Defects engineering of layered double hydroxide-based electrocatalyst for water splitting

doi:10.1016/S1872-2067(23)64557-7

Abstract

Abstract:

Layered double hydroxide (LDH)-based materials are considered as promising electrocatalysts for water splitting due to the advantages of unique layered structure, flexible tunability, high specific surface area and distinct electron distribution. However, the low conductivity and limited active sites hinder the industrial applications of LDH-based electrocatalysts. On the other hand, defect engineering is an effective strategy to tune the local surface microstructure and electronic structure, which can efficiently address the drawbacks of LDH. Unfortunately, a comprehensive overview of defect engineering in LDH-based materials is still rarely reported. Herein, this paper reviews the research progress of LDH with various types of defects and its regulation strategies in recent years. Furthermore, the relationship between the catalytic activity, stability, morphology, structure, composition, and defect types of LDH are systematically discussed, aiming to deepen the understanding of the mechanism of defect-mediated LDH. Finally, the main challenges and opportunities for defect design in LDH are emphasized to shed light on the future applications.

Key words: Water splitting, Electrocatalysis, Layered double hydroxide, Defect engineering, Oxygen evolution reaction, Hydrogen evolution reaction

Junhao Yang, Lulu An, Shuang Wang, Chenhao Zhang, Guanyu Luo, Yingquan Chen, Huiying Yang, Deli Wang. Defects engineering of layered double hydroxide-based electrocatalyst for water splitting[J]. Chinese Journal of Catalysis, 2023, 55: 116-136.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(23)64557-7

https://www.cjcatal.com/EN/Y2023/V55/I12/116

Figures/Tables 12

Fig. 1. (a) HER and OER of electrocatalytic water splitting. (b) Volmer-Tafel reaction route (left) and Volmer-Heyrovsky reaction route (right) for HER (inner circle is for alkaline condition and the outer circle is for acidic condition). Reproduced with permission [9]. Copyright 2020, American Chemical Society. (c) Volcano plot of the exchange current density as a function of the DFT-calculated Gibbs free energy of adsorbed atomic hydrogen. Reproduced with permission [26]. Copyright 2007, The American Association for the Advancement of Science. AEM reaction route (d) and LOM pathway (e) for OER (inner circle is for alkaline condition and the outer circle is for acidic condition). Reproduced with permission [27?-29]. Copyright 2021, Wiley-VCH GmbH. Copyright 2020, The Royal Society of Chemistry. Copyright 2019, American Chemical Society. (f) Volcano plot of overpotential for OER as a function of oxygenated reaction intermediates. Reproduced with permission [30]. Copyright 2011, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Fig. 2. (a) Structure model of the host layer of LDH (The red ball represents oxygen, the green ball represents divalent metal ions, and the blue ball represents trivalent metal ions). (b) The mechanism of metal dissolution in NiFe LDH during CV (left) and CA (right) process. Summary of the activity loss and metal dissolution by CV processes (c) and CA processes (d), respectively. Elemental mapping images for NiFe LDH before (e) and after (f) stability test. (b-f) Reproduced with permission [60]. Copyright 2021, Wiley-VCH GmbH.

Fig. 3. The common types of defects in LDH. The process of anion vacancies formation (a) and cation vacancies (b). (a) Reproduced with permission [79]. Copyright 2022, John Wiley & Sons Ltd. (b) Reproduced with permission [25]. Copyright 2023, Yingying Hao et al. (c) Schematic illustration of the formation process of cavities. SEM (d) and TEM (e) images after introduction of cavities. Reproduced with permission [22]. Copyright 2018, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (f) HRTEM for atomic vacancies. Reproduced with permission [70]. Copyright 2019, The Royal Society of Chemistry. (g) HRTEM image after introduction of lattice distortion. Reproduced with permission [23]. Copyright 2023, Elsevier B. V.

Fig. 4. Plasma etching method. (a) H2O DBD plasma. Reproduced with permission [67]. Copyright 2017, WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim. (b) Nitrogen glow discharge plasma etching. Reproduced with permission [86]. Copyright 2021, Elsevier Ltd.

Fig. 5. Alkaline etching method combined with Ru single atoms (a) and electrodeposition method (b) and corresponding schematic diagram of water splitting (c). (a) Reproduced with permission [24]. Copyright 2021, Wiley-VCH GmbH. (b,c) Reproduced with permission [59]. Copyright 2021, Panlong Zhai et al. Alkaline etching method for creating defects (d) and corresponding enhancement mechanisms of the defects creation processes (e). Reproduced with permission [44]. Copyright 2022, American Chemical Society. (f) Laser shock method. Reproduced with permission [93]. Copyright 2022, Wiley-VCH GmbH.

Fig. 6. (a) Complexation-extraction method using methyl-isorhodanate and (b) tributylphosphine. (a) Reproduced with permission [74]. Copyright 2020, Elsevier Ltd. (b) Reproduced with permission [25]. Copyright 2023, Yingying Hao et al. (c) Gas-phase acid etching method. Reproduced with permission [77]. Copyright 2022, American Chemical Society. (d) Non-equilibrium precipitation [85]. Reproduced with permission. Copyright 2021, Wiley-VCH GmbH.

Fig. 7. (a) Charge density distribution for the valence band maximum of NiO-VNi. (b) Schematic view of the Ni and O atoms relaxation around VNi in NiTi mixed metal oxide nanosheets (O atoms move outward, and Ni atoms move inward to VNi.). Reproduced with permission [103]. Copyright 2016, American Chemical Society. (c) ECSA-normalized CV curves. Reproduced with permission [21]. Copyright 2021, Wiley-VCH GmbH. (d) Cation vacancies result in longer Ni-Fe distances and shorter M-O bonds. (e) k3-weighted Fourier-transformed EXAFS R-space patterns (indicating Fe?Fe/Ni is much longer in bond length compared with those in the pristine NiFe-LDH or Fe2O3). Reproduced with permission [60]. Copyright 2021, Wiley-VCH GmbH.

