非晶相电催化剂在电解水领域的研究进展

doi:10.1016/S1872-2067(23)64486-9

催化学报 ›› 2023, Vol. 51: 5-48.DOI: 10.1016/S1872-2067(23)64486-9

非晶相电催化剂在电解水领域的研究进展

王潇涵^a, 田汉^b^,^*(), 余旭^b, 陈立松^c, 崔香枝^a^,^b^,^*(), 施剑林^b

^a中国科学院大学杭州高等研究院, 化学与材料科学学院, 浙江杭州310024
^b中国科学院上海硅酸盐研究所, 高性能陶瓷与超微结构国家重点实验室, 上海200050
^c华东师范大学化学与分子工程学院, 上海市绿色化学与化工过程绿色化重点实验室, 上海200062

收稿日期:2023-04-29 接受日期:2023-07-03 出版日期:2023-08-18 发布日期:2023-09-11
通讯作者: *电子信箱: cuixz@mail.sic.ac.cn (崔香枝), tianhan@mail.sic.ac.cn (田汉)
基金资助:
国家自然科学基金(52172110);上海市科委“科技创新行动计划”港澳台科技合作项目(21520760500);上海市人力资源和社会保障局“超级博士后”激励计划(2021411);中国科学院特别研究助理资助项目.

Advances and insights in amorphous electrocatalyst towards water splitting

Xiaohan Wang^a, Han Tian^b^,^*(), Xu Yu^b, Lisong Chen^c, Xiangzhi Cui^a^,^b^,^*(), Jianlin Shi^b

^aSchool of Chemistry and Materials Science, Hangzhou Institute for Advanced Study, University of Chinese Academy of Sciences, Hangzhou 310024, Zhejiang, China
^bState Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai 200050, China
^cShanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, China

Received:2023-04-29 Accepted:2023-07-03 Online:2023-08-18 Published:2023-09-11
Contact: *E-mail: cuixz@mail.sic.ac.cn (X. Cui), tianhan@mail.sic.ac.cn (H. Tian).
About author:Xiangzhi Cui received her Ph.D. degree in 2009 at Shanghai Institute of Ceramics, Chinese Academy of Sciences, and has been working at the institute since then. Now she is a full professor of the Institute. Her main research interest includes the structural design and synthesis of nanostructured composites, and the electrochemical catalysis for clean energy.
Han Tian received his Ph.D. degree in 2021 at Shanghai Institute of Ceramics, Chinese Academy of Sciences, and has been working as a postdoctor at the institute since then. His main research interest includes the structural design and synthesis of nanostructured composites in water splitting and proton exchange membrane fuel cells.
Supported by:
National Natural Science Foundation of China(52172110);“Scientific and Technical Innovation Action Plan” China Science & Technology Cooperation Project of Shanghai Science and Technology Committee(21520760500);“Super Postdoctoral Incentive Program” of Shanghai Municipal Human Resources and Social Security Bureau(2021411);Special Research Assistant Grant Project from Chinese Academy of Sciences

