title: Synergistically Enhanced Electrocatalytic Activity of Sandwich-like N-Doped Graphene/Carbon Nanosheets Decorated by Fe and S for Oxygen Reduction Reaction.
abstract: Although N-doped graphene-based electrocatalysts have shown good performance for oxygen reduction reaction (ORR), they still suffer from the single-type active site in the as-prepared catalyst, limited accessible active surface area because of easy aggregation of graphene, and harsh condition for preparation process of graphene. Therefore, further developing a novel type of graphene-based electrocatalyst by a facile and environmentally benign method is highly anticipated. Herein, we first fabricate a sandwich-like graphene/carbon hybrid using graphene oxide (GO) and nontoxic starch. Then the graphene/carbon hybrid undergoes postprocessing with iron(III) chloride (FeCl3) and potassium sulfocyanide (KSCN) to acquire N-doped graphene/carbon nanosheets decorated by Fe and S. The resultant displays the features of interpenetrated three-dimensional hierarchical architecture composed of abundant sandwich-like graphene/carbon nanosheets and low graphene content in as-prepared sample. Remarkably, the obtained catalyst possesses favorable kinetic activity due to the unique structure and synergistic effect of N, S, and Fe on ORR, showing high onset potential, low Tafel slope, and nearly four-electron pathway. Meanwhile, the catalyst exhibits strong methanol tolerance and excellent long-term durability. In view of the multiple active sites, unique hierarchical structure, low graphene content, and outstanding electrochemical activity of the as-prepared sample, this work could broaden the thinking to develop more highly efficient graphene/carbon electrocatalysts for ORR in fuel cells.
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Bao
authors.initials: B
authors.lastname: Men
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Yanzhi
authors.initials: Y
authors.lastname: Sun
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Jia
authors.initials: J
authors.lastname: Liu
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Yang
authors.initials: Y
authors.lastname: Tang
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Yongmei
authors.initials: Y
authors.lastname: Chen
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Pingyu
authors.initials: P
authors.lastname: Wan
authors.affiliation: National Fundamental Research Laboratory of New Hazardous Chemicals Assessment and Accident Analysis, Institute of Applied Electrochemistry, Beijing University of Chemical Technology , Beijing 100029, China.
authors.forename: Junqing
authors.initials: J
authors.lastname: Pan
keywords: electrocatalytic activity; graphene/carbon nanosheets; multiple active sites; oxygen reduction reaction; synergistic effect