Synergistic Effects of Strain and Oxygen Vacancies in Nanofiber Electrodes for Enhanced High-Temperature Electrochemical Ethane Dehydrogenation

IF 11.3 1区化学 Q1 CHEMISTRY, PHYSICAL

ACS Catalysis Pub Date : 2025-05-30 DOI:10.1021/acscatal.5c02377

Yongjian Ye, Xuepeng Xiang, Zilin Ma, Nian Zhang, Shijun Zhao, Wonyoung Lee, Youmin Guo, Jaroslaw Milewski, Yan Chen

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引用次数: 0

Abstract

Direct ethane dehydrogenation (EDH) via protonic ceramic electrolysis cells (PCEC) represents a promising strategy for ethylene production. The practical application of this technique nevertheless is hindered by the scarcity of high-performance anode materials. In this work, PrBa_0.5Sr_0.5Co_1.5Fe_0.5O_5+δ (PBSCF) nanofibers are synthesized as PCEC anodes, which exhibit high activity toward EDH, achieving an ethylene selectivity as high as 93.8% and an ethane conversion of 63.7% at 535 mA cm^–2 and 700 °C. The combination of advanced spectroscopic techniques and density functional theory calculations reveals the presence of compressive strain in the nanofibers. This strain weakens the metal–oxygen bonds and shifts the O 2p band center closer to the Fermi level, thereby facilitating the formation of oxygen vacancies. The synergistic effect of compressive strain and oxygen vacancies enhances C₂H₆ adsorption and promotes the dehydrogenation steps for C₂H₄ production. The obtained knowledge can be broadly applied to the design of nanostructured electrocatalysts for other high-temperature electrochemical devices.

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应变和氧空位在纳米纤维电极中增强高温电化学乙烷脱氢的协同效应

通过质子陶瓷电解电池（PCEC）进行乙烷直接脱氢（EDH）是一种很有前途的乙烯生产策略。然而，高性能阳极材料的缺乏阻碍了该技术的实际应用。在本研究中，制备了PrBa0.5Sr0.5Co1.5Fe0.5O5+δ (PBSCF)纳米纤维作为PCEC阳极，其对EDH具有较高的活性，在535 mA cm-2和700℃条件下，乙烯选择性高达93.8%，乙烷转化率为63.7%。结合先进的光谱技术和密度泛函理论计算，揭示了纳米纤维中存在压缩应变。这种应变削弱了金属-氧键，使o2p能带中心更靠近费米能级，从而促进了氧空位的形成。压缩应变和氧空位的协同作用增强了C2H6的吸附，促进了C2H4生产的脱氢步骤。所获得的知识可以广泛应用于其他高温电化学器件的纳米结构电催化剂的设计。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

ACS Catalysis CHEMISTRY, PHYSICAL-

CiteScore

20.80

自引率

6.20%

发文量

1253

审稿时长

1.5 months

期刊介绍： ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.