纳米Li_2ZrO_3吸收剂原位移除CO_2强化水煤气变换反应制氢  

Li_2ZrO_3 Nanoparticles as Absorbent for in-Situ Removal of CO_2 in Water-Gas Shift Reaction to Enhance H_2 Production

作　　者：张元卓[1] 于兹瀛[1] 张富民[1] 肖强[1] 钟依均[1] 朱伟东[1] 

机构地区：[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

出　　处：《催化学报》2012年第9期1572-1577,共6页

基　　金：国家自然科学基金重点项目(21036006);国家重点基础研究发展计划(973计划)前期专项(2009CB626607);教育部“长江学者和创新团队发展计划”创新团队(IRT0980);浙江省自然科学基金杰出青年团队项目(R4080084)~~

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823K,0.1MPa和H2O/CO=4的条件下,在SE-WGS过程一步制得纯度高于98%的H,验证了吸附强化反应进程制高纯氢的可行性.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 LizZrO3 absor- bent 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 applica- tion 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 H20/CO molar ratio of 4, demonstrating the concept of SERP for H2 production.

关 键 词：制氢 二氧化碳 吸收剂 水煤气变换反应 锆酸锂 

分 类 号：O643.36[理学—物理化学]