Preparation of palladium-based catalyst by plasma-assisted atomic layer deposition and its applications in CO2 hydrogenation reduction

Shouxian Tang, Di Tian, Zheng Li, Zhengduo Wang, Bowen Liu, jiushan Cheng, Zhongwei Liu
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Abstract

Supported Pd catalyst is an important noble metal material in recent years due to its high catalytic performance in CO2 hydrogenation. An fluidized-bed plasma assisted atomic layer deposition (FP-ALD) process is reported to fabricate Pd nanoparticle catalyst over γ-Al2O3 or Fe2O3/γ-Al2O3 support, using palladium hexafluoroacetylacetonate as the Pd precursor and H2 plasma as counter-reactant. Scanning transmission electron microscopy exhibits that high-density Pd nanoparticles are uniformly dispersed over Fe2O3/γ-Al2O3 support with an average diameter of 4.4 nm. The deposited Pd-Fe2O3/γ-Al2O3 shows excellent catalytic performance for CO2 hydrogenation in a dielectric barrier discharge reactor. Under a typical condition of H2 to CO2 ratio of 4 in the feed gas, the discharge power of 19.6 W, and gas hourly space velocity of 10000 h-1, the conversion of CO2 is as high as 16.3 % with CH3OH and CH4 selectivities of 26.5 % and 3.9 %, respectively.
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等离子体辅助原子层沉积制备钯基催化剂及其在二氧化碳加氢还原中的应用
由于在二氧化碳加氢过程中具有很高的催化性能,负载钯催化剂是近年来一种重要的贵金属材料。本研究采用流化床等离子体辅助原子层沉积(FP-ALD)工艺,以六氟乙酰丙酮钯为钯前驱体,以 H2 等离子体为反应剂,在 γ-Al2O3 或 Fe2O3/γ-Al2O3 载体上制备了钯纳米颗粒催化剂。扫描透射电子显微镜显示,高密度钯纳米粒子均匀地分散在 Fe2O3/γ-Al2O3 载体上,平均直径为 4.4 纳米。沉积的 Pd-Fe2O3/γ-Al2O3 在介质阻挡放电反应器中对 CO2 加氢具有优异的催化性能。在原料气中 H2 与 CO2 的比例为 4、放电功率为 19.6 W、气体时空速度为 10000 h-1 的典型条件下,CO2 的转化率高达 16.3%,CH3OH 和 CH4 的选择性分别为 26.5% 和 3.9%。
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