论文总字数：25327字

摘 要

固体氧化物电解池（SOEC，Solid oxide electrolysis cell）能够在中高温下将电能和热能转化为化学能，是一种效率高、污染小的能源转化装置。它可以以H₂O和CO₂作为原料，高效电解生产合成气（H₂和CO）。作为关键的燃料极材料，ABO₃型钙钛矿La_0.6Ce_0.4FeO₃具有良好的催化活性，因而是SOEC燃料极材料的合适选择。本课题就是以La_0.6Ce_0.4FeO₃为基础材料，通过在A位缺位B位掺杂脱溶的方式，来寻找镧-铈-铁-镍最佳的非化学计量比，探究具有优异电化学性能的SOEC燃料极材料。

本文通过合成A位缺位的La_0.6Ce_0.3Fe_0.95Ni_0.05O₃材料，在H₂还原条件下原位脱溶Ni纳米颗粒对燃料极进行修饰。XRD结果表明，在不同合成温度（1200℃、1300℃、1400℃）下，1300℃下合成的材料主晶相结晶度较高、杂峰较少。脱溶后的La_0.6Ce_0.3Fe_0.95Ni_0.05O₃样品的XRD表明Ni可以在镧-铈-铁材料体系中成功脱溶。探究在不同温度下（700℃、800℃、900℃）原位脱溶纳米颗粒的颗粒分布和大小的影响，并通过制备半电池、对称电池测试Ni脱溶对于电极在CO₂气氛下极化阻抗的影响，测试对比未脱溶和Ni脱溶表面修饰电极材料的电解性能。

关键词：固体氧化物电解池；燃料极材料；钙钛矿材料；原位脱溶

Effect of in situ exsolution Ni nanoparticles on the properties of La_0.6Ce_0.3Fe_0.95Ni_0.05O₃ fuel electrode materials

Abstract

The solid oxide electrolytic cell (SOEC, Solid oxide electrolysis cell) is a high-efficiency, low-polluting energy conversion device capable of converting electrical and thermal energy into chemical energy at medium and high temperatures. It can produce syngas (H₂ and CO) efficiently and electrolysis with H₂O and CO₂ as raw materials. As a key fuel electrode material, La_0.6Ce_0.4FeO₃ has good catalytic activity and is an appropriate choice for SOEC fuel electrode materials. This topic is based on La_0.6Ce_0.4FeO₃ material, through the optimization of A-bit and B-site, to find the best non-chemical measurement ratio of lanthanum-iron-nickel, to explore the excellent electrochemical performance of SOEC fuel electrode materials.

In this paper, the fuel electrode is modified by synthesizing the Material La_0.6Ce_0.3Fe_0.95Ni_0.05O₃, which is exsoluted under H₂ reduction conditions. The XRD results show that the main crystal phase crystallization and the lower peak of the synthetic material at 1300℃ are higher at different synthetic temperatures (1200℃, 1300℃, 1400℃). XRD of the desoluble La_0.6Ce_0.3Fe_0.95Ni_0.05O₃ sample shows that Ni can successfully exsoluted in this material system. To investigate the effect of particle distribution and size of exsoluted nanoparticles in situ at different temperatures (700℃, 800℃, 900℃), and to test the electrolysis performance of the un-exsoluted and exsoluted Ni surface-modified electrodes by testing the effect of Ni exsolution on the polarization impedance of the electrode under the CO₂ atmosphere by preparing half cells and full cells tests.

Key Words: Solid oxide electrolysis cell: Fuel electrode materials: Perovskite material:

In-situ exsolution

目 录

摘 要 I

Abstract II

第一章 绪论 1

1.1 引言 1

1.2 固体氧化物电解池的运行原理 1

1.3固体氧化物电解池的主要材料 2

1.3.1 氧电极材料 2

1.3.2 电解质材料 3

1.3.3 中间材料 4

1.3.4 燃料极材料 4

1.4 常见的固体氧化电解池燃料极钙钛矿材料 4

1.4.1 层状钙钛矿型结构燃料极材料 5

1.4.2 简单钙钛矿型结构燃料极材料 5

1.5 ABO₃型钙钛矿燃料极材料改性方法 8

1.5.1 变价金属离子掺杂 8

1.5.2 活性粒子浸渍 9

1.5.3 原位脱溶 10

1.6 研究意义及目的 11

第二章 实验及表征方法 12

2.1 实验原料 12

2.2 实验设备 12

2.3 实验方法及步骤 13

2.3.1 固相法制备粉料 13

2.3.2 燃料极浆料的制备 13

2.3.3 YSZ电解质片的制备 14

2.3.4半电池的制备 14

2.3.5对称电池的制备 14

2.3.6 单电池制备 14

2.3.7 电导率条的制备 14

2.4 表征方法 15

2.4.1 X射线衍射（XRD）分析 15

2.4.2 极化阻抗 15

2.4.3 电导率 15

2.4.4 扫描电子显微镜（SEM）分析 16

2.4.5 电解性能测试 16

第三章 结果与讨论 17

3.1 XRD分析 17

3.2 半电池测试 19

3.3 对称电池测试 21

3.3 电导率测试 21

3.4 单电池测试 22

3.5 稳定性测试 22

第四章 结论与展望 23

4.1 结论 23

4.2 展望 23

参考文献 24

致谢 28

第一章 绪论

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