【摘 要】
：
Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction (ORR) is extremely important for promoting the commercialized applications of such catalysts.In this work,t
【机 构】
：
School of Materials Science and Engineering, China University of Petroleum(East China), Qingdao 2665
论文部分内容阅读
Facile preparation of cost-effective and durable porous carbon-supported non-precious-metal/nitrogen electrocatalysts for oxygen reduction reaction (ORR) is extremely important for promoting the commercialized applications of such catalysts.In this work,the FeCl3-containing porphyrinato iron-based covalent porous polymer (FeCl3.FePor-CPP) was fabricated in-situ onto porous corncob biomass supports via a simple one-pot method.Subsequent thermal-reduction pyrolysis at 700 ℃-900 ℃ with CO2 gas as an activating agent resulted in Fe2O3-decorated and N-doped graphitic carbon composite Fe2O3@NC&bio-C with a high degree of graphitization of Fe-involved promotion during pyrolysis (Fe2O3 =FeCl3.FePor-CPP derived Fe2O3;NC =N-doped graphene analog;bio-C =the corncob-derived hierarchically porous graphitic biomass carbon framework).The derived α-Fe2O3 and γ-Fe2O3 nanocrystals (5-10nm particle diameter)were all immobilized on the N-doped bio-C micro/nanofibers.Notably,the Fe2O3@NC&bio-C obtained at the pyrolysis temperature of 800 C (Fe2O3@NC&bio-C-g00),exhibited unusual ORR catalytic efficiency via a 4-electron pathway with the onset and half-wave potentials of 0.96V and 0.85V vs.RHE,respectively.In addition,Fe2O3@NC&bio-C-800 also exhibited a high and stable limiting current density of-6.0mAcm-2,remarkably stability (larger than 91％ retention after 10000s),and good methanol tolerance.The present work represents one of the best results for iron-based biomass material ORR catalysts reported to date.The high ORR activity is attributed to the uniformly distributed α-Fe2O3 and y-Fe2O3 nanoparticles on the N-enriched carbon matrix with a large specific surface area of 772.6m2 g-1.This facilitates favor faster electron movement and better adsorption of oxygen molecules on the surface of the catalyst.Nevertheless,comparative studies on the structure and ORR catalytic activity of Fe2O3@NC&bioC-800 with Fe2O3@bio-C-800 and NC&bio-C-800 clearly highlight the synergistic effect of the coexisting Fe2O3 nanocrystals,NC and bio-C on the ORR performance.
其他文献
In the light of wireless and non-fossil society based on portable electronics, electric vehicles, and smart grids, secondary batteries with higher energy density, faster charge, and safer operation are pursued persistently [1].Nowadays, commercial lithium
Structural and compositional design of core-shell structure is an effective strategy towards enhanced catalysis.Herein,amorphous MnO2 nanosheets and K+-intercalated layered MnO2 nanosheets are controllably assembled over Fe2O3 spindles,in which the MnO2 n
A series of Pt/C catalysts for proton exchange membrane fuel cells (PEMFCs) with various metal Ioadings is synthesized by a microwave-assisted polyol process via mixing an extremely stable platinum colloid (＞ 3 months\' shelf life) from single batch pre
Carbon materials have been widely used as electrodes,but the mechanistic roles are still not clear due to the complexity of the carbon surface chemistry.Herein we clarify that intrinsic material properties of carbon have to be activated by extrinsic facto
Metal-organic framework (MOF) derived hybrid materials have been developed as an efficient non-noblemetal electrocatalysts for clean energy conversion systems.In this work,a Co-based MOF containing nitrogen and oxygen heteroatoms (Co-NOMOF) mixed with the
Ordered hierarchical architectures are attractive candidates for electrochemical energy storage applications.Herein,a facile self-template strategy is applied to prepare Fe7Se8 architectures with a monolithic structure via a self-synthesized single precur
Lithium metal is a promising anode material owing to its very low electrochemical potential and ultrahigh specific capacity.However,the growth of lithium dendrites could result in a short lifespan,low coulombic efficiency,and potential safety hazards duri
A new benzothiadiazole-based D-A-D hole transport material (DTBT) has been designed and synthesized with a more planar structure by introducing of thiophene bridges.The results indicate a lower band gap and quite higher hole mobility for the DTBT.Furtherm
Understanding of the oxygen reduction reaction (ORR) mechanism for single atom catalysts is pivotal for the rational design of non-precious metal cathode materials and the commercialization of fuel cells.Herein,a series of non-precious metal electmcatalys
The development of bifunctional oxygen electrocatalysts with high efficiency,high stability,and low cost is of great significance to the industrialization of rechargeable Zn-air batteries.A widely accepted view is that the oxygen reduction reaction (ORR)