Surface chlorine doped perovskite-type cobaltate lanthanum for water oxidation

doi:10.1016/S1872-2067(21)64004-4

Chinese Journal of Catalysis ›› 2022, Vol. 43 ›› Issue (6): 1485-1492.DOI: 10.1016/S1872-2067(21)64004-4

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Surface chlorine doped perovskite-type cobaltate lanthanum for water oxidation

Wei Shen^a^,^†, Jing Jin^a^,^†, Yang Hu^a, Yichao Hou^a, Jie Yin^a, Zhenhui Ma^b, Yong-Qing Zhao^a, Pinxian Xi^a^,^*()

^aState Key Laboratory of Applied Organic Chemistry, Frontiers Science Center for Rare Isotopes, Key Laboratory of Nonferrous Metal Chemistry and Resources Utilization of Gansu Province, College of Chemistry and Chemical Engineering, Lanzhou University, Lanzhou 730000, Gansu, China
^bDepartment of Physics, Beijing Technology and Business University, Beijing 100048, China

Received:2021-11-13 Accepted:2021-11-13 Online:2022-06-18 Published:2022-04-14
Contact: Pinxian Xi
About author:First author contact:
作者简介:^† Contributed equally to this work.
Supported by:
National Natural Science Foundation of China(21931001);National Natural Science Foundation of China(21922105);National Natural Science Foundation of China(51771085);National Natural Science Foundation of China(51801088);Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province(2019ZX-04);111 Project(B20027);Fundamental Research Funds for the Central Universities(lzujbky-2021-pd04);Fundamental Research Funds for the Central Universities(lzujbky-2021-it12);Fundamental Research Funds for the Central Universities(lzujbky-2021-37);China Postdoctoral Science Foundation(2021M691375);China National Postdoctoral Program for Innovative Talents(BX20200157)

Abstract

Abstract:

Rationally manipulating the in-situ formed catalytically active surface of catalysts remains a great challenge for a highly efficient water electrolysis. Here, we report a cationic oxidation method which can adjust the leaching of the in-situ catalyst and promote the reconstruction of dynamic surface for the oxygen evolution reaction (OER). The chlorine doping can reduce the possibility of triggering in-situ cobalt oxidation and chlorine leaching, leading to a transformation of the surface chlorine doped LaCoO₃ (Cl-LaCoO₃) into an intricate amorphous (oxygen) hydroxide phase. And thus, Cl-LaCoO₃ nanocrystals shows an ultralow overpotential of 342 mV at the current density of 10 mA cm ^-2 and Tafel slope of 76.2 mV dec^-1. Surface reconstructed Cl-LaCoO₃ is better than many of the most advanced OER catalysts and has proven significant stability. This work provides a new prospect for designing a high-efficiency electrocatalyst with optimized perovskite-structure in renewable energy system.

Key words: Surface reconstruction, LaCoO₃, Chlorine doped, Hollow cube, Oxygen evolution reaction

Wei Shen, Jing Jin, Yang Hu, Yichao Hou, Jie Yin, Zhenhui Ma, Yong-Qing Zhao, Pinxian Xi. Surface chlorine doped perovskite-type cobaltate lanthanum for water oxidation[J]. Chinese Journal of Catalysis, 2022, 43(6): 1485-1492.

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URL: https://www.cjcatal.com/EN/10.1016/S1872-2067(21)64004-4

https://www.cjcatal.com/EN/Y2022/V43/I6/1485

Figures/Tables 4

Fig. 1. XRD patterns (a), SEM (b), HRTEM (c,d), EDS mapping (e,f) images of La, Co, O, Cl. SAED pattern (g) and atomic resolution HAADF-STEM image (h) and corresponding EDS elemental mapping images (i) of hollow cube structure LaCoO3 and Cl-LaCoO3.

Fig. 2. Raman spectra (a), crystal structure (b), XPS spectra (c) of Cl-LaCoO3. XPS spectra of La 3d5/2 (d), Co 2p3/2 (e) and O 1s (f) for those obtained catalysts.

Fig. 3. (a) Scheme of experimental setup for in-situ Raman spectrometry. (b,c) In-situ Raman signals during OER. (d) IR-corrected LSV curves for OER in 1.0 mol/L KOH. (e) Schematic diagram of self-driven surface reconstruction. (f) Comparison of merit with respect to both kinetics (Tafel slope) and activity. (g) Total ECSA of LSV curves for OER in 1.0 mol/L KOH. (h) Chronoamperometric response for OER. (i) EIS curves of LaCoO3 and Cl-LaCoO3.

Fig. 4. SEM and TEM (a), HRTEM (b), SAED pattern (c) of Cl-LaCoO3 after OER. (d) EELS before and after OER in 1.0 mol/L KOH. (e,f) EDS mapping images of La, Co, O, Cl of those obtained catalysts after OER.

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Surface chlorine doped perovskite-type cobaltate lanthanum for water oxidation

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