Dopant-Induced Charge Redistribution on the 3D Sponge-like Hierarchical Structure of Quaternary Metal Phosphides Nanosheet Arrays Derived from Metal–Organic Frameworks for Natural Seawater Splitting,ACS Applied Materials & Interfaces

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Dopant-Induced Charge Redistribution on the 3D Sponge-like Hierarchical Structure of Quaternary Metal Phosphides Nanosheet Arrays Derived from Metal–Organic Frameworks for Natural Seawater Splitting
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2024-01-05 , DOI: 10.1021/acsami.3c15117
Thuy Tien Nguyen Tran _{1,

2,

3} , Thuy-Kieu Truong ₄ , Jianmin Yu ₅ , Lishan Peng ₅ , Xinghui Liu ₆ , Linh Ho Thuy Nguyen _{2,

3} , Sungkyun Park ₇ , Yoshiyuki Kawazoe ₈ , Thang Bach Phan _{2,

3} , Nhu Hoa Thi Tran _{1,

3} , Nam Hoang Vu _{1,

3} , Ngoc Quang Tran _{2,

3}

Affiliation

Dopant-induced electron redistribution on transition metal-based materials has long been considered an emerging new electrocatalyst that is expected to replace noble-metal-based electrocatalysts in natural seawater electrolysis; however, their practical applications remain extremely daunting due to their sluggish kinetics in natural seawater. In this work, we developed a facile strategy to synthesize the 3D sponge-like hierarchical structure of Ru-doped NiCoFeP nanosheet arrays derived from metal–organic frameworks with remarkable hydrogen evolution reaction (HER) performance in natural seawater. Based on experimental results and density functional theory calculations, Ru-doping-induced charge redistribution on the surface of metal active sites has been found, which can significantly enhance the HER activity. As a result, the 3D sponge-like hierarchical structure of Ru–NiCoFeP nanosheet arrays achieves low overpotentials of 52, 149, and 216 mV at 10, 100, and 500 mA cm^–2 in freshwater alkaline, respectively. Notably, the electrocatalytic activity of the Ru–NiCoFeP electrocatalyst in simulated alkaline seawater and natural alkaline seawater is nearly the same as that in freshwater alkaline. This electrocatalyst exhibits superior catalytic properties with outstanding stability under a high current density of 85 mA cm^–2 for more than 100 h in natural seawater, which outperforms state-of-the-art 20% Pt/C at high current density. Our work provides valuable guidelines for developing a low-cost and high-efficiency electrocatalyst for natural seawater splitting.

中文翻译：

天然海水分裂金属有机框架衍生的四元金属磷化物纳米片阵列的 3D 海绵状分层结构上的掺杂剂诱导电荷重新分布

过渡金属基材料上的掺杂诱导电子重新分布长期以来被认为是一种新兴的新型电催化剂，有望取代天然海水电解中的贵金属基电催化剂；然而，由于它们在天然海水中的缓慢动力学，其实际应用仍然极其令人畏惧。在这项工作中，我们开发了一种简单的策略来合成源自金属有机框架的 Ru 掺杂 NiCoFeP 纳米片阵列的 3D 海绵状分层结构，在天然海水中具有显着的析氢反应 (HER) 性能。基于实验结果和密度泛函理论计算，发现Ru掺杂引起金属活性位点表面的电荷重新分布，可以显着增强HER活性。因此，Ru-NiCoFeP 纳米片阵列的 3D 海绵状分层结构在淡水碱性条件下在 10、100 和 500 mA cm ^–2下分别实现了 52、149 和 216 mV 的低过电势。值得注意的是，Ru-NiCoFeP电催化剂在模拟碱性海水和天然碱性海水中的电催化活性与在淡水碱性水中的电催化活性几乎相同。这种电催化剂在天然海水中在85 mA cm ^–2的高电流密度下表现出优异的催化性能和出色的稳定性超过100小时，在高电流密度下优于最先进的20% Pt/C。我们的工作为开发用于自然海水分解的低成本且高效的电催化剂提供了宝贵的指导。

更新日期：2024-01-05

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