Ni-Fe/Ti和Ni-Fe-S/Ti的制备及其电催化水分解性能

doi:10.13208/j.electrochem.190114

电化学（中英文） ›› 2020, Vol. 26 ›› Issue (1): 136-147. doi: 10.13208/j.electrochem.190114

Ni-Fe/Ti和Ni-Fe-S/Ti的制备及其电催化水分解性能

陆杭烁¹, 何小波²^,³, 银凤翔¹^,²^,³^,^*(), 李国儒²

^1. 北京化工大学化学工程学院,北京 100029
^2. 常州大学石油化工学院,江苏省绿色催化材料与技术重点实验室,江苏常州 213164
^3. 北京化工大学常州先进材料研究院,江苏常州 213164

收稿日期:2019-01-14 修回日期:2019-04-01 发布日期:2019-04-02 出版日期:2020-02-28
通讯作者: 银凤翔 E-mail:yinfx@cczu.edu.cn
基金资助:
国家自然科学基金项目(21706010);江苏省自然科学基金面上项目(BK20161200)

Preparations of Nickel-Iron Hydroxide/Sulfide and Their Electrocatalytic Performances for Overall Water Splitting

Hang-shuo LU¹, Xiao-bo HE²^,³, Feng-xiang YIN¹^,²^,³^,^*(), Guo-ru LI²

^1. College of Chemical Engineering, Beijing University of Chemical Technology, Beijing 100029, China
^2. Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, Jiangsu, China
^3. Changzhou Institute of Advanced Materials, Beijing University of Chemical Technology, Changzhou 213164, Jiangsu, China

Received:2019-01-14 Revised:2019-04-01 Online:2019-04-02 Published:2020-02-28
Contact: Feng-xiang YIN E-mail:yinfx@cczu.edu.cn

摘要/Abstract

摘要：

以钛网为基底,采用电沉积法制备了Ni-Fe/Ti析氧电极,然后将得到的Ni-Fe/Ti电极通过固相硫化制备了Ni-Fe-S/Ti析氢电极. 分别考察了电沉积液中Ni²⁺/Fe³⁺离子摩尔浓度比和硫脲加入量对Ni-Fe/Ti和Ni-Fe-S/Ti结构和电化学性能的影响. 结果表明,随着电沉积液中Ni²⁺含量的增加,Ni-Fe/Ti电极析氧性能先增强后减弱,Ni9Fe1/Ti电极具有最好的析氧性能;随着硫脲加入量的增加,Ni-Fe-S/Ti电极析氢性能呈现先增强后减弱的趋势,Ni9Fe1S0.25/Ti电极具有最好的析氢性能. 在50 mA·cm^-2下,Ni9Fe1/Ti电极的析氧过电位为280 mV,Ni9Fe1S0.25/Ti电极的析氢过电位为269 mV,且均具有很好的稳定性. 将Ni9Fe1/Ti与Ni9Fe1S0.25/Ti分别作为阳极和阴极进行电催化全水分解,电流密度达到50 mA·cm^-2所需电势仅1.69 V,表现出很好的全水解催化性能.

关键词: 镍铁氢氧化物, 镍铁硫化物, 氧气析出反应, 氢气析出反应, 电催化全水分解

Abstract:

The Ni-Fe/Ti oxygen evolution electrode was prepared by electrodeposition on a titanium mesh substrate. Then, the as prepared Ni-Fe/Ti electrode was used to derive the Ni-Fe-S/Ti hydrogen evolution electrode through solid phase sulfuration. The effects of the molar ratio of Ni²⁺ to Fe³⁺ in the electrolyte and the amount of thiourea on the structures and electrochemical performances of Ni-Fe/Ti and Ni-Fe-S/Ti electrodes were investigated. The results show that the oxygen evolution performance of Ni-Fe/Ti electrode was first increased and then decreased with the increase of nickel ion content in the electrolyte. The Ni9Fe1/Ti electrode exhibited the best oxygen evolution performance. With the increase of thiourea addition, the hydrogen evolution performance of Ni-Fe-S/Ti electrode was increased firstly and then decreased. The Ni9Fe1S0.25/Ti electrode showed the best hydrogen evolution performance. To achieve a current density of 50 mA·cm^-2, an overpotential of 280 mV was required for oxygen evolution reaction (OER) with the Ni9Fe1/Ti electrode, while 269 mV for hydrogen evolution reaction (HER) with the Ni9Fe1S0.25/Ti electrode, both with good stabilities. Accordingly, the Ni9Fe1/Ti and Ni9Fe1S0.25/Ti electrode were used as anodes and cathodes, respectively, for overall water splitting tests. The current density of 50 mA·cm^-2 was achieved at a voltage of 1.69 V, showing the good catalytic performance of overall water splitting.

Key words: nickel-iron hydroxide, nickel-iron sulfide, oxygen evolution reaction, hydrogen evolution reaction, overall water splitting

中图分类号:

O646

陆杭烁, 何小波, 银凤翔, 李国儒. Ni-Fe/Ti和Ni-Fe-S/Ti的制备及其电催化水分解性能[J]. 电化学（中英文）, 2020, 26(1): 136-147.

Hang-shuo LU, Xiao-bo HE, Feng-xiang YIN, Guo-ru LI. Preparations of Nickel-Iron Hydroxide/Sulfide and Their Electrocatalytic Performances for Overall Water Splitting[J]. Journal of Electrochemistry, 2020, 26(1): 136-147.

