Chinese Journal of Catalysis ›› 2023, Vol. 44: 7-49.DOI: 10.1016/S1872-2067(22)64149-4
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Hui Sua,b,1, Jing Jianga,b,1, Shaojia Songc, Bohan Ana,b, Ning Lia,b, Yangqin Gaoa,b, Lei Gea,b,*()
Received:
2022-07-11
Accepted:
2022-09-01
Online:
2023-01-18
Published:
2022-12-08
Contact:
Lei Ge
About author:
Lei Ge (College of New Energy and Materials, China University of Petroleum Beijing) received his B.S. in 2002 and Ph.D degree in 2006 from Tianjin University. At the end of 2006, he joined the faculty of Department of Materials Science and Engineering, China University of Petroleum Beijing. From 2011 to 2012, he did postdoctoral research at The University of California at Riverside. His research interests currently focus on new materials and energy photocatalysis, electrocatalysis with emphasis on design of new catalysts and control of morphology, microstructure and reaction mechanism for hydrogen production, environmental pollutants degradation, etc. Some of his recent progresses include the novel approaches to design cocatalysts decorated photocatalysts with controllable microstructures, the synthesis of novel hollow structured materials with superior catalytic performance, preparation of metal and nonmetal ions doped electrocatalysts derived from MOFs with high overwall water splitting performance. He has coauthored more than 120 peer-reviewed papers. He was invited as a young member of the editorial board of Chin. J. Catal. Since 2020.Supported by:
Hui Su, Jing Jiang, Shaojia Song, Bohan An, Ning Li, Yangqin Gao, Lei Ge. Recent progress on design and applications of transition metal chalcogenide-associated electrocatalysts for the overall water splitting[J]. Chinese Journal of Catalysis, 2023, 44: 7-49.
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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(22)64149-4
Fig. 1. (a) Schematic diagram of an electrolyzer. (b,c) Volcano plots for the HER and OER catalysts. (d?f) Mechanism of HER/OER electrocatalysis in two different media. Reprinted with permission from Ref. [82]. Copyright 2018, Elsevier B.V.
Fig. 2. (a) Synthesis chart of heterostructured MoS2-Ni3S2 HNRs/NF composites. Reprinted with permission from Ref. [99]. Copyright 2017, American Chemical Society. (b) Schematic illustration of the Co9S8/WS2 composites. Reprinted with permission from Ref. [100]. Copyright 2017, Royal Society of Chemistry. (c?e) The preparation of metal sulfides on NF by different methods. Reprinted with permission from Ref. [103?-105]. Copyright 2019, Wiley-VCH GmbH. Copyright 2017, Copyright 2018, Elsevier. B.V.
Fig. 3. Scheme of the whole LPE process containing immersion, insertion, exfoliation, and stabilization. Reprinted with permission from Ref. [115]. Copyright 2016, Wiley-VCH GmbH.
Fig. 4. (a) Process for buildup of multilayer films by the LBL method. Reprinted with permission from Ref. [117]. Copyright 2018, American Chemical Society. (b) Mechanism illustration of electrochemically exfoliating bulk NiPS3 crystals in tetra-n-butylammonium salts solution. Reprinted with permission from Ref. [118]. Copyright 2019, Wiley-VCH GmbH. (c) Schematic illustration of the exfoliation process. Reprinted with permission from Ref. [119]. Copyright 2019, Elsevier. B.V.
Fig. 5. (a) Synthesis of Fe-S/NGF composite. Reprinted with permission from Ref. [123]. Copyright 2021, Science Citation Index Expanded. (b) Synthesis of the C-N-MoS2/CC-700. Reprinted with permission from Ref. [124]. Copyright 2021, Royal Society of Chemistry. (c) Schematic illustration of CoS2, Se:CoS2?x and CoSe1?x electrodes. Reprinted with permission from Ref. [121]. Copyright 2021, Royal Society of Chemistry. (d) The synthetic process of N-CoS2 and CoS2. Reprinted with permission from Ref. [122]. Copyright 2019, Wiley-VCH GmbH. (e) A schematic diagram showing preparation process of samples. Reprinted with permission from Ref. [125]. Copyright 2021, Springer Nature.
Fig. 6. (a) Schematic of the MoS2-NiS2/G. Reprinted with permission from Ref. [130]. Copyright 2020, Royal Society of Chemistry. (b) Schematic of the P-doped MoS2. Reprinted with permission from Ref. [131]. Copyright 2022, Springer Nature.
Fig. 7. (a?c) The process of NH3 stripping S-V-S. Reprinted with permission from Ref. [153]. Copyright 2011, American Chemical Society (d,f) SEM image of MoS2 nanostructures of original growth and chemical exfoliation. (e) Schematic diagram of phase transition from 2H-MoS2 to 1T MoS2 in partial semiconductor induced by P atoms. Reprinted with permission from Ref. [161]. Copyright 2018, Wiley-VCH GmbH.
