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Searching General Sufficient‐and‐Necessary Conditions for Ultrafast Hydrogen‐Evolving Electrocatalysis
Author(s) -
Guan Daqin,
Zhou Jing,
Hu Zhiwei,
Zhou Wei,
Xu Xiaomin,
Zhong Yijun,
Liu Bo,
Chen Yuhui,
Xu Meigui,
Lin HongJi,
Chen ChienTe,
Wang JianQiang,
Shao Zongping
Publication year - 2019
Publication title -
advanced functional materials
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 6.069
H-Index - 322
eISSN - 1616-3028
pISSN - 1616-301X
DOI - 10.1002/adfm.201900704
Subject(s) - catalysis , materials science , electrocatalyst , transition metal , oxygen , octahedron , oxygen evolution , hydrogen , rational design , chemical physics , nanotechnology , chemistry , crystallography , crystal structure , electrochemistry , biochemistry , organic chemistry , electrode
The development of cost‐effective and high‐performance electrocatalysts for the hydrogen evolution reaction (HER) is one critical step toward successful transition into a sustainable green energy era. Different from previous design strategies based on single parameter, here the necessary and sufficient conditions are proposed to develop bulk non‐noble metal oxides which are generally considered inactive toward HER in alkaline solutions: i) multiple active sites for different reaction intermediates and ii) a short reaction path created by ordered distribution and appropriate numbers of these active sites. Computational studies predict that a synergistic interplay between the ordered oxygen vacancies (at pyramidal high‐spin Co 3+ sites) and the O 2p ligand holes (OLH; at metallic octahedral intermediate‐spin Co 4+ sites) in RBaCo 2 O 5.5+ δ (δ = 1/4; R = lanthanides) can produce a near‐ideal HER reaction path to adsorb H 2 O and release H 2 , respectively. Experimentally, the as‐synthesized (Gd 0.5 La 0.5 )BaCo 2 O 5.75 outperforms the state‐of‐the‐art Pt/C catalyst in many aspects. The proof‐of‐concept results reveal that the simultaneous possession of ordered oxygen vacancies and an appropriate number of OLH can realize a near‐optimal synergistic catalytic effect, which is pivotal for rational design of oxygen‐containing materials.