Deep Eutectic Solvent-Mediated Electrocatalysts for Water Splitting
Abstract
:1. Introduction
Type | Composition | Terms | Example | Ref. |
---|---|---|---|---|
Type I | R1R2R3R4N+·X–+MClx | X is a Lewis base, generally a halide anion; M = Zn, Sn, Fe, Al, Ga, In, etc. | ChCl/ZnCl2 | [24] |
Type II | R1R2R3R4N+·X–+MClx·yH2O | X is a Lewis base, generally a halide anion; M = Cr, Co, Cu, Ni, Fe, etc | ChCl/NiCl2·6H2O | [24] |
Type III | R1R2R3R4N+·X–+HBD | HBDs include RCONH2, RCOOH, ROH, etc | ChCl/urea, ChCl/EG, ChCl/glycerol | [25] |
Type IV | MClx·yH2O+HBD | M = Zn, Sn, Fe, Al, etc; HBDs include RCONH2, RCOOH, ROH, etc | [25] | |
Type V | nonionic, molecular HBAs +HBDs | thymol/menthol thymol/lidocaine | [26] |
- (1)
- DESs are considered emerging green solvents and promisingly soft templates [37]. This is because DESs have special properties. Firstly, they exhibit fine solubility for metal salts, so that they are beneficial in synthesizing catalysts. Secondly, the low vapor pressure and high thermal stability of DESs allow the progress of reactions at high temperature and ambient pressure, avoiding the danger of high pressure. Thirdly, owing to the hydrogen bond, highly ionic strength and the viscosity of DESs, the microenvironment is different from that in conventional solvents. The supramolecular nature of DESs can tune structures and sizes of micro/nanomaterials.
- (2)
- DESs can serve as active reactants to prepare catalysts. Their designability makes them P, S, N, C or metals sources (such as Fe, Co, Ni and so on) to form phosphides, sulfides, nitrides, carbides or metal-based catalysts [38,39]. Compared with traditional heteroatom sources, they are safe and green. Moreover, owing to the influence of the special liquid structure of DESs during the reaction process, the obtained products show different structures and performance from those obtained from the conventional reactants. In addition, the conversion of DESs into electrocatalysts can reduce waste emissions and simplify operation processes.
- (3)
- The unique physicochemical characteristics of DESs result in different nucleation and growth mechanisms from those in conventional solvents through charge neutralization, changes in reduction potential as well as chemical activity, and determination of growth along the preferred crystallographic directions. In addition, DESs are able to change the activity order of metals, leading to some displacement reactions that cannot occur in aqueous solutions being undertaken in DESs [40].
2. Deep Eutectic Solvents as Both Green Solvents and Structure-Directed Reagents Simultaneously for the Preparation of HER and OER Electrocatalysts
Catalyst | Applied DES | Preparation Method | Catalytic Performance | ||||||||
---|---|---|---|---|---|---|---|---|---|---|---|
HER | OER | Water Splitting | |||||||||
