Research progress of anionic vacancies in electrocatalysts for oxygen evolution reaction

doi:10.1016/S1872-2067(24)60157-9

Chinese Journal of Catalysis ›› 2024, Vol. 66: 110-138.DOI: 10.1016/S1872-2067(24)60157-9

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Research progress of anionic vacancies in electrocatalysts for oxygen evolution reaction

Ya’nan Xia^a, Jingqi Chi^a^,^*(), Junheng Tang^a, Xiaobin Liu^a^,^c, Zhenyu Xiao^a^,^b, Jianping Lai^a^,^b, Lei Wang^a^,^b^,^*()

^aKey Laboratory of Eco-chemical Engineering, International Science and Technology Cooperation Base of Eco-chemical Engineering and Green Manufacturing, College of Chemical Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^bCollege of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China
^cCollege of Environment and Safety Engineering, Qingdao University of Science and Technology, Qingdao 266042, Shandong, China

Received:2024-07-15 Accepted:2024-09-09 Online:2024-11-18 Published:2024-11-10
Contact: *E-mail: chijingqi@qust.edu.cn (J. Chi),inorchemwl@qust.edu.cn (L. Wang).
About author:Jingqi Chi received her B. S. degree and Ph.D. degree from the State Key Laboratory of Heavy Oil Processing, China University of Petroleum (East China). She is currently an associate professor at Qing dao University of Science and Technology. Her research interests focus on the design and synthesis of transition metal-based nanostructures and porous MOFs materials for electrochemical applications.
Lei Wang was awarded a Ph.D. in chemistry from Jilin University in 2006 under the supervision of Prof. Shouhua Feng. He worked as a Postdoctoral Scholar in Shandong University, the State Key Laboratory of Crystal Materials from 2008 to 2010. He is currently a professor at Qingdao University of Science and Technology. His research interests mainly focus on the design and synthesis of functional organic-inorganic hybrids and porous MOFs materials, as well as their applications in photocatalysis, electrocatalysis, lithium-ion battery, etc.
Supported by:
National Natural Science Foundation of China(52072197);National Natural Science Foundation of China(52174283);National Natural Science Foundation of China(22301156);Natural Science Foundation of Shandong Province(ZR2021QE165);Youth Innovation and Technology Foundation of Shandong Higher Education Institutions, China(2019KJC004);Major Scientific and Technological Innovation Project(2019JZZY020405);Major Basic Research Program of Natural Science Foundation of Shandong Province(ZR2020ZD09);Shandong Province "Double-Hundred Talent Plan"(WST2020003);Taishan Scholar Young Talent Program(tsqn201909114);University Youth Innovation Team of Shandong Province(202201010318)

Abstract

Abstract:

Renewable energy conversion as well as water electrolysis technologies are constrained by the fact that kinetics are always slow in the electrocatalytic oxygen evolution reaction (OER). There are numerous means and strategies for the enhancement of OER activity. In this paper, we systematically review the important role of anionic vacancies in enhancing the OER activity of catalysts: increasing catalyst conductivity, improving electrical conductivity, and enhancing intermediate adsorption. In order to better detect the presence of vacancies in the samples, the principle of vacancy detection is reviewed in detail in terms of both spectroscopic and microscopic characterization, and the methods of vacancy formation as well as the factors influencing the concentration of vacancies are summarized in detail. In addition, the challenges and new directions for the study of anionic vacancies are provided.

Key words: Anionic vacancy, Oxygen evolution reaction, Characterization, Introduction strategy, Detection method

Ya’nan Xia, Jingqi Chi, Junheng Tang, Xiaobin Liu, Zhenyu Xiao, Jianping Lai, Lei Wang. Research progress of anionic vacancies in electrocatalysts for oxygen evolution reaction[J]. Chinese Journal of Catalysis, 2024, 66: 110-138.

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Figures/Tables 23

Fig. 1. OER mechanism of AEM (a), LOM (b-e), and OPM (f) in alkaline condition.

Fig. 2. Summary of methods for introducing anionic vacancies using different strategies [41??-44]. Reprinted with permission from Ref. [41]. Copyright 2023, Elsevier; Reprinted with permission from Ref. [43]. Copyright 2022, Elsevier; Reprinted with permission from Ref. [44]. Copyright 2018, American Chemical Society.

