direct methanol oxidation play an essential role in the electrochemical energy conversion systems for their application in a wide range of portable applications. Consequently, Cu-doped NiO thin films on fluorine-doped tin oxide (FTO) were successfully prepared by the co-sputtering deposition technique, using various deposition times (300, 600, 900, and 1200 seconds), and producing films of different thicknesses (30, 55, 90, and 120 nm, respectively). X-ray diffraction (XRD) revealed the ideal crystallinity of the structure of the prepared films and was used to observe the effect of the thickness of the films on the crystal size. Energy-dispersive X-ray spectroscopy (EDS) confirmed the purity of the deposited film without any contamination. Field emission scanning electron microscopy (FESEM) images confirmed the film thickness increase with increasing deposition time. The surface roughness value of the Cu-NiO 1200 film was found to be 3.2 nm based on the atomic force microscopy (AFM) measurements. The deposited thin films of different thicknesses have been used as electrocatalysts for methanol oxidation at various concentrations of methanol (0, 0.5, 1, and 2 M), and displayed the highest electrocatalytic performance in 1 M methanol. Cu-doped NiO thin films have the advantage as electrocatalysts where they can be used directly without adding any binder or conducting agents, this is because Cu-doped NiO is deposited with high adhesion and strong electrical contact to the FTO substrate. A clear impact on the catalytic activity with increasing film thickness and a correlation between the film thickness and its catalytic activity was observed. The current density increased by about 60% for the Cu-NiO 1200 sample compared to Cu-NiO 300 sample, with the lowest onset potential of 0.4 V vs. Ag/AgCl. All deposited thin films of different thicknesses exhibited high stability at 0.6 V in 1 M methanol. This will open the window toward using physical deposition techniques for optimizing the electrocatalytic activity of different catalysts for electrocatalytic applications.
| S-EPMC10074234 | biostudies-literature
Project description:Recently, concern has been raised over the transport, transformation, and fate of carbon nanodots (CNDs) after their release into the environment. Their toxicity towards organisms and humans has recently been addressed as an important issue. In this study, a metabolomic approach was employed to obtain an insight into the effect of CNDs (either pristine or doped with nitrogen and nitrogen/sulfur) on zebrafish. Embryos were exposed to concentrations corresponding to lethal concentration (LC) LC50 (550, 400, and 150 μg mL-1), LC50/2 (275, 200, and 75 μg mL-1), and LC50/4 (138, 100, and 38 μg mL-1) of the three CNDs (non-doped, N-doped, and N,S-codoped, respectively) to scrutinize the interactions of the CNDs with the larvae. Numerous differences in the metabolic pathways were recorded in all cases. Seven metabolic pathways were detected in the control larvae. When the larvae were exposed to concentrations equal to LC50, LC50/2, and LC50/4 of non-doped CNDs, 12, 12, and 3 metabolic pathways were detected, respectively. In the case of N-doped CNDs, 4, 7, and 4 pathways were detected, while in the case of N,S-codoped CNDs, 8, 5, and 5 pathways were detected when exposed to concentrations of LC50, LC50/2, and LC50/4, respectively. In all cases, certain metabolic pathways were altered while others were either down-regulated or up-regulated. Some of these changes include the activation of alanine, aspartate, and glutamate metabolism, aminoacyl-tRNA biosynthesis, butanoate metabolism, D-glutamine, and D-glutamate metabolism, glutathione metabolism, selenoamino acid metabolism, valine, leucine, and isoleucine degradation pathways. Moreover, the deactivation of starch and sucrose metabolism, the glycine, serine, and threonine metabolism, among others, were recorded. Our findings underline the importance to further study the impact of CNDs on marine organisms. As zebrafish has been shown to share many similarities with humans in bioprocesses and genome, it can be assumed that CNDs may also pose a threat to human health.
| S-EPMC7918839 | biostudies-literature
Project description:Molecularly well-defined Ni sites at heterogeneous interfaces were derived from the incorporation of Ni2+ ions into heteroatom-doped graphene. The molecular Ni sites on graphene were redox-active. However, they showed poor activity toward oxygen evolution reaction (OER) in KOH aqueous solution. We demonstrated for the first time that the presence of Fe3+ ions in the solution could bond at the vicinity of the Ni sites with a distance of 2.7 Å, generating molecularly sized and heterogeneous Ni-Fe sites anchored on doped graphene. These Ni-Fe sites exhibited markedly improved OER activity. The Pourbaix diagram confirmed the formation of the Ni-Fe sites and revealed that the Ni-Fe sites adsorbed HO- ions with a bridge geometry, which facilitated the OER electrocatalysis.