Catalyst | Preparation strategy | Electrolyte | Overpotential (mV) | Tafel slope (mV dec‒1) | Ref. |
---|---|---|---|---|---|
monolayer MoS2 | hydrothermal synthesis | 0.1 mol L‒1 KOH | 200 | 73 | [ |
Co-Ni3S2 | solvothermal-electrodeposition | 1 mol L‒1 KOH | 80 | 43 | [ |
Co3O4/MoS2 | hydrothermal | 1 mol L‒1 KOH | 205 | 98 | [ |
Ni-N0.19S | vapor-assisted treatment | 1 mol L‒1 KOH | 125 | 42 | [ |
CoMoSx | hydrothermal | 1 mol L‒1 KOH | 89 | 94 | [ |
Ni-Fe-S | solvothermal | 1 mol L‒1 KOH | 115 | 108 | [ |
MoS2/Co3S4 | hydrothermal | 1 mol L‒1 KOH | 90 | 61 | [ |
MoS2-NiS2 | solid-state synthesis | 1 mol L‒1 KOH | 141 | 77 | [ |
NiS0.5Se0.5 | hydrothermal | 1 mol L‒1 KOH | 70 | 78 | [ |
N-CoS2/G | hydrothermal | 1 mol L‒1 KOH | 109 | 69 | [ |
FeS2/CoS2 | vapor-deposition | 1 mol L‒1 KOH | 78 | 44 | [ |
MoS2/NiS2 | hydrothermal | 1 mol L‒1 KOH | 62 | 80 | [ |
PtSA-Ni3S2 | solvothermal | 1 mol L‒1 KOH | 80 | 34 | [ |
Co3S4@FNC-Co | hydrothermal | 1 mol L‒1 KOH | 140 | 103 | [ |
NiPS3 | electrochemical exfoliation | 1 mol L‒1 KOH | 53 | 38 | [ |
MoS2/CoS2 | hydrothermal | 1 mol L‒1 KOH | 71 | 60 | [ |
MoS2/RGO | hydrothermal synthesis | 0.5 mol L‒1 H2SO4 | 100 | 41 | [ |
1T phase MoS2 | chemical exfoliation | 0.5 mol L‒1 H2SO4 | 200 | 40 | [ |
VS2 nanosheets | one-pot hydrothermal | 0.5 mol L‒1 H2SO4 | 43 | 36 | [ |
MoSe2/MoS2 | hydrothermal | 0.5 mol L‒1 H2SO4 | 162 | 61 | [ |
S-RhNi | hydrothermal | 0.5 mol L‒1 H2SO4 | 44 | 24 | [ |
Fe-Ni3S2 | hydrothermal | 0.5 mol L‒1 H2SO4 | 198 | 42 | [ |
N-MoSx | hydrothermal | 0.5 mol L‒1 H2SO4 | 143 | 57 | [ |
Mn-CoS2 | hydrothermal | 0.5 mol L‒1 H2SO4 | 43 | 34 | [ |
Co:FeS2/CoS | solvothermal | 0.5 mol L‒1 H2SO4 | 69 | 46 | [ |
Fe-NiS2 | electrocatalytic/photocatalytic | 0.5 mol L‒1 H2SO4 | 121 | 37 | [ |
MoS2/VG | microwave-assisted | 0.5 mol L‒1 H2SO4 | 85 | 42 | [ |
CoSeS@NC | calcination | 0.5 mol L‒1 H2SO4 | 115 | 43 | [ |
CNT/VS2-MoS2 | hydrothermal sol-gel processes | 0.5 mol L‒1 H2SO4 | 215 | 64 | [ |
CoMoS4NS | solvothermal | 1.0 mol L‒1 PBS | 183 | 116 | [ |
Table 1 Summary of metal sulfide catalysts for hydrogen evolution reaction.
