Recent developments in the use of single-atom catalysts for water splitting

doi:10.1016/S1872-2067(20)63619-1

Abstract

Abstract:

Electrochemical water splitting is regarded as the most promising approach to produce hydrogen. However, the sluggish electrochemical reactions occurring at the anode and cathode, namely, the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER), respectively, consume a tremendous amount of energy, seriously hampering its wide application. Recently, single-atom catalysts (SACs) have been proposed to effectively enhance the kinetics of these two reactions. In this minireview, we focus on the recent progress in SACs for OER and HER applications. Three classes of SACs have been reviewed, i.e., alloy-based SACs, carbon-based SACs and SACs supported on other compounds. Different factors affecting the activities of SACs are also highlighted, including the inherent element property, the coordination environment, the geometric structure and the loading amount of metal atoms. Finally, we summarize the current problems and directions for future development in SACs.

Key words: Single-atom catalyst, Electrochemical water splitting, Inherent element property, Coordination environment, Geometric structure

Yao Wang, Xun Huang, Zidong Wei. Recent developments in the use of single-atom catalysts for water splitting[J]. Chinese Journal of Catalysis, 2021, 42(8): 1269-1286.

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Figures/Tables 8

Fig. 1. Activity trends towards hydrogen evolution (a) and oxygen evolution (b). Panel (a) reprinted with permission from ref. [64] Copyright 2015, The Royal Society of Chemistry. Panel (b) reprinted with permission from Ref. [67] Copyright 2011, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Table 1 Recent progress in SACs for electrochemical water splitting.

Reaction	Catalyst	Electrolyte	Overpotential	Re啊啊啊f.
HER	Ir₁@Co/NC	1 M KOH	0.060 V @10 mA cm^-2	[37]
	Ru-NC-700	1 M KOH	0.012 V @10 mA cm^-2	[41]
	A-Ni@DG	0.5 M H₂SO₄	0.070 V @10 mA cm^-2	[49]
	Pt₁/MC	0.5 M H₂SO₄	0.065 V @100 mA cm^-2	[52]
	W-SAC	0.5 M H₂SO₄	0.105 V @10 mA cm^-2	[69]
	Pt-1T’MoS₂	0.5 M H₂SO₄	0.180 V @10 mA cm^-2	[70]
	A-CoPt-NC	0.5 M H₂SO₄	0.027 V @10 mA cm^-2	[71]
	A-CoPt-NC	1 M KOH	0.050 V @10 mA cm^-2	[71]
	Pt/np-Co_0.85Se	1 M phosphate buffer solutions (PBS)	0.050 V @10 mA cm^-2	[72]