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Project description:In this work, high-level heteroatom doped two-dimensional hierarchical carbon architectures (H-2D-HCA) are developed for highly efficient Li-ion storage applications. The achieved H-2D-HCA possesses a hierarchical 2D morphology consisting of tiny carbon nanosheets vertically grown on carbon nanoplates and containing a hierarchical porosity with multiscale pore size. More importantly, the H-2D-HCA shows abundant heteroatom functionality, with sulfur (S) doping of 0.9% and nitrogen (N) doping of as high as 15.5%, in which the electrochemically active N accounts for 84% of total N heteroatoms. In addition, the H-2D-HCA also has an expanded interlayer distance of 0.368 nm. When used as lithium-ion battery anodes, it shows excellent Li-ion storage performance. Even at a high current density of 5 A g-1, it still delivers a high discharge capacity of 329 mA h g-1 after 1,000 cycles. First principle calculations verifies that such unique microstructure characteristics and high-level heteroatom doping nature can enhance Li adsorption stability, electronic conductivity and Li diffusion mobility of carbon nanomaterials. Therefore, the H-2D-HCA could be promising candidates for next-generation LIB anodes.
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Project description:Heteroatom-doped porous carbon membranes (HPCMMs) with a tailor-made pore architecture, chemical composition, atomic structural order, and surface state represent an exciting family of porous carbon materials for diverse potential applications in catalysis, water treatment, biofiltration, energy conversion/storage, and so forth. Conventional porous carbon membranes possess intrinsic structural integrity, interconnectivity, and chemical purity across the atomic-to-macro world and have been popularly incorporated into devices as separators or chemically inert conductive supports, circumventing otherwise the inevitable complicated processing and structure weakness of their fine powderous counterpart. Motivated by the distinguished heteroatom-doping effect that revolutionizes the chemical and physical nature of carbon materials, the HPCMM research surges very recently, and focuses not only on the eminent conductive supports or separators but also on electro(co)catalysts in energy devices. Synergy of the porous nature, incorporation of heteroatoms, and the membrane state creates a vivid profile pattern and new task-specific usage. It is also noteworthy that the inherent structural merits of HPCMMs plus a high electron conductivity imbue them as a reliable binder-free model electrode to derive the intrinsic structure-property relationship of porous carbons in electrochemical environments, excluding the complex and adverse factors in association with polymer binders in carbon powder-based electrodes. HPCMMs are of both intense academic interest and practical value because of their well-defined properties endowed by controllable structure and porosity at both atomic and macroscopic scales in a membrane form. The sole aim of this article is to bring this group of porous carbon materials to the forefront so their comprehensive properties and functions can be better understood to serve the carbon community to address pressing materials challenges in our society. In this Account, we highlight the latest discovery and proceedings of HPCMMs, particularly the advancements in how to tailor structures and properties of HPCMMs by rational structure design of porous polymer membranes as sacrificial template built up especially from heteroatom-rich poly(ionic liquid)s (PILs). We will also stress the carbonization craft and the state-of-the-art electrochemical applications for HPCMMs. Key factors and thoughts in heteroatom doping and porous systems in HPCMMs are discussed. A future perspective of the challenges and promising potential of HPCMMs is cast on the basis of these achievements.
| S-EPMC7640738 | biostudies-literature
Project description:A series of platinum catalysts supported on carbon nanofibers with various heteroatom dopings were synthesized to investigate the effect of the local platinum environment on the catalytic activity and selectivity in aqueous phase reforming (APR) of ethylene glycol (EG). Typical carbon dopants such as oxygen, nitrogen, sulfur, phosphorus, and boron were chosen based on their ability to bring acidic or basic functional groups to the carbon surface. In situ X-ray absorption spectroscopy (XAS) was used to identify the platinum oxidation state and platinum species formed during APR of EG through multivariate curve resolution alternating least-squares analysis, observing differences in activity, selectivity, and platinum local environment among the catalysts. The platinum-based catalyst on the nitrogen-doped carbon support demonstrated the most favorable properties for H2 production due to high Pt dispersion and basicity (H2 site time yield 22.7 h-1). Direct Pt-N-O coordination was identified by XAS in this catalyst. The sulfur-doped catalyst presented Pt-S contributions with the lowest EG conversion rate and minimal production of the gas phase components. Boron and phosphorus-doped catalysts showed moderate activity, which was affected by low platinum dispersion on the carbon support. The phosphorus-doped catalyst showed preferential selectivity to alcohols in the liquid phase, associated with the presence of acid sites and Pt-P contributions observed under APR conditions.
| S-EPMC10949196 | biostudies-literature
Project description:We report herein that zinc and cobalt bimetallic-organic-framework (BMOF) crystalline micro-rods are able to be constructed instantly with the eco-friendly glutamate ligand and building unit of double metallic ions. After carbonization and acid leaching of these precursors, the resultant heteroatom-doped porous carbon occupies not only the enriched mesopore architectures but the ultrathin graphitic networks. Moreover, due to cyclizing dehydration reaction of the glutamate ligand upon thermal conversion, the predominant pyrrolic and pyridinic nitrogen atom sites within the carbon lattices are achieved. The supercapacitor electrodes from these carbonaceous materials without any conductive addictive deliver an impressive specific gravimetric capacitance of 230 F g-1 and a specific areal capacitance of 50 μF cm-2 at a current density of 1 A g-1 in alkaline aqueous electrolyte.
| S-EPMC9064546 | biostudies-literature