Catalyst | Preparation strategy | Electrolyte | Overpotential (mV) | Tafel slope (mV dec‒1) | Ref. |
---|---|---|---|---|---|
monolayer MoS2 | hydrothermal synthesis | 0.1 mol L‒1 KOH | 200 | 73 | [ |
Co-Ni3S2 | solvothermal-electrodeposition | 1 mol L‒1 KOH | 80 | 43 | [ |
Co3O4/MoS2 | hydrothermal | 1 mol L‒1 KOH | 205 | 98 | [ |
Ni-N0.19S | vapor-assisted treatment | 1 mol L‒1 KOH | 125 | 42 | [ |
CoMoSx | hydrothermal | 1 mol L‒1 KOH | 89 | 94 | [ |
Ni-Fe-S | solvothermal | 1 mol L‒1 KOH | 115 | 108 | [ |
MoS2/Co3S4 | hydrothermal | 1 mol L‒1 KOH | 90 | 61 | [ |
MoS2-NiS2 | solid-state synthesis | 1 mol L‒1 KOH | 141 | 77 | [ |
NiS0.5Se0.5 | hydrothermal | 1 mol L‒1 KOH | 70 | 78 | [ |
N-CoS2/G | hydrothermal | 1 mol L‒1 KOH | 109 | 69 | [ |
FeS2/CoS2 | vapor-deposition | 1 mol L‒1 KOH | 78 | 44 | [ |
MoS2/NiS2 | hydrothermal | 1 mol L‒1 KOH | 62 | 80 | [ |
PtSA-Ni3S2 | solvothermal | 1 mol L‒1 KOH | 80 | 34 | [ |
Co3S4@FNC-Co | hydrothermal | 1 mol L‒1 KOH | 140 | 103 | [ |
NiPS3 | electrochemical exfoliation | 1 mol L‒1 KOH | 53 | 38 | [ |
MoS2/CoS2 | hydrothermal | 1 mol L‒1 KOH | 71 | 60 | [ |
MoS2/RGO | hydrothermal synthesis | 0.5 mol L‒1 H2SO4 | 100 | 41 | [ |
1T phase MoS2 | chemical exfoliation | 0.5 mol L‒1 H2SO4 | 200 | 40 | [ |
VS2 nanosheets | one-pot hydrothermal | 0.5 mol L‒1 H2SO4 | 43 | 36 | [ |
MoSe2/MoS2 | hydrothermal | 0.5 mol L‒1 H2SO4 | 162 | 61 | [ |
S-RhNi | hydrothermal | 0.5 mol L‒1 H2SO4 | 44 | 24 | [ |
Fe-Ni3S2 | hydrothermal | 0.5 mol L‒1 H2SO4 | 198 | 42 | [ |
N-MoSx | hydrothermal | 0.5 mol L‒1 H2SO4 | 143 | 57 | [ |
Mn-CoS2 | hydrothermal | 0.5 mol L‒1 H2SO4 | 43 | 34 | [ |
Co:FeS2/CoS | solvothermal | 0.5 mol L‒1 H2SO4 | 69 | 46 | [ |
Fe-NiS2 | electrocatalytic/photocatalytic | 0.5 mol L‒1 H2SO4 | 121 | 37 | [ |
MoS2/VG | microwave-assisted | 0.5 mol L‒1 H2SO4 | 85 | 42 | [ |
CoSeS@NC | calcination | 0.5 mol L‒1 H2SO4 | 115 | 43 | [ |
CNT/VS2-MoS2 | hydrothermal sol-gel processes | 0.5 mol L‒1 H2SO4 | 215 | 64 | [ |
CoMoS4NS | solvothermal | 1.0 mol L‒1 PBS | 183 | 116 | [ |
Catalyst | Preparation strategy | Current density (mA cm‒2) | Overpotential (mV) | Tafel slope (mV dec‒1) | Ref. |
---|---|---|---|---|---|
Co3O4/MoS2 | solvothermal | 20 | 230 | 45 | [ |
Ni-Fe-S | solvothermal | 10 | 223 | 41 | [ |
NiS2/Fe7S8 | calcination | 50 | 330 | 51 | [ |
MoS2-NiS2 | solid-state synthesis | 10 | 320 | 82 | [ |
Co3S4@FNC-Co | hydrothermal | 10 | 250 | 78 | [ |
CoS1.97-CeO2 | hydrothermal | 10 | 264 | 49 | [ |
NiS0.5Se0.5 | hydrothermal | 10 | 257 | 61 | [ |
MoS2/NiS2 | hydrothermal | 10 | 278 | 91 | [ |
N-CoS2/G | hydrothermal | 10 | 260 | 56 | [ |
FeS2/CoS2 | vapor-deposition | 100 | 302 | 49 | [ |
CoMoOS | solvothermal | 10 | 281 | 75 | [ |
N,S-Graphdiyne | pyrolysis | 10 | 299 | 62 | [ |
Co-CuS0.7 | fast thermolysis | 10 | 270 | 130 | [ |
Ni3S2/VS4 | solvothermal | 50 | 317 | 43 | [ |
NiMoS | hydrothermal | 10 | 260 | 68 | [ |
P-NiS2 | phosphidation | 20 | 225 | 86 | [ |
Ni-Ni3S2 | hydrothermal | 10 | 284 | 56 | [ |
Fe-Ni3S2 | hydrothermal | 10 | 213 | 33 | [ |
Mo-Ni3S2/NixPy | solvothermal | 50 | 238 | 60 | [ |
Ni3S2/MnS | hydrothermal | 10 | 228 | 46 | [ |
Ni3S2-NGQDs/NF | microwave synthetic | 10 | 216 | 95 | [ |
CeOx/CoS | solvothermal | 100 | 418 | 50 | [ |
NiCo2S4/ZnS | calcination | 10 | 220 | 47 | [ |
Ni-Co9S8 | hydrothermal | 50 | 300 | 106 | [ |
MoS2/Fe5Ni4S8 | electrochemical deposition | 10 | 204 | 45 | [ |
Se-(NiCo)Sx/(OH)x | solvothermal | 10 | 155 | 33 | [ |
Fe(OH)3/Ni9S8 | electrochemical deposition | 10 | 206 | 81 | [ |
Co9S8-V3S4 | hydrothermal | 10 | 232 | 59 | [ |
Fe-Ni3S2 | SACVT | 10 | 267 | 103 | [ |
CoMoSx | hydrothermal | 100 | 345 | — | [ |
Table 2 Summary of metal sulfide catalysts for oxygen evolution reaction.