摘要/Abstract

摘要：

化石燃料短缺和环境污染引发了人们对可持续、清洁和高效新能源的关注. 氢具有能量密度高、燃烧产物清洁等优点, 是一种重要的能源载体, 具有替代化石燃料的潜力. 在各种制氢方法中, 电解水制氢是获取高纯氢气的有效技术, 其包含阴极析氢反应(HER)和阳极析氧反应(OER). 为了实现高效的电化学水分解, 需要使用高效的电催化剂以克服HER和OER的热力学势垒并降低制氢电耗. 目前, 广泛使用的HER和OER催化剂分别是Pt和RuO₂/IrO₂基金属或金属氧化物, 该类贵金属催化剂的高成本和稀缺性严重限制了其在水分解制氢中的广泛应用. 此外, 金红石型RuO₂和IrO₂在阳极高电位下可溶于酸性和碱性电解质溶液中, 致使催化活性下降, 因此, 亟需发展新型高效且稳定的电解水催化剂.
相较于目前报道的晶相电解水催化剂材料, 非晶相催化剂材料没有严格限定的晶体结构, 并具有硬度低、比表面积大和化学稳定性好等优点, 特别是其含有大量随机取向的化学键和表面暴露的缺陷, 可以显著提高活性位点数量, 优化反应物的吸脱附, 因此在电催化领域具有良好的应用前景. 自20世纪80年代末以来, 一系列非晶相材料被成功制备出来且用于HER, OER和全解水中. 考虑到当前非晶相电催化剂在电解水领域取得的进展, 本综述对其合成方法、稳定策略、性能评估、机制探索和理论研究等进行了系统的总结. 阐述了酸性和碱性条件下HER和OER的反应过程和机理, 介绍了非晶电催化剂材料的制备方法, 以及提升其稳定性的策略. 重点介绍了含贵金属(Pt, Pd和Ir等)和非贵金属(Fe, Co, Ni和Mo等)基非晶态电催化剂在HER, OER和全解水中的性能评价, 以及采用能带理论和第一性原理相结合阐述相应的电催化机理. 深入讨论了当前非晶态电催化剂在电解水实际应用中遇到的关键问题, 如非晶催化剂所面临的导电率低、稳定性差(尤其是高电流下)、制备困难、缺乏深入的催化机制研究和工业化前景不明朗等问题, 简要地指出了该领域未来的研究方向: (1)高导电材料的引入. 为了解决非晶材料导电性差的问题, 可考虑引入高导电介质或引入特殊导电结构(如核壳结构等). (2)新颖的合成策略(非晶/结晶结构集成、非晶表面涂覆和创造离子缺陷等). (3)非晶材料结构高度可调的合理使用. 非晶催化剂的结构具有高度可调性, 在催化过程中易发生相转变, 可考虑合理诱导其可控转变. (4)先进的表征手段(原位电镜、原位拉曼、原位XPS和同步辐射等)的开发. (5)理论计算工具(进一步引入机器学习、材料基因组等理论)的使用. (6)更多应用层面的探索. 通过研究催化机制加深对非晶催化剂结构的认知, 提高稳定性, 一方面探究其在实际环境条件(高/低温、高/低pH)下的电解水性能, 另一方面将其扩展到甲醇、甘油等小分子氧化应用中的探究. 综上, 本综述旨在更好地理解非晶相电催化剂在电解水领域的研究现状、机理研究以及存在的挑战等, 从而推动非晶相电催化剂在未来电解水领域中的实际应用.

关键词: 非晶相催化剂, 缺陷工程, 电解水, 析氢反应, 析氧反应

Abstract:

Amorphous materials can markedly enhance the active site amount and optimize the adsorption and desorption of reactants owing to the special structural characteristics of large numbers of randomly oriented bonds and surface-exposed defects. Therefore, many amorphous electrocatalysts have emerged for effectively catalyzing water splitting. Considering the advancement of novel in-situ techniques and theoretical density functional theory calculations, significant progress emerging in amorphous electrocatalysts for water splitting needs to be summarized urgently. Herein, the recent progress of amorphous catalyst materials in water splitting has been systematically reviewed, emphasizing key issues of synthesis methods, stabilization strategies, performance evaluation, mechanistic understanding, integrated experiments, and theoretical studies in water splitting, including hydrogen evolution reaction, oxygen evolution reaction, and overall water splitting. This study focuses on these topics to present the most updated results and the perspectives and challenges for the future development of amorphous electrocatalysts toward water splitting.

Key words: Amorphous catalyst, Defect engineering, Water splitting, Hydrogen evolution reaction, Oxygen evolution reaction

王潇涵, 田汉, 余旭, 陈立松, 崔香枝, 施剑林. 非晶相电催化剂在电解水领域的研究进展[J]. 催化学报, 2023, 51: 5-48.

Xiaohan Wang, Han Tian, Xu Yu, Lisong Chen, Xiangzhi Cui, Jianlin Shi. Advances and insights in amorphous electrocatalyst towards water splitting[J]. Chinese Journal of Catalysis, 2023, 51: 5-48.

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图/表 37

Fig. 1. Overview of amorphous materials for water splitting.

