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1.
A novel OER electrocatalyst, namely oxygen‐incorporated amorphous cobalt sulfide porous nanocubes (A‐CoS4.6O0.6 PNCs), show advantages over the benchmark RuO2 catalyst in alkaline/neutral medium. Experiments combining with calculation demonstrate that the desirable O* adsorption energy, associated with the distorted CoS4.6O0.6 octahedron structure and the oxygen doping, contribute synergistically to the outstanding electrocatalytic activity.  相似文献   

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The development of low‐cost, efficient, and stable electrocatalysts for the oxygen reduction reaction (ORR) is desirable but remains a great challenge. Herein, we made a highly reactive and stable isolated single‐atom Fe/N‐doped porous carbon (ISA Fe/CN) catalyst with Fe loading up to 2.16 wt %. The catalyst showed excellent ORR performance with a half‐wave potential (E 1/2) of 0.900 V, which outperformed commercial Pt/C and most non‐precious‐metal catalysts reported to date. Besides exceptionally high kinetic current density (J k) of 37.83 mV cm−2 at 0.85 V, it also had a good methanol tolerance and outstanding stability. Experiments demonstrated that maintaining the Fe as isolated atoms and incorporating nitrogen was essential to deliver the high performance. First principle calculations further attributed the high reactivity to the high efficiency of the single Fe atoms in transporting electrons to the adsorbed OH species.  相似文献   

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Designing highly efficient electrocatalysts for oxygen evolution reaction (OER) plays a key role in the development of various renewable energy storage and conversion devices. In this work, we developed metallic Co4N porous nanowire arrays directly grown on flexible substrates as highly active OER electrocatalysts for the first time. Benefiting from the collaborative advantages of metallic character, 1D porous nanowire arrays, and unique 3D electrode configuration, surface oxidation activated Co4N porous nanowire arrays/carbon cloth achieved an extremely small overpotential of 257 mV at a current density of 10 mA cm−2, and a low Tafel slope of 44 mV dec−1 in an alkaline medium, which is the best OER performance among reported Co‐based electrocatalysts to date. Moreover, in‐depth mechanistic investigations demonstrate the active phases are the metallic Co4N core inside with a thin cobalt oxides/hydroxides shell during the OER process. Our finding introduces a new concept to explore the design of high‐efficiency OER electrocatalysts.  相似文献   

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The development of highly efficient metal‐free carbon electrocatalysts for the oxygen reduction reaction (ORR) is one very promising strategy for the exploitation and commercialization of renewable and clean energy, but this still remains a significant challenge. Herein, we demonstrate a facile approach to prepare three‐dimensional (3D) N‐doped carbon with a sp3/sp2 carbon interface derived from ionic liquids via a simple pyrolysis process. The tunable hybrid sp3 and sp2 carbon composition and pore structures stem from the transformation of ionic liquids to polymerized organics and introduction of a Co metal salt. Through tuning both composition and pores, the 3D N‐doped nanocarbon with a high sp3/sp2 carbon ratio on the surface exhibits a superior electrocatalytic performance for the ORR compared to that of the commercial Pt/C in Zn–air batteries. Density functional theory calculations suggest that the improved ORR performance can be ascribed to the existence of N dopants at the sp3/sp2 carbon interface, which can lower the theoretical overpotential of the ORR.  相似文献   

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Electrochemically functional porous membranes of low cost are appealing in various electrochemical devices used in modern environmental and energy technologies. Herein we describe a scalable strategy to construct electrochemically active, hierarchically porous carbon membranes containing atomically dispersed semi‐metallic Se, denoted SeNCM. The isolated Se atoms were stabilized by carbon atoms in the form of a hexatomic ring structure, in which the Se atoms were located at the edges of graphitic domains in SeNCM. This configuration is different from that of previously reported transition/noble metal single atom catalysts. The positively charged Se, enlarged graphitic layers, robust electrochemical nature of SeNCM endow them with excellent catalytic activity that is superior to state‐of‐the‐art commercial Pt/C catalyst. It also has long‐term operational stability for hydrazine oxidation reaction in practical hydrazine fuel cell.  相似文献   