Catalyst | Preparation strategy | Current density (mA cm‒2) | Overpotential (mV) | Tafel slope (mV dec‒1) | Ref. |
---|---|---|---|---|---|
Co3O4/MoS2 | solvothermal | 20 | 230 | 45 | [ |
Ni-Fe-S | solvothermal | 10 | 223 | 41 | [ |
NiS2/Fe7S8 | calcination | 50 | 330 | 51 | [ |
MoS2-NiS2 | solid-state synthesis | 10 | 320 | 82 | [ |
Co3S4@FNC-Co | hydrothermal | 10 | 250 | 78 | [ |
CoS1.97-CeO2 | hydrothermal | 10 | 264 | 49 | [ |
NiS0.5Se0.5 | hydrothermal | 10 | 257 | 61 | [ |
MoS2/NiS2 | hydrothermal | 10 | 278 | 91 | [ |
N-CoS2/G | hydrothermal | 10 | 260 | 56 | [ |
FeS2/CoS2 | vapor-deposition | 100 | 302 | 49 | [ |
CoMoOS | solvothermal | 10 | 281 | 75 | [ |
N,S-Graphdiyne | pyrolysis | 10 | 299 | 62 | [ |
Co-CuS0.7 | fast thermolysis | 10 | 270 | 130 | [ |
Ni3S2/VS4 | solvothermal | 50 | 317 | 43 | [ |
NiMoS | hydrothermal | 10 | 260 | 68 | [ |
P-NiS2 | phosphidation | 20 | 225 | 86 | [ |
Ni-Ni3S2 | hydrothermal | 10 | 284 | 56 | [ |
Fe-Ni3S2 | hydrothermal | 10 | 213 | 33 | [ |
Mo-Ni3S2/NixPy | solvothermal | 50 | 238 | 60 | [ |
Ni3S2/MnS | hydrothermal | 10 | 228 | 46 | [ |
Ni3S2-NGQDs/NF | microwave synthetic | 10 | 216 | 95 | [ |
CeOx/CoS | solvothermal | 100 | 418 | 50 | [ |
NiCo2S4/ZnS | calcination | 10 | 220 | 47 | [ |
Ni-Co9S8 | hydrothermal | 50 | 300 | 106 | [ |
MoS2/Fe5Ni4S8 | electrochemical deposition | 10 | 204 | 45 | [ |
Se-(NiCo)Sx/(OH)x | solvothermal | 10 | 155 | 33 | [ |
Fe(OH)3/Ni9S8 | electrochemical deposition | 10 | 206 | 81 | [ |
Co9S8-V3S4 | hydrothermal | 10 | 232 | 59 | [ |
Fe-Ni3S2 | SACVT | 10 | 267 | 103 | [ |
CoMoSx | hydrothermal | 100 | 345 | — | [ |
Catalyst | Preparation strategy | Reaction/J (mA cm‒2) | Potential (V) | Ref. |
---|---|---|---|---|
MoS2/NiS2||MoS2/NiS2 | hydrothermal | 10 | 1.59 | [ |
NiS||NiS2 | hydrothermal | 10 | 1.58 | [ |
Ni0.33 Co0.67S2||NiCo2O4 | hydrothermal | 10 | 1.69 | [ |
NiS||Ni2P2S6 | calcination | 10 | 1.64 | [ |
MoS2||NiS | reflux reaction | 10 | 1.64 | [ |
MoS2/NiS||MoS2/NiS | solvothermal | 10 | 1.61 | [ |
MoS2-NiS2||MoS2-NiS2 | template-assisted | 10 | 1.64 | [ |
Co-MoS2||Co-MoS2 | vapor-phase hydrothermal | 10 | 1.45 | [ |
CoMoSx/NF||CoMoSx/NF | in situ metathesis reaction | 500 | 1.89 | [ |
Ni2P-Ni3S2||Ni2P-Ni3S2 | hydrothermal | 10 | 1.5 | [ |
N-CoS2/NF||N-CoS2/NF | hydrothermal | 10 | 1.5 | [ |
N-NiMoO4/NiS2||N-NiMoO4/NIS2 | solvent-thermal | 10 | 1.6 | [ |
CoS2-MoS2||CoS2-MoS2 | hydrothermal | 10 | 1.6 | [ |
Ni3S2/MnO2||Ni3S2/MnO2 | hydrothermal | 10 | 1.52 | [ |
CoSx-Ni3S2||CoSx-Ni3S2 | hydrothermal | 100 | 1.63 | [ |
Co9S8/Ni3S2||Co9S8/Ni3S2 | in situ vulcanization | 10 | 1.64 | [ |
Se-MnS/NiS||Se-MnS/NiS | electrodeposition | 10 | 1.47 | [ |
Cu@Cu2S||Cu@Cu2S | electrodeposition | 20 | 1.61 | [ |
NiCo2S4||NiCo2S4 | solvothermal | 10 | 1.6 | [ |
CuCo2S4||CuCo2S4 | hydrothermal | 10 | 1.58 | [ |
P-CoNi2S4||P-CoNi2S4 | gas-phase phosphorization | 10 | 1.54 | [ |
Co-Ni3S2||Co-Ni3S2 | topochemical conversion strategy | 10 | 1.54 | [ |
Ni-Mo-S||Ni-Mo-S | electroplating | 100 | 2.0 | [ |
Co9S8@NOSC||Co9S8@NOSC | hydrothermal | 20 | 1.74 | [ |
NiFe/(Ni,Fe)3S2||NiFe/(Ni,Fe)3S2 | anodic aluminum oxide | 400 | 1.9 | [ |
Co3S4||Ni:Co3S4 | electroplating | 10 | 1.7 | [ |
Table 3 Summary of metal sulfide catalysts for overall water splitting.
