电解水金属单原子催化剂的研究进展

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

催化学报 ›› 2021, Vol. 42 ›› Issue (8): 1269-1286.DOI: 10.1016/S1872-2067(20)63619-1

电解水金属单原子催化剂的研究进展

王尧^a^,^b, 黄寻^b^,^*(), 魏子栋^b

^a四川大学新能源与低碳技术研究院, 四川成都 610065
^b重庆大学化学化工学院, 重庆市化工过程清洁能源与资源利用重点实验室, 重庆 400044

收稿日期:2020-09-23 接受日期:2020-10-24 出版日期:2021-08-18 发布日期:2020-12-10
通讯作者: 黄寻
作者简介:^*. 电话/传真: (023)65678931; 电子信箱: huangxun@cqu.edu.cn
基金资助:
国家自然科学基金(21761162015);国家自然科学基金(91834301);国家自然科学基金(21908148);四川省科技项目(2020YJ0088);中央高校基本科研业务费专项资金

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

Yao Wang^a^,^b, Xun Huang^b^,^*(), Zidong Wei^b

^aInstitute of New-Energy and Low-Carbon Technology, Sichuan University, Chengdu 610065, Sichuan, China
^bChongqing Key Laboratory of Chemical Process for Clean Energy and Resource Utilization, College of Chemistry and Chemical Engineering, Chongqing University, Chongqing 400044, China

Received:2020-09-23 Accepted:2020-10-24 Online:2021-08-18 Published:2020-12-10
Contact: Xun Huang
About author:^*. Tel/Fax: +86-23-65678931; E-mail:huangxun@cqu.edu.cn
Supported by:
This work was supported by the National Natural Science Foundation of China(21761162015);This work was supported by the National Natural Science Foundation of China(91834301);This work was supported by the National Natural Science Foundation of China(21908148);Sichuan Science and Technology Program(2020YJ0088);the Fundamental Research Funds for the Central Universities

摘要/Abstract

摘要：

氢能因其能量密度高、清洁无污染等特点, 作为替代化石燃料的能源载体得到了广泛的研究. 如何清洁高效地制备氢气受到了大量研究者的关注. 当前, 以化石能源的热反应所得副产氢气是主要来源. 然而, 采用该类方法不仅不能摆脱化石能源的使用以及温室气体的排放, 还会造成生产氢气的纯度不高, 碳氧化物杂质浓度过高的问题, 严重影响氢气的后续使用. 采用可再生能源(太阳能、风能等)所产富余电, 进行电解水制氢, 产生的氢气不含碳氧化合物杂质, 纯度很高, 可以真正实现碳的零排放, 被认为是未来氢气来源的重要方式. 目前, 电解水制氢在制氢市场的所占份额较小, 而造成这样局面的主要因素是该过程中的高能耗问题. 为了降低能耗, 开发高效催化剂加速两个电极上的电解反应的动力学尤为重要. 近年, 金属单原子催化剂(SACs)因其独特的结构, 在很多研究中被用作电解水催化剂, 进而开发出大量高性能的金属单原子电解水催化剂.
本文综述了近年SACs在电解水催化方面的应用. 首先, 针对电解水反应本身, 总结了阴阳极两侧的电极反应机制以及影响电极催化性能的关键吸附中间物种; 然后, 根据载体的不同, 即合金、碳以及其它化合物将SACs分为三类, 总结了相关电解水催化研究现状, 并且针对不同类型SACs目前的发展情况, 提出了它们各自存在的问题. 其次, 进一步总结了影响SACs电解水催化活性的因素, 提出了四种决定SACs催化性能的影响因子, 分别为金属原子的固有元素性质、配位环境、几何结构和负载量; 同时讨论了这四类影响因素对SACs催化活性的影响机制, 总结了调控各类影响因素的方法, 为SACs的设计提出了一些建议. 最后, 展望了SACs在电解水催化中的应用, 探讨了SACs在催化剂设计及催化机制研究方面的问题, 提出了SACs在电解水催化中的未来发展方向.

关键词: 单原子催化剂, 电解水, 固有元素性质, 配位环境, 几何结构

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

王尧, 黄寻, 魏子栋. 电解水金属单原子催化剂的研究进展[J]. 催化学报, 2021, 42(8): 1269-1286.

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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图/表 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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电解水金属单原子催化剂的研究进展

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

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