Fig. 3. (a) Mechanism diagram of phosphorus vacancy formation process. HRTEM images of Fe-Ni2P (b) and intensity maps of P vacancies in the corresponding regions (c) [48]. Reprinted with permission from Ref. [48]. Copyright 2023, John Wiley and Sons. In situ Raman images (d) and the EPR results (e) of the ZnOx. (f) H2O adsorption energy simulations of ZnOx with and without vacancies [49]. Reprinted with permission from Ref. [49]. Copyright 2024, Elsevier. (g) Comparison of EIS images of different samples. (h) Simulation of intermediate adsorption during OER of FeCo2Ni-Ov. (i) Reaction potentials and d-band center for different samples [52]. Reprinted with permission from Ref. [52]. Copyright 2021, Elsevier.

Fig. 4. Schematic synthesis (a) and HRTEM images (b) of Mo(SSe)2-x/G. (c) Gibbs free energy diagrams of H adsorption for different samples [55]. Reprinted with permission from Ref. [55]. Copyright 2023, Elsevier. (d) Schematic preparation of MoSe2-x/ZnSe@C with anionic vacancies and heterojunction. (e) Schematic diagram of the process of preparing vacancies by calcination. (f,g) HRTEM image of MoSe2-x/ZnSe@C, where red circles represent Se vacancies [56]. Reprinted with permission from Ref. [56]. Copyright 2023, John Wiley and Sons.

Fig. 5. (a) Simulation of electrochemical measurement process. (b) XRD plots of different voltage treated NiO. (c) CV polarization curves for different samples [60]. Reprinted with permission from Ref. [60]. Copyright 2020, Elsevier. Mechanistic diagram of the synthesis of HEOs by conventional methods (d) and low-temperature plasma methods (e). (f) Isothermal curves of N2 adsorption and desorption for different samples [61]. Reprinted with permission from Ref. [61]. Copyright 2021, John Wiley and Sons. Schematic distribution of BVO charge carriers (g) without and (h) with oxygen vacancies [62]. Reprinted with permission from Ref. [62]. Copyright 2024, Elsevier.

Fig. 6. (a) Diagram of the mechanism of oxygen vacancy formation in CeO2 [67]. Reprinted with permission from Ref. [67]. Copyright 2024, Elsevier. (b) Mechanistic diagram of oxygen vacancy formation in Co3O4 [70]. Reprinted with permission from Ref. [70]. Copyright 2016, John Wiley and Sons. (c) Single-vacancy OER mechanism diagram [71]. Reprinted with permission from Ref. [71]. Copyright 2024, John Wiley and Sons. (d,e) Multi-vacancies aggregation model diagram [72]. Reprinted with permission from Ref. [72]. Copyright 2023, AIP Publishing. (f) Synergistic model of anionic vacancies and cationic vacancies [73] Reprinted with permission from Ref. [73]. Copyright 2020, John Wiley and Sons.

Fig. 7. (a) EPR spectra of SrTiO3 at different temperatures [74]. Reprinted with permission from Ref. [74]. Copyright 2014, American Chemical Society. (b) EPR spectra of SrTiO3 at different temperatures [75]. Reprinted with permission from Ref. [75]. Copyright 2019, Elsevier. (c) STM image of the alignment status of a single S vacancy in MoS2 [76]. Reprinted with permission from Ref. [76]. Copyright 2020, American Chemical Society. (d) Comparison of the density of states of Mo atoms with different distributions of S vacancies in MoS2. STM image of the alignment status of a single S vacancy in MoS2 (e) and the image of the arrangement status of linear S vacancies in MoS2 (f) [77]. Reprinted with permission from Ref. [77]. Copyright 2017, John Wiley and Sons. (g) ESR plots for different concentrations of phosphorus doping. (h) LSV polarization curves for different PV concentrations [79]. Reprinted with permission from Ref. [79]. Copyright 2022, John Wiley and Sons. (i) CoP charge density difference cross section with and without vacancies [82]. Reprinted with permission from Ref. [82]. Copyright 2023, John Wiley and Sons.