Electrolyte | η (mV)@ Current Density (mA cm−2) | Tafel Slope (mV dec−1) | Electrolyte | η (mV)@ Current Density (mA cm−2) | Tafel Slope (mV dec−1) | Electrolyte | Potential (V)@ Current Density (mA cm−2) | Ref. | |||
Ni | ChCl/Urea | Electrodeposition | 1 M KOH | 153@30 | 185 | –– | –– | –– | –– | –– | [57] |
Ni/TiO2 | ChCl/EG | Electrodeposition | 1 M NaOH | –– | 122 | –– | –– | –– | –– | –– | [58] |
Ni/Ni(OH)2 | ChCl/EG | Electrodeposition | 1 M KOH | 110@10 | 83.9 | 1 M KOH | 290@10 | 120.9 | –– | –– | [59] |
NiSx | ChCl/EG | Electrodeposition | 1 M KOH | 54@10 | 54 | –– | –– | –– | –– | –– | [60] |
Ni | ChCl/EG | GRR | 1 M KOH | 170@10 | 98.5 | –– | –– | –– | –– | –– | [61] |
Ni3S2 | ChCl/EG | GRR | 1 M KOH | 60.8@10 | 67.5 | –– | –– | –– | –– | –– | [62] |
Ni3S2 | ChCl/EG | GRR | 0.5 M H2SO4 | 63.5@10 | 91.6 | –– | –– | –– | –– | –– | [62] |
NiPx | ChCl/EG | Electrodeposition | 1 M KOH | 105@10 | 44.7 | –– | –– | –– | –– | –– | [64] |
Ni–P | ChCl/EG | Electrodeposition | 1 M KOH | 105@50 | 72.9 | –– | –– | –– | –– | –– | [65] |
Ni–Mo | ChCl/EG | Electrodeposition | 1 M KOH | 63@20 | 49 | 1 M KOH | 335@20 | 108 | 1 M KOH | 1.59@10 | [66] |
Ni–Mo–Cu | ChCl/Urea | Electrodeposition | 1 M KOH | 93@10 | 105 | –– | –– | –– | –– | –– | [67] |
Ni–Cu | ChCl/EG | Electrodeposition | 1 M KOH | 128@10 | 57.2 | –– | –– | –– | –– | –– | [68] |
Ni–Co–Sn | ChCl/EG | Electrodeposition | 1 M KOH | –– | 121 | –– | –– | –– | –– | –– | [69] |
Ni–Fe | ChCl/EG | Electrodeposition | 0.1 M KOH | 316@10 | 62 | –– | –– | –– | –– | –– | [70] |
Ni–Fe | ChCl/Urea | Electrodeposition | 0.5 M NaOH | 256@10 | 140.1 | 0.5 M NaOH | 406@10 | 84.4 | –– | –– | [71] |
Cox–Ni(OH)2 | ChCl/EG | Electrodeposition | 1 M KOH | 106@10 | 98.2 | 1 M KOH | 330@100 | 126.7 | –– | –– | [72] |
NiCo2O4 | ChCl/Glycerol | Calcining method | –– | –– | –– | 1 M KOH | 320@10 | 67 | –– | –– | [73] |
(FeCoNiCuZn)(C2O4)· 2H2O | Polyethylene glycol (PEG)/Oxalic acid | Ionothermal method | 1 M KOH | 334@10 | 67.93 | [74] | |||||
NiCoxSy | ChCl/EG | Electrodeposition | 1 M KOH | 65@10 | 62.5 | 1 M KOH | 300@20 | 109 | 1M KOH | 1.57@10 | [75] |
S–NiFe2O4/Ni3Fe | ChCl/EG | Electrodeposition | –– | –– | –– | 1 M KOH | 260@10 | 35 | 1 M KOH | 1.52@10 | [76] |
NiCoxSy | ChCl/EG | Electrodeposition | 1 M KOH | 65@20 | 54 | 1 M KOH | 270@20 | 35 | 1 M KOH | 1.57@10 | [77] |
Co | ChCl/Malonic acid | Electrodeposition | –– | –– | –– | 1 M KOH | 350@10 | 76 | –– | –– | [78] |
P–Co | ChCl–EG | Electrodeposition | 1 M KOH | 65@10 | 69.2 | 1 M KOH | 320@10 | 91.15 | 1 M KOH | 1.59@10 | [79] |
Co–O/Co–Se | ChCl/Urea | Electrodeposition | 1 M KOH | 85@10 | 71.9 | 1 M KOH | 340@10 | 67.6 | 1 M KOH | 1.65@10 | [80] |
Co–S | ChCl/EG | Electrodeposition | 1 M KOH | 59@10 | 65 | 1 M KOH | 307@50 | 66.4 | 1 M KOH | 1.69@50 | [81] |
