NiAlNd catalysts for CO2 methanation derived from the layered double hydroxide precursor
Jinglin CHENG, Xiaoming GUO, Tao MENG, Xu HU, Liang LI, Yanzhe WANG, Wenzhu HUANG
【无机化学学报】doi: 10.11862/CJIC.20240152
The glycol solvent -thermal method prepared a serial of NiAlNd catalysts based on layered double hydrox-ides (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+ hin-dered 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.
关键词: CO2 methanation, layered double hydroxide, NiAl catalyst, neodymium, active site
ZSM-5分子筛中铝分布与孔结构协同催化生物乙醇制丙烯
茹薏, 孟涛, 薛招腾, 毛东森
【无机化学学报】doi: 10.11862/CJIC.20250255
采用水热法成功将镁(Mg)引入ZSM-5分子筛骨架结构中,系统考察了Mg含量对分子筛孔的结构、酸性质、骨架铝(framework aluminum,AlF)分布及催化生物乙醇制丙烯(bioethanol to propylene,ETP)反应性能的影响。结果表明,随着Mg含量的增加,分子筛介孔体积显著增大,结晶度略有下降。氨气程序升温脱附(NH3-TPD)和吡啶红外(Py-IR)分析结果显示,Mg的引入有效降低了分子筛总酸量和强酸强度,同时提高了Brønsted酸的比例。固体核磁共振(27Al MAS NMR)和紫外可见漫反射光谱(UV-Vis DRS)表明,Mg的引入促使AlF从通道交叉处向正弦或直通道迁移,并减少了铝对(aluminum pair,Alpair)的形成。催化反应评价结果显示,适量Mg改性的分子筛(2-MgHZ5)表现出最优的ETP性能,丙烯选择性从改性前的ZSM-5(HZ5)的26.8%提高至29.5%,丙烯选择性维持在不低于10%的时间更是从HZ5的15 h显著延长至30 h,这归因于其适中的酸强度、丰富的介孔结构以及Al分布的优化有效抑制了芳烃循环和积碳生成,促进了烯烃-环戊二烯循环路径。
关键词: ZSM-5分子筛, 杂原子镁, 酸性质, 铝分布, 生物乙醇制丙烯

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