	Mo₂TiC₂T_x-Pt_SA	0.5 M H₂SO₄	0.077 V @100 mA cm^-2	[73]
	Mo₂TiC₂T_x-Pt_SA	0.5 M PBS	0.061 V @10 mA cm^-2	[73]
	Pt/p-MWCNTs	0.5 M H₂SO₄	0.044 V @10 mA cm^-2	[74]
	NiSA-MoS₂	1 M KOH	0.098 V @10 mA cm^-2	[75]
	NiSA-MoS₂	0.5 M H₂SO₄	0.110 V @10 mA cm^-2	[75]
	Ru@Co-SAs/N-C	1 M KOH	0.007 V @10 mA cm^-2	[76]
		0.5 M H₂SO₄	0.057 V @10 mA cm^-2
		1 M PBS	0.055 V @10 mA cm^-2
	ALD50Pt/NGNs	0.5 M H₂SO₄	0.050 V @16 mA cm^-2	[77]
	Ni/GD	0.5 M H₂SO₄	0.088 V @10 mA cm^-2	[78]
	Fe/GD	0.5 M H₂SO₄	0.066 V @10 mA cm^-2	[78]
	Pt₁/hNCNC-2.92	0.5 M H₂SO₄	0.015 V @10 mA cm^-2	[79]
	Co₁/PCN	1 M KOH	0.138 V @10 mA cm^-2	[80]
	SANi-PtNWs	1 M KOH	0.070 V @11mA cm^-2	[81]
	Co-substituted Ru	1 M KOH	0.013 V @11mA cm^-2	[82]
	Pt₁/OLC	0.5 M H₂SO₄	0.038 V @11mA cm^-2	[83]
	RuAu-0,2	1 M KOH	0.024 V @11mA cm^-2	[84]
	Fe-N₄ SAs/NPC	1 M KOH	0.202 V @10 mA cm^-2	[85]
	PtSA-NT-NF	1 M PBS	0.024 V @10 mA cm^-2	[86]
	Ru SAs@PN	0.5 M H₂SO₄	0.024 V @10 mA cm^-2	[87]
	Cu@MoS₂	0.5 M H₂SO₄	0.131 V @10 mA cm^-2	[88]
	Ru-MoS₂/CC	1 M KOH	0.041 V @10 mA cm^-2	[89]
		0.5 M H₂SO₄	0.061 V @10 mA cm^-2
		1 M PBS	0.114 V @10 mA cm^-2
	Pt SASs/AG	0.5 M H₂SO₄	0.012 V @10 mA cm^-2	[90]
	CoSAs/PTF-600	0.5 M H₂SO₄	0.094 V @10 mA cm^-2	[91]
	SACo-N/C	1 M KOH	0.178 V @10 mA cm^-2	[92]
	SACo-N/C	0.5 M H₂SO₄	0.169 V @10 mA cm^-2	[92]
	RuSA-N-S-Ti₃C₂T_x	0.5 M H₂SO₄	0.151 V @10 mA cm^-2	[93]
	Mo₁N₁C₂	0.1 M KOH	0.132 V @10 mA cm^-2	[94]
OER	Ir₁@Co/NC	1 M KOH	0.260 V @10 mA cm^-2	[37]
	Ru-N-C	0.5 M H₂SO₄	0.267 V @10 mA cm^-2	[40]
	CoIr-0.2	1 M PBS	0.373 V @10 mA cm^-2	[42]
	A-Ni@DG	1 M KOH	0.270 V @10 mA cm^-2	[49]
	P-O/FeN₄-CNS	0.1 M KOH	0.390 V @10 mA cm^-2	[54]
	Fe-N₄ SAs/NPC	1 M KOH	0.440 V @10 mA cm^-2	[85]
	Au@Ni₂P-350°C	1 M KOH	0.240 V @10 mA cm^-2	[95]
	Co-C₃N₄@CS	1 M KOH	0.470 V @50 mA cm^-2	[96]
	Co-Fe-N-C.	1 M KOH	0.309 V @10 mA cm^-2	[97]
	Co-C₃N₄/CNT	1 M KOH	0.380 V @10 mA cm^-2	[98]
	CoNi-SAs/NC	1 M KOH	0.340 V @10 mA cm^-2	[99]
	Au₁N_x	0.1 M KOH	0.450 V @10 mA cm^-2	[100]
	w-Ni(OH)₂	1 M KOH	0.273 V @10 mA cm^-2	[101]
	Ni-NHGF	1 M KOH	0.331 V @10 mA cm^-2	[102]
	Ru₁-Pt₃Cu	0.1 M HClO₄	0.220 V @10 mA cm^-2	[103]
	Ru/CoFe-LDH	1 M KOH	0.198 V @10 mA cm^-2	[104]
	0.5 wt% Pt/NiO	1 M KOH	0.358 V @10 mA cm^-2	[105]
	Ir@Co	1 M KOH	0.273 V @10 mA cm^-2	[106]
	HCM@Ni-N.	1 M KOH	0.304 V @10 mA cm^-2	[107]
	SCoNC	0.1 M KOH	0.310 V @10 mA cm^-2	[108]
	Co-N_x/C NRA	0.1 M KOH	0.300 V @10 mA cm^-2	[109]

