Intrinsic Specific Activity Enhancement for Bifunctional Electrocatalytic Activity toward Oxygen and Hydrogen Evolution Reactions via Structural Modification of Nickel Organophosphonates

化学 双功能 电催化剂 吡嗪 配体(生物化学) 无机化学 金属 析氧 组合化学 有机化学 电化学 催化作用 立体化学 电极 物理化学 受体 生物化学
作者
Poojita,Tanmay Rom,Rathindranath Biswas,Krishna Kanta Haldar,Avijit Kumar Paul
出处
期刊:Inorganic Chemistry [American Chemical Society]
卷期号:63 (8): 3795-3806 被引量:4
标识
DOI:10.1021/acs.inorgchem.3c03960
摘要

A comprehensive knowledge of the structure–activity relationship of the framework material is decisive to develop efficient multifunctional electrocatalysts. In this regard, two different metal organophosphonate compounds, [Ni(Hhedp)2]·4H2O (I) and [Ni3(H3hedp)2(C4H4N2)3]·6H2O (II) have been isolated through one-pot hydrothermal strategy by using H4hedp (1-hydroxyethane 1,1-diphosphonic acid) and N-donor auxiliary ligand (pyrazine; C4H4N2). The structures of synthesized materials have been established through single-crystal X-ray diffraction studies, which confirm that compound I formed a one-dimensional molecular chain structure, while compound II exhibited a three-dimensional extended structure. Further, the crystalline materials have participated as efficient electrocatalysts for the oxygen evolution and hydrogen evolution reactions (OER and HER) as compared to the state-of-the-art electrocatalyst RuO2. The electrocatalytic OER and HER performances show that compound II displayed better electrocatalytic performances toward OER (η10 = 305 mV) and HER (η10 = 230 mV) in alkaline (1 M KOH) and acidic (0.5 M H2SO4) media, respectively. Substantially, the specific activity has been assessed in order to measure the inherent electrocatalytic activity of the title electrocatalyst, which displays an enrichment of fourfold higher activity of compound II (0.64 mA/cm2) than compound I (0.16 mA/cm2) for the OER experiments. Remarkably, inclusion of an auxiliary pyrazine ligand into the metal organophosphonate structure (compound II) not only offers higher dimensionality along with significant enhancement of the overall bifunctional electrocatalytic performances but also improves the long-term stability, which is noteworthy for the family of hybrid framework materials.
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