Enhancing Direct Electrochemical CO2 Electrolysis by Introducing A-Site Deficiency for the Dual-Phase Pr(Ca)Fe(Ni)O3−δ Cathode

IF 13 2区材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY Energy & Environmental Materials Pub Date : 2024-02-11 DOI:10.1002/eem2.12715

Wanhua Wang, Haixia Li, Ka-Young Park, Taehee Lee, Dong Ding, Fanglin Chen

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Abstract

High-temperature CO₂ electrolysis via solid oxide electrolysis cells (CO₂–SOECs) has drawn special attention due to the high energy convention efficiency, fast electrode kinetics, and great potential in carbon cycling. However, the development of cathode materials with high catalytic activity and chemical stability for pure CO₂ electrolysis is still a great challenge. In this work, A-site cation deficient dual-phase material, namely (Pr_0.4Ca_0.6)_xFe_0.8Ni_0.2O_3−δ (PCFN, x = 1, 0.95, and 0.9), has been designed as the fuel electrode for a pure CO₂–SOEC, which presents superior electrochemical performance. Among all these compositions, (Pr_0.4Ca_0.6)_0.95Fe_0.8Ni_0.2O_3−δ (PCFN95) exhibited the lowest polarization resistance of 0.458 Ω cm² at open-circuit voltage and 800 °C. The application of PCFN95 as the cathode in a single cell yields an impressive electrolysis current density of 1.76 A cm⁻² at 1.5 V and 800 °C, which is 76% higher than that of single cells with stoichiometric Pr_0.4Ca_0.6Fe_0.8Ni_0.2O_3−δ (PCFN100) cathode. The effects of A-site deficiency on materials' phase structure and physicochemical properties are also systematically investigated. Such an enhancement in electrochemical performance is attributed to the promotion of effective CO₂ adsorption, as well as the improved electrode kinetics resulting from the A-site deficiency.

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通过引入双相 Pr(Ca)Fe(Ni)O3-δ 阴极的 A 盐缺失来增强直接电化学二氧化碳电解能力

通过固体氧化物电解槽进行高温二氧化碳电解（CO2-SOECs）具有能量转化效率高、电极动力学速度快、碳循环潜力大等特点，因此受到特别关注。然而，开发具有高催化活性和化学稳定性的纯 CO2 电解阴极材料仍然是一个巨大的挑战。本研究设计了 A 位阳离子缺陷双相材料，即 (Pr0.4Ca0.6)xFe0.8Ni0.2O3-δ（PCFN，x = 1、0.95 和 0.9），作为纯 CO2-SOEC 的燃料电极，该材料具有优异的电化学性能。在所有这些成分中，(Pr0.4Ca0.6)0.95Fe0.8Ni0.2O3-δ（PCFN95）在开路电压和 800 °C 下的极化电阻最低，为 0.458 Ω cm2。在单电池中使用 PCFN95 作为阴极，在 1.5 V 和 800 ℃ 条件下可获得 1.76 A cm-2 的惊人电解电流密度，比使用化学计量 Pr0.4Ca0.6Fe0.8Ni0.2O3-δ （PCFN100）阴极的单电池高出 76%。此外，还系统地研究了 A 位缺陷对材料相结构和物理化学性能的影响。电化学性能的提高归因于 A 位缺失促进了二氧化碳的有效吸附以及电极动力学的改善。

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来源期刊

Energy & Environmental Materials MATERIALS SCIENCE, MULTIDISCIPLINARY-

CiteScore

17.60

自引率

6.00%

发文量

期刊介绍： Energy & Environmental Materials (EEM) is an international journal published by Zhengzhou University in collaboration with John Wiley & Sons, Inc. The journal aims to publish high quality research related to materials for energy harvesting, conversion, storage, and transport, as well as for creating a cleaner environment. EEM welcomes research work of significant general interest that has a high impact on society-relevant technological advances. The scope of the journal is intentionally broad, recognizing the complexity of issues and challenges related to energy and environmental materials. Therefore, interdisciplinary work across basic science and engineering disciplines is particularly encouraged. The areas covered by the journal include, but are not limited to, materials and composites for photovoltaics and photoelectrochemistry, bioprocessing, batteries, fuel cells, supercapacitors, clean air, and devices with multifunctionality. The readership of the journal includes chemical, physical, biological, materials, and environmental scientists and engineers from academia, industry, and policy-making.