Fig. 9. HRTEM image of F-FeCoPV@IF (a) and magnified image of the corresponding region (b) [89]. Reprinted with permission from Ref. [89]. Copyright 2023, Elsevier. (c) HAADF-STEM image in PtTe2 NSs (upper inset represents Te vacancies at certain line intensities, lower right inset represents Pt and Te atomic columns, lower left inset represents contrast visualization of vacancies in PtTe2 NSs). (d) STM diagram of Cu2O/Au (111). (e) AFM image of the presence of S vacancies in MoS2 sample, pink circle and blue circle representing the impassable current density [94]. Reprinted with permission from Ref. [94]. Copyright 2022, American Chemical Society. (f) ABF-STEM images of P-Pt/STO samples (Red dots indicate oxygen vacancies). (g) The enlarged area of the red dashed box in Figs. 9(f) and (h) the line profile along the dashed arrow in Fig. 9(g) [95]. Reprinted with permission from Ref. [95]. Copyright 2022, Elsevier.

Fig. 10. XPS spectra of N 1s (a) and O 1s (b) of Vo-Co(OH)2/CoN and comparison sample [100]. Reprinted with permission from Ref. [100]. Copyright 2023, Springer Nature. XANES spectral profile of the K-edge of Co (c) and Corresponding K3-weighted EXAFS fitting curves (d) [103]. Reprinted with permission from Ref. [103]. Copyright 2023, Elsevier. (e) EPR curves of O-MoS2 and comparison sample [106]. Reprinted with permission from Ref. [106]. Copyright 2020, Elsevier. (f) Raman spectra of L-Co3O4 and comparison sample [108]. Reprinted with permission from Ref. [108]. Copyright 2021, Elsevier. (g) In situ UV Raman spectra of Ce-LDH materials during calcination at different temperatures. (h) UV Raman spectra of different samples [109]. Reprinted with permission from Ref. [109]. Copyright 2022, Elsevier. (i) Positron annihilation spectra of N-(Zn,en)VO and comparison sample [112]. Reprinted with permission from Ref. [112]. Copyright 2022, John Wiley and Sons.

Sample	τ₁ (ps)	τ₂ (ps)	τ₃ (ps)	I₁ (%)	I₂ (%)	I₃ (%)
N-(Zn,en)VO	199	374	2.332	25.0	73.1	1.9
(Zn,en)VO	201	360	2.189	32.2	65.4	2.4

Fig. 12. (a) TEM images of RuO2@Co3O4 samples. (b) Differential charge density images of RuO2@Co3O4 samples. (c) Density of d-orbital states for different samples [115]. Reprinted with permission from Ref. [115]. Copyright 2024, Elsevier. (d) LSV polarization curves for OER of different samples. (e) Gibbs free energy diagrams of the OER process for different sample models. (f) Projected density of d-orbital states for different samples [116]. Reprinted with permission from Ref. [116]. Copyright 2024, Elsevier. (g) Plots of the heterogeneous interface model and vacancy distribution for Co9Se8/FeNiSe. (h) LSV curve of Co9Se8/FeNiSe [117]. Reprinted with permission from Ref. [117]. Copyright 2024, Elsevier.

Fig. 13. (a) LSV polarization curves of NiFe LDHs samples with oxygen vacancies. (b) Conductivity versus potential curves for different samples [118]. Reprinted with permission from Ref. [118]. Copyright 2023, American Chemical Society. (c) Nyquist plots for different samples. (d) Ea values for different samples [119]. Reprinted with permission from Ref. [119]. Copyright 2022, John Wiley and Sons. (e) LSV polarization curves of different samples. (f) Differential charge density images of NiFe2O4-Vo-P samples. (g) OER Gibbs free energy of different samples at different potentials [120]. Reprinted with permission from Ref. [120]. Copyright 2023, Elsevier.

Fig. 14. (a) Tafel slopes for different samples. (b) Geometrical configuration of different samples. (c) Free energy diagrams of the HER process for different samples [121]. Reprinted with permission from Ref. [121]. Copyright 2021, Elsevier. (d) OER LSV polarization curves for different samples. (e) XPS plots of O 1s from different samples [122]. Reprinted with permission from Ref. [122]. Copyright 2022, American Chemical Society. (f) DOS plots of different samples [123]. Reprinted with permission from Ref. [123]. Copyright 2022, John Wiley and Sons. (g) Relationship between Sr and O vacancies in the OER process. (h) Difference in adsorption energy of OH* intermediates between samples [124]. Reprinted with permission from Ref. [124]. Copyright 2023, Elsevier.

