短纤维状FeOOH催化剂的正仲氢催化转化性能OA
Catalytic performance of short-fiberous FeOOH for ortho-para hydrogen conversion
FeOOH作为一种广泛使用的正仲氢转化催化剂,一般采用无机铁盐与无机强碱共沉淀法制备,但该方法存在碱金属阳离子残留量大、材料比表面积难以调控等不足.为解决以上问题,采用有机碱四甲基氢氧化铵(TMAH)替代无机碱NaOH与氯化铁反应制备了FeOOH-T,用于正仲氢催化转化,并通过XRD、N2吸/脱附、HRTEM和ICP等手段对制备的催化剂进行了表征.结果表明,FeOOH-T的比表面积最大可达294 m2/g,其微观粒子呈短纤维状,且晶粒具有弱结晶相态.TMAH用于合成FeOOH可以有效避免碱金属阳离子大量残留,所得产物在洗涤1次的情况下,Na+含量仅为商业催化剂(FeOOH-F)的18%,有利于大幅减少含盐污水的排放.在20 K及氢气流量为2000 mL/min条件下,FeOOH-T、FeOOH-F催化下,装置出口处仲氢物质的量分数分别为92.06%、88.61%,正氢转化率分别为92.22%、88.77%;且在相同转化温度下,随着氢气流量增大,FeOOH-T催化活性下降幅度较小,总体上表现出最优的催化性能.
As a widely used catalyst for ortho-para hydrogen conversion,FeOOH is generally prepared by co-precipitation of inorganic iron salts with inorganic strong bases.However,this method has drawbacks such as large residual amounts of alkali metal cations and difficulty in regulating the specific surface area of the material.To solve these problems,an organic base,tetramethylammonium hydroxide(TMAH),was used to react with ferric chloride instead of NaOH for the preparation of FeOOH-T,which was applied to ortho-para hydrogen catalytic conversion.The catalyst was characterized by series of techniques,including XRD,N2 adsorption/desorption,HRTEM and ICP.The results show that the specific surface area of FeOOH-T can reach a maximum of 294 m2/g,and its microcrystalline grains are short fiber-like with a weakly crystalline phase.Using TMAH for FeOOH synthesis can effectively avoid large residual amount of alkali metal cations.After one-time washing,the Na⁺ content of the product is only 18%of that of commercial catalyst(FeOOH-F),which is conducive to significantly reducing the discharge of salt-containing wastewater.Mole fraction of para-hydrogen at the outlet of the device catalyzed by FeOOH-T and FeOOH-F is 92.06%and 88.61%,and the ortho-hydrogen conversion rate is 92.22%and 88.77%at 20 K and hydrogen flow rate of 2000 mL/min.Additionally,at the same conversion temperature,FeOOH-T shows the smallest decline in catalytic activity with increasing hydrogen flow rate,demonstrating overall optimal catalytic performance.
关瑞彤;杨卫亚;张雁玲;王姝凡;谷明镝;孙京;周明东
沈阳化工大学 化学工程学院,辽宁 沈阳 110142||中石化(大连)石油化工研究院有限公司,辽宁 大连 116045中石化(大连)石油化工研究院有限公司,辽宁 大连 116045中石化(大连)石油化工研究院有限公司,辽宁 大连 116045中石化(大连)石油化工研究院有限公司,辽宁 大连 116045中石化(大连)石油化工研究院有限公司,辽宁 大连 116045沈阳化工大学 化学工程学院,辽宁 沈阳 110142沈阳化工大学 化学工程学院,辽宁 沈阳 110142
化学化工
仲氢正仲氢转化铁基催化剂FeOOH催化活性
para-hydrogenortho-para hydrogen conversioniron-based catalystFeOOHcatalytic activity
《低碳化学与化工》 2026 (3)
97-102,6
中国石化氢能重大专项(122415).
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