CoSx | Ethanedithiol/n–Butylamine | CO2–assited solution–processed method | –– | –– | –– | 1 M KOH | 302@10 | 64.8 | –– | –– | [82] |
CoV2O6 | ChCl/Malonic acid | Calcining method | –– | –– | –– | 1 M KOH | 324@10 | –– | –– | –– | [83] |
CoFe–LDH | ChCl/Urea | Water injection method | –– | –– | 0.5 M KOH | Onset overpotential 510 | –– | –– | –– | [88] | |
FexCo3–x(PO4)2 | ChCl/Urea | Electrodeposition | 1 M KOH | 108.1@100 | 30.3 | 1 M KOH | 310@10 | 40.2 | 1 M KOH | 1.62@10 | [91] |
FexCo3–x(PO4)2 | ChCl/Urea | Electrodeposition | 0.5 M H2SO4 | 128.8@100 | 42.4 | –– | –– | –– | –– | –– | [91] |
FexCo3–x(PO4)2 | ChCl/Urea | Electrodeposition | 1 M Phosphate–buffered saline (PBS) | 291.5@100 | 117.6 | –– | –– | –– | –– | –– | [91] |
FeSx | ChCl/EG | Electrodeposition | –– | –– | –– | 1 M KOH | 340@10 | –– | –– | –– | [92] |
Fe7S8/Fe2O3 | ChCl/glycerol | Calcining method | –– | –– | –– | 1 M KOH | 229@10 | 49 | –– | –– | [93] |
S–MnOx/Mn | ChCl/EG | Electrodeposition and in–situ electrochemical oxidation | –– | –– | –– | 1 M KOH | 435@10 | 89.97 | –– | –– | [94] |
LaCoO3 | ChCl/Malonic acid | Calcining method | –– | –– | –– | 1 M NaOH | 390@10 | 55.8 | [95] | ||
Pt–Pd@Ag | ChCl/EG | GRR and Electrodeposition | 0.5 M H2SO4 | 28.1@10 | 31.2 | –– | –– | –– | –– | –– | [97] |
Pt–Pd@Ag | ChCl/EG | GRR and Electrodeposition | 1.0 M PBS | 34.8@10 | 32.2 | –– | –– | –– | –– | –– | [97] |
Pt–Pd@Ag | ChCl/EG | GRR and Electrodeposition | 1 M KOH | 23.8@10 | 32.5 | –– | –– | –– | –– | –– | [97] |
Ru | ChCl/urea | Electrodeposition | 0.5 M H2SO4 | 65.7@10 | 97 | –– | –– | –– | –– | –– | [99] |
MoS2 | A series of sugar–based natural DESs | Mechanical stirring | –– | –– | –– | 0.5 M H2SO4 | 339@10 | 94 | –– | –– | [105] |
3. Deep Eutectic Solvents as Reactive Reagents of Metal Electrocatalysts for HER and OER
3.1. Deep Eutectic Solvents as Heteroatom Sources to Prepare Metal Electrocatalysts
3.2. Hydrated Metal Chloride-Based Deep Eutectic Solvents as Metal Sources to Prepare Metal Electrocatalysts
4. Conclusions and Perspectives
4.1. Dialectically Understand the Greenness of DESs and Maximize Their Greenness through Reasonable Design and Effective Control Conditions
4.2. Requiring Further Understanding of the Structure-Composition-Performance Relationship
4.3. Exploring Research on the Preparation of Single-Atom Catalysts in DESs
Author Contributions
Funding
Institutional Review Board Statement
Informed Consent Statement
Data Availability Statement
Conflicts of Interest
References
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Catalyst | Applied DES | Preparation Method | Catalytic Performance | ||||||||
---|---|---|---|---|---|---|---|---|---|---|---|
HER | OER | Water Splitting | |||||||||
Electrolyte | η (mV)@ Current Density (mA cm−2) | Tafel Slope (mV dec−1) | Electrolyte | η (mV)@ Current Density (mA cm−2) | Tafe l Slope (mV dec−1) | Electrolyte | Potential (V)@ Current Density (mA cm−2) | Ref. | |||
