Nitrogen and Phosphate Co‐doped Graphene as Efficient Bifunctional Electrocatalysts by Precursor Modulation Strategy for Oxygen Reduction and Evolution Reactions

双功能 杂原子 石墨烯 化学 析氧 电化学 催化作用 碳纤维 电催化剂 金属 氧化还原 无机化学 材料科学 组合化学 纳米技术 电极 有机化学 物理化学 复合材料 戒指(化学) 复合数
作者
Xiaoran Zhang,Xiao Zhang,Xue Xiang,Can Pan,Qing‐Hao Meng,Chao Hao,Zhi Qun Tian,Pei Kang Shen,San Ping Jiang
出处
期刊:ChemElectroChem [Wiley]
卷期号:8 (17): 3262-3272 被引量:13
标识
DOI:10.1002/celc.202100599
摘要

Abstract Heteroatoms doped carbon‐based metal‐free catalysts are important candidates as alternatives for precious group metal (PGM) catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) – two of the most important reactions in electrochemical energy conversion and storage areas. Despite the significant efforts in developing heteroatoms doped metal‐free electrocatalysts with enhanced electrocatalytic activity, few studies focus on their bifunctional activities for ORR and OER due to the unclear catalytic mechanism and complicated active sites configurations. Herein, a series of nitrogen and phosphate co‐doped carbon‐based catalysts (NP/C) are successfully synthesized via a precursor modulation strategy. In this method, 5‐aminouracil, 2, 6‐diaminopyridine and 1, 3‐diaminobenzene are selected to modulate pyridinic N (N P ), graphitic N (N G ) and pyrrolic N (N PY ) sites, respectively, while phytic acid is used as P sites. The results demonstrate that the N and P co‐doped graphene with N P +N G +P configuration shows increased ORR performance, and on the other hand, the N P +N PY +P configuration enhances OER. Density functional theory (DFT) calculation demonstrates that different NP configurations formed by precursor modulation induce different electronic structure on surrounding carbon atoms, providing a possibility to manipulate intermediates energy in reaction pathway for ORR and OER. This study sheds new light on revealing the intrinsic correlation between active site configurations and catalytic bifunctional activity and selectivity of graphene based electrocatalysts for oxygen redox reactions.
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