MOF衍生CoSe<sub>2</sub>基电催化剂的制备及其电解水性能研究进展

李筱霏; 赵恩德; 彭少波; 朱雨辰; 蔡琳; 乔靓

doi:10.13801/j.cnki.fhclxb.20230328.001

MOF衍生CoSe₂基电催化剂的制备及其电解水性能研究进展

doi: 10.13801/j.cnki.fhclxb.20230328.001

长春大学　理学院，材料设计与量子模拟吉林省高校重点实验室，长春 130022

基金项目: 国家自然科学基金(52172145)；吉林省科技发展计划项目(YDZJ202101ZYTS165；20230402066GH)

详细信息

通讯作者:
乔靓，博士，教授，硕士生导师，研究方向为能源与催化材料　E-mail: qiaol@ccu.edu.cn

中图分类号: TB331；TQ151.1
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出版历程
- 收稿日期: 2023-02-13
- 修回日期: 2023-03-10
- 录用日期: 2023-03-17
- 网络出版日期: 2023-03-28
- 刊出日期: 2023-08-15

Research progress of synthesis of metal organic framework derived CoSe₂-based electrocatalysts for overall water splitting

Key Laboratory of Materials Design and Quantum Simulation, College of Science, Changchun University, Changchun 130022, China

Funds: National Natural Science Foundation of China (52172145); Science and Technology Development Project of Jilin Province (YDZJ202101ZYTS165; 20230402066GH)

摘要

摘要: 氢能是未来替代化石能源的最理想新能源，电化学水分解是目前最有效的制氢方法。为实现电解水制氢和制氧的大规模推广和应用，首要任务是设计开发高效、稳定、低成本的电解水催化剂。过渡金属硫族化合物因其固有的电催化活性和丰富的化学相组成已成为理想的电解水催化剂，其中具有层状结构的CoSe₂是最具代表性的过渡金属硒化物。金属有机骨架(MOF)具有高度有序的多孔结构和较大的比表面积，采用MOF为前驱体制备得到的MOF衍生CoSe₂电催化剂可以继承其MOF前驱体的结构优势。这种MOF衍生制备方法是进一步提高CoSe₂电解水催化活性的有效手段。本文综述了国内外近年来MOF衍生CoSe₂基电催化剂电解水性能的重要研究进展，简要介绍了CoSe₂的晶体结构和相变调控，叙述了MOF衍生CoSe₂基电催化剂的制备方法，重点阐述了调控其电解水析氢和析氧催化性能的改性手段，并对未来MOF衍生CoSe₂基电催化材料在电解水领域的发展进行了展望。
- CoSe₂ /
- 金属有机骨架 /
- 制备 /
- 电解水 /
- 析氢反应 /
- 析氧反应
Abstract: Hydrogen energy is considered as the most ideal alternative renewable energy of fossil energy in the future. Electrochemical water splitting is the most effective approach to produce hydrogen. Design and development of high-efficient, stable and low-cost electrocatalyst is of significant urgence and importance to realize the large-scale production of hydrogen and oxygen from water splitting. Transition metal chalcogenides have become ideal electrocatalysts for water splitting due to their intrinsic electrocatalytic activities and abundant chemical phase compositions, among which CoSe₂ with layered structure is the most representative transition metal selenides. Metal organic frameworks (MOFs) possess highly-ordered porous structures and large specific surface area. The MOF-derived CoSe₂ electrocatalysts can inherit the structural advantages of their MOF precursors. These kinds of MOF-derived synthetic methods are the most effective method to further improve the electrocatalytic activity of water splitting. This review summarizes the recent significant advances of MOF derived CoSe₂-based electrocatalysts for overall water splitting. The crystal structure and phase transformation of CoSe₂ are briefly introduced, and the synthetic methods of MOF derived CoSe₂-based electrocatalysts are described. Furthermore, the effective ways to enhance the performance of hydrogen evolution reaction and oxygen evolution reaction of MOF derived CoSe₂-based electrocatalysts are emphatically elucidated. Finally, future research perspectives of MOF derived CoSe₂-based electrocatalysts in the field of water splitting are prospected.
- CoSe₂ /
- metal organic framework /
- synthesis /
- overall water splitting /
- hydrogen evolution reaction /
- oxygen evolution reaction

HTML全文

图 1 电解水装置示意图

HER—Hydrogen evolution reaction; OER—Oxygen evolution reaction

Figure 1. Schematic illustration of conventional water electrolyzer

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图 2 立方黄铁矿型 (a) 和正交白铁矿型 (b) CoSe₂的晶体结构^[31]

Figure 2. Crystal structures of CoSe₂ in cubic pyrite-type phase (a) and orthorhombic marcasite-type phase (b)^[31]