Catalyst | Preparation strategy | Reaction/J (mA cm‒2) | Potential (V) | Ref. |
---|---|---|---|---|
MoS2/NiS2||MoS2/NiS2 | hydrothermal | 10 | 1.59 | [ |
NiS||NiS2 | hydrothermal | 10 | 1.58 | [ |
Ni0.33 Co0.67S2||NiCo2O4 | hydrothermal | 10 | 1.69 | [ |
NiS||Ni2P2S6 | calcination | 10 | 1.64 | [ |
MoS2||NiS | reflux reaction | 10 | 1.64 | [ |
MoS2/NiS||MoS2/NiS | solvothermal | 10 | 1.61 | [ |
MoS2-NiS2||MoS2-NiS2 | template-assisted | 10 | 1.64 | [ |
Co-MoS2||Co-MoS2 | vapor-phase hydrothermal | 10 | 1.45 | [ |
CoMoSx/NF||CoMoSx/NF | in situ metathesis reaction | 500 | 1.89 | [ |
Ni2P-Ni3S2||Ni2P-Ni3S2 | hydrothermal | 10 | 1.5 | [ |
N-CoS2/NF||N-CoS2/NF | hydrothermal | 10 | 1.5 | [ |
N-NiMoO4/NiS2||N-NiMoO4/NIS2 | solvent-thermal | 10 | 1.6 | [ |
CoS2-MoS2||CoS2-MoS2 | hydrothermal | 10 | 1.6 | [ |
Ni3S2/MnO2||Ni3S2/MnO2 | hydrothermal | 10 | 1.52 | [ |
CoSx-Ni3S2||CoSx-Ni3S2 | hydrothermal | 100 | 1.63 | [ |
Co9S8/Ni3S2||Co9S8/Ni3S2 | in situ vulcanization | 10 | 1.64 | [ |
Se-MnS/NiS||Se-MnS/NiS | electrodeposition | 10 | 1.47 | [ |
Cu@Cu2S||Cu@Cu2S | electrodeposition | 20 | 1.61 | [ |
NiCo2S4||NiCo2S4 | solvothermal | 10 | 1.6 | [ |
CuCo2S4||CuCo2S4 | hydrothermal | 10 | 1.58 | [ |
P-CoNi2S4||P-CoNi2S4 | gas-phase phosphorization | 10 | 1.54 | [ |
Co-Ni3S2||Co-Ni3S2 | topochemical conversion strategy | 10 | 1.54 | [ |
Ni-Mo-S||Ni-Mo-S | electroplating | 100 | 2.0 | [ |
Co9S8@NOSC||Co9S8@NOSC | hydrothermal | 20 | 1.74 | [ |
NiFe/(Ni,Fe)3S2||NiFe/(Ni,Fe)3S2 | anodic aluminum oxide | 400 | 1.9 | [ |
Co3S4||Ni:Co3S4 | electroplating | 10 | 1.7 | [ |
Fig. 8. (a) Schematic illustration of the synthesis route for the Co9S8/Zn0.8Co0.2S@C. (b) FESEM image of Zn-Co-ZIFs. (c) High-magnification FESEM images of Co9S8/Zn0.8Co0.2S@C. Electrochemical performance of ZnS@C, Zn0.8Co0.2S@C, Co9S8/Zn0.8Co0.2S@C, Co9S8@C, physical mixture, and IrO2@C. (d) Electrochemical performance of ZnS@C, Zn0.8Co0.2S@C, Co9S8/Zn0.8Co0.2S@C, Co9S8@C, physical mixture, and IrO2@C. (e) The current density as a function of scan rate in the charge process. Reprinted with permission from Ref. [278]. Copyright 2018, Elsevier. B.V. (f) Polarization curves of Ni3Sn2S2@Ni3S2, Ni3S2, Pt/C NF and bare NF. (g) Tafel plots of Ni3S2, Ni3Sn2S2@Ni3S2 and Pt/C NF. Reprinted with permission from Ref. [279]. Copyright 2020, Elsevier. B.V. (h) DFT-optimized structures of MoS2/Co9S8 interfaces:MoS2 (001) parallel to Co9S8 (001) and (001) MoS2 perpendicular to Co9S8 (001). Atom colors: Mo, black; Co, blue; and S, yellow. Co-termination at the interface results in the most stable structure. (i) Calculated densities of electronic states for MoS2/Co9S8interfaces with Co termination and with Co9S8. (j) Gibbs free energy changes for four steps of OER at 0 V vs. standard hydrogen electrode. Reprinted with permission from Ref. [280]. Copyright 2019, American Chemical Society.
