Uncovering the Promotion of CeO2/CoS1.97 Heterostructure with Specific Spatial Architectures on Oxygen Evolution Reaction

Tengyuan Dai; Xin Zhang; Mingzi Sun; Bolong Huang; Nan Zhang; Pengfei Da; Rui Yang; Zidong He; Wei Wang; Pinxian Xi; Chun-Hua Yan

doi:10.1002/adma.202102593

Uncovering the Promotion of CeO₂/CoS_1.97 Heterostructure with Specific Spatial Architectures on Oxygen Evolution Reaction

Tengyuan Dai, Xin Zhang, Mingzi Sun, Bolong Huang^*, Nan Zhang, Pengfei Da, Rui Yang, Zidong He, Wei Wang, Pinxian Xi^*, Chun-Hua Yan

^*Corresponding author for this work

Research output: Journal Publications and Reviews › RGC 21 - Publication in refereed journal › peer-review

186 Citations (Scopus)

Abstract

Structural engineering and compositional controlling are extensively applied in rationally designing and fabricating advanced freestanding electrocatalysts. The key relationship between the spatial distribution of components and enhanced electrocatalysis performance still needs further elaborate elucidation. Here, CeO₂ substrate supported CoS_1.97 (CeO₂-CoS_1.97) and CoS_1.97 with CeO₂ surface decorated (CoS_1.97-CeO₂) materials are constructed to comprehensively investigate the origin of spatial architectures for the oxygen evolution reaction (OER). CeO₂-CoS_1.97 exhibits a low overpotential of 264 mV at 10 mA cm⁻² due to the stable heterostructure and faster mass transfer. Meanwhile, CoS_1.97-CeO₂ has a smaller Tafel slope of 49 mV dec⁻¹ through enhanced adsorption of OH⁻, fast electron transfer, and in situ formation of Co(IV)O₂ species under the OER condition. Furthermore, operando spectroscopic characterizations combined with theoretical calculations demonstrate that spatial architectures play a distinguished role in modulating the electronic structure and promoting the reconstruction from sulfide to oxyhydroxide toward higher chemical valence. The findings highlight spatial architectures and surface reconstruction in designing advanced electrocatalytic materials. © 2021 Wiley-VCH GmbH

Original language	English
Article number	2102593
Journal	Advanced Materials
Volume	33
Issue number	42
Online published	3 Sept 2021
DOIs	https://doi.org/10.1002/adma.202102593
Publication status	Published - 21 Oct 2021
Externally published	Yes

Funding

T.D. and X.Z. contributed equally to this work. The authors acknowledge the support from the National Natural Science Foundation of China (no. 21931001 and 21922105), Special Fund Project of Guiding Scientific and Technological Innovation Development of Gansu Province (2019ZX-04), and the 111 Project (B20027). B.H. acknowledges the support of the Natural Science Foundation of China (NSFC) (no. 21771156), and the Early Career Scheme (ECS) fund (grant no. PolyU 253026/16P) from the Research Grant Council (RGC) in Hong Kong.

Research Keywords

heterostructures
oxygen evolution reaction
spatial architectures
structure-performance relationships
surface reconstruction

RGC Funding Information

RGC-funded

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

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10.1002/adma.202102593

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Cite this

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title = "Uncovering the Promotion of CeO2/CoS1.97 Heterostructure with Specific Spatial Architectures on Oxygen Evolution Reaction",

abstract = "Structural engineering and compositional controlling are extensively applied in rationally designing and fabricating advanced freestanding electrocatalysts. The key relationship between the spatial distribution of components and enhanced electrocatalysis performance still needs further elaborate elucidation. Here, CeO2 substrate supported CoS1.97 (CeO2-CoS1.97) and CoS1.97 with CeO2 surface decorated (CoS1.97-CeO2) materials are constructed to comprehensively investigate the origin of spatial architectures for the oxygen evolution reaction (OER). CeO2-CoS1.97 exhibits a low overpotential of 264 mV at 10 mA cm−2 due to the stable heterostructure and faster mass transfer. Meanwhile, CoS1.97-CeO2 has a smaller Tafel slope of 49 mV dec−1 through enhanced adsorption of OH−, fast electron transfer, and in situ formation of Co(IV)O2 species under the OER condition. Furthermore, operando spectroscopic characterizations combined with theoretical calculations demonstrate that spatial architectures play a distinguished role in modulating the electronic structure and promoting the reconstruction from sulfide to oxyhydroxide toward higher chemical valence. The findings highlight spatial architectures and surface reconstruction in designing advanced electrocatalytic materials. {\textcopyright} 2021 Wiley-VCH GmbH",

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AU - Dai, Tengyuan

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AU - Huang, Bolong

AU - Zhang, Nan

AU - Da, Pengfei

AU - Yang, Rui

AU - He, Zidong

AU - Wang, Wei

AU - Xi, Pinxian

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AB - Structural engineering and compositional controlling are extensively applied in rationally designing and fabricating advanced freestanding electrocatalysts. The key relationship between the spatial distribution of components and enhanced electrocatalysis performance still needs further elaborate elucidation. Here, CeO2 substrate supported CoS1.97 (CeO2-CoS1.97) and CoS1.97 with CeO2 surface decorated (CoS1.97-CeO2) materials are constructed to comprehensively investigate the origin of spatial architectures for the oxygen evolution reaction (OER). CeO2-CoS1.97 exhibits a low overpotential of 264 mV at 10 mA cm−2 due to the stable heterostructure and faster mass transfer. Meanwhile, CoS1.97-CeO2 has a smaller Tafel slope of 49 mV dec−1 through enhanced adsorption of OH−, fast electron transfer, and in situ formation of Co(IV)O2 species under the OER condition. Furthermore, operando spectroscopic characterizations combined with theoretical calculations demonstrate that spatial architectures play a distinguished role in modulating the electronic structure and promoting the reconstruction from sulfide to oxyhydroxide toward higher chemical valence. The findings highlight spatial architectures and surface reconstruction in designing advanced electrocatalytic materials. © 2021 Wiley-VCH GmbH

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