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图 3 (a) CoSe₂微球合成过程示意图；(b) CoSe₂-450微球的SEM图像；(c) CoSe₂微球和商业IrO₂在320 mV至390 mV过电位下的转换频率(TOF)；(d) CoSe₂-450和商业IrO₂ 1000次循环前后的线性扫描伏安曲线(插图为330 mV过电位下的电流密度-时间曲线)^[26]

BTC^3–—1, 3, 5-benzenetricarboxylic ion; MOFs—Metal organic frameworks; RHE—Reversible hydrogen electrode

Figure 3. (a) Schematic illustration of the synthetic strategy for the CoSe₂ microspheres; (b) SEM image of CoSe₂-450 microsphere; (c) Turnover frequency (TOF) of CoSe₂ microspheres and commercial IrO₂ at different overpotentials from 320 mV to 390 mV; (d) Linear sweep voltammetry curves for the 1st and1000th potential cycles of CoSe₂-450 and commercial IrO₂(Inset: Current-time curves at overpotential of 330 mV)^[26]

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图 4 ZIF-67 (a)、Fe-ZIF-67 (b) 和Fe-CoSe₂@NC (c) 的SEM图像；(d) Fe-CoSe₂@NC合成示意图，包括Fe³⁺蚀刻ZIF-67和随后的煅烧硒化；(e) CoSe₂@NC和Fe-CoSe₂@NC的线性扫描伏安曲线；(f) CoSe₂和Fe-CoSe₂的氢吸附吉布斯自由能图(插图为在CoSe₂(右)和Fe-CoSe₂(左)中Co位点上的氢吸附分子结构)^[48]

j—Current density; E—Potential; NC—N doped carbon

Figure 4. SEM images of ZIF-67 (a), Fe-ZIF-67 (b) and Fe-CoSe₂@NC (c); (d) Schematic illustration of the synthetic process of Fe-CoSe₂@ NC, involving Fe³⁺ etching of ZIF-67 and the following thermal selenization; (e) Linear sweep voltammetry curves of CoSe₂@NC and Fe-CoSe₂@NC; (f) Calculated free-energy diagrams of the hydrogen evolution reaction of pristine CoSe₂ and Fe-doped CoSe₂ (Inset: Molecular structures with H adsorption on the Co site of CoSe₂ (right) and Fe-CoSe₂ (left))^[48]

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图 5 CoSe₂/FeSe₂@C异质结构的合成过程示意图 (a) 和SEM图像 (b)；CoSe₂/FeSe₂@C、商业RuO₂、CoFe₂O₄@C、CoSe₂@C及FeSe₂@C的线性扫描伏安曲线 (c) 和Tafel斜率 (d)^[55]

Figure 5. Schematic illustration of the synthetic process (a) and SEM image (b) of CoSe₂/FeSe₂@C heterostructure; Linear sweep voltammetry curves (c) and Tafel slopes (d) of CoSe₂/FeSe₂@C, commercial RuO₂, CoFe₂O₄@C, CoSe₂@C and FeSe₂@C^[55]

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图 6 CoSe₂@NC-NR/CNT的合成过程示意图 (a)、SEM (b) 和TEM (c) 图像^[59]；CoSe₂@NC-CNT的合成过程示意图 (d) 和TEM图像 (e)^[60]

CNT—Carbon nanotubes; ZIF-67—Zeolitic imidazolate framework-67; NC-NR—N-doped carbon nanorod; PVP—Polyvinyl pyrrolidone

Figure 6. Schematic illustration of the synthetic process (a), SEM (b) and TEM (c) images of CoSe₂@NC-NR/CNT^[59]; Schematic illustration of the synthetic process (d) and TEM image (e) of CoSe₂@NC-CNT^[60]

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图 7 Zn掺杂CoSe₂/CFC的合成过程示意图 (a) 和SEM图像 (b)；CoSe₂/CFC、Zn掺杂CoSe₂/CFC的线性扫描伏安曲线 (c) 和Tafel斜率 (d)^[63]

MOF_ZnCo—ZnCo metal organic framework

Figure 7. Schematic illustration of the synthetic process (a) and SEM image (b) of Zn-doped CoSe₂/CFC; Linear sweep voltammetry curves (c) and Tafel slopes (d) of CoSe₂/CFC and Zn-doped CoSe₂/CFC^[63]

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图 8 花状MOF衍生CoSe₂ (MOF-D CoSe₂)的SEM图像 ((a)~(c)) 及其示意图 (d)；(e) MOF-D CoSe₂、CoSe₂和商业Pt/C的析氢反应(HER)线性扫描伏安曲线；(f) MOF-D CoSe₂、Co-MOF、CoSe₂和RuO₂的析氧反应(OER)线性扫描伏安曲线^[69]