Fig. 2. Schematic diagram of the HER mechanism. Reaction path interpretation of generating H2 gas for Volmer-Tafel (1+2+3) and Volmer-Heyrovsky (1+4) routes in acidic media. Reaction path interpretation of generating H2 gas for both Volmer-Tafel (5+6+7) and Volmer-Heyrovsky (5+8) routes in alkaline media.

Fig. 3. (a) Trassati’s volcano plot for the hydrogen evolution reaction in acid solutions. j00 denotes the exchange current density, and EMH the energy of hydride formation. (b) Volcano plots for hydrogen evolution alkaline aqueous solutions. Note that ascending and descending branch are reversed with respect to (a). Reprinted with permission from Ref. [49]. Copyright 2014, Beilstein Institute.

Fig. 4. AEM (a) and LOM (b) plots of OER in acidic and alkaline media. Red color indicates lattice oxygen on the electrode surface and blue color indicates oxide in solution.

Fig. 5. The adsorption energy scaling relations between oxygen-containing intermediates. (a) Plot of adsorption energies of HOO* and HO* on metal oxides. Hollow symbols represent the adsorption energy on the clean surfaces: perovskites (circle), rutiles (triangle), MnxOy (square), anatase (diamond), Co3O4 (+). The solid symbols represent the adsorption energies on high coverage surfaces. (b) The volcano relationship between ΔGO* ? ΔGHO* and OER activity for major oxides. Reproduced with permission from Ref. [50]. Copyright 2022, Springer Nature.

Fig. 6. The development strategy of amorphous electrocatalysts.

Table 1 Synthetic methods for amorphous electrocatalysts.

Amorphous metal	Catalyst	Synthetic method	Ref.
Precious metal	amorphous Pt nanospheres	one-step stirring method	[32]
	Pd-Cu-S	chemical dealloying method	[62]
	PdNi-S/C	chemical reduction loading method	[63]
	RuO₂-doped Ti/IrO₂-ZrO₂	sol-gel method	[64]
Fe	FeMoPC	electrochemical activation-dealloying	[65]
	FeB, FeSiB, FeCoSiB	plunge cooling method	[66]
	CC@FeOOH-NTs-240 °C	template electro-etching method	[67]
	a-Co₂Fe	chemical reduction method	[68]
Co	Co-30Ni-B	chemical reduction method	[69]
	Co-Mo-S	hydrothermal method	[70]
	Co₂P/CoMoP_x-NF	electrodeposition method	[71]
	CoO_x(Ce)	electrostatic spray deposition method	[72]
	PA-CoS_x(OH)_y	etching and sulfurization	[73]
Ni	NiP/Poplar	electroless plating method	[74]
	Ni-OH/P	chemical reduction loading method	[75]
	NiFe(OH)_x/CP	electrochemical deposition method	[76]
Mo	a-MoS_x	aging approach	[77]
	MoS₃/MWCNT-NC	wet chemistry method	[78]
	N-doped a-MoS_x	chemical reduction method	[79]
Other	WP/Ti	chemical reduction method	[80]
	Cu-A-TiO₂	alternating pulse deposition method	[81]
	TaO_x/Ti	thermal decomposition method	[82]

Fig. 7. (a) Schematic illustration of synthesis process for amorphous cobalt boron alloy (a-CoBx). SEM (b), TEM (c), HAADF-TEM (d) images, elemental mapping (e,f), HRTEM (g) and SAEM (h) images of a-CoBx. Reproduced with permission from Ref. [84]. Copyright 2020, Royal Society of Chemistry.

Fig. 8. (a) Schematic illustration of synthesis process for amorphous Ni-B hollow spheres. SEM (b,d,f) and TEM (c,e,g) micrographs of the polystyrene microspheres before and after Ni-B deposition. Reproduced with permission from Ref. [86]. Copyright 2005, Royal Society of Chemistry.

