片状NiFeCo-LDH-Ti6C3.75复合催化剂的制备及电催化析氧性能

doi:10.15541/jim20220688

摘要/Abstract

摘要：

氧析出反应(OER)是电解水的关键反应, 但其动力学过程缓慢, 限制了电解水的快速发展。因此, 设计和构筑高效的OER催化剂对电解水至关重要。本研究以硝酸钴、硝酸镍、硝酸铁、尿素及Ti₆C_3.75为原料, 采用简单的一步水热法制备了片状Co²⁺离子掺杂的NiFe双金属氢氧化物偶联Ti₆C_3.75的(NiFeCo-LDH-Ti₆C_3.75)OER催化剂。NiFeCo-LDH-Ti₆C_3.75催化剂呈片状堆叠结构, 有利于暴露更多活性位点, 引入Co²⁺和Ti₆C_3.75可以降低Ni、Fe位点的电子密度。得益于此, NiFeCo-LDH-Ti₆C_3.75催化剂表现出优异的OER活性, 在20 mA·cm^-2电流密度下的过电势仅为290 mV, 并且Tafel斜率低至87.84 mV·dec^-1, 具有较快的反应动力学。并且其电荷转移电阻较低, 电荷转移速率较高。此外, NiFeCo-LDH-Ti₆C_3.75催化剂在20 mA·cm^-2条件下经过6000圈加速老化测试后过电势仅增加约 7 mV, 表现出卓越的循环稳定性。

关键词: NiFe-LDH, 钴掺杂, Ti₆C_3.75掺杂

Abstract:

Oxygen evolution reaction (OER) is the key reaction for water splitting, but its slow kinetics limitsits application. Therefore, rational design and construction of efficient OER catalysts are crucial for water splitting. Here, a Co²⁺ ion doped NiFe layered double hydroxides coupled Ti₆C_3.75 (NiFeCo-LDH-Ti₆C_3.75) catalyst was prepared by a simple one-step hydrothermal method using cobalt nitrate, nickel nitrate, iron nitrate, urea, and Ti₆C_3.75 as raw materials. NiFeCo-LDH-Ti₆C_3.75 catalyst showed a lamellar stacking structure, which is facilitating exposing more active sites. Introduction of Co²⁺ and Ti₆C_3.75 reduced the electronic density of Ni and Fe sites of NiFeCo-LDH-Ti₆C_3.75 catalyst. Benefiting from these features, the NiFeCo-LDH-Ti₆C_3.75 catalyst exhibits excellent OER activity with an overpotential of merely 290 mV at a current density of 20 mA·cm^-2 and a Tafel slope of 87.84 mV·dec^-1 with faster reaction kinetics. NiFeCo-LDH-Ti₆C_3.75 catalyst shows a relatively low charge transfer resistance, which means a fast charge transfer efficiency. Furthermore, after 6000 cycles of accelerated aging test at 20 mA·cm^-2, the overpotential only increased ~7 mV, indicating excellent cycle stability of NiFeCo-LDH-Ti₆C_3.75.

Key words: NiFe-LDH, Co doping, Ti₆C_3.75 doping

中图分类号:

TB331
O614

李光兰, 王天宇, 刘一辰, 路中发. 片状NiFeCo-LDH-Ti₆C_3.75复合催化剂的制备及电催化析氧性能[J]. 无机材料学报, 2023, 38(7): 823-829.

LI Guanglan, WANG Tianyu, LIU Yichen, LU Zhongfa. Layered NiFeCo-LDH-Ti₆C_3.75 Catalyst: Preparation and Performance for Oxygen Evolution Reaction[J]. Journal of Inorganic Materials, 2023, 38(7): 823-829.

图/表 6

图1 NiFeCo-LDH-Ti6C3.75制备流程示意图

Fig. 1 Preparation process of NiFeCo-LDH-Ti6C3.75

图2 NiFeCo-LDH-Ti6C3.75的(a) SEM、(b) TEM、(c) HRTEM及(d) SAED照片

Fig. 2 (a) SEM, (b) TEM, (c) HRTEM, and (d) SAED images of NiFeCo-LDH-Ti6C3.75

图3 NiFeCo-LDH-Ti6C3.75的EDS谱图(a)和元素映射照片(b)

Fig. 3 (a) EDS spectrum and (b) elemental mapping images of NiFeCo-LDH-Ti6C3.75

图4 NiFeCo-LDH-Ti6C3.75、NiFe-LDH-Ti6C3.75和NiFeCo-LDH的XRD谱图

Fig. 4 XRD patterns of NiFeCo-LDH-Ti6C3.75, NiFe-LDH- Ti6C3.75, and NiFeCo-LDH catalysts

图5 NiFeCo-LDH-Ti6C3.75、NiFe-LDH-Ti6C3.75和NiFeCo-LDH的(a)XPS总谱图, (b)Ni2p和(c)Fe2p的XPS高分辨谱图, (d)NiFeCo-LDH-Ti6C3.75和NiFeCo-LDH的Co2p的XPS高分辨谱图

Fig. 5 (a) Total survey, high resolution (b) Ni2p and (c) Fe2p XPS spectra for NiFeCo-LDH-Ti6C3.75, NiFe LDH-Ti6C3.75 and NiFeCo-LDH catalysts, (d) Co2p XPS spectra for NiFeCo-LDH-Ti6C3.75 and NiFeCo-LDH catalysts

图6 NiFeCo-LDH-Ti6C3.75、NiFe-LDH-Ti6C3.75、NiFeCo-LDH和RuO2催化剂的电化学性能

Fig. 6 Electrochemical performance of NiFeCo-LDH-Ti6C3.75, NiFe-LDH-Ti6C3.75, NiFeCo-LDH, and RuO2 catalysts (a) LSV curves, (b) overpotential at 20and 50 mA·cm-2, and (c) Tafel slopes of NiFeCo-DH-Ti6C3.75, NiFe LDH-Ti6C3.75, NiFeCo-LDH, and RuO2 catalysts; (d) EIS and (e) Cdl of NiFeCo-DH-Ti6C3.75, NiFe LDH-Ti6C3.75, and NiFeCo-LDH; (f) Accelerated aging curves of NiFeCo-LDH-Ti6C3.75 before and after 6000 cycles

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片状NiFeCo-LDH-Ti₆C_3.75复合催化剂的制备及电催化析氧性能

Layered NiFeCo-LDH-Ti₆C_3.75 Catalyst: Preparation and Performance for Oxygen Evolution Reaction

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