Low-Coordinated Conductive ZnCu Metal-Organic Frameworks for Highly Selective H2O2 Electrosynthesis,Small

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Low-Coordinated Conductive ZnCu Metal-Organic Frameworks for Highly Selective H2O2 Electrosynthesis
Small ( IF 13.0 ) Pub Date : 2024-05-21 , DOI: 10.1002/smll.202403808
Zhihao Pei ₁ , Yunxiang Li _{1,

2} , Guilan Fan ₃ , Yan Guo ₃ , Deyan Luan ₂ , Xiaojun Gu ₃ , Xiong Wen David Lou ₂

Affiliation

Direct electrosynthesis of hydrogen peroxide (H₂O₂) with high production rate and high selectivity through the two-electron oxygen reduction reaction (2e⁻ORR) offers a sustainable alternative to the energy-intensive anthraquinone technology but remains a challenge. Herein, a low-coordinated, 2D conductive Zn/Cu metal-organic framework supported on hollow nanocube structures (ZnCu-MOF (H)) is rationally designed and synthesized. The as-prepared ZnCu-MOF (H) catalyst exhibits substantially boosted electrocatalytic kinetics, enhanced H₂O₂ selectivity, and ultra-high Faradaic efficiency for 2e⁻ORR process in both alkaline and neutral conditions. Electrochemical measurements, operando/quasi in situ spectroscopy, and theoretical calculation demonstrate that the introduction of Cu atoms with low-coordinated structures induces the transformation of active sites, resulting in the beneficial electron transfer and the optimized energy barrier, thereby improving the electrocatalytic activity and selectivity.

中文翻译：

用于高选择性 H2O2 电合成的低配位导电 ZnCu 金属有机框架

通过双电子氧还原反应（^2e-ORR）以高生产率和高选择性直接电合成过氧化氢（H₂O₂）为能源密集型蒽醌技术提供了一种可持续的替代方案，但仍然是一个挑战。在此，合理设计并合成了一种支撑在空心纳米立方体结构（ZnCu-MOF （H））上的低配位 2D 导电 Zn/Cu 金属有机框架。所制备的 ZnCu-MOF （H）催化剂在碱性和中性条件下均表现出显着增强的电催化动力学、增强的 H₂O₂ 选择性和 ^2e-ORR 工艺的超高法拉第效率。电化学测量、原位/准原位光谱和理论计算表明，引入具有低配位结构的 Cu 原子会诱导活性位点的转变，从而产生有益的电子转移和优化的能垒，从而提高电催化活性和选择性。

更新日期：2024-05-21

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