Fig. 9. Mechanical and self-healing properties of copolymers with different E (ethylene), AHexP (hexylanisyl propylene), and ANaphP (methoxynaphthyl propylene) contents. (a) Glass transition temperature (Tg) versus ANaphP content. (b) Stress-strain curves of copolymers with different AHexP/ANaphP/E ratios. (c) Self-healing tests of terpolymer P1 in air at 25 °C. (d) Self-healing tests of terpolymer P4 in air at 25 °C. The AHexP/ANaphP ratio in the terpolymers could be adjusted by changing the initial monomer feed ratio, affording a series of three-component copolymers with different AHexP/ANaphP/E ratios (P1: 21/19/60, P2: 31/10/59, P3: 11/28/61) and similar molecular weights (P1: Mn = 165 × 103 g mol?1, P2: Mn = 151 × 103 g mol?1, P3: Mn = 124 × 103 g mol?1). Reproduced with permission from Ref. [97]. Copyright 2021, John Wiley and Sons.

P	Mn (10³)	[A^HexP]/[A^NaphP]/[E](mol%)	T_g (°C)
P_EH	164	36/0/64	‒31
P_EN	115	0/41/59	52
P_EH + P_EN	—	—	‒28,50
P1	165	21/19/60	0
P2	151	31/10/59	‒13
P3	124	11/28/61	25

Fig. 10. Polarization curves of different catalysts in 0.5 mol L?1 H2SO4 (a), 1.0 mol L?1 PBS (b) and 1.0 mol L?1 KOH (c). (d) Chronopotential curves obtained over Pt-Pd@NPA at a low current density of 10 mA cm?2 for 50 h (red curve) and at high current density of 1000 mA cm?2 over 100 h without IR correction. Inset: the polarization curves of the Pt-Pd@NPA and Pt/C catalysts, initially and after 10000 CV cycles ranging from 200 to ?200 mV vs. RHE at 100 mV s?1. All the current densities are normalized with the electrode's geometric surface area. (e) TOF values of Pd@NPA and Pt-Pd@NPA compared with both precious and non-precious-based representative catalysts in acidic solution. (f) Top view atomic structure models of Ag (111), Pt (111), Pd (111), Pd@Ag (111), Pt@Ag (111) and Pt-Pd@Ag (111) with H*. (g) Free-energy diagram for hydrogen evolution at equilibrium (U = 0). (h) Volcano plots of j0 as a function of the ?G*H for the as-synthesized Pt-Pd@NPA, Pd@NPA, and common metal catalysts. Reproduced with permission from Ref. [104]. Copyright 2018, Royal Society of Chemistry.

Electrocatalyst	Overpotential (mV) at 10 mA cm^‒2	Tafel slope (mV dec^‒1)	Ref.
AC-Ir NSs	17	27	[106]
Ir@CON	13.4	27	[107]
IrCo-PHNC	21	26.6	[108]
Ru@C₂N	22	30	[109]
Pd/Cu-Pt	22.8	25	[110]
RhP₂@PNC	38	38	[111]
Rh-MoS₂	47	24	[112]
Ru-MoO₂	55	44	[113]
Pt@NHPCP	57	27	[114]
Rh/Si NW	80	24	[115]
Pt ML Ag NF/Ni foam	70	53	[116]
Pt-MoS₂	53	40	[117]

Fig. 11. (a) The schematic illustration of the FeP/FeOx structure. (b) Adsorption energy of water on FeP and FeP/FeO interface. (c) The ΔGH* diagrams for the FeP/FeO interface. (d) Minimum-energy paths for water dissociation on FeP and FeP/FeO interface with structures for initial state (IS), transition state (TS) and final state (FS). Reproduced with permission from Ref. [124]. Copyright 2018, Royal Society of Chemistry.

Fig. 12. (a?d) Charge density difference of CoSe2, CoP, orthorhombic crystalline CoSe2/crystalline CoP heterojunction (CoSe2/c-CoP), and orthorhombic crystalline CoSe2/amorphous CoP heterojunction (CoSe2/a-CoP). The purple, grey-green, and brown spheres denote Co, Se, and P atoms, respectively. The yellow and cyan contours represent charge accumulation and dilution, respectively. (e) ΔGH on different sites of CoSe2, CoP, CoSe2/c-CoP, and CoSe2/a-CoP. (f) The reaction pathway of the HER process. (g) Projected DOS of CoSe2/a-CoP. (h) DOS of the Co 3d band. The vertical lines mark the positions of d-band center. Reproduced with permission from Ref. [125]. Copyright 2022, John Wiley and Sons.

