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在新型三维交叉花状框架内设计三元钴镍铁层状双氢氧化物以实现析氧反应中的高效催化性能。

Designing ternary Co-Ni-Fe layered double hydroxides within a novel 3D cross-flower framework for efficient catalytic performance in oxygen evolution reaction.

作者信息

Liu Shuo, Zhang Yufan, Hao Lin, Nsabimana Anaclet, Shen Shigang

机构信息

State Key Laboratory of New Pharmaceutical Preparations and Excipients, Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of Education, Key Laboratory of Analytical Science and Technology of Hebei Province, School of Eco-Environment, College of Chemistry and Materials Science, Hebei University, 071002 Baoding, PR China.

State Key Laboratory of New Pharmaceutical Preparations and Excipients, Key Laboratory of Medicinal Chemistry and Molecular Diagnosis of the Ministry of Education, Key Laboratory of Analytical Science and Technology of Hebei Province, School of Eco-Environment, College of Chemistry and Materials Science, Hebei University, 071002 Baoding, PR China.

出版信息

J Colloid Interface Sci. 2025 Jan 15;678(Pt C):924-933. doi: 10.1016/j.jcis.2024.09.185. Epub 2024 Sep 24.

Abstract

In this study, we synthesized novel three-dimensional (3D) cross-flowered Co-Ni metal-organic framework (Co-Ni-MOF) precursors using the chemical precipitation method. Subsequently, we obtained Co-Ni-Fe layered double hydroxides (Co-Ni-Fe-LDHs) through an ion exchange strategy, which preserved their original morphology while consisting of ultrathin layered hydroxide nanosheets. The interlayer spacing of the LDH lamellar structure was finely tuned by varying the ratios of Co to Ni. The results demonstrated that Co-Ni-Fe LDHs, characterized by a unique three-dimensional cross-shaped structure and an optimal composition ratio of Co:Ni = 2:1, exhibited increased interlayer spacing. This structural characteristic contributed to their excellent electrochemical performance, positioning them as optimal electrode materials for catalytic oxygen evolution reactions (OER). Our observations revealed that Co-Ni-Fe-LDHs exhibited remarkable OER activity, characterized by a low Tafel slope of 41.82 mV dec, a low overpotential of 322 mV at a current density of 10 mA cm, and outstanding stability over a 48-hour period. In-situ Raman spectroscopy results indicated that the active site of the composite was γ-CoOOH. Additionally, the room temperature stirring and standing strategy employed in this study is easier to scale up and yields a higher quantity of reaction products compared to traditional high-temperature and high-pressure conditions. This investigation provides novel insights into the design and fabrication of Co-Ni-Fe-LDHs catalyst with 3D cross-flower structures, demonstrating enhanced electrocatalytic activity and commendable stability. These findings suggest promising applications in the field of electrolyzed water.

摘要

在本研究中,我们采用化学沉淀法合成了新型三维(3D)交叉花状钴镍金属有机框架(Co-Ni-MOF)前驱体。随后,通过离子交换策略获得了钴镍铁层状双氢氧化物(Co-Ni-Fe-LDHs),其保留了原始形态,同时由超薄层状氢氧化物纳米片组成。通过改变钴与镍的比例,对LDH层状结构的层间距进行了精细调节。结果表明,具有独特三维十字形结构且钴与镍最佳组成比为2:1的Co-Ni-Fe LDHs表现出层间距增加。这一结构特征有助于其优异的电化学性能,使其成为催化析氧反应(OER)的最佳电极材料。我们的观察结果表明,Co-Ni-Fe-LDHs表现出显著的OER活性,其特征在于低塔菲尔斜率为41.82 mV dec,在电流密度为10 mA cm时过电位低至322 mV,并且在48小时内具有出色的稳定性。原位拉曼光谱结果表明,该复合材料的活性位点为γ-CoOOH。此外,与传统的高温高压条件相比,本研究采用的室温搅拌和静置策略更易于扩大规模,且反应产物产量更高。本研究为具有3D交叉花状结构Co-Ni-Fe-LDHs催化剂的设计和制备提供了新的见解,展示了增强的电催化活性和良好的稳定性。这些发现表明在电解水领域具有广阔的应用前景。

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