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Vol. 10 No. 1 (2018)

Creation of Triple Hierarchical Micro-Meso-Macroporous N-doped Carbon Shells with Hollow Cores Toward the Electrocatalytic Oxygen Reduction Reaction

https://doi.org/10.1007/s40820-017-0157-1
Ruohao Xing
School of Materials Science and Engineering, Shanghai University, 99 Shangda Road, Shanghai 200444, People’s Republic of China
Tingsheng Zhou
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, People’s Republic of China
Yao Zhou
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, People’s Republic of China
Ruguang Ma
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, People’s Republic of China
Qian Liu
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, People’s Republic of China
Jun Luo
School of Materials Science and Engineering, Shanghai University, 99 Shangda Road, Shanghai 200444, People’s Republic of China
Jiacheng Wang
State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, People’s Republic of China

Corresponding Author: Jiacheng Wang

jiacheng.wang@mail.sic.ac.cn

Nano-Micro Letters, Vol. 10 No. 1 (2018), Article Number: 3

Abstract

A series of triple hierarchical micro-meso-macroporous N-doped carbon shells with hollow cores have been successfully prepared via etching N-doped hollow carbon spheres with CO2 at high temperatures. The surface areas, total pore volumes and micropore percentages of the CO2-activated samples evidently increase with increasing activation temperature from 800 to 950 °C, while the N contents show a contrary trend from 7.6 to 3.8 at%. The pyridinic and graphitic nitrogen groups are dominant among various N-containing groups in the samples. The 950 °C-activated sample (CANHCS-950) has the largest surface area (2072 m2 g−1), pore volume (1.96 cm3 g−1), hierarchical micro-mesopore distributions (1.2, 2.6 and 6.2 nm), hollow macropore cores (~91 nm) and highest relative content of pyridinic and graphitic N groups. This triple micro-meso-macropore system could synergistically enhance the activity because macropores could store up the reactant, mesopores could reduce the transport resistance of the reactants to the active sites, and micropores could be in favor of the accumulation of ions. Therefore, the CANHCS-950 with optimized structure shows the optimal and comparable oxygen reduction reaction (ORR) activity but superior methanol tolerance and long-term durability to commercial Pt/C with a 4e−-dominant transfer pathway in alkaline media. These excellent properties in combination with good stability and recyclability make CANHCSs among the most promising metal-free ORR electrocatalysts reported so far in practical applications.


Highlights:


1 A series of triple hierarchical micro-meso-macroporous N-doped carbon shells have been successfully prepared via etching N-doped hollow carbon spheres with CO2 at high temperatures.
2 The activated sample has the large surface area and pore volume, hierarchical micro-mesopore distributions, hollow macropore cores and controllable nitrogen contents.
3 The optimized sample shows the comparable oxygen reduction reaction activity but superior methanol tolerance and long-term durability to commercial Pt/C with a 4e−-dominant transfer pathway in alkaline media.

Keywords

Hierarchical pores Hollow cores N doping Electrocatalysis Oxygen reduction reaction
Xing, Ruohao, Tingsheng Zhou, Yao Zhou, Ruguang Ma, Qian Liu, Jun Luo, and Jiacheng Wang. 2017. “Creation of Triple Hierarchical Micro-Meso-Macroporous N-Doped Carbon Shells With Hollow Cores Toward the Electrocatalytic Oxygen Reduction Reaction”. Nano-Micro Letters 10 (1):3. https://doi.org/10.1007/s40820-017-0157-1.
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