Fig. 9. (a,b) Characterization, chemical analysis and SEM image for (Co1?xNix)(S1?yPy)2/GO. (c,e) The OER and HER polarization curves of Ni3S2@NGCLs/NF. (d,f) The stability tests of OER and HER. (g) Linear sweeping voltammetry curve of Ni3S2@NGCLs/NF bifunctional catalyst and noble metal catalyst. (h) 1.5 V dry-cell battery assisted water-splitting device. (i) Calculated free-energy diagram of HER over Ni3S2, Ni3S2@C, Ni3S2@NC, at equilibrium potential. (j) Free-energy diagram for the four steps of the OER on the Ni3S2, Ni3S2@C, Ni3S2@NC surface at U = 1.23 V. Reprinted with permission from Ref. [284,288]. Copyright 2018, Wiley-VCH GmbH.
Fig. 10. (a) Illustration of the fabrication of 3D-networked heterostructured Ni2P/Ni3S2 HNAs composites and SAED pattern of High-resolution TEM images. (b,e) HER/OER polarization curves of NF, Ni2P, Ni3S2, Ni(OH)2/Ni3S2, and Pt/C. (c,d) Gibbs free-energy diagrams for H adsorption and calculated electronic density of states. Reprinted with permission from Ref. [253]. Copyright 2018, Elsevier. B.V. (f,g) TEM image, and HRTEM image of Co9S8/S-CNTs. Reprinted with permission from Ref. [289]. Copyright 2019, Wiley-VCH GmbH. (h,i) HRTEM at the boundary of Mo2C and MoS2 and scanning transmission electron microscopy of (MoS2)0.125Mo2C. Reprinted with permission from Ref. [290]. Copyright 2018, Elsevier. B.V.
Fig. 11. (a) Schematic illustration of the synthesis process for V-doped NiS2. (b) TEM images of 10% VNS. (c) PXRD patterns of bare NiS2 and 10% VNS (inset: zoomed-in view of XRD patterns). (d) Ni K-edge XANES of bare NiS2 and 10% VNS (inset: zoomed-in view of the Ni K-edge XANES). (e) FT V K-edge FT(k3(χ(k))) of VS2 and 10% VNS. (f,g) LSV polarization curves of bare NiS2, IrO2, Pt/C, and 10% VNS for OER and HER. (h) LSV curves of the typical two-electrode system by using nickel foam supported 10% VNS as both the cathode and anode in 1 mol L?1 KOH. Reprinted with permission from Ref. [295]. Copyright 2017, American Chemical Society.
Fig. 12. (a) Schematic of the formation of NF/T(Ni3S2/MnS-O) on NF. (b) ESR spectra of NF/MnO2, NF/Ni3S2/MnS and NF/T(Ni3S2/MnS-O). (c,e) Schematics of the HER/OER pathways with Mn and Ni atoms adjacent to OV as active sites. (d,f) LSV curves of NF/T(Ni3S2/MnS-O), NF/Ni3S2/MnS, NF/MnO2, and commercial Pt/C/IrO2 in 1.0 mol L?1 KOH. Reprinted with permission from Ref. [298]. Copyright 2019, Elsevier. B.V. (g) Schematic illustration of the synthesis of S-NiFe2O4. (h) ESR spectra of NiFe2O4 and S-NiFe2O4. (i) IR-corrected LSV curves of NiFe2O4, NiS2/FeS2, and S-NiFe2O4 for HER in 1.0 mol L?1 KOH. (j) The PDOS of S-NiFe2O4. (k) The bond length distribution of NiFe2O4 and S-NiFe2O4. (l) Energy diagram for HER with the S-NiFe2O4 electrocatalyst in an alkaline environment. Reprinted with permission from Ref. [299]. Copyright 2021, Wiley-VCH GmbH.
Fig. 13. (a) Scheme for the preparation of Co3S4 PNSvac. (b) LSV curves of Co3S4 PNSvac. Reprinted with permission from Ref. [301]. Copyright 2018, American Chemical Society. HER free energy diagram for different Co sites (c) and Ni sites (d). Reprinted with permission from Ref. [134]. Copyright 2017, American Chemical Society. (e) LSV polarization curves of pure CoS2, N-doped CoS2, and platinum in 0.5 mol L?1 H2SO4. (f) Stability testing of catalytic materials. (g) Illustration of the creation of S vacancies in the basal plane of MoS2. S is removed with a two-step process in the form of H2S. The created S vacancies can serve as active sites for HER. (h) The calculated surface free energy of pristine MoS2/CoMoP2 (Black line), MoS2/CoMoP2 with S vacancies (MoSx/CoMoP2), and with a hydrogen adsorbed on the S vacancy (MSx(H)/CoMoP2). (i) Characterizations of defected MoS2 nanosheets. (j) High-resolution TEM image of an ultrathin layer of defected MoS2-7H. Reprinted with permission from Ref. [58]. Copyright 2021, Springer Nature.
