Preparation of Metallic Ni3N Nanoparticles and Its Electrooxidation Performance for Ethylene Glycol★

doi:10.6023/A23050202

Acta Chimica Sinica ›› 2023, Vol. 81 ›› Issue (11): 1471-1477.DOI: 10.6023/A23050202 Previous Articles Next Articles

Special Issue: 庆祝《化学学报》创刊90周年合辑

Article

金属性Ni₃N纳米粒子的制备与乙二醇电氧化性能^★

杨镇鸿, 干晓娟, 王书哲, 段君元, 翟天佑, 刘友文^*()

华中科技大学材料科学与工程学院材料成形与模具技术全国重点实验室武汉 430074

投稿日期:2023-05-05 发布日期:2023-08-14
作者简介:
^†共同第一作者
^★庆祝《化学学报》创刊90周年.
基金资助:
大学生创新创业训练计划(S202210487007); 国家自然科学基金(22071069)

Preparation of Metallic Ni₃N Nanoparticles and Its Electrooxidation Performance for Ethylene Glycol^★

Zhenhong Yang, Xiaojuan Gan, Shuzhe Wang, Junyuan Duan, Tianyou Zhai, Youwen Liu()

State Key Laboratory of Material Processing and Die & Mould Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074

Received:2023-05-05 Published:2023-08-14
Contact: *E-mail: ywliu@hust.edu.cn
About author:
^†These authors contributed equally to this work
^★Dedicated to the 90th anniversary of Acta Chimica Sinica.
Supported by:
College Student Innovation and Entrepreneurship Training Program(S202210487007); National Natural Science Foundation of China(22071069)

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Abstract

Coupled small molecule electrocatalytic oxidation reaction can not only reduce anode overpotential, improve hydrogen evolution reaction (HER) efficiency, but also produce high value-added chemicals, which is an effective strategy to improve the performance of electrocatalytic water splitting. The development of non-noble metal based electrocatalysts with high conductivity and low oxidation potential is the key issue. Herein, Ni₃N nanoparticles (Ni₃N-NPs) with low oxidation potential and high conductivity were prepared by annealing and nitriding Ni(OH)₂ nanosheets precursors. Compared with Ni(OH)₂, Ni₃N-NPs has a smaller Faraday resistance, a lower oxidation potential, a smaller Tafel slope (29 mV•dec^–1), and exhibits the better electrocatalytic oxidation performance towards ethylene glycol (EG). At 1.36 V, the Faraday efficiency of electrocatalytic EG oxidation to formate reached 91.16%. The structure of Ni₃N-NPs before and after the electrocatalytic oxidation reaction was characterized in detail by X-ray diffractometer (XRD), transmission electron microscope (TEM) and X-ray photoelectron spectroscopy (XPS). It was found that in the electrocatalytic EG oxidation process, the surface of Ni₃N-NPs was oxidized into NiOOH, while EG underwent dehydrogenation and oxidation to form formic acid on the catalyst surface, and the NiOOH was synchronously reduced by H and converted into Ni(OH)₂. In addition, Ni₃N-NPs has good universality for electrocatalytic oxidation of small organic molecules.

Key words: electrocatalysis, water splitting, ethylene glycol, Ni(OH)₂, Ni₃N

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Zhenhong Yang, Xiaojuan Gan, Shuzhe Wang, Junyuan Duan, Tianyou Zhai, Youwen Liu. Preparation of Metallic Ni₃N Nanoparticles and Its Electrooxidation Performance for Ethylene Glycol^★[J]. Acta Chimica Sinica, 2023, 81(11): 1471-1477.

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Fig. & Tab. 8

Figure 1. Phase and structure characterization of Ni3N nanoparticles (Ni3N-NPs). (a) XRD pattern; (b) Raman spectrum; (c) TEM and (d) HRTEM images

Figure 2. Electrocatalytic EG oxidation performance of Ni3N-NPs. (a) LSV curve with or without EG; (b) LSV curve of electrocatalytic EG oxidation for Ni3N-NPs and Ni(OH)2; (c) Tafel slopes; (d) chronopotential curve at 10 mA?cm–2; (e) Cdl values, and (f) normalized LSV curves

Figure 3. (a) Nyquist diagram with or without EG; (b) Ni3N-NPs and Ni(OH)2 Nyquist diagram at 1.4 V; (c) Nyquist diagram and (d) Bode diagram of Ni3N-NPs; (e) Nyquist diagram and (f) Bode diagram of Ni(OH)2 under different potentials; (g) charge transfer diagram (EDL stands for double layer) and equivalent circuit diagram; (h) the relationships between Rct and potential; (i) the relationship between Rp and potential

Figure 4. (a) 1H NMR spectra of EG oxidation products at different potentials; (b) Faraday efficiency of EG oxidation to formate at different potentials; (c) LSV curves of the electrolytic water splitting with or without EG; (d) cell voltage required by different current densities

Figure 5. (a) Charge density diagram of Ni3N; (b) state density of Ni3N; (c) band diagram of Ni3N; (d) LSV curve of OER of Ni3N-NPs and Ni(OH)2 in 1 mol/L KOH

Figure 6. (a) TEM and (b~d) HRTEM images of Ni3N-NPs after electrocatalytic EG oxidation reaction

Figure 7. Schematic diagram of Ni3N-NPs electrocatalytic oxidation reaction towards EG

Figure 8. LSV curves of Ni3N-NPS electrocatalytic oxidation (a) methanol, (b) urea and (c) benzyl alcohol; (d) the current densities of electrocatalytic oxidation of various organic small molecule at 1.4 V

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金属性Ni₃N纳米粒子的制备与乙二醇电氧化性能^★

Preparation of Metallic Ni₃N Nanoparticles and Its Electrooxidation Performance for Ethylene Glycol^★

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金属性Ni3N纳米粒子的制备与乙二醇电氧化性能★