Developing an efficient single-atom material (SAM) synthesis and exploring the energy-related catalytic reaction are important but still challenging. A polymerization-pyrolysis-evaporation (PPE) strategy was developed to synthesize N-doped porous carbon (NPC) with anchored atomically dispersed Fe-N catalytic sites. This material was derived from predesigned bimetallic Zn/Fe polyphthalocyanine. Experiments and calculations demonstrate the formed Fe-N site exhibits superior trifunctional electrocatalytic performance for oxygen reduction, oxygen evolution, and hydrogen evolution reactions. In overall water splitting and rechargeable Zn-air battery devices containing the Fe-N SAs/NPC catalyst, it exhibits high efficiency and extraordinary stability. This current PPE method is a general strategy for preparing M SAs/NPC (M=Co, Ni, Mn), bringing new perspectives for designing various SAMs for catalytic application.
The development of highly active and stable bifunctional noble-metal-based electrocatalysts for the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) is a crucial goal for clean and renewable energy, which still remains challenging. Herein, we report an efficient and stable catalyst comprising a Co single atom incorporated in an RuO 2 sphere for HER and OER, in which the Co single atom in the RuO 2 sphere was confirmed by XAS, AC-STEM, and DFT. This tailoring strategy uses a Co single atom to modify the electronic structures of the surrounding Ru atoms and thereby remarkably elevates the electrocatalytic activities. The catalyst requires ultralow overpotentials, 45 mV for HER and 200 mV for OER, to deliver a current density of 10 mA cm À 2 . The theoretical calculations reveal that the energy barriers for HER and OER are lowered after incorporation of a cobalt single atom.
Herein, a facile and cost-effective strategy for hydrothermal synthesis of three-dimensional (3D) MoS2 with adequate active edge sites and advanced hydrogen evolution reaction (HER) performance using polypyrrole (PPy) as template is reported. The MoS2 is first thermally nucleated using hexaammonium heptamolybdate tetrahydrate (NH4)6Mo7O24·4H2O and thiourea as precursor in the presence of PPy, and then they are further annealed to remove PPy at higher temperature to generate 3D MoS2-P. Morphology and composition characterizations reveal that the 3D MoS2-P exhibits a nanoflower morphology. It presents larger stretched “thin folding leaves” and higher mesoporous volume of 0.608 cm3 g−1 than the MoS2 without PPy as template. Importantly, the 3D MoS2-P shows enhanced HER catalytic activity (onset potential at −100 mV) than previously reports that MoS2-based HER catalysts. The large “thin folding leaves” possessing efficient edge active sites and defects are responsible to for the enhanced HER performance, while the high mesoporous volume facilitates the transfer of reaction substrate. Our study provides a facile and cost-effective method for synthesis of 3D MoS2 with advanced HER performances, which has great potential for larger-scale production and practical industrial applications.
Bulky and strong electron-donating dibutylamino groups were incorporated onto the peripheral positions of one of the two phthalocyanine ligands in the bis(phthalocyaninato) terbium complex, resulting in the isolation of heteroleptic double-decker (Pc)Tb{Pc[N(CH)]} {Pc = phthalocyaninate; Pc[N(CH)] = 2,3,9,10,16,17,23,24-octakis(dibutylamino)phthalocyaninate} with the nature of an unsymmetrical molecular structure, a square-antiprismatic coordination geometry, an intensified coordination field strength, and the presence of organic radical-f interaction. As a total result of all these factors, this sandwich-type tetrapyrrole lanthanide single-ion magnet (SIM) exhibits an overall enhanced magnetic performance including a high blocking temperature (T) of 30 K and large effective spin-reversal energy barrier of U = 939 K, rendering it the best sandwich-type tetrapyrrole lanthanide SIM reported thus far.
Developing an efficient single-atom material (SAM) synthesis and exploring the energy-related catalytic reaction are important but still challenging.Apolymerization-pyrolysisevaporation (PPE) strategy was developed to synthesize Ndoped porous carbon (NPC) with anchored atomically dispersed Fe-N 4 catalytic sites.T his material was derived from predesigned bimetallic Zn/Fep olyphthalocyanine. Experiments and calculations demonstrate the formed Fe-N 4 site exhibits superior trifunctional electrocatalytic performance for oxygen reduction, oxygen evolution, and hydrogen evolution reactions.Inoverall water splitting and rechargeable Znair battery devices containing the Fe-N 4 SAs/NPC catalyst, it exhibits high efficiency and extraordinary stability.T his current PPE method is ag eneral strategy for preparing M SAs/NPC (M = Co,N i, Mn), bringing new perspectives for designing various SAMs for catalytic application.
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