Table 1 Recent progress in SACs for electrochemical water splitting.

Reaction	Catalyst	Electrolyte	Overpotential	Re啊啊啊f.
HER	Ir₁@Co/NC	1 M KOH	0.060 V @10 mA cm^-2	[37]
	Ru-NC-700	1 M KOH	0.012 V @10 mA cm^-2	[41]
	A-Ni@DG	0.5 M H₂SO₄	0.070 V @10 mA cm^-2	[49]
	Pt₁/MC	0.5 M H₂SO₄	0.065 V @100 mA cm^-2	[52]
	W-SAC	0.5 M H₂SO₄	0.105 V @10 mA cm^-2	[69]
	Pt-1T’MoS₂	0.5 M H₂SO₄	0.180 V @10 mA cm^-2	[70]
	A-CoPt-NC	0.5 M H₂SO₄	0.027 V @10 mA cm^-2	[71]
	A-CoPt-NC	1 M KOH	0.050 V @10 mA cm^-2	[71]
	Pt/np-Co_0.85Se	1 M phosphate buffer solutions (PBS)	0.050 V @10 mA cm^-2	[72]
	Mo₂TiC₂T_x-Pt_SA	0.5 M H₂SO₄	0.077 V @100 mA cm^-2	[73]
	Mo₂TiC₂T_x-Pt_SA	0.5 M PBS	0.061 V @10 mA cm^-2	[73]
	Pt/p-MWCNTs	0.5 M H₂SO₄	0.044 V @10 mA cm^-2	[74]
	NiSA-MoS₂	1 M KOH	0.098 V @10 mA cm^-2	[75]
	NiSA-MoS₂	0.5 M H₂SO₄	0.110 V @10 mA cm^-2	[75]
	Ru@Co-SAs/N-C	1 M KOH	0.007 V @10 mA cm^-2	[76]
		0.5 M H₂SO₄	0.057 V @10 mA cm^-2
		1 M PBS	0.055 V @10 mA cm^-2
	ALD50Pt/NGNs	0.5 M H₂SO₄	0.050 V @16 mA cm^-2	[77]
	Ni/GD	0.5 M H₂SO₄	0.088 V @10 mA cm^-2	[78]
	Fe/GD	0.5 M H₂SO₄	0.066 V @10 mA cm^-2	[78]
	Pt₁/hNCNC-2.92	0.5 M H₂SO₄	0.015 V @10 mA cm^-2	[79]
	Co₁/PCN	1 M KOH	0.138 V @10 mA cm^-2	[80]
	SANi-PtNWs	1 M KOH	0.070 V @11mA cm^-2	[81]
	Co-substituted Ru	1 M KOH	0.013 V @11mA cm^-2	[82]
	Pt₁/OLC	0.5 M H₂SO₄	0.038 V @11mA cm^-2	[83]
	RuAu-0,2	1 M KOH	0.024 V @11mA cm^-2	[84]
	Fe-N₄ SAs/NPC	1 M KOH	0.202 V @10 mA cm^-2	[85]
	PtSA-NT-NF	1 M PBS	0.024 V @10 mA cm^-2	[86]
	Ru SAs@PN	0.5 M H₂SO₄	0.024 V @10 mA cm^-2	[87]
	Cu@MoS₂	0.5 M H₂SO₄	0.131 V @10 mA cm^-2	[88]
	Ru-MoS₂/CC	1 M KOH	0.041 V @10 mA cm^-2	[89]
		0.5 M H₂SO₄	0.061 V @10 mA cm^-2
		1 M PBS	0.114 V @10 mA cm^-2
	Pt SASs/AG	0.5 M H₂SO₄	0.012 V @10 mA cm^-2	[90]
	CoSAs/PTF-600	0.5 M H₂SO₄	0.094 V @10 mA cm^-2	[91]
	SACo-N/C	1 M KOH	0.178 V @10 mA cm^-2	[92]
	SACo-N/C	0.5 M H₂SO₄	0.169 V @10 mA cm^-2	[92]
	RuSA-N-S-Ti₃C₂T_x	0.5 M H₂SO₄	0.151 V @10 mA cm^-2	[93]
	Mo₁N₁C₂	0.1 M KOH	0.132 V @10 mA cm^-2	[94]
OER	Ir₁@Co/NC	1 M KOH	0.260 V @10 mA cm^-2	[37]
	Ru-N-C	0.5 M H₂SO₄	0.267 V @10 mA cm^-2	[40]
	CoIr-0.2	1 M PBS	0.373 V @10 mA cm^-2	[42]
	A-Ni@DG	1 M KOH	0.270 V @10 mA cm^-2	[49]
	P-O/FeN₄-CNS	0.1 M KOH	0.390 V @10 mA cm^-2	[54]
	Fe-N₄ SAs/NPC	1 M KOH	0.440 V @10 mA cm^-2	[85]
	Au@Ni₂P-350°C	1 M KOH	0.240 V @10 mA cm^-2	[95]
	Co-C₃N₄@CS	1 M KOH	0.470 V @50 mA cm^-2	[96]
	Co-Fe-N-C.	1 M KOH	0.309 V @10 mA cm^-2	[97]
	Co-C₃N₄/CNT	1 M KOH	0.380 V @10 mA cm^-2	[98]
	CoNi-SAs/NC	1 M KOH	0.340 V @10 mA cm^-2	[99]
	Au₁N_x	0.1 M KOH	0.450 V @10 mA cm^-2	[100]
	w-Ni(OH)₂	1 M KOH	0.273 V @10 mA cm^-2	[101]
	Ni-NHGF	1 M KOH	0.331 V @10 mA cm^-2	[102]
	Ru₁-Pt₃Cu	0.1 M HClO₄	0.220 V @10 mA cm^-2	[103]
	Ru/CoFe-LDH	1 M KOH	0.198 V @10 mA cm^-2	[104]
	0.5 wt% Pt/NiO	1 M KOH	0.358 V @10 mA cm^-2	[105]
	Ir@Co	1 M KOH	0.273 V @10 mA cm^-2	[106]
	HCM@Ni-N.	1 M KOH	0.304 V @10 mA cm^-2	[107]
	SCoNC	0.1 M KOH	0.310 V @10 mA cm^-2	[108]
	Co-N_x/C NRA	0.1 M KOH	0.300 V @10 mA cm^-2	[109]