Fig. 14. (a) Schematic of the design process of the samples. (b?g) XRD, XPS, TEM images and OER/HER polarization curves of the samples. (h) The Bader charge density difference and electron transference of Cu-Ni3S2/Co3S4. (i) Mechanism diagram of electronic coupling between Co and Ni in Cu-Ni3S2/Co3S4. (j) Calculated free energy diagram of OER intermediates. (k) Calculated free energy diagram of H adsorption for Cu-Ni3S2/Co3S4. Reprinted with permission from Ref. [303]. Copyright 2021, Elsevier. B.V.
Fig. 15. (a,b) Calculated ΔGH* diagram of the HER. (c,d) The calculated free-energy diagram of the OER on Co and Ni sites. Reprinted with permission from Ref. [306]. Copyright 2021, Elsevier. B.V. (e) A two-electrode configuration for overall water splitting. (f) OER polarization curves of materials. (g) XPS S 2p spectra of Fe17.5%-Ni3S2/NF before and after OER. Reprinted with permission from Ref. [63]. Copyright 2018, American Chemical Society.
Fig. 16. (a) Schematic illustration of the samples. Electron microscope analysis: (b) SEM images; (c) Atomic-resolution HAADF-STEM image; (d) FT of the Mo K-edge EXAFS spectra of Mo foil, MoO3, and Mo-Co9S8@C; (e) OER polarization curves. (f) The durability measurements for the catalyst; (g) Comparison with other OER electrocatalysts of the overpotentials; (h) HER polarization curves in 0.5 mol L?1 H2SO4; (i) Overall water splitting characteristics; (j) Optical photograph of overall water splitting using Mo-Co9S8@C/CC powered by an AA battery. Reprinted with permission from Ref. [308]. Copyright 2019, Wiley-VCH GmbH.
Fig. 17. (a) Calculated density of states for samples. (b) The Cdl of N-Ni3S2/NF and Ni3S2/NF. (c,d) Calculated HER/water adsorption energy for the materials, respectively. Reprinted with permission from Ref. [311]. Copyright 2017, Wiley-VCH GmbH. (e) Schematic illustration. (f) Reaction energy of H adsorption. Reprinted with permission from Ref. [312]. Copyright 2018, Wiley-VCH GmbH. (g) Free energy diagram of HER of (Ni,Fe)3S2/NF and P-(Ni,Fe)3S2/NF. (h) Projected DOS on the (2?10) surface of (Ni,Fe)3S2/NF and P-(Ni,Fe)3S2/NF. (i,j) LSV curves of materials. Reprinted with permission from Ref. [313]. Copyright 2019, American Chemical Society.
Fig. 18. (a?d) The DFT calculation results of the B-Fe7S8/FeS2 electrocatalysts. (a) Free energies of hydrogen adsorption on both S and Fe sites of the FeS2, Fe7S8, B-Fe7S8, and B-Fe7S8/FeS2 electrocatalysts. (b) The electronic density of states of the Fe7S8, B-Fe7S8, and B-Fe7S8/FeS2 electrocatalysts. Dependence of free energies of hydrogen adsorption on the d-band centers of Fe-3d state (c) and the p-band centers of S-3p state (d). (e) Schematic illustration of the synthesis steps of the B-Fe7S8/FeS2 electrocatalysts. The normalized XANES spectra (f) and FT-EXAFS curves (g) at the Fe K-edge of a Fe foil, the FeS2, and B-Fe7S8/FeS2 electrocatalysts. (h) The iR-corrected HER polarization curves. (i) The Cdl values of the FeS2 and B-Fe7S8/FeS2 electrocatalysts. (j) Schematics of the HER pathway on the B-Fe7S8/FeS2 electrocatalysts in alkaline media. (k) The corresponding free energy diagrams of the B-Fe7S8/FeS2 electrocatalysts toward alkaline HER on the B-Fe7S8 side, the FeS2 side, and the B-Fe7S8/FeS2 heterointerface. Reprinted with permission from Ref. [315]. Copyright 2021, Wiley-VCH GmbH.
Fig. 19. (a,b) Typical field emission scanning electron microscopy (FE-SEM) and TEM images of CoS2. Reprinted with permission from Ref. [316]. Copyright 2018, Wiley-VCH GmbH. (c) LSV curves recorded with iR correction for different catalysts. (d) Scheme of the preparation of Fe/P-CoS2 PCNW. Reprinted with permission from Ref. [317]. Copyright 2022, Royal Society of Chemistry. (e) K-L plots of CoSx@Cu2MoS4-MoS2/NSG at different potentials. (f,g) LSVs of materials for HER/OER in 0.1 mol L?1 KOH at a scan rate of 10 mV s?1. Reprinted with permission from Ref. [320]. Copyright 2020, Wiley-VCH GmbH.
