镍铁氢氧化物-磷化钴复合电极电催化分解水研究

doi:10.15541/jim20230432

无机材料学报 ›› 2024, Vol. 39 ›› Issue (4): 374-382.DOI: 10.15541/jim20230432 CSTR: 32189.14.10.15541/jim20230432

所属专题：【能源环境】氢能材料(202409)

镍铁氢氧化物-磷化钴复合电极电催化分解水研究

杨博¹^,²^,³(), 吕功煊¹(), 马建泰³

1.中国科学院兰州化学物理研究所, 羰基合成与选择氧化国家重点实验室, 兰州 730000
2.中国科学院大学, 北京 100049
3.兰州大学化学化工学院, 兰州 730000

收稿日期:2023-09-22 修回日期:2023-11-23 出版日期:2024-04-20 网络出版日期:2023-12-04
通讯作者: 吕功煊, 教授. E-mail: gxlu@lzb.ac.cn
作者简介:杨博(1989-), 男, 博士研究生. E-mail: yangbo18@licp.cas.cn
基金资助:
国家重点研发计划(2022YFB3803600);国家自然科学基金(22272189);国家自然科学基金(22102200)

Electrocatalytic Water Splitting over Nickel Iron Hydroxide-cobalt Phosphide Composite Electrode

YANG Bo¹^,²^,³(), LÜ Gongxuan¹(), MA Jiantai³

1. State Key Laboratory for Oxo Synthesis and Selective Oxidation, Lanzhou Institute of Chemical Physics, Chinese Academy of Sciences, Lanzhou 730000, China
2. University of Chinese Academy of Sciences, Beijing 100049, China
3. College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, China

Received:2023-09-22 Revised:2023-11-23 Published:2024-04-20 Online:2023-12-04
Contact: LÜ Gongxuan, professor. E-mail: gxlu@lzb.ac.cn
About author:YANG Bo (1989–), male, PhD candidate. E-mail: yangbo18@licp.cas.cn
Supported by:
National Key R&D Program of China(2022YFB3803600);National Natural Science Foundation of China(22272189);National Natural Science Foundation of China(22102200)

摘要/Abstract

摘要：

本研究采用水热-磷化-电化学沉积法在磷化钴表面构筑了金属氢氧化物层, 制备了NiFeOH/CoP/NF复合电极, 考察了复合电极电解水制氢的性能。在1.0 molּ/L的KOH介质中, NiFeOH/CoP/NF复合电极表现出良好的催化电解水性能。在电流密度为100 mA/cm²时, NiFeOH/CoP/NF复合电极电催化析氢(HER)和析氧反应(OER)所需的过电势分别为141和372 mV。在电流密度为10 mA/cm²时, NiFeOH/CoP/NF同时用作阴极和阳极电解水所需电压仅为1.61 V。NiFeOH保护层增强了CoP在电解水反应中的活性和稳定性, NiFeOH/CoP/NF复合电极在恒电流电解中表现出高的HER和OER稳定性, 活性可维持60000 s, 性能未见明显衰减。将NiFeOH/CoP/NF两电极电解池与GaAs太阳能电池组成光伏-电解水系统, 该系统在100 mW/cm²模拟光照条件下, 太阳能至氢能转化效率达到18.0%, 并可稳定运行200 h。

关键词: 磷化钴, 金属氢氧化物保护层, 电催化水分解, 稳定性

Abstract:

NiFeOH/CoP/NF composite electrode was fabricated by constructing a metal hydroxide layer on the surface of cobalt phosphide via hydrothermal, phosphating, and electrodeposition methods. The electrolytic water splitting to hydrogen performance by as-prepared electrode was investigated in 1.0 mol/L KOH medium. NiFeOH/CoP/NF composite electrode exhibited excellent water electrolysis performance, and the required overpotentials for HER and OER at 100 mA/cm²current density were 141 and 372 mV, respectively. When NiFeOH/CoP/NF electrode served as both cathode and anode for water splitting, only 1.61 V voltage was required to reach current density of 10 mA/cm². Because NiFeOH protection layer enhanced the electrocatalytic activity and stability of CoP for water splitting, NiFeOH/CoP/NF composite electrode exhibited high stability during the galvanostatic electrolysis in the HER and OER, and its activity could maintain 60000 s without significant performance degradation. The photovoltaic-electrolytic water cell constructed with two NiFeOH/CoP/NF electrodes and GaAs solar cell showed 18.0% efficiency of solar to hydrogen under 100 mW/cm² simulated solar irradiation and worked stably for 200 h.

Key words: cobalt phosphide, metal hydroxide protection layer, electrocatalytic water splitting, stability

中图分类号:

O646
O643

杨博, 吕功煊, 马建泰. 镍铁氢氧化物-磷化钴复合电极电催化分解水研究[J]. 无机材料学报, 2024, 39(4): 374-382.

YANG Bo, LÜ Gongxuan, MA Jiantai. Electrocatalytic Water Splitting over Nickel Iron Hydroxide-cobalt Phosphide Composite Electrode[J]. Journal of Inorganic Materials, 2024, 39(4): 374-382.