Fig. 13. Structure models and hydrogen adsorption free energies at different sites of [Mo3S13]2?, [Mo6S24]2? clusters and at the [Mo3S13]/Ni3S2 interface. (a) Structure models. (b,c) The diagrams for hydrogen adsorbed at different sites of the clusters, composite and 2H MoS2 slab. Electrochemical results of the a-MoSx-Ni3S2 composite. (d,e) Different-current range LSV curves. (f) Tafel plots of the as-prepared a-MoSx-Ni3S2, Ni3S2/NF, MoS2/NF and NF in 1 mol L?1 KOH. Reproduced with permission from Ref. [133]. Copyright 2019, Royal Society of Chemistry.

Fig. 14. Polarization curves (a) and the corresponding Tafel plots (b), electrochemical impedance spectra (c), electrochemical capacitance calculated from CV (d), TOF value (e) of typical a-MoSx and Sbr-MoSx with bridging S contents in the range from 51% to 67%; (f) HER activity of 67% Sbr-MoSx before and after cycling test. Reproduced with permission from Ref. [77]. Copyright 2019, Elsevier. Polarization curves (g) and the corresponding Tafel plots (h). (i) Electrochemical impedance spectra of MoSx/NCNT and bare MoSx at ?0.2 V versus RHE from 5 MHz to 10 mHz. Reproduced with permission from Ref. [137]. Copyright 2014, American Chemical Society.

Fig. 15. Electrochemical tests in 1 mol L?1 KOH solution. IR-corrected polarization curves (a) and Tafel plots (b) of Cu-A-TiO2, M-TiO2, CuO NW/CF, 20% Pt/C, and CF at 2 mV s?1. (c) Polarization curves for the Cu-A-TiO2 before and after 5000 CV cycles. The inset in panel (c) shows stability testing of Cu-A-TiO2 by chronopotentiometry at static current densities of 10 and 50 mA cm?2. (d) Water adsorption free energy (ΔGH2O), water dissociation energy barrier (ΔGW), and hydrogen adsorption free energy (ΔGH*) on M-TiO2 (001), A-TiO2, and Cu-A-TiO2. Partial electronic density of states (PDOS) of O 2p (e) and total electronic density of states (TDOS) (f) calculated for M-TiO2, A-TiO2, and Cu-A-TiO2. The Fermi level is set at 0 eV. Reproduced with permission from Ref. [81]. Copyright 2020, American Chemical Society. (g,h) Polarization curves of CoW(OH)x, Co(OH)x, and W(OH)x, along with Pt/C and blank Ni foam for comparison. (i) Stability test of CoW(OH)x at the current density of ?20 mA cm?2. Reproduced with permission from Ref. [138]. Copyright 2018, American Chemical Society.

Fig. 16. HER catalysts at different levels of development over time.

Fig. 17. (a) Schematic diagram of the electronic activity enhancement in amorphous structure. (b) Local structural configurations of initial reactant, intermediates or final product on the amorphous RuTe2 surface. (c) Schematic illustration of the OER process under acidic and alkaline conditions. (d) The free energetic pathways for acidic OER at U = 0 V. (e) The alkaline OER pathway at U = 0 V. (f) The OER pathways of acidic and alkaline conditions at U = 1.23 V. Reproduced with permission from Ref. [151]. Copyright 2019, Springer Nature.

Electrocatalyst	Overpotential (mV) at 10 mA cm^‒2	Tafel slope (mV dec^‒1)	Ref.
SnCoFe-Ar	300	42.3	[155]
NCoM-SS-Ar	340	51	[156]
Ni_1.5Sn@triMPO₄-R	240	45.2	[157]
CeO_x/CoO_x	313	66	[158]
NiO/CoN PINWs	300	44.5	[159]
Mo₅₁Ni₄₀Fe₉ NBs	257	51	[160]
Ni/Ni(OH)₂	270	53	[161]
Co₃O₄/CeO₂	270	60	[162]
W₂N/WC	320	122.8	[163]
LaNiO₃	189	36	[164]
Ru/CoFe-LDHs	197	39	[165]
e-ICLDH@GDY	216	43.6	[166]
CoP-MNA	290	65	[167]
Fe-Mn-O NSs/CC	273	63.9	[168]
F/BCN	222	87	[169]
FeOOH(Se)/IF	287	54	[170]
Co_xMo_y@NC	330	46.1	[171]
Ir/CoNiB	178	35.1	[154]