Figure 8. SEM images ((a)-(c)) and the corresponding schematic illustration (d) of flower-shaped MOF-derived CoSe₂ (MOF-D CoSe₂); (e) Linear sweep voltammetry curves for the hydrogen evolution reaction (HER) of MOF-D CoSe₂, bare CoSe₂, and commercial Pt/C; (f) Linear sweep voltammetry curves for the oxygen evolution reaction (OER) of MOF-D CoSe₂, Co-MOF, bare CoSe₂ and RuO₂^[69]

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表 1 MOF衍生CoSe₂基电催化剂电解水析氢和析氧性能

Table 1. Electrocatalytic HER and OER performance of MOF derived CoSe₂-based electrocatalysts

Electrocatalyst	Electrolyte	Overpotential^a/mV		Cell voltage^a/V	Morphology of CoSe₂	Ref.
Electrocatalyst	Electrolyte	HER	OER	Cell voltage^a/V	Morphology of CoSe₂	Ref.
CoSe₂-NC NSs	1.0 mol/L KOH	75	247	1.54	Nanoparticles	[23]
CoSe₂-450	1.0 mol/L KOH	—	330	—	Microspheres	[26]
CoSe₂-160	0.5 mol/L H₂SO₄	156	—	—	Microcubes	[27]
CoSe₂-160	1.0 mol/L KOH	—	328	—	Microcubes	[27]
CoSe₂@N/C-CNT	0.5 mol/L H₂SO₄	185	—	—	Nanoparticles	[28]
CoSe₂@N/C-CNT	1.0 mol/L KOH	—	340	—	Nanoparticles	[28]
(Ni, Co)Se₂/C	1.0 mol/L KOH	87	245	—	Hollow rhombic dodecahedra	[47]
(Ni, Co)Se₂/C	1.0 mol/L and 6.0 mol/L KOH	—	—	1.58	Hollow rhombic dodecahedra	[47]
Fe-CoSe₂@NC	0.5mol/L H₂SO₄	143	—	—	Rhombic dodecahedra	[48]
(Ni, Co)Se₂	3.0 mol/L KOH	—	278	—	Nanoparticles	[49]
Zn_0.1Co_0.9Se₂	0.5 mol/L H₂SO₄	140	—	—	Hollow dodecahedra	[50]
Zn_0.1Co_0.9Se₂	1.0 mol/L KOH	—	340	—	Hollow dodecahedra	[50]
CoSe₂/(NiCo)Se₂	0.5 mol/L H₂SO₄	200^b	—	—	Nanocubes	[52]
RuSe₂-CoSe₂	1.0 mol/L KOH	—	200	1.61^b	Nanosheets	[53]
FeSe₂-CoSe₂/CoSe₂	1.0 mol/L KOH	—	260	—	Yolk-shell nanoboxes	[54]
CoSe₂/FeSe₂@C	1.0 mol/L KOH	—	291	—	Nanoparticles	[55]
(Co, Fe)Se₂	1.0 mol/L KOH	124	—	—	Hollow polyhedra	[56]
CoSe₂/MoSe₂	1.0 mol/L KOH	168	—	—	Hollow nanospheres	[57]
CoSe₂/CNTs	1.0 mol/L KOH	190	300	1.75	Nanosheets	[61]
CoSe₂@rGO	1.0 mol/L KOH	—	296	—	—	[62]
CoSe₂/CFC	1.0 mol/L KOH	—	356	—	Nanosheets	[63]
CoSe₂/CF	1.0 mol/L KOH	95	297	1.63	Nanoparticles	[64]
CC/MOF-CoSe₂@MoSe₂ CoSe₂@MoSe₂	1.0 mol/L KOH	109.87	183.81	1.53	Core of the core-shell	[65]
CoSe₂@DC	0.5 mol/L H₂SO₄	132	—	—	Nanoparticles	[68]
MOF-D CoSe₂	0.5 mol/L H₂SO₄	195	—	—	Flower-like nanoplates	[69]
MOF-D CoSe₂	1.0 mol/L KOH	—	320	—	Flower-like nanoplates	[69]
Notes: NC NSs—Nitrogen doped carbon nanosheets; N/C-CNT—N-doped graphitized carbon carbon nanotube; CNTs—Carbon nanotubes; rGO—Reduced graphene oxide; CFC—Carbon fabric collector; CF—Carbon fiber; CC/MOF—Metal organic framework on carbon cloth; DC—Defective carbon; MOF-D—Metal organic framework-derived; a—The overpotential and cell voltage are obtained at the current density of 10 mA·cm^-2; b—The overpotential and cell voltage are obtained at the current density of 50 mA·cm^-2.

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