Fig. 2. (a) The synthetic procedure, the EXAFS spectra of the Co K-edge and OER performance of cobalt-based SACs by using KCl particles as the growth seeds; reprinted with permission from Ref. [108] Copyright 2019, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) The synthetic procedure, the EXAFS spectra of the Co K-edge and OER performance of SACs electrode without any binders; reprinted with permission from Ref. [139] Copyright 2011, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) The synthetic procedure, HAADF-STEM image and HER performance of cobalt based SACs prepared by Co2+-SCN- compound and C3N4 precursors; reprinted with permission from Ref. 92 Copyright 2019, Science China Press. Published by Elsevier B.V. and Science China Press. (d) The HER performance of single platinum atoms supported on single-wall carbon nanotubes and the adsorption of Pt onto (14,0) SWNT and graphene. Reprinted with permission from Ref. [151] Copyright 2017, American Chemical Society.

Fig. 3. (a) HAADF signal analysis, EXAFS spectra of the Pt K-edge O and mass activity for 0.5 wt% Pt/Ni, and simulated OER element steps proceeded at the Pt-doped γ-NiOOH and the corresponding energy profiles of the OER at 1.23 V. Reprinted with permission from Ref. [105] Copyright 2018, The Royal Society of Chemistry. (b) HAADF-STEM and OER performance for single gold atoms-doped NiFe(OH)2, and simulated OER element steps and the corresponding energy profiles on the surface of single gold atoms-doped NiFe(OH)2. Reprinted with permission from Ref. [161] Copyright 2018, American Chemical Society. (c) The OER performance of single tungsten atoms-doped Ni(OH)2 nanosheets, and simulated OER element steps and the corresponding energy profiles for single tungsten atoms-doped Ni(OH)2 nanosheets and Ni(OH)2 nanosheets. Reprinted with permission from Ref. [101] Copyright 2019, Springer Nature. (d) The charge density difference on the Ni/Cr2CO2 surface and the schematic of the single metal atoms anchored on Cr2CO2 surface for overall water splitting. Reprinted with permission from Ref. [165] Copyright 2019, American Chemical Society.

Fig. 4. (a) The volcano curve of exchange current as a function of the Gibbs free energy for hydrogen binding on different active sites on the GDY monolayer. (b) Activity trends toward OER, the negative maximum potential-determining step was plotted against the (ΔGO* - ΔGOH*) step; reproduced with permission from Ref. [173] Copyright 2019 WILEY‐VCH Verlag GmbH & Co. KGaA, Weinheim. (c) The relation between currents (log(i0)) and ΔGH* indicates a volcano curve. Reprinted with permission from Ref. [175] Copyright 2015, The Royal Society of Chemistry. (d) Downshift of the conduction band (CB) upon addition of a single Co and Ni metal atom at the Mo atop site, respectively. Reprinted with permission from Ref. [176] Copyright 2018, The Royal Society of Chemistry.

Fig. 5. The HER volcano curve (a) and OER volcano plot (b) for various low-coordinated transition metals/graphene composite. Reprinted with permission from Ref. [187] Copyright 2017, The Royal Society of Chemistry. (c) Gibbs free energy diagram of HER and DFT optimized geometry of Pt-S4 complexes in the presence of water (black) and CO (red). Reprinted with permission from Ref. [189] Copyright 2018, American Chemical Society. (d) OER performance of Co-Fe double-atom catalyst; Inset: proposed model for the formation of Co-Fe double-atom catalyst. Reprinted with permission from Ref. [97] Copyright 2019, American Chemical Society.

Fig. 6. SEM (a) and HAADF-STEM (b) images of SS-Co-SAC NSAs. Reprinted with permission from Ref. [203] Copyright 2019, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (c) TEM image and the corresponding EDS maps of Mo-SAC. (d) HAADF-STEM images of Mo-SAC. Reprinted with permission from Ref. [94] Copyright 2017, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim. (e) FESEM and ADF-STEM image of HCM@Ni-N. (f) HAADF-STEM image of HCM@Ni-N. Reprinted with permission from Ref. [107] Copyright 2019, Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fig. 7. (a) The cascade anchoring strategy for the synthesis of M-NC SACs. Reprinted with permission from Ref. [48] Copyright 2019, Springer Nature. (b) Six typical configurations of [PtCl6]2- on different supports with different nitrogen atoms in micropores and corresponding calculated free energies. Reprinted with permission from Ref. [79] Copyright 2019, Springer Nature. (c) Schematic illustration of the iced-photochemical process and HER performance of the corresponding prepared SACs (scale bar, 2 nm). Reprinted with permission from Ref. [52] Copyright 2017, Springer Nature.

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