Fig. 15. Three mechanisms of OER two-dimensional activity diagram AEM (a), LOM-OVSM (b) and LOM-SMSM (c). (d) Comparison of theoretical and actual overpotential [125]. (e) OER mechanism diagram for Ni0.3Fe0.7-LDH@NF (LOM). (f) Schematic diagram of OER relative performance of different catalysts. (g) OER free energy barrier diagram of different surfaces of NiFe-LDH by LOM [126]. Reprinted with permission from Ref. [126]. Copyright 2023, Elsevier.

Fig. 16. (a) Water molecular adsorption and charge density of NiCo2O4 sample with oxygen vacancy. (b) LSV polarization curve of different NiCo2O4 nanosheets. (c) XRD of NiCo2O4 nanosheets with oxygen vacancies and bulk NiCo2O4 [138]. (d) O 1s XPS spectra of pristine and reduced Co3O4 nanosheets (e) Polarization curves of as-prepared O-vacancy-rich Co3O4 (O-Co3O4) with other catalysts. (f) The calculated OER free energy of the Co3O4 structure with/without oxygen vacancy [145]. Reprinted with permission from Ref. [145]. Copyright 2017, John Wiley and Sons. (g) Comparison of OER LSV curves of Co0.025-NiFe-LDH/NF and NiFe-LDH/NF. (h) O 1s XPS spectra of Co0.025-NiFe-LDH/NF and NiFe-LDH. (i) Partial density of states of Co0.025-NiFe-LDH (left) and NiFe-LDH (right) [135]. Reprinted with permission from Ref. [135]. Copyright 2021, Elsevier.

Fig. 17. (a) Fourier transform filtered atomic resolution images of different diffraction points. (b) Represents the different atomic intensity distribution images in (a). (c) Polarization curves for different samples. (d) Raman spectra of different samples. (e) Gibbs free energy for the Co9S8-ZnS model at U = 0 [146]. Reprinted with permission from Ref. [146]. Copyright 2022, American Chemical Society. (f) EPR images of different samples. (g) Polarization curves for different samples. (h) Adsorption model of Vs-(Fe, Ni)3S4. (i) Gibbs free energy of different samples during OER at Fe and Ni sites [147]. Reprinted with permission from Ref. [147]. Copyright 2024, Elsevier.

Fig. 18. (a) HRTEM images of CoXPV@NC samples. (b) Mechanism diagram of P vacancy formation in CoXPV@NC samples. (c) In-situ Raman spectra of CoXPV@NC samples [148]. Reprinted with permission from Ref. [148]. Copyright 2020, Elsevier. (d) EPR images of samples at different reduction times. (e) Comparison of LSV curves of different samples. (f) XPS curve of O 1s of samples after OER [152]. Reprinted with permission from Ref. [152]. Copyright 2021, Elsevier. (g) OER polarization curves for LSV. (h) Application resistance diagrams for different samples. (i) Comparative OER kinetic studies of different samples [155]. Reprinted with permission from Ref. [155]. Copyright 2023, John Wiley and Sons.

Fig. 19. (a) Comparison of polarization curves standardized by ECSA. (b) Comparison of total DOS for different samples. (c) OER Gibbs free energy of FeOOH and Se2(2C)-FeOOH [82]. Reprinted with permission from Ref. [82]. Copyright 2023, John Wiley and Sons. (d) R-space Ag K-edge EXAFS spectra of AgSA-NiSe2. (e) In situ Raman spectroscopy of AgSA-NiSe2 samples. (f) Free energy diagrams of NiSe2 and AgSA-NiSe2 OER processes [166]. Reprinted with permission from Ref. [166]. Copyright 2024, Elsevier. (g) Local HRTEM of Mo-Co9Se8@NiSe/NF-60 sample. (h) Comparison of EPR images of different samples. (i) Comparison of LSV polarization curves of different samples. (j) Comparison of d-band centers for different samples [168]. Reprinted with permission from Ref. [168]. Copyright 2023, Royal Society of Chemistry.

Fig. 20. (a) Comparison of EPR of different samples. (b) HRTEM images of o-CoTe2?P@HPC/CNTs samples. (c) Comparison of LSV of OER for different samples [170]. Reprinted with permission from Ref. [170]. Copyright 2020, American Chemical Society. (d) Top and side views of the G/BNNs sample and the corresponding charge density distribution. (e) Energy band structure of G/BNNs. (f) Comparison of LSV of OER for different samples [171]. Reprinted with permission from Ref. [171]. Copyright 2023, John Wiley and Sons.