Fig. 20. (a) Calculated free energy diagram of OER intermediates. (b) The optimal reaction paths of several catalytic materials for HER. (c) Schematic diagram of the preparation process of the catalysts. (d,e) HAADF-STEM images of Ru-NiCo2S4, Ru-NiCo2S4?x. (f) XANES of Ru K-edge of Ru-NiCo2S4 and Ru-NiCo2S4?x with Ru metal foil and RuO2 as references. (g) FT EXAFS spectra in R-space. (h,i) OER/HER polarization curves of NiCo2S4, NiCo2S4?x, Ru-NiCo2S4, Ru-NiCo2S4?x, and NF. (j,k) Polarization curves and stability test of Ru-NiCo2S4?x//Ru-NiCo2S4 with different metals toward overall water splitting. Reprinted with permission from Ref. [321]. Copyright 2021, Wiley-VCH GmbH.
Fig. 21. (a) Calculated PDOS of PtSA-Ni3S2, Ni3S2, and Pt foil with aligned Fermi level EF. (b) The free energy diagrams of H2O and H adsorbing on the surface of PtSA-Ni3S2, Ni3S2, and Pt foil. (c) LSV polarization curves of PtSA-Ni3S2@Ag NWs, PtSA-Ni3S2@NF, Ni3S2@Ag NWs, Ag NWs, and Pt/C@NF. (d) Schematic illustration of the in-situ preparation of Ni3S2 phase via sulfuration reaction of metallic Ni on Ag nanowires. (e) FT-EXAFS of Pt K-edge EXAFS signal substrate followed by the electrochemical anchoring of single-atom Pt. (f) Atomic-resolution HAADF-STEM images of PtSA-Ni3S2. Reprinted with permission from Ref. [324]. Copyright 2021, Wiley-VCH GmbH. (g) Single S-vacancies in different agglomerations at the concentration of 12.50%. (h) Schematic of the chemical etching process to introduce single S-vacancies. (i) STEM image together with the line profiles extracted from the areas marked with purple rectangles of a CVD-grown monolayer MoS2 flake film after etching. (j) EPR spectra of etched MoS2 with different etching durations compared to P-MoS2. (k) Electrochemical HER performance of P-MoS2 and MoS2?x. (l) LSV curves of MoS2-60 s before and after 1000 cyclic voltammetry. Reprinted with permission from Ref. [325]. Copyright 2020, American Chemical Society.
Fig. 22. (a) Schematic illustration for the formation mechanism of Ru-MoS2-Mo2C. (b) CS-TEM images of Ru-MoS2-Mo2C nanosheet. (c?e) LSV measurement of different materials for HER/OER and overall water splitting in 1.0 mol L?1 KOH medium. (f) ?GH* comparison between active sites in the structure of Ru-MoS2-Mo2C material model. Reprinted with permission from Ref. [326] Copyright 2021, Elsevier. B.V. (g) Schematic illustration of the fabrication of the CoSAs-MoS2/TiN hybrid. (h) The corresponding structure configurations for the two steps of HER in alkaline condition on Co active sites of CoSAs-MoS2. (i) The Gibbs free-energy diagram for the two steps of HER in alkaline conditions on different sites of the MoS2 and CoSAs-MoS2. (j?l) LSV measurement of different materials for HER/OER and overall water splitting in 1.0 mol L?1 KOH medium. (m) Corresponding stability. Reprinted with permission from Ref. [327]. Copyright 2021, Wiley-VCH GmbH.
Fig. 23. (a) Preparation of (Fe,Co)/N-C. (b) Magnified HAADF-STEM of (Fe,Co)/N-C, showing Fe-Co dual sites dominant in (Fe,Co)/N-C. Reprinted with permission from Ref. [329]. Copyright 2017, American Chemical Society. (c) Schematic illustration for the two-step synthesis of Fe2-N-C. (d) Magnified HAADF-STEM of Fe2N-C. Reprinted with permission from Ref. [331]. Copyright 2019, Elsevier. B.V.
Fig. 24. (a) Electron configuration of 3d orbital. (b) Magnetic exchange sketch. (c) The orbital interaction between Co and *OH under different spin configuration. (d) Polarization curves of the Co0.8Mn0.2-MOF with different times of MS. (e) The spin density distribution of Co0.8Mn0.2-MOF. (f) The theoretical simulation of heating process between conventional annealing treatment and magnetic stimulation. (g) The potential of OER for Co0.8Mn0.2-MOF at 100 mA cm?2. Reprinted with permission from Ref. [334]. Copyright 2021, Springer Nature. (h) LSV curves of CoFe2O4 with and without a constant magnetic field (10000 Oe) under different temperatures. (i) The spin-polarization mechanisms in OER with starting from the step of O* + OH? → *OOH + e? step. Reprinted with permission from Ref. [335]. Copyright 2021, Springer Nature.
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