Fig. 18. Polarization curves (a,b) and the corresponding Tafel plots (c) of various catalysts in 1 mol L?1 KOH solution. Reproduced with permission from Ref. [181]. Copyright 2018, Elsevier. (d) The surface distribution of OH- concentration of NiFe-ANR with different scales. (e) The distribution of OH- in the internal channels of NiFe-ANR. (f) The surface distribution of OH- concentration of NiFe-ANNR with different scales. (g) The current density distribution on the surface of NiFe-ANR with different scales. (h) The current density distribution in the internal channels of NiFe-ANR. (i) The current density distribution on the surface of NiFe-ANNR with different scales. Reproduced with permission from Ref. [184]. Copyright 2023, John Wiley and Sons.

Fig. 19. (a) SEM images of CoOx(Ce). Polarization curves (b) and Tafel slopes (c) of CoOx(Ce), CoOx, and RuO2. (d) Current-time curve of CoOx(Ce) recorded in a potentiostatic electrolysis experiment. Inset of (d) shows the LSV curves measured before and after a potentiostatic electrolysis experiment. (e) Comparison of theoretical and detected volume of oxygen generated from a potentiostatic electrolysis. All potentials are corrected with IR drop. EIS spectra (f), Cdl (g), JECSA (h), and Arrhenius plots (i) of CoOx(Ce) and CoOx. All measurements were carried out in 1 mol L?1 KOH solution. Reproduced with permission from Ref. [72]. Copyright 2019, Royal Society of Chemistry.

Fig. 20. Electrochemical performance in the OER. (a) Cyclic voltammograms of Zn;NiFeOxHy. Only the curves obtained at the 1st (purple line), 2nd (blue line), 10th (green line), 50th (yellow line), 100th (orange line), and 150th (red line) scans are shown. The inset exhibits the magnified CVs for the initial and final cycles. The arrow denotes the voltammograms for the forward scan. (b) CV of Zn, NiFeOxHy, and Ni foil. Chronoamperometry curves of various catalysts at a specific potential (c), where the initial current density is 10 mA cm?2 and the corresponding Tafel plots (d). Reproduced with permission from Ref. [204]. Copyright 2020, American Chemical Society. (e) OER polarization curves of NiFe/Ni, NiFeIr0.02/Ni, NiFeIr0.03/Ni, and NiFeIr0.05/Ni NW@NSs catalysts. (f) Required overpotentials at current densities of 10.0 and 100 mA cm?2. (g) Schematic illustration of the OER process for the NiFeIrx/Ni model. Ni* at the NiFeIrx/Ni model is the active site. (h) Gibbs free energy diagram of the OER process on Ni active site for NiFe/Ni and NiFeIrx/Ni models at U = 0 V, pH = 14, and 0 °C. Reproduced with permission from Ref. [205]. Copyright 2020, American Chemical Society.

Fig. 21. Polarization curves (a) and the corresponding Tafel plots (b) of different electrodes. (c) Current density vs time (i-t) curves of Mo-FeS NSs at 1.45 and 1.55 V vs. RHE, respectively, and LSV curves before and after 1000 cycles (inset). Free energy diagram of three simulated models at U = 0, FeS (d), Mo-FeS NPs (e) and Mo-FeS NSs (f). The blue, red, purple, green, and orange balls denote S, Fe, Mo, O, and H, respectively. Projected DOS of pristine FeS (g), Mo-FeS-NPs (h), and Mo-FeS-NSs (i) (the Fermi level is set to zero). Reproduced with permission from Ref. [213]. Copyright 2020, American Chemical Society.

