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多杂原子掺杂碳材料对氧还原反应催化活性的增强作用。

Enhancement of ORR catalytic activity by multiple heteroatom-doped carbon materials.

作者信息

Kim Dae-wook, Li Oi Lun, Saito Nagahiro

机构信息

Department of Materials, Physics and Energy Engineering, Nagoya University, Furo-cho, Chikusa-ku, Nagoya, Japan.

出版信息

Phys Chem Chem Phys. 2015 Jan 7;17(1):407-13. doi: 10.1039/c4cp03868a.

Abstract

Heteroatom-doped carbon matrices have been attracting significant attention due to their superior electrochemical stability, light weight and low cost. Hence, in this study, various types of heteroatom, including single dopants of N, B and P and multiple dopants of B-N and P-N with a carbon matrix were synthesized by an innovative method named the solution plasma process. The heteroatom was doped into the carbon matrix during the discharge process by continuous dissociation and recombination of precursors. The chemical bonding structure, ORR activity and electrochemical performance were compared in detail for each single dopant and multiple dopants. According to the Raman spectra, the carbon structures were deformed by the doped heteroatoms in the carbon matrix. In comparison with N-doped structures (NCNS), the ORR potential of PN-doped structures (PNCNS) was positively shifted from -0.27 V to -0.24 V. It was observed that doping with N decreased the bonding between P and C in the matrix. The multiple doping induced additional active sites for ORR which further enhanced ORR activity and stability. Therefore, PNCNS is a promising metal-free catalyst for ORR at the cathode in a fuel cell.

摘要

杂原子掺杂的碳基体因其卓越的电化学稳定性、轻质和低成本而备受关注。因此,在本研究中,通过一种名为溶液等离子体工艺的创新方法,合成了包括N、B和P的单一掺杂剂以及B-N和P-N与碳基体的多种掺杂剂在内的各种类型的杂原子。在放电过程中,通过前驱体的连续解离和重组,杂原子被掺杂到碳基体中。对每种单一掺杂剂和多种掺杂剂的化学键结构、氧还原反应(ORR)活性和电化学性能进行了详细比较。根据拉曼光谱,碳基体中的掺杂杂原子使碳结构发生了变形。与N掺杂结构(NCNS)相比,P-N掺杂结构(PNCNS)的ORR电位从-0.27 V正向移动至-0.24 V。据观察,掺杂N会降低基体中P与C之间的键合。多种掺杂诱导了额外的ORR活性位点,进一步增强了ORR活性和稳定性。因此,PNCNS是一种有前景的用于燃料电池阴极ORR的无金属催化剂。

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