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Although multilayer films have been extensively reported, most compositions have been limited to non‐catalytically active materials (e.g. polymers, proteins, lipids, or nucleic acids). Herein, we report the preparation of binder‐free multilayer metallic mesoporous films with sufficient accessibility for high electrocatalytic activity by using a programmed electrochemical strategy. By precisely tuning the deposition potential and duration, multilayer mesoporous architectures consisting of alternating mesoporous Pd layers and mesoporous PdPt layers with controlled layer thicknesses can be synthesized within a single electrolyte, containing polymeric micelles as soft templates. This novel architecture, combining the advantages of bimetallic alloys, multilayer architectures, and mesoporous structures, exhibits high electrocatalytic activity for both the methanol oxidation reaction (MOR) and the ethanol oxidation reaction (EOR).  相似文献   

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The synthesis of highly microporous, epoxy‐functionalized porous organic polymers (ep‐POPs) by a one‐pot, catalyst‐free Diels–Alder cycloaddition polymerization is reported. The high oxygen content of ep‐POPs offer efficient hydrogen‐bonding sites for water molecules, thus leading to high water‐uptake capacities up to 39.2–42.4 wt % under a wide temperature range of 5–45 °C, which covers the span of climatic conditions and manufacturing applications in which such materials might be used. Importantly, ep‐POPs demonstrated regeneration temperatures as low as 55 °C, as well as excellent water stability, recyclability, and high specific surface areas up to 852 m2 g−1.  相似文献   

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Recent developments in the field of microporous and mesoporous materials show the potential for applications in the area of environment protection, renewable energy exploitation, and health care.  相似文献   

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Trimetallic oxyhydroxides are one of the most effective materials for oxygen evolution reaction (OER) catalysis, a key process for water splitting. Herein, we describe a facile wet‐chemical method to directly grow a series of coralloid trimetallic oxyhydroxides on arbitrary substrates such as nickel foam (NF) and carbon nanotubes (CNTs). The amount of iron in these oxyhydroxide sponges on NF and CNTs was precisely controlled, revealing that the electrocatalytic activity of the WCoFe trimetallic oxyhydroxides depends on the Fe amount in a volcano‐like fashion. The optimized W0.5Co0.4Fe0.1/NF catalyst exhibited an overpotential of only 310 mV to deliver a large current density of 100 mA cm−2 and a very low Tafel slope of 32 mV dec−1. It also showed superior stability with negligible activity decay after use in the OER for 21 days (>500 h). X‐ray photoelectron spectroscopy revealed that the addition of Fe leads to an on average lower Co oxidation state, which contributes to the enhanced OER performance.  相似文献   

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An iron oxide decorated nickel iron alloy nanoparticle/porous graphene hybrid exhibits high electrocatalytic activity and excellent durability toward oxygen evolution reaction (OER). It displays a low overpotential of 274 mV at 10 mA cm−2, and low Tafel slope of 37 mV dec−1, showing a superior performance to the state-of-the-art RuO2 OER electrocatalyst.  相似文献   

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In this study, we successfully synthesized CuxCoyS supraparticles (SPs) on the nanoscale featuring multiple pores inside and strong absorption from 400 to 900 nm. Porous CuxCoyS SPs produced the highest reactive oxygen species (ROS) yield (1.39) when illuminated with near‐infrared (NIR) light. Furthermore, we demonstrated that CuxCoyS SPs could be used to identify cancer cells through intracellular telomerase‐responsive fluorescence (FL) imaging in living cells. Because the CuxCoyS SPs were associated with telomerase‐responsive bioimaging and high ROS production, they can be efficiently used in the diagnosis and therapy of tumors with high selectivity and excellent therapeutic effects in vivo. This study provides a new vision for the creation of multifunctional SPs, which can be used as cellular sensors and control tools for pathologies across a broad range of biological systems.  相似文献   

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Russian Journal of Electrochemistry - At present, the graphene hybrid as electrode material demonstrates the efficient performance for oxygen evolution reaction (OER). OER influences some important...  相似文献   

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