基于层状双氢氧化物前驱体的CO2甲烷化NiAlNd催化剂 |
NiAlNd catalysts for CO2 methanation derived from the layered double hydroxide precursor |
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摘要: 采用乙二醇溶剂热法合成了一系列基于层状双氢氧化物前驱体(LDHs)的NiAlNd催化剂。Nd的引入大大提高了CO2甲烷化的低温催化活性。在 T=210 ℃,WHSV(weight hourly space velocity)=24 000 mL·g-1·h-1,p=100 kPa的条件下,NiAlNd-0.4催化剂上CO2转化率达到83.9%。Nd3+取代部分Al3+阻碍了前驱体中LDHs结构的形成,同时也减小了焙烧后催化剂的粒径。Nd的加入削弱了NiO与Al2O3之间的相互作用,促进了NiO的还原,提高了Ni的本征活性。此外,Nd的添加提高了催化剂表面碱性位的数目,从而增强了对CO2的吸附。随着Nd掺杂量的增加,还原后的催化剂中金属Ni的表面积呈火山形变化。Ni活性位的数目和本征活性同时影响NiAlNd催化剂的催化活性。 |
关键词: CO2甲烷化 层状双氢氧化物 NiAl催化剂 Nd 活性位 |
基金项目: 上海科促会联盟计划项目(No.LM201848)和上海应用技术大学协同创新基金(No.XTCX2023-04)资助。 |
Abstract: The glycol solvent-thermal method prepared a serial of NiAlNd catalysts based on layered double hydroxides (LDHs) precursor. The introduction of Nd greatly promoted the catalytic activity for CO2 methanation at low temperatures. The CO2 conversion on the NiAlNd 0.4 catalyst reached 83.9% under the reaction condition: T= 210 ℃, WHSV (weight hourly space velocity)=24 000 mL·g-1·h-1, p=100 kPa. The substitution of Nd3+ for Al3+ hindered the formation of LDHs structure in the precursor but decreased the particle size of the calcined catalyst. The interaction between NiO and Al2O3 was weakened with the introduction of Nd, resulting in better NiO component reducibility and high intrinsic activity of the Ni site. Moreover, the presence of Nd increased the number of surface basic sites of the catalyst, thus increasing the adsorption of CO2. With the increase in Nd, the surface area of metallic Ni in the reduced catalyst takes on a volcano-shape variation trend. The catalytic activities of NiAlNd catalysts are affected by the number and intrinsic activity of Ni sites simultaneously. |
Keywords: CO2 methanation layered double hydroxide NiAl catalyst neodymium active site |
投稿时间:2024-05-02 修订日期:2024-07-11 |
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程菁琳,郭晓明,孟涛,胡旭,李亮,王彦哲,黄文珠.基于层状双氢氧化物前驱体的CO2甲烷化NiAlNd催化剂[J].无机化学学报,2024,40(8):1592-1602. |
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