图/表 9

图1 电极制备过程示意图(a)及Co前驱体/NF(b, e)、CoP/NF(c, f)和NiFeOH/CoP/NF-200s(d, g)的SEM照片(b~d)和XRD谱图(e~g)

Fig. 1 Synthesis diagram of electrodes (a), SEM images (b-d) and XRD patterns (e-g) of Co precursor/NF (b, e), CoP/NF (c, f), and NiFeOH/CoP/NF-200s (d, g)

图2 Co前驱体/NF、CoP/NF和NiFeOH/CoP/NF-200s的Ni2p(a)、Co2p(b)、P2p(c)和Fe2p(d) XPS谱图

Fig. 2 Ni2p(a), Co2p(b), P2p(c), and Fe2p(d) XPS spectra of Co precursor/NF, CoP/NF, and NiFeOH/CoP/NF-200s

图3 单独NF、Co前驱体/NF、CoP/NF和NiFeOH/CoP/NF-200s的HER电化学性质

Fig. 3 HER electrocatalytic properties of bare NF, Co precursor/NF, CoP/NF, and NiFeOH/CoP/NF-200s (a) LSV curves; (b) Corresponding Tafel plots; (c) Nyquist plots at -0.20 V (vs. RHE); (d) Chronopotentiometry plots of CoP/NF and NiFeOH/CoP/NF-200s at the current density of -10 mA/cm2

图4 单独NF、Co前驱体/NF、CoP/NF和NiFeOH/CoP/NF-200s的OER电化学性质

Fig. 4 OER electrocatalytic properties of bare NF, Co precursor/NF, CoP/NF, and NiFeOH/CoP/NF-200s (a) LSV curves; (b) Corresponding Tafel plots; (c) Nyquist plots at the potential of 1.60 V (vs. RHE); (d) Chronopotentiometry plots of CoP/NF and NiFeOH/CoP/NF-200s at the current density of 10 mA/cm2

图5 NiFeOH/CoP/NF-200s||NiFeOH/CoP/NF-200s两电极全分解水的电化学性质, 以及两电极电解池与GaAs太阳能电池组成光伏-电催化系统的太阳能制氢效率

Fig. 5 Electrocatalytic overall water splitting properties of NiFeOH/CoP/NF-200s||NiFeOH/CoP/NF-200s two electrode system and hydrogen production efficiency of the photovoltaic-electrocatalytic system consisting of two electrode cell and GaAs solar cell (a) LSV curve; (b) Long term chronopotentiometry plot at current density of 10 mA/cm2; (c) Galvanostatic electrocatalytic hydrogen and oxygen evolution curves, Faradic efficiency (FE), and electricity to hydrogen efficiency curves (ETH); (d) Hydrogen, oxygen evolution and corresponding solar to hydrogen efficiency curves of a photovoltaic-electrocatalytic system consisting of NiFeOH/CoP/NF-200s||NiFeOH/CoP/NF-200s electrocatalytic cell and GaAs solar cell

图S1 Co前驱体/NF、CoP/NF和NiFeOH/CoP/NF-200s的TEM表征

Fig. S1 TEM characterization of Co precursor/NF, CoP/NF, and NiFeOH/CoP/NF-200s (a-c) TEM images of (a) Co precursor/NF, (b) CoP/NF, and (c) NiFeOH/CoP/NF-200s; (d-f) HRTEM images of (d) Co precursor/NF, (e) CoP/NF, and (f) NiFeOH/CoP/NF-200s; (g, h) SAED images in crystalline (1) and amorphous (2) areas of (f); (i) HAADF-STEM image and (j) Ni, Fe, Co, P, O element mappings of NiFeOH/CoP/NF-200s

图S2 CoP/NF和不同电沉积时间制备的NiFeOH/CoP/NF-xs的阴极LSV曲线(a), 电流密度差对扫描速率作图计算单独NF、Co前驱体/NF、CoP/NF和NiFeOH/CoP/NF-200s的双层电化学电容(b)

Fig. S2 Cathode LSV curves of CoP/NF, and NiFeOH/CoP/NF-xs prepared with different electrodeposition time (a), and current density difference versus scan rate to calculate the double layer capacities (Cdls) of bare NF, Co precursor/NF, CoP/NF, and NiFeOH/CoP/NF-200s (b)

图S3 CoP/NF和不同电沉积时间制备的NiFeOH/CoP/NF-xs电极的阳极LSV曲线(a)及NiFeOH/CoP/NF-200s阴、阳极恒电流反应后的XRD和SEM表征(b~d)

Fig. S3 Anode LSV curves of CoP/NF and NiFeOH/CoP/NF-xs prepared with different electrodeposition time (a), XRD and SEM characterization of NiFeOH/CoP/NF-200s after cathode and anode chronopotentiometry test (b-d) (b) XRD spectra after HER and OER; (c) SEM image after HER; (d) SEM image after OER

图S4 NiFeOH/CoP/NF-200s电极在HER和OER恒电流反应前后的XPS表征

Fig. S3 XPS characterization of NiFeOH/CoP/NF-200s before and after HER and OER chronopotentiometry test (a) Ni2p; (b) Co2p; (c) P2p; (d) Fe2p

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镍铁氢氧化物-磷化钴复合电极电催化分解水研究

Electrocatalytic Water Splitting over Nickel Iron Hydroxide-cobalt Phosphide Composite Electrode

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