Table 2 Summary of OER catalysts optimized for different anionic vacancies.

Catalysts	Vacancy	Performance	Ref.
Ru/d-NiFe LDH	O_V	220 mV/10 mA cm^-2	[172]
Co₃O₄	O_V	320 mV/10 mA cm^-2	[173]
300-h/Co/CC	O_V	280 mV/10 mA cm^-2	[174]
Ni_0.3Fe_0.7-LDH@NF	O_V	184 mV/10 mA cm^-2	[126]
S-CeO₂	O_V	190 mV/10 mA cm^-2	[175]
N-ZnCo₂O_4-_δ-350	O_V	406 mV/10 mA cm^-2	[176]
v-NiFe LDH	O_V	210 mV/10 mA cm^-2	[177]
NiCoPi	O_V	254 mV/10 mA cm^-2	[178]
Co(OH)₂/WO_x	O_V	208 mV/10 mA cm^-2	[179]
Ni-S-5	O_V	142 mV/10 mA cm^-2	[180]
CoMoO₄-Ov	O_V	296 mV/10 mA cm^-2	[181]
HEOs-Ov	O_V	284 mV/10 mA cm^-2	[182]
Sr₂Co₂O₅	O_V	370 mV/10 mA cm^-2	[183]
2D d-MHOFs	O_V	207 mV/10 mA cm^-2	[184]
V_O-Cubic-Co₃O₄	O_V	375 mV/10 mA cm^-2	[185]
β-FeOOH	O_V	232 mV/10 mA cm^-2	[186]
Fe₁Co₁O_x	O_V	225 mV/10 mA cm^-2	[187]
Co₃O₄	O_V	367 mV/10 mA cm^-2	[188]
MNC	O_V	250 mV/10 mA cm^-2	[189]
Fe₂O₃@CeO₂-O_V	O_V	172 mV/10 mA cm^-2	[190]
Fe-Ni₂P(P_V)	P_V	290 mV/10 mA cm^-2	[191]
V-doped NiCoP	P_V	246 mV/10 mA cm^-2	[192]
D-Ni₅P₄\|Fe	P_V	217 mV/10 mA cm^-2	[193]
CoP-B1	P_V	297 mV/10 mA cm^-2	[152]
Fe-Ni₂P	P_V	190 mV/10 mA cm^-2	[194]
Ni₂P/Cu₃P	P_V	370 mV/10 mA cm^-2	[148]
V_P-Co-MoP@MXene	P_V	265 mV/10 mA cm^-2	[195]
Fe-Ni₂P-V_P	P_V	289 mV/10 mA cm^-2	[196]
NiFe(OH)_x/NiP_x/NF	P_V	220 mV/10 mA cm^-2	[197]
Co_0.68Fe_0.32P-60	P_V	259 mV/10 mA cm^-2	[198]
P-NiS₂-500	S_V	340 mV/10 mA cm^-2	[199]
P-CoS	S_V	280 mV/10 mA cm^-2	[200]
S_V-Ni₃S_2-_xP_x_-4	S_V	216 mV/10 mA cm^-2	[201]
Bi₂S₃	S_V	374 mV/10 mA cm^-2	[202]
H-V_S-Co₃S₄	S_V	270 mV/10 mA cm^-2	[203]
Ru-FeNi₂S₄	S_V	253 mV/10 mA cm^-2	[204]
V_S-Ni₃S₂/MoS₂	S_V	180 mV/10 mA cm^-2	[205]
Co₉S₈-ZnS/NTC	S_V	290 mV/10 mA cm^-2	[146]
d-PtSe₂	Se_V	310 mV/10 mA cm^-2	[206]
Co_0.85Se_1-_x@C	Se_V	231 mV/10 mA cm^-2	[207]
A-NiSe₂\|P	Se_V	272 mV/10 mA cm^-2	[208]
CoSe₂	Se_V	284 mV/10 mA cm^-2	[209]
o-CoTe2\|P@HPC/CNTs	Te_V	241 mV/10 mA cm^-2	[170]

Fig. 21. Prospective images of anionic vacancies on OER catalysts [211?-213]. Reprinted with permission from Ref. [212]. Copyright 2023, John Wiley and Sons. Reprinted with permission from Ref. [213]. Copyright 2024, American Chemical Society.

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Research progress of anionic vacancies in electrocatalysts for oxygen evolution reaction

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