催化学报

催化学报 ›› 2012, Vol. 33 ›› Issue (9): 1572-1577.DOI: 10.3724/SP.J.1088.2012.20352

• 研究论文 • 上一篇    下一篇

纳米 Li2ZrO3 吸收剂原位移除 CO2 强化水煤气变换反应制氢

张元卓, 于兹瀛, 张富民a, 肖强, 钟依均, 朱伟东b   

  1. 浙江师范大学物理化学研究所, 先进催化材料教育部重点实验室, 浙江金华 321004
  • 收稿日期:2012-03-26 修回日期:2012-06-14 出版日期:2012-09-11 发布日期:2012-09-11

Li2ZrO3 Nanoparticles as Absorbent for in-Situ Removal of CO2 in Water-Gas Shift Reaction to Enhance H2 Production

ZHANG Yuanzhuo, YU Ziying, ZHANG Fumina, XIAO Qiang, ZHONG Yijun, ZHU Weidongb   

  1. Key Laboratory of the Ministry of Education for Advanced Catalysis Materials, Institute of Physical Chemistry, Zhejiang Normal University, Jinhua 321004, Zhejiang, China
  • Received:2012-03-26 Revised:2012-06-14 Online:2012-09-11 Published:2012-09-11

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摘要： 采用浸渍法制备了在水煤气变换 (WGS) 反应中具有高催化活性的 Ni/γ-Al2O3 催化剂, 使用柠檬酸法合成出高效 CO2 吸收剂 Li2ZrO3 纳米材料. 在固定床微反应器上对 WGS 和吸附强化水煤气变换 (SE-WGS) 反应制氢过程进行了比较研究. 前者只使用 20% Ni/γ-Al2O3 催化剂, 而后者将 20% Ni/γ-Al2O3 催化剂与纳米 Li2ZrO3 吸收剂混合装填. 结果表明, 纳米 Li2ZrO3 具有比已报道的 CO2 吸收剂更快的吸收速率及优异的吸脱附循环稳定性, 可应用于吸附强化过程, 通过原位吸收 WGS 反应产生的 CO2, 使得反应超越化学平衡限制, 直接制得高纯度 H2. 在 823 K, 0.1 MPa 和 H2O/CO = 4 的条件下, 在 SE-WGS 过程一步制得纯度高于 98% 的 H2, 验证了吸附强化反应进程制高纯氢的可行性.

关键词: 制氢, 二氧化碳, 吸收剂, 水煤气变换反应, 锆酸锂

Abstract: Ni/γ-Al2O3 catalyst with high activity in water-gas shift (WGS) reaction was prepared by an impregnation method, and nano-sized Li2ZrO3 absorbent with excellent CO2 capture properties was synthesized by a citrate sol-gel method. Two processes, WGS over 20% Ni/γ-Al2O3 catalyst alone and sorption-enhanced WGS (SE-WGS) over 20% Ni/γ-Al2O3 catalyst admixing with nano-sized Li2ZrO3 absorbent in a fixed-bed microreactor, towards the production of H2 were compared. The nano-sized Li2ZrO3 absorbent shows better CO2 capture properties than other CO2 absorbents reported so far in terms of uptake rate and reusability. Based on these excellent properties, the application of the developed Li2ZrO3 absorbent in sorption-enhanced reaction process (SERP) for the in-situ removal of CO2 produced from WGS leads to the equilibrium shift of the reaction to the production of H2 with high purity. The H2 purity higher than 98% can be achieved by SE-WGS at 823 K, a total pressure of 0.1 MPa, and a H2O/CO molar ratio of 4, demonstrating the concept of SERP for H2 production.

Key words: hydrogen production, carbon dioxide, absorbent, water-gas shift reaction, lithium zirconate