Nan Yanli, He Yuanyuan, Zhang Zihan, Wei Jian, Zhang Yubin
School of Material Science and Engineering, Shaanxi Key Laboratory of Nano Materials and Technology, Xi'an University of Architecture and Technology Xi'an 710055 China
Ningbo University of Finance and Economics Ningbo 315175 China
RSC Adv. 2021 Nov 3;11(56):35463-35471. doi: 10.1039/d1ra06458d. eCollection 2021 Oct 28.
The development of efficient, cost-effective and stable N-doped carbon material with catalytic activity as an excellent catalyst for the oxygen evolution reaction (OER) is critical for renewable energy systems. In this study, the unique tip-half-closed N-doped carbon nanohorns (THC-N-CNHs) were firstly produced by the positive pressure-assisted arc discharge method using N as the nitrogen source. Benefitting from the novel tip-half-closed structure and sufficient porosity, the specific surface area (SSA) of THC-N-CNHs is calculated to be 670 m g without any further treatment, which is three times larger than that of traditional tip-closed CNHs. More importantly, the content of nitrogen can achieve ∼1.98 at% with noticeable pyridinic-N enrichment, increasing the number of active sites for the OER. Furthermore, the three-dimensional spherical feature and the unique pore structure for THC-N-CNHs lead to the fast transportation of electrons, and facile release of the evolved O bubbles during the OER process. Therefore, THC-N-CNHs exhibit excellent electrocatalytic activity toward the OER, with an overpotential of 328 mV at 10 mA cm, which is superior to that of most N-doped carbon material-based electrocatalysts. Meanwhile, the resulting catalyst also shows excellent durability after long-term cycling. Finally, we emphasize that THC-N-CNHs can be promising candidates as cheap, industrially scalable catalytic scaffolds for OER application.
开发具有催化活性的高效、经济高效且稳定的氮掺杂碳材料作为析氧反应(OER)的优异催化剂对于可再生能源系统至关重要。在本研究中,首先采用以N为氮源的正压辅助电弧放电法制备了独特的尖端半封闭氮掺杂碳纳米角(THC-N-CNHs)。受益于新颖的尖端半封闭结构和充足的孔隙率,未经任何进一步处理的THC-N-CNHs的比表面积(SSA)经计算为670 m²/g,比传统的尖端封闭CNHs大三倍。更重要的是,氮含量可达到约1.98 at%,吡啶氮显著富集,增加了OER的活性位点数量。此外,THC-N-CNHs的三维球形特征和独特的孔结构导致电子快速传输,并在OER过程中使析出的O气泡易于释放。因此,THC-N-CNHs对OER表现出优异的电催化活性,在10 mA/cm²时过电位为328 mV,优于大多数基于氮掺杂碳材料的电催化剂。同时,所得催化剂在长期循环后也表现出优异的耐久性。最后,我们强调THC-N-CNHs作为用于OER应用的廉价、可工业规模化的催化支架有很大潜力。