Fe-Co(OH)2/Fe2O3 异质结构中吸附演化与晶格氧机制的耦合增强电化学水氧化,Advanced Functional Materials

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Fe-Co(OH)2/Fe2O3 异质结构中吸附演化与晶格氧机制的耦合增强电化学水氧化
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2023-09-01 , DOI: 10.1002/adfm.202305243
Sisi Xin ₁ , Yu Tang ₂ , Baohua Jia ₃ , Zhengfu Zhang ₁ , Chengping Li ₁ , Rui Bao ₁ , Caiju Li ₁ , Jianhong Yi ₁ , Jinsong Wang _{1,

4} , Tianyi Ma ₃

Affiliation

析氧反应（OER）仍然是电催化水分解制氢的瓶颈。然而，传统的吸附演化机制（AEM）由于尺度关系而具有缓慢的反应动力学，而晶格氧机制（LOM）由于晶格氧的逃逸而引发不稳定的结构。本文提出了一种概念验证的Fe-Co(OH) ₂ /Fe ₂ O _{3异质结构，其中AEM之后的Fe-Co(OH)}₂可以完成快速去质子化过程，而LOM之后的Fe ₂ O ₃可以触发O ─O耦合步骤。_{结合理论和实验研究证实，Fe-Co(OH) 2} /Fe ₂ O ₃结的空间电荷重新分布可以协同优化吸附和晶格氧，AEM和LOM的耦合机制可以同步促进OER活性和稳定性。结果，Fe-Co(OH) ₂ /Fe ₂ O _{3异质结构表现出优异的OER性能，仅219和249 mV的低过电势即可达到10和100 mA cm}^-2的电流密度。具体而言，Fe-Co(OH) ₂ /Fe ₂ O _{3电催化剂在100 mA cm}^-2的大电流密度下保持100小时优异的长期稳定性。这项工作为突破传统开放教育资源机制的限制铺平了道路。

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Coupling Adsorbed Evolution and Lattice Oxygen Mechanism in Fe-Co(OH)2/Fe2O3 Heterostructure for Enhanced Electrochemical Water Oxidation

Oxygen evolution reaction (OER) remains a bottleneck for electrocatalytic water-splitting to generate hydrogen. However, the traditional adsorbed evolution mechanism (AEM) possesses sluggish reaction kinetics due to the scaling relationship, while lattice oxygen mechanism (LOM) triggers an unstable structure due to the escaping of lattice oxygen. Herein, a proof-of-concept Fe-Co(OH)₂/Fe₂O₃ heterostructure is put forward, where Fe-Co(OH)₂ following AEM can complete rapidly deprotonation process while Fe₂O₃ following LOM can trigger O─O coupling step. Combining the theoretical and experimental investigation confirmed that the redistributed space-charge of Fe-Co(OH)₂/Fe₂O₃ junction can optimize synergistically adsorbed and lattice oxygen, the coupling mechanism of AEM and LOM can facilitate synchronously the OER activity and stability. As a result, the Fe-Co(OH)₂/Fe₂O₃ heterostructure shows excellent OER performance with low overpotential of only 219 and 249 mV to reach a current density of 10 and 100 mA cm⁻². Specifically, the Fe-Co(OH)₂/Fe₂O₃ electrocatalyst maintains excellent long-term stability for 100 h at a large current density of 100 mA cm⁻². This work paves an avenue to break through the limit of the conventional OER mechanism.

更新日期：2023-09-01

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