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阐明氮磷共掺杂碳对复合尖晶石NiFeO在碱性介质中氧还原反应的影响。

Elucidating the effects of nitrogen and phosphorus co-doped carbon on complex spinel NiFeO towards oxygen reduction reaction in alkaline media.

作者信息

Mbokazi Siyabonga Patrick, Matthews Thabo, Zheng Haitao, Chabalala Makhaokane Paulina, Zikhali Memory, Mugadza Kudzai, Gwebu Sandile, Mekuto Lukhanyo, Maxakato Nobanathi Wendy

机构信息

Department of Chemical Sciences, University of Johannesburg, Doornfontein, 2028, South Africa.

Energy Centre, Council for Scientific and Industrial Research (CSIR), Pretoria, 0001, South Africa.

出版信息

Heliyon. 2024 Jul 30;10(15):e35483. doi: 10.1016/j.heliyon.2024.e35483. eCollection 2024 Aug 15.

Abstract

The study presents for the first time complex spinel NiFeO nanoparticles supported on nitrogen and phosphorus co-doped carbon nanosheets (NPCNS) prepared using sol gel and the carbonization of graphitic carbon nitride with lecithin as a highly active and durable electrocatalyst for oxygen reduction reaction. The physicochemical properties of complex spinel NiFeO on NPCNS and subsequent nanomaterials were investigated using techniques such as X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, and transmission electron microscopy. The electrochemical activity of the electrocatalysts was evaluated using hydrodynamic linear sweep voltammetry, cyclic voltammetry, electrochemical impedance spectroscopy, and chronoamperometry. The electrocatalytic performance of the NiFeO/NPCNS nanohybrid electrocatalyst is dominated by the 4e transfer mechanism, with an onset potential of 0.92 V vs. RHE, which is closer to that of the Pt/C, and a current density of 7.81 mA/cm that far exceeds that of the Pt/C. The nanohybrid demonstrated the best stability after 14 400 s, outstanding durability after 521 cycles, and the best ability to oxidize methanol and remove CO from its active sites during CO tolerance studies. This improved catalytic activity can be attributed to small nanoparticle sizes of the unique complex spinel nickel ferrite structure, NFe/Ni coordination of nanocomposite, high dispersion, substantial ECSA of 47.03 mF/cm, and synergy caused by strong metal-support and electronic coupling interactions.

摘要

该研究首次展示了负载在氮磷共掺杂碳纳米片(NPCNS)上的复合尖晶石NiFeO纳米颗粒,其通过溶胶凝胶法以及以卵磷脂为原料对石墨相氮化碳进行碳化制备而成,是一种用于氧还原反应的高活性且耐用的电催化剂。采用X射线衍射、傅里叶变换红外光谱、X射线光电子能谱和透射电子显微镜等技术对NPCNS上的复合尖晶石NiFeO及后续纳米材料的物理化学性质进行了研究。使用流体动力学线性扫描伏安法、循环伏安法、电化学阻抗谱和计时电流法对电催化剂的电化学活性进行了评估。NiFeO/NPCNS纳米杂化电催化剂的电催化性能由4e转移机制主导,相对于可逆氢电极(RHE)的起始电位为0.92 V,这与Pt/C的起始电位相近,且电流密度为7.81 mA/cm²,远远超过Pt/C的电流密度。该纳米杂化物在14400 s后表现出最佳稳定性,在521次循环后具有出色的耐久性,并且在CO耐受性研究中表现出最佳的氧化甲醇和从其活性位点去除CO的能力。这种催化活性的提高可归因于独特复合尖晶石镍铁氧体结构的小纳米颗粒尺寸、纳米复合材料的NFe/Ni配位、高分散性、47.03 mF/cm²的高电化学活性表面积(ECSA)以及强金属-载体和电子耦合相互作用所产生的协同效应。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/6c17/11334865/4955fae625eb/ga1.jpg

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