Investigation of nickel iron layered double hydroxide for water oxidation in different pH electrolytes

doi:10.1016/S1872-2067(22)64190-1

Chinese Journal of Catalysis ›› 2023, Vol. 44: 127-138.DOI: 10.1016/S1872-2067(22)64190-1

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Investigation of nickel iron layered double hydroxide for water oxidation in different pH electrolytes

Qixian Xie^a, Dan Ren^b, Lichen Bai^c, Rile Ge^d, Wenhui Zhou^d, Lu Bai^e, Wei Xie^e, Junhu Wang^d^,^*(), Michael Grätzel^b, Jingshan Luo^a^,^*()

^aInstitute of Photoelectronic Thin Film Devices and Technology, Key Laboratory of Photoelectronic Thin Film Devices and Technology of Tianjin, Ministry of Education Engineering Research Center of Thin Film Photoelectronic Technology, Renewable Energy Conversion and Storage Center, Nankai University, Tianjin 300350, China
^bLaboratory of Photonics and Interfaces, Institute of Chemical Sciences and Engineering, École Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, Switzerland
^cLaboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), 1015 Lausanne, Switzerland
^dCenter for Advanced Mössbauer Spectroscopy, Mössbauer Effect Data Center, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China
^eKey Laboratory of Advanced Energy Materials Chemistry (Ministry of Education), College of Chemistry, Nankai University, Tianjin 300071, China

Received:2022-06-13 Accepted:2022-08-04 Online:2023-01-18 Published:2022-12-08
Contact: Junhu Wang, Jingshan Luo
Supported by:
National Key Research and Development Program of China(2019YFE0123400);National Key Research and Development Program of China(2018YFB1502003);Excellent Young Scholar Fund from the National Science Foundation of China(22122903);Tianjin Distinguished Young Scholar Fund(20JCJQJC00260);“111” Project(B16027);scholarship from the China Scholarship Council;Gebert Rüf Stiftung under Microbials scheme ‘Solar-Bio Fuels’(GRS-080/19);Early Postdoc Research Fellowship from the Swiss National Science Foundation(P2ELP2_199800);National Science Foundation of China(21961142006);International Partnership Program of Chinese Academy of Sciences(121421KYSB20170020)

Abstract

Abstract:

Nickel iron layered double hydroxide (NiFe LDH) is one of the best oxygen evolution reaction (OER) catalysts in alkaline electrolytes. However, it performs poorly in neutral electrolytes, and the detailed mechanism is still unclear. Herein, we introduce electrochemical measurements, operando surface enhanced Raman spectroscopy and operando ⁵⁷Fe Mössbauer spectroscopy to elucidate the mechanism of NiFe LDH for OER process in different pH electrolytes. Our results show that even though there exist Ni³⁺ and Fe⁴⁺ species, the NiFe LDH based electrocatalysts still show worse OER performance in neutral electrolytes than in alkaline conditions. Combining the electrochemical measurements with spectroscopic investigations, we demonstrated that the rate-determining step (RDS) of OER on NiFe LDH based electrocatalysts is from *O to *OOH in alkaline medium while *OH formation is the RDS in neutral conditions. Our work provides new insights into elucidating the OER mechanism in different pH electrolytes.

Key words: Nickel Iron layered double hydroxide, Oxygen evolution reaction, Operando surface enhanced Raman spectroscopy, Operando ⁵⁷Fe M?ssbauer spectroscopy

Qixian Xie, Dan Ren, Lichen Bai, Rile Ge, Wenhui Zhou, Lu Bai, Wei Xie, Junhu Wang, Michael Grätzel, Jingshan Luo. Investigation of nickel iron layered double hydroxide for water oxidation in different pH electrolytes[J]. Chinese Journal of Catalysis, 2023, 44: 127-138.

Figures/Tables 5

Fig. 1. Electrochemical OER performance and operado spectroscopic measurements of the pristine NiFe LDH. Cyclic voltammetry curves (a) and Tafel slopes (b) of NiFe LDH tested in the different electrolytes (0.1 mol L?1 KOH, pH = 13; 0.1 mol L?1 BBS, pH = 9.2; 0.1 mol L?1 PBS, pH = 7, the scan rate is 10 mV s?1). The operando SERS of NiFe LDH acquired in the potential range from 1.0?1.7 V vs. RHE in 0.1 mol L?1 KOH (c), 0.1 mol L?1 BBS (d), 0.1 mol L?1 PBS (e) (potential step size is 100 mV); the operando 57Fe Mo?ssbauer spectra of NiFe LDH collected at different pH electrolytes: (f) 1.57 V vs. RHE, 0.1 mol L?1 KOH, pH = 13. (g) 2.17 V vs. RHE, 0.1 mol L?1 BBS, pH 9.2; (h) 2.17 V vs. RHE, 0.1 mol L?1 PBS, pH = 7.

Fig. 2. Spectroscopic characterizations of NiFe CVA500 sample. XPS spectra results of Ni 2p (a), Fe 2p (b), ex-situ Raman spectra (c), and ex-situ 57Fe Mo?ssbauer spectrum (d) of NiFe CVA500.

Fig. 3. Electrochemical OER performance and in-situ/operando spectroscopy measurements of the NiFe CVA500. (a) CV curves of NiFe CVA500 in the different pH electrolytes. (b) Tafel slopes of the NiFe CVA500 samples in the different pH electrolytes; operando Raman spectra of pristine NiFe CVA500 acquired in the potential range 1.0?1.7 V vs. RHE in 0.1 mol L?1 KOH (c), 0.1 mol L?1 BBS (d), and 0.1 mol L?1 PBS (e). The measurements were performed potentiostatically. Operando Mo?ssbauer spectra of NiFe CVA500 collected at high potential in different pH electrolytes: (f) 0.1 mol L?1 PBS, pH = 7.0 (2.17V vs. RHE). (g) 0.1 mol L?1 BBS, pH = 9.2 (2.17 V vs. RHE). (h) 0.1 mol L?1 KOH, pH = 13 (1.77 V vs. RHE).

Fig. 4. Electrochemical response to methanol of pristine NiFe LDH in different electrolytes (0.5 mol L?1 KOH/BBS/PBS with and without 0.5 mol L?1 methanol). CV curves for NiFe LDH in different electrolytes: (a) 0.5 mol L?1 KOH; (c) 0.5 mol L?1 BBS; (e) 0.5 mol L?1 PBS. Schematic energy profile for the NiFe based electrocatalysts for OER process in different pH conditions: (b) the alkaline condition; (d) the near neutral condition; (f) the neutral condition. The inset Figure shows enlarged CV curves at the low current region, and the scan rate is 50 mV s?1 (the solid line is with 0.5 mol L?1 methanol, and the dashed line is without methanol).

Fig. 5. Proposed mechanism of NiFe LDH electrocatalyst for OER in different pH electrolytes.

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Investigation of nickel iron layered double hydroxide for water oxidation in different pH electrolytes

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