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室温合成镍铁-六亚甲基四胺作为晶格氧参与的高效析氧反应电催化剂。

Room-temperature synthesis of NiFe-hexamethylenetetramine as lattice oxygen involved electrocatalyst for efficient oxygen evolution reaction.

作者信息

Zhang Yuehua, Wang Jialin, Guan Peng, Ye Qing, Zhao Yanxia, Cheng Yongliang

机构信息

Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an 710127, China.

Key Laboratory of Synthetic and Natural Functional Molecule of the Ministry of Education, College of Chemistry and Materials Science, Northwest University, Xi'an 710127, China.

出版信息

J Colloid Interface Sci. 2025 Jul 15;690:137287. doi: 10.1016/j.jcis.2025.137287. Epub 2025 Mar 9.

Abstract

The design and synthesis of an oxygen evolution reaction (OER) electrocatalyst following lattice oxygen mechanism (LOM) through a straightforward strategy is crucial for achieving efficient electrocatalytic hydrogen production; however, it remains a formidable challenge. Herein, a novel and highly efficient LOM-based OER electrocatalyst, NiFe-hexamethylenetetramine (NiFe-HMT) coordination compound, is fabricated through a straightforward co-precipitation strategy at room temperature within 30 min. The obtained NiFe-HMT exhibits remarkable OER activity with low overpotentials of 269 and 352 mV to achieve 100 and 1000 mA cm, respectively. Experimental results and theoretical calculations reveal that the incorporation of Fe can effectively activate the lattice oxygen in the reconstructed oxyhydroxides, thereby shifting the OER pathway from adsorbate evolution mechanism to LOM. Additionally, compared with NiFe-LDH, NiFe-HMT is more favorable for forming highly active oxyhydroxides and exhibits more significant lattice oxygen activity. Furthermore, NiFe-HMT can be scaled up to more than 10 g in a single batch and stored stability for over 142 days without any significant decline in activity, thereby indicating its potential for large-scale implementation. This study provides valuable insights into developing high-performance OER electrocatalysts following the LOM pathway.

摘要

通过直接的策略设计和合成遵循晶格氧机制(LOM)的析氧反应(OER)电催化剂对于实现高效的电催化制氢至关重要;然而,这仍然是一个巨大的挑战。在此,通过在室温下30分钟内采用直接的共沉淀策略制备了一种新型高效的基于LOM的OER电催化剂,即NiFe-六亚甲基四胺(NiFe-HMT)配位化合物。所制备的NiFe-HMT表现出显著的OER活性,在达到100和1000 mA cm时的过电位分别低至269和352 mV。实验结果和理论计算表明,Fe的掺入可以有效激活重构羟基氧化物中的晶格氧,从而将OER途径从吸附质析出机制转变为LOM。此外,与NiFe-LDH相比,NiFe-HMT更有利于形成高活性的羟基氧化物,并且表现出更显著的晶格氧活性。此外,NiFe-HMT可以单次批量扩大到10 g以上,并且储存稳定性超过142天,活性没有任何显著下降,从而表明其大规模应用的潜力。这项研究为开发遵循LOM途径的高性能OER电催化剂提供了有价值的见解。

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