Fig. 22. (a) Free energies of Co2+ → Co3+ → Co4+ evolution in various Co-Fe-Cr (oxy)hydroxides. (b) Theoretical OER volcano plot. (c) Optimized β-CoOOH (101-4) models considered for DFT calculations. Red, white, blue, brown, and teal spheres represent O, H, Co, Fe, and Cr atoms, respectively. OER catalytic performance atlases of CoaFebCrc (oxy)hydroxides measured in 1 mol L?1 KOH electrolyte based on η10 (d), Tafel slope (e), and TOF (f) at the η of 300 mV. Reproduced with permission from Ref. [219]. Copyright 2021, John Wiley and Sons.

Fig. 23. OER catalysts at different levels of development over time.

Fig. 24. DFT calculations. Schematic illustration of the proposed OER mechanism (a,b) and Gibbs free energy diagram (c,d) for Ru (a,c) and Ru-O (b,d) sites on Ru1/D-NiFe LDH. The lavender box step is the rate-determining step. Reproduced with permission from Ref. [223]. Copyright 2021, Springer Nature.

Catalyst	Cell Voltage (V)	Ref.
RuIrO_x	1.47	[228]
Ni-Fe NPs	1.47	[229]
CoMoNiS-NF	1.54	[230]
R-NiCo₂O₄	1.61	[231]
CoP/NCNHP	1.64	[232]
CoMnO@CN	1.5	[233]
RuCu NSs	1.49	[234]
Co/β-Mo₂C@N-CNTs	1.64	[235]
VOOH/NF	1.62	[236]
Co₃O₄-MTA	1.63	[237]
Cu@NiFe LDH	1.54	[238]
EG/Co_0.85Se/NiFe LDH	1.67	[239]
MoO₃/Ni-NiO	1.55	[240]
Ni/Ni(OH)₂	1.59	[241]
W₂N/WC	1.58	[242]
Cr-doped FeNi-P/NCN	1.50	[243]
δ-FeOOH NSs/NF	1.62	[244]
CoS_x@Cu₂MoS₄-MoS₂/NSG	1.6	[245]
Ni-ZIF/Ni-B	1.54	[246]
Mo-Co₉S₈@C	1.56	[247]
Co@N-CS/N-HCP	1.545	[248]
NiFe LDH@NiCoP	1.57	[249]
sNiCoP/NF	1.58	[250]
CoFe@NiFe LDH	1.59	[251]
S-CoO_x	1.63	[252]
Zn_1-_xFe_x-LDH	1.62	[253]
NiCoFeB	1.81	[254]
Ru₁/D-NiFe LDH	1.44	[223]

Fig. 25. (a) Schematic illustration of FeS/IF as a pre-catalyst for generating active electrocatalysts for both HER and OER. (b) Measurement of adhesive forces of hydrogen bubbles with Fe-H2cat. (c) The contact angle of hydrogen bubbles with Fe-H2cat in 1 mol L?1 KOH solution. (d) Schematic illustration of the enhanced HER activity in the presence of Fe-H2cat. Possible H* adsorption sites on the O-covered Fe (111) slab (e) and the O/S-covered Fe (111) slab (f). All of the top sites (indicated by the element symbol) and top-shallow bridge sites (denoted as “b”) on the surfaces are considered. (g) Calculated free-energy diagram of HER at the equilibrium potential for Pt (111), FeS (001), O-covered Fe (111), and O/S-covered Fe (111) surfaces. Reproduced with permission from Ref. [257]. Copyright 2018, Elsevier.

Fig. 26. (a) Panoramic SEM images of GA. (b) Schematic illustration of a rechargeable Zn-air battery. (c) Scheme of the structure characterization of the self-driven OWS device. (d) The open-circuit plots for zinc-air battery performance of CoNx/NGA acting as the air cathode in comparison with the noble metal RuO2 + Pt/C catalyst. (e) Charging and discharging polarization curves. (f) Energy density plots at 50 mA cm?2. (g) Long-term cycling performance at 10 mA cm?2. (h) Oxygen and hydrogen evolution rates in the integrated device. Reproduced with permission from Ref. [261]. Copyright 2019, Elsevier.