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链接本文: https://electrochem.xmu.edu.cn/CN/10.13208/j.electrochem.190114

https://electrochem.xmu.edu.cn/CN/Y2020/V26/I1/136

图/表 15

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表8

Sample	Molar ratio of Ni²⁺/Fe³⁺	Deposition potential/ V(vs. Ag/AgCl)	Deposition time/min	Thiourea/g	Temperature of sulfuration/°C	Loading/ (mg·cm^-2)
Ni0Fe10/Ti	0:10	-1	20	—	—	0.2
Ni3Fe7/Ti	3:7	-1	20	—	—	2.3
Ni6Fe4/Ti	6:4	-1	20	—	—	3.0
Ni9Fe1/Ti	9:1	-1	20	—	—	7.4
Ni10Fe0/Ti	10:0	-1	20	—	—	7.0
Ni9Fe1S0.1/Ti	9:1	-1	20	0.10	200	8.2
Ni9Fe1S0.25/Ti	9:1	-1	20	0.25	200	7.9
Ni9Fe1S0.5/Ti	9:1	-1	20	0.50	200	8.1

Electrode	η₅₀/mV	Tafel slope/(mV·dec^-1)	C_dl/(mF·cm^-2)
Ti	—	—	0.25
Ni0Fe10/Ti	940	110	0.25
Ni3Fe7/Ti	503	80	0.17
Ni6Fe4/Ti	323	38	0.48
Ni9Fe1/Ti	280	30	5.16
Ni10Fe0/Ti	340	113	3.45

Electrode	Substrate	Current density/ (mA·cm^-2)	η/mV	Tafel slope/(mV·dec^-1)	KOH/ ( mol·L^-1)	Ref.
Ni9Fe1/Ti	Ti mesh	50	280	30	0.1	This work
NiFe LDH	Ni foam	10	240	—	1	[9]
NiCo-LDH	Ni foam	10	420	113	0.1	[10]
Cu@NiFe LDH	Cu foam	100	280	27.8	1	[11]
Ni(OH)₂	Ni foam	50	330	150	1	[31]
Ni70Fe30(H)	Glassy carbon	10	292	30.4	0.1	[30]
CoNi(OH)_x	Cu foil	10	280	77	1	[32]
NiMo HNRs	Ti mesh	10	310	47	1	[33]
IrO_x/C	Glassy carbon	10	326	41.7	0.1	[30]

Electrode	η_-50/mV	Tafel slope/ (mV·dec^-1)	C_dl/ (mF·cm^-2)
Ni9Fe1/Ti	498	158	0.79
Ni9Fe1S0.1/Ti	379	145	17.68
Ni9Fe1S0.25/Ti	269	126	13.52
Ni9Fe1S0.5/Ti	347	131	4.31

Electrode	Substrate	Current density/ (mA·cm^-2)	η/mV	Tafel slope/(mV·dec^-1)	KOH/ ( mol·L^-1)	Ref.
Ni9Fe1S0.25/Ti	Ti mesh	50	269	126	0.1	This work
NiFeS	Ni foam	10	180	53	1	[16]
NiFeP	Ni foam	10	87	48	1	[34]
Fe_0.1-NiS₂NA	Ti mesh	50	~300	108	1	[31]
NiMoS₄	Ti mesh	50	263	97	0.1	[35]
NiCo₂S₄ nanowire	Ni foam	10	210	58.9	1	[36]
Ni₅P₄	Ni foil	10	150	53	1	[37]
NiSe	Ni foam	10	96	120	1	[38]
Pt/C	Ti mesh	50	~180	58	0.1	[35]

Ni-Fe/Ti和Ni-Fe-S/Ti的制备及其电催化水分解性能

Preparations of Nickel-Iron Hydroxide/Sulfide and Their Electrocatalytic Performances for Overall Water Splitting

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Metrics

Electrode	Ti	Ni0Fe10/Ti	Ni3Fe7/Ti	Ni6Fe4/Ti	Ni9Fe1/Ti	Ni10Fe0/Ti
R_s/(Ω·cm²)	4.95	2.75	4.01	3.58	2.45	4.02
R_ct/(Ω·cm²)	7.85	4.61	3.90	3.05	2.83	1.98

Electrode	Ni9Fe1/Ti	Ni9Fe1S0.1/Ti	Ni9Fe1S0.25/Ti	Ni9Fe1S0.5/Ti
R_s/(Ω·cm²)	2.69	1.90	1.34	2.50
R_ct/(Ω·cm²)	7.65	7.88	7.56	7.55

Electrode	Substrate	Current density/(mA·cm^-2)	Voltage/V	KOH/ ( mol·L^-1)	Ref.
Ni9Fe1/Ti(+)\|\|Ni9FeS0.25/Ti(-)	Ti mesh	50	1.69	0.1	This work
IrO₂(+)\|\|Pt(-)	Cu foam	50	~1.70	1	[11]
NiFe LDH	Ni foam	10	1.70	1	[21]
Co₂VO₄(+)\|\|Co/VN(-)	Glassy carbon	10	1.65	1	[40]
NiFe LDH@NiCoP	Ni foam	10	1.57	1	[22]
Ni₃S₂	Ni foam	10	1.76	1	[23]
NiCo_3-_xS₄/Ni₃S₄	Ni foam	10	1.53	1	[24]
NiCo_3-_xS₄/Ni₃S₄	Ni foam	100	1.8	1	[24]

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