Fig. 8. (a) Scheme of the enhancement mechanisms of the defects creation processes. Reproduced with permission [49]. Copyright 2020, Ning Zhang et al. (b) Schematic electronic configuration of the Ni2+ and Ni3+ cations in NiO6. Reproduced with permission [103]. Copyright 2016, American Chemical Society. (c) Chronoamperometry data for NiFe LDH with different types of defects. DFT calculated dissolution energy of metal atoms in NiFe LDH with M2+ vacancies (d) and M3+ vacancies (e). Reproduced with permission [60]. Copyright 2021, Wiley-VCH GmbH.

Fig. 9. (a) Multiple cation vacancies are created through a non-equilibrium precipitation method. (b) Adsorption configurations of OER steps over NiFe-LDH with no defect, mono-cationic defect, and di-cationic defect, respectively. Reproduced with permission [85]. Copyright 2023, Wiley-VCH GmbH. (c) The evolution of cation defects from VM to VMOH and then to VMOH-H along with increasing applied voltage. (d) Adsorption energies of various intermediates on the pristine and the various defective NiFe LDH models. Reproduced with permission [21]. Copyright 2021, Wiley-VCH GmbH.

Fig. 10. (a) Partial density of state of pristine NiFe LDH and NiFe LDH with Fe and O vacancies. (b) Atomic structure illustration of NiFe LDH with Fe and O vacancies. (c) Electron density distribution of NiFe LDH without vacancies (top) and NiFe LDH with vacancies. Reproduced with permission [58]. Copyright 2021, Elsevier B. V. (d) Atomic structure illustration of NiFe LDH with doped Ce and lattice distortion. (e) Gibbs free energy diagram for the four steps of OER on NiFe LDH with doped Ce and lattice distortion. Reproduced with permission [23]. Copyright 2023, Elsevier B. V. (f) Pt single atoms can be anchored to the Fe vacancies. Reproduced with permission [101]. Copyright 2021, Wiley-VCH GmbH.

Table 1 Defect-engineered LDH-based electrocatalysts in alkaline electrolytes for the OER.

Catalyst	Defect type ^a	Overpotential (mV) (@10 mA cm^-2)	Stability ^b(h) (@mA cm^-2)	Ref.
PM-LDH	V_M, V_O, cavity	230	100 @10	[78]
Ru₁/D-NiFeLDH	V_M³⁺	189	100 @100	[59]
NiFe-LDH-NSs/NF-200	V_M³⁺, V_O, cavity	170	40 @10	[109]
CoFe LDHs-Ar	V_M, V_O	266	N/A	[76]
H₂O-Plasma Exfoliated LDHs	V_M, V_O, cavity	232	11.1 @20	[67]
cd-NiFe LDH-NaBH₄	V_M²⁺, V_O	205	36 @10	[44]
Pt/Ni_xFe LDHs	V_M²⁺	186	70 @10‒200	[119]
MNF-LDH-laser	V_M²⁺, cavity	220	10 @10	[93]
A-NiFe/NF	V_M, cavity	N/A	75 @100	[77]
v-L-LDH	V_M, V_O	150	60 @20	[74]
NiCo LDH-V_Ni/CC	V_M²⁺	227	100 @10	[75]
CoFe_{1/3 V}-LDH	V_M	241	18 @10	[120]
d-NiFe LDH	V_M, cavity	230	36 @10	[21]
EE-NiFe-LDH array	V_M²⁺, V_O	205	24 @100	[58]
SAV-NiCu_x-LDH	V_M	290	50 @10	[70]
NiFe-LDH/ATO-air plasma	V_O	312	N/A	[121]
Pt-Ni₂Fe₁-24	V_M²⁺	243	N/A	[101]
d-NiFe-LDH-150	V_M²⁺	243	12 @15	[25]
E-CoFe LDHs	V_M²⁺	300	10 @10	[96]
Ni_vacFe_vac-LDH	V_M²⁺, V_M³⁺	230	100 @110	[60]
NiFe LDHs-V_Ni	V_M	229	N/A	[108]
d-NiFe-LDH	V_M	170	900 @10	[85]
v-NiFe LDH	V_O, cavity	195	26 @10	[99]
v-Ce/CoFe LDH	V_O, cavity	73	N/A	[57]
NiFe-LDH-Ti₄O₇	V_M, V_O	270	30 @45	[122]
Ni_0.3Fe_0.7 LDH@NF	V_M, V_O	184	84 @10	[110]
P-V-NiFe LDH NSA	V_M, V_O	19	100 @10	[123]
5% Ce-doped LDH	V_O	340	24 @10	[124]
v-NiFe LDH	V_M, V_O	370	100 @50	[97]
Defective NiFe LDH	V_O, cavity	250	11.1 @20	[22]
NiFeCe LDH@CP	lattice distortion	232	70 @20	[23]
Ru₁/D-NiFeLDH (HER)^c	V_M³⁺	18	100 @100	[59]
Pt/Ni_xFe LDHs (HER)	V_M²⁺	5	N/A	[119]
NiCo LDH-V_Ni/CC (HER)	V_M²⁺	195	100 @10	[75]
CoFe_{1/3 V}-LDH (HER)	V_M	72	24 @10	[120]
v-NiFe LDH (HER)	V_M and V_O	87	N/A	[97]

Fig. 11. Outlook for defect engineering in LDH.

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