Identification of catalytic sites for oxygen reduction and oxygen evolution in N-doped graphene materials: Development of highly efficient metal-free bifunctional electrocatalyst

被引:1086
|
作者
Yang, Hong Bin [1 ]
Miao, Jianwei [1 ]
Hung, Sung-Fu [2 ]
Chen, Jiazang [1 ]
Tao, Hua Bing [1 ]
Wang, Xizu [3 ]
Zhang, Liping [1 ]
Chen, Rong [1 ]
Gao, Jiajian [1 ]
Chen, Hao Ming [2 ]
Dai, Liming [4 ]
Liu, Bin [1 ]
机构
[1] Nanyang Technol Univ, Sch Chem & Biomed Engn, 62 Nanyang Dr, Singapore 637459, Singapore
[2] Natl Taiwan Univ, Dept Chem, 1,Sec 4,Roosevelt Rd, Taipei 10617, Taiwan
[3] ASTAR, IMRE, 08-03,2 Fusionopolis Way, Singapore 138634, Singapore
[4] Case Western Reserve Univ, Dept Macromol Sci & Engn, 10900 Euclid Ave, Cleveland, OH 44106 USA
来源
SCIENCE ADVANCES | 2016年 / 2卷 / 04期
基金
新加坡国家研究基金会; 美国国家科学基金会;
关键词
IN-SITU; NITROGEN; WATER; EDGE; SULFUR; OXIDE; ELECTROCHEMISTRY; NANOPARTICLES; CONVERSION; SUBSTRATE;
D O I
10.1126/sciadv.1501122
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
Oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are critical to renewable energy conversion and storage technologies. Heteroatom-doped carbon nanomaterials have been reported to be efficient metal-free electrocatalysts for ORR in fuel cells for energy conversion, as well as ORR and OER in metal-air batteries for energy storage. We reported that metal-free three-dimensional (3D) graphene nanoribbon networks (N-GRW) doped with nitrogen exhibited superb bifunctional electrocatalytic activities for both ORR and OER, with an excellent stability in alkaline electrolytes (for example, KOH). For the first time, it was experimentally demonstrated that the electron-donating quaternary N sites were responsible for ORR, whereas the electron-withdrawing pyridinic N moieties in N-GRW served as active sites for OER. The unique 3D nanoarchitecture provided a high density of the ORR and OER active sites and facilitated the electrolyte and electron transports. As a result, the as-prepared N-GRW holds great potential as a low-cost, highly efficient air cathode in rechargeable metal-air batteries. Rechargeable zinc-air batteries with the N-GRW air electrode in a two-electrode configuration exhibited an open-circuit voltage of 1.46 V, a specific capacity of 873 mAh g(-1), and a peak power density of 65 mW cm(-2), which could be continuously charged and discharged with an excellent cycling stability. Our work should open up new avenues for the development of various carbon-based metal-free bifunctional electrocatalysts of practical significance.
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页数:11
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