Thermally Labile Organic-Soluble Heterometal Diorganophosphate-Derived Efficient Electrocatalysts for the Oxygen Evolution Reaction

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL Chemistry of Materials Pub Date : 2024-06-18 DOI:10.1021/acs.chemmater.4c00536

Savi Chaudhary, and , Ramaswamy Murugavel*,

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Abstract

Heterometal phosphates are burgeoning electrocatalysts and cathode materials in energy storage and conversion devices. In this work, we demonstrate a novel and clean synthetic route for substoichiometric lithium-deficient metastable Cmcm-Li_0.65(7)Co_1.16(2)PO₄ (Li-Co-P-HEX) and metaphosphate P2₁2₁2₁-LiCo(PO₃)₃ (Li-Co-P-BT), starting from the same starting material [LiCo(dtbp)₃] (dtbp = di-tert-butyl phosphate) through a thermolytic single-source precursor approach. The heterometal organophosphate [LiCo(dtbp)₃] decomposed into different phases of inorganic heterometal phosphates by employing a solution and solid-state thermal treatment. The solution-processed Li-deficient orthophosphate exhibits superior oxygen evolution reaction activity, delivering a current density of 10 mA cm^–2 at an overpotential of 294 mV, outperforming other reported lithium–cobalt phosphates for water oxidation. The enhanced performance of the Cmcm-Li_0.65(7)Co_1.16(2)PO₄ as an electrocatalyst elucidates the synergistic effect generated by the structure, composition, and morphology.

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用于氧进化反应的热敏性有机可溶性异金属二甘磷酸盐高效电催化剂

杂金属磷酸盐是能量存储和转换设备中新兴的电催化剂和阴极材料。在这项工作中，我们通过热解单源前驱体方法，从相同的起始材料[LiCo(dtbp)3]（dtbp = 磷酸二叔丁酯）出发，展示了一种新颖、清洁的亚计量缺锂陨石 Cmcm-Li0.65(7)Co1.16(2)PO4（Li-Co-P-HEX）和偏磷酸盐 P212121-LiCo(PO3)3（Li-Co-P-BT）的合成路线。通过溶液和固态热处理，杂金属有机磷酸盐[LiCo(dtbp)3]分解成不同相的无机杂金属磷酸盐。溶液处理的缺锂正磷酸盐表现出卓越的氧进化反应活性，在 294 mV 的过电位下可提供 10 mA cm-2 的电流密度，优于其他已报道的用于水氧化的锂钴磷酸盐。作为一种电催化剂，Cmcm-Li0.65(7)Co1.16(2)PO4 性能的提高阐明了结构、组成和形态所产生的协同效应。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.