Short Hydrogen Bonds on Reconstructed Nanocrystal Surface Enhance Oxygen Evolution Activity

Yang, Jinlong; Zheng, Jiaxin; Xu, Ming; Zhuo, Zengqing; Yang, Wanli; Wang, Lin -Wang; Dai, Liming; Lu, Jun; Amine, Khalil; Pan, Feng

doi:10.1021/acscatal.7b02814

Title: Short Hydrogen Bonds on Reconstructed Nanocrystal Surface Enhance Oxygen Evolution Activity

Journal Article · Mon Nov 20 00:00:00 EST 2017 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.7b02814· OSTI ID:1461413

Yang, Jinlong ^[1]; Zheng, Jiaxin ^[1]; Xu, Ming ^[1]; Zhuo, Zengqing ^[2];

^[3]; Wang, Lin -Wang ^[3]; Dai, Liming ^[4];

^[5];

^[1]

Peking Univ., Shenzhen (People's Republic of China)
Peking Univ., Shenzhen (People's Republic of China); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Case Western Reserve Univ., Cleveland, OH (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Here, water splitting to generate hydrogen and oxygen gas is critical to renewable energy technologies, including fuel cells and rechargeable metal–air batteries. The oxygen evolution reaction (OER) has long been the bottleneck of water splitting because of its high overpotential (η) and sluggish kinetics, and development of efficient, stable, and non-noble-metal-based OER catalysts has been an extensively studied topic. Here, we propose short hydrogen bonds on reconstructed nanocrystal surface to enhance oxygen evolution activity by investigating three types of phase structures (β_II, β_I, and γ₀) of Li₂CoSiO₄ (LCS) nanoparticles as OER electrocatalysts. Among them, the β_II-LCS outperforms the previously reported Co-based catalysts and the state-of-the-art IrO₂ catalyst for OER in the alkaline condition. Our experiments combined with ab initio calculations indicated that due to the line-linked arrangement of Co active sites at the surface of β_II-LCS, short hydrogen bonds (2.54 Å) are formed and linked into a network at the reconstructed surface by rotating the flexible CoO4 tetrahedra after surface delithiation, thus facilitating proton transfer and dissociation, leading to a unique dual-center catalytic pathway with low theoretical thermodynamic overpotential (0.35 eV) for the OER process.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Vehicle Technologies Office (EE-3V)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1461413

Journal Information:: ACS Catalysis, Vol. 8, Issue 1; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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Core-Shell Structured NiCo ₂ O ₄ @FeOOH Nanowire Arrays as Bifunctional Electrocatalysts for Efficient Overall Water Splitting Li, Man; Tao, Leiming; Xiao, Xin ChemCatChem, Vol. 10, Issue 18 https://doi.org/10.1002/cctc.201800606	journal	August 2018
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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
nanocrystal surface
oxygen evolution activity
proton transfer and dissociation
short hydrogen bond
βII-Li2CoSiO4

Title: Short Hydrogen Bonds on Reconstructed Nanocrystal Surface Enhance Oxygen Evolution Activity

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