La0.5Sr0.5Co0.8Fe0.2O3 | Glucose/Urea | Calcining method | –– | –– | –– | 1.0 M KOH | 304@10 | 62.9 | –– | –– | [115] |
Co@NPC | ChCl/Urea/Gluconic acid ternary | Calcining method | 1 M KOH | 215@10 | 70 | 1 M KOH | 430@10 | 87 | 1 M KOH | 1.74@10 | [116] |
Iron alkoxide | ChCl/Glycerol | Ionothermal method | –– | –– | –– | 1 M KOH | 280@10 | 47 | –– | –– | [117] |
NiCo2S4 | PEG 200/Thiourea | Ionothermal method | –– | –– | –– | 1 M KOH | 337@10 | 64 | –– | –– | [123] |
NiS/Graphene | NiCl2·6H2O/PEG 200 | Calcining method | 1 M KOH | 70@10 | 50.1 | 1 M KOH | 300@10 | 55.8 | 1 M KOH | 1.54@10 | [126] |
NiS2/Graphene | NiCl2·6H2O/Malonic acid | Calcining method | 1 M KOH | 57@10 | 47 | 1 M KOH | 294@10 | 54 | 1 M KOH | 1.52@10 | [127] |
Ni2P/Graphene | NiCl2·6H2O/Malonic acid | Calcining method | 1 M KOH | 103@10 | 56.5 | 1 M KOH | 275@20 | 56.2 | 1 M KOH | 1.51@10 | [128] |
N–C/NiS2 | NiCl2·6H2O/Urea | Calcining method | 1 M KOH | 78@10 | 63.4 | 1 M KOH | 264@10 | 51.3 | 1 M KOH | 1.53@10 | [129] |
NiFe–LDH | FeCl3·6H2O/Urea | Dip**–redox method | 1 M KOH | 160@10 | 42 | 1 M KOH | –– | –– | 1 M KOH | 1.61@10 | [130] |
NiFe–LDH/N–C | NiCl2·6H2O/FeCl3· 6H2O/Urea/Water | Ionothermal method | –– | –– | –– | 0.1 M KOH | 363@500 | 49.8 | –– | –– | [132] |
[Co(NH3)4CO3]Cl | CoCl2·6H2O/Urea | Calcining method | –– | –– | –– | 1 M KOH | 291@10 | 65 | –– | –– | [136] |
N,S,O–C/Co9S8 | CoCl2·6H2O/Thiourea | Calcining method | 1.0 M KOH | 53@10 | 31 | –– | –– | –– | –– | –– | [137] |
N,S,O–C/Co9S8 | CoCl2·6H2O/Thiourea | Calcining method | 1.0 M PBS | 103@10 | 91.2 | –– | –– | –– | –– | –– | [137] |
N,S,O–C/Co9S8 | CoCl2·6H2O/Thiourea | Calcining method | 0.5 M H2SO4 | 68@10 | 45.3 | –– | –– | –– | –– | –– | [137] |
FeCoNi–NS | FeCl3·6H2O/CoCl26H2O/NiCl2·6H2O/L–cysteine | Calcining method | –– | –– | –– | 1 M KOH | 251@10 | 58 | –– | –– | [141] |
High–entropy metal phosphides | [P4444]Cl/Ethylene glycol/Five equimolar hydrated metal chlorides | Eutectic solvent method | 1 M KOH | 136@10 | 85.5 | 1 M KOH | 320@10 | 60.8 | 1 M KOH | 1.78@100 | [142] |
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Zhang, C.; Fu, Y.; Gao, W.; Bai, T.; Cao, T.; **, J.; **n, B. Deep Eutectic Solvent-Mediated Electrocatalysts for Water Splitting. Molecules 2022, 27, 8098. https://doi.org/10.3390/molecules27228098
Zhang C, Fu Y, Gao W, Bai T, Cao T, ** J, **n B. Deep Eutectic Solvent-Mediated Electrocatalysts for Water Splitting. Molecules. 2022; 27(22):8098. https://doi.org/10.3390/molecules27228098
Chicago/Turabian StyleZhang, Chenyun, Yongqi Fu, Wei Gao, Te Bai, Tianyi Cao, Jianjiao **, and Bingwei **n. 2022. "Deep Eutectic Solvent-Mediated Electrocatalysts for Water Splitting" Molecules 27, no. 22: 8098. https://doi.org/10.3390/molecules27228098