Uncovering Atomic‐Scale Stability and Reactivity in Engineered Zinc Oxide Electrocatalysts for Controllable Syngas Production,Advanced Energy Materials

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Uncovering Atomic‐Scale Stability and Reactivity in Engineered Zinc Oxide Electrocatalysts for Controllable Syngas Production
Advanced Energy Materials ( IF 24.4 ) Pub Date : 2020-06-10 , DOI: 10.1002/aenm.202001381
Rahman Daiyan ₁ , Emma Catherine Lovell ₁ , Bosi Huang ₂ , Muhammad Zubair ₁ , Joshua Leverett ₁ , Qingran Zhang ₁ , Sean Lim ₃ , Jonathan Horlyck ₁ , Jianbo Tang ₁ , Xunyu Lu ₁ , Kourosh Kalantar‐Zadeh ₁ , Judy N. Hart ₂ , Nicholas M. Bedford ₁ , Rose Amal ₁

Affiliation

In this study, scalable, flame spray synthesis is utilized to develop defective ZnO nanomaterials for the concurrent generation of H₂ and CO during electrochemical CO₂ reduction reactions (CO₂RR). The designed ZnO achieves an H₂/CO ratio of ≈1 with a large current density (j ) of 40 mA cm⁻² during long‐term continuous reaction at a cell voltage of 2.6 V. Through in situ atomic pair distribution function analysis, the remarkable stability of these ZnO structures is explored, addressing the knowledge gap in understanding the dynamics of oxide catalysts during CO₂RR. Through optimization of synthesis conditions, ZnO facets are modulated which are shown to affect reaction selectivity, in agreement with theoretical calculations. These findings and insights on synthetic manipulation of active sites in defective metal‐oxides can be used as guidelines to develop active catalysts for syngas production for renewable power‐to‐X to generate a range of fuels and chemicals.

中文翻译：

在可控制合成气生产的工程氧化锌电催化剂中发现原子尺度的稳定性和反应性

在这项研究中，可扩展的火焰喷涂合成技术被用于开发有缺陷的ZnO纳米材料，以在电化学CO ₂还原反应（CO ₂ RR）中同时生成H ₂和CO 。设计的ZnO在2.6 V电池电压下长期连续反应期间，具有40 mA cm ^-2的大电流密度（j），H ₂ / CO比达到≈1 。通过原位原子对分布函数分析，探索了这些ZnO结构的出色稳定性，解决了在了解CO ₂期间氧化物催化剂动力学方面的知识差距RR。通过优化合成条件，可以调节ZnO晶面，与理论计算结果一致，这些ZnO晶面会影响反应的选择性。这些关于缺陷金属氧化物中活性位点的合成操纵的发现和见解可以用作开发用于可再生能源X的合成气生产以生产各种燃料和化学品的活性催化剂的指南。

更新日期：2020-07-28

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