Polymer nanosheets derived porous carbon nanosheets as high efficient electrocatalysts for oxygen reduction reaction. 2018

Wenbei Zhang, and Sai Sun, and Lingyun Yang, and Chenbao Lu, and Yafei He, and Chao Zhang, and Ming Cai, and Yefeng Yao, and Fan Zhang, and Xiaodong Zhuang
State Key Laboratory of Metal Matrix Composites & Shanghai Key Laboratory of Electrical Insulation and Thermal Ageing, School of Chemistry and Chemical Engineering, Shanghai Jiao Tong University, Dongchuan Road 800, 200240 Shanghai, China.

Porous carbon nanosheets and corresponding heteroatom doped porous carbon nanosheets have shown great potential as active materials for energy conversion and storage in recent years. However, it remains great challenge to prepare such kind of new two-dimensional (2D) polymer nanosheets without using any templates. In this work, thiadiazole-containing expanded heteroazaporphyrinoid was designed as the building blocks for preparation of free-standing N/S-containing polymer nanosheets (PN) without using any templates. Most importantly, such PN can coordinate with transition metal ions to prepare Fe, N, and S containing PN-Fe. By using these PN-Fe as precursors, Fe/N/S co-doped porous carbon nanosheets (PCN-FeNS) can be facilely prepared by direct pyrolysis under inert condition. The N and S contents of PCN-FeNS can reach up to 6.4 at.% and 0.8 at.%, respectively. For proof-of-concept, PCN-FeNS were further used as electrochemical catalysts for oxygen reduction reaction (ORR) in both alkaline and neutral media. Benefiting from the high surface area and rich-doping character, PCN-FeNS exhibited relatively high half-wave potential of down to 0.71 V, via a four-electron transfer mechanism (n = 3.87 at 0.65 V), as well as high diffusion limiting current density (JL = 5.02 mA cm-2), which are comparable to commercial precious metal based electrocatalysts. This study not only offers a new method to prepare conjugated polymer nanosheets, but also provides a new strategy to fabricate Fe/N/S co-doped porous carbon nanosheets for versatile energy-related applications.

UI MeSH Term Description Entries
D007501 Iron A metallic element with atomic symbol Fe, atomic number 26, and atomic weight 55.85. It is an essential constituent of HEMOGLOBINS; CYTOCHROMES; and IRON-BINDING PROTEINS. It plays a role in cellular redox reactions and in the transport of OXYGEN. Iron-56,Iron 56
D009584 Nitrogen An element with the atomic symbol N, atomic number 7, and atomic weight [14.00643; 14.00728]. Nitrogen exists as a diatomic gas and makes up about 78% of the earth's atmosphere by volume. It is a constituent of proteins and nucleic acids and found in all living cells.
D010084 Oxidation-Reduction A chemical reaction in which an electron is transferred from one molecule to another. The electron-donating molecule is the reducing agent or reductant; the electron-accepting molecule is the oxidizing agent or oxidant. Reducing and oxidizing agents function as conjugate reductant-oxidant pairs or redox pairs (Lehninger, Principles of Biochemistry, 1982, p471). Redox,Oxidation Reduction
D010100 Oxygen An element with atomic symbol O, atomic number 8, and atomic weight [15.99903; 15.99977]. It is the most abundant element on earth and essential for respiration. Dioxygen,Oxygen-16,Oxygen 16
D011108 Polymers Compounds formed by the joining of smaller, usually repeating, units linked by covalent bonds. These compounds often form large macromolecules (e.g., BIOPOLYMERS; PLASTICS). Polymer
D002244 Carbon A nonmetallic element with atomic symbol C, atomic number 6, and atomic weight [12.0096; 12.0116]. It may occur as several different allotropes including DIAMOND; CHARCOAL; and GRAPHITE; and as SOOT from incompletely burned fuel. Carbon-12,Vitreous Carbon,Carbon 12,Carbon, Vitreous
D002384 Catalysis The facilitation of a chemical reaction by material (catalyst) that is not consumed by the reaction. Catalyses
D003035 Cobalt A trace element that is a component of vitamin B12. It has the atomic symbol Co, atomic number 27, and atomic weight 58.93. It is used in nuclear weapons, alloys, and pigments. Deficiency in animals leads to anemia; its excess in humans can lead to erythrocytosis. Cobalt-59,Cobalt 59
D000077319 Pyrolysis High temperature decomposition without addition of extra air or oxygen. It yields syngas, bio-oil and bio-char. Pyrolyses
D001372 Aza Compounds Organic chemicals where carbon atoms have been replaced by nitrogen atoms. Compounds, Aza

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