Fig. 27. Theoretical insights of amorphous-crystalline coupling and d/p-band center regulation. (a) Schematic illustration of amorphous-crystalline heterostructure for promoting d/p-band center regulation. (b) CoBOx/NiSe heterostructure model. DOS of (c) NiSe and CoBOx, and (d) CoBOx/NiSe. (e) Planar average potential in CoBOx/NiSe along Z direction. d-p orbital level of surface atoms (f) and d-p band center difference (Δ?d-p) values (g) in CoBOx and CoBOx/NiSe. Reproduced with permission from Ref. [271]. Copyright 2023, John Wiley and Sons.

Fig. 28. (a) The k3-weighted R-space FT spectra for Co K-edge EXAFS of CoMoSx, CoS and Co foil. (b) The k2-weighted R-space FT spectra for Mo K-edge EXAFS of CoMoSx, MoS2 and Mo foil. EXAFS fitting in R space for CoMoSx in (d) Co K-edge and (e) Mo K-edge. (c) Comparisons between the experimental K-edge XANES spectra of CoMoSx and the theoretical spectra calculated based on CoS6 and CoS5 moieties. Some of the main features reproduced are highlighted at points a?c. (f) Proposed model of CoMoSx, yellow: S, gray: Mo, blue: Co, red: O. Reproduced with permission from Ref. [272]. Copyright 2019, John Wiley and Sons.

Table 6 Structural parameters extracted from the Co K-edge EXAFS fitting of CoMoSx. (CN is the coordination number with an error of 20%; R is the bond length between central atoms and surrounding coordination atoms; σ2 is Debye-Waller factor (a measure of thermal and static disorder in absorber-scatterer distances); R factor is used to value the goodness of the fitting. Reproduced with permission from Ref. [272]. Copyright 2019, John Wiley and Sons.)

Sample	Shell	CN	R (Å)	σ²(×10^‒3A²)	R factor
CoS₂	Co-S	6	2.31	—	—
CoMoS_x	Co-S	4.7	2.31	6.9	1.86%
(NH₄)₂Mo₃S₁₃·2H₂O	Mo-S	7	2.43	4.6	0.04%
(NH₄)₂Mo₃S₁₃·2H₂O	Mo-Mo	2	2.75	2.9	0.04%
MoS₂	Mo-S	6	2.41	—	—
CoMoS_x	Mo-O	2.0	2.22	6.8	1.99%
	Mo-S	5.0	2.34	8.9
	Mo-Mo	1.9	2.73	9.6

Fig. 29. Electrocatalytic performances for OWS in 1 mol L?1 KOH. (a) OWS LSV curves. (b) Comparison of the cell voltages at a current density of 100 mA cm?2 for OWS. (c) Constant current electrolysis at a current density of 20 mA cm?2 using FeOOH/Cr-NiCo2O4/NF as both cathode and anode. Reproduced with permission from Ref. [275]. Copyright 2020, Springer Nature. (d) LSV curves of RuCu NSs/C, RuCu NPs/C and Ir/C||Pt/C for OWS in 1 mol L?1 KOH, 0.1 mol L?1 KOH, 0.5 mol L?1 H2SO4 and 0.05 mol L?1 H2SO4, respectively. Potentials (e) and Tafel slopes (g) of RuCu NSs/C, RuCu NPs/C and Ir/C||Pt/C in different electrolytes calculated from corresponding polarization curves. (f) Chronopotentiometry tests of RuCu NSs/C, RuCu NPs/C and Ir/C||Pt/C in 1 mol L?1 KOH at 10 mA cm?2. Reproduced with permission from Ref. [234]. Copyright 2019, John Wiley and Sons.

Fig. 30. OWS catalysts at different levels of development over time.

Fig. 31. In-situ Raman spectra of Ni9S8/Ni3S2/NF-20 (a) and Ni3S2/NF-5 (b) in 1.0 mol L?1 KOH as a function of different potentials. Reproduced with permission from Ref. [280]. Copyright 2023, John Wiley and Sons. (c) Algorithm framework of SOAP-ML model construction. Reproduced with permission from Ref. [284]. Copyright 2022, Royal Society of Chemistry.

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非晶相电催化剂在电解水领域的研究进展

Advances and insights in amorphous electrocatalyst towards water splitting

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