无机材料学报

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质子陶瓷膜反应器的制备及低温氨分解性能研究

唐阳1, 刘立敏1,2, 周晓亮1,2,3, 张搏3, 蒋星洲1, 贾浩义1, 罗延麟庆1   

  1. 1.西南石油大学 化学化工学院,成都 610500;
    2.天府永兴实验室,成都 611130;
    3.新疆理工学院 能源化工工程学院,阿克苏 843100
  • 收稿日期:2025-02-14 修回日期:2025-04-17
  • 通讯作者: 刘立敏(1976-), 副教授. E-mail: liulimin_ly@126.com
  • 作者简介:唐 阳(2001-), 男, 硕士研究生. E-mail: 2630565355@qq.com
  • 基金资助:
    国家重点研发计划(2021YFB4001502); 国家自然科学基金(22075231); 天府永兴实验室组织研究项目(2023KJGG09)

Proton Ceramic Membrane Reactor: Preparation and Low-temperature Ammonia Decomposition Performance

TANG Yang1, LIU Limin1,2, ZHOU Xiaoliang1,2,3, ZHANG Bo3, JIANG Xingzhou1, JIA Haoyi1, LUO Yanlinqing1   

  1. 1. College of Chemistry and Chemical Engineering, Southwest Petroleum University, Chengdu 610500, China;
    2. Tianfu Yongxing Laboratory, Chengdu 611130, China;
    3. College of Energy and Chemical Engineering, Xinjiang Institute of Technology, Akesu 843100, China
  • Received:2025-02-14 Revised:2025-04-17
  • Contact: LIU Limin (1976-), associate professor. E-mail:liulimin_ly@126.com
  • About author:Tang Yang (2001-), male, Master candidate. E-mail:2630565355@qq.com
  • Supported by:
    National Key Research and Development Program of China (2021YFB4001502); National Natural Science Foundation of China (22075231); Tianfu Yongxing Laboratory Organized Research Project Funding (2023KJGG09)

摘要: 氨气(NH3)作为一种储氢材料,具有高储氢密度、易液化等优点,因此利用氨分解制氢是一种理想的氢气(H2)制备方法。但传统氨分解的工作温度过高,中低温下NH3转化效率过低且H2纯度较低,无法实现H2的有效制取。本研究通过共压法制备了具有多孔电极Ni-BZCY/BZCY/Ni-BZCY(BZCY:BaZr0.1Ce0.7Y0.2O3-δ)对称结构的质子陶瓷膜反应器(PCMR)。在600 ℃时,PCMR在H2与NH3气氛下分别实现了0.11和0.23 Ω·cm2的极化阻抗(Rp),在0.8 V外加电压下其电流密度分别达到1.87和1.56 A·cm-2;在300 ℃、0.8 V外加电压下,H2与NH3中的电流密度仍能分别达到0.16和0.06 A·cm-2。通过共压法所制备的PCMR在600 ℃下的NH3分解转化效率达到80%,比裸催化剂材料提升了8%,在350 ℃仍能实现0.3%的提升,即使在300 ℃也表现出约1%的NH3转化效率。本研究为实现低温氨分解制氢提供了新的思路。

关键词: 氨分解制氢, 低温, 质子陶瓷膜反应器, 电化学性能, 质子传输

Abstract: Ammonia (NH3) has been considered as a hydrogen storage material due to high hydrogen storage density and ease to liquefaction, thus hydrogen (H2) production by ammonia decomposition is an ideal method for hydrogen preparation. However, traditional ammonia decomposition technologies face challenges such as high operating temperatures, low efficiency at moderate temperatures, and difficulties in hydrogen purification. In this study, proton ceramic membrane reactor (PCMR) with symmetric structure of porous electrode Ni-BZCY/BZCY/Ni-BZCY (BZCY : BaZr0.1Ce0.7Y0.2O3-δ) was prepared by co-pressing method. At 600 ℃, PCMR exhibited polarization impedances (Rp) of 0.11 and 0.23 Ω·cm2 in H2 and NH3 atmospheres, respectively, with corresponding current densities of 1.87 and 1.56 A·cm-2 at an applied voltage of 0.8 V. Even at 300 ℃ and 0.8 V, the current densities in H2 and NH3 remained at 0.16 and 0.06 A·cm-2, respectively. The NH3 conversion efficiency of PCMR reached 80% at 600 °C, improving by 8% compared to bare catalyst material. Even at 350 °C, an additional improvement of 0.3% can still be attained, and the NH3 conversion efficiency of about 1% was demonstrated even at 300 ℃. This study provides a novel approach to low-temperature ammonia decomposition for hydrogen production.

Key words: hydrogen production by ammonia decomposition, low-temperature, proton ceramic membrane reactor, electrochemical properties, proton transport

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