Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions

IF 6.4 3区 环境科学与生态学 Q2 ENERGY & FUELS
Xiao Fan , Kaiying Wang , Xiaoqing He , Shiguang Li , Miao Yu , Xinhua Liang
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引用次数: 1

Abstract

A series of palladium-modified (Pd-modified) CuO-ZnO-Al2O3 (CZA) catalysts with various Pd loadings (0.3 wt% to 2.4 wt%) were prepared using the wetness impregnation method, on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydrotalcite-like phases (CZA-zH), and CuO-ZnO-Al2O3 metal oxide nanoparticles (CZA-MO). Enhancement on catalytic activity can be observed on both Pd-modified CZA catalysts in a temperature range of 180–240 °C for methanol synthesis via CO2 hydrogenation. Pd/CZA-zH catalysts exhibited a more efficient and stable production of methanol at a relatively low reaction temperature of 180 °C for 100 hrs of reaction. The improvement of activity is mainly ascribed to a higher surface area and abundant oxygen-containing functional groups (e.g., –OH) of CZA-zH support, which is beneficial for better adsorption and distribution of Pd promoter. Hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy results demonstrated a better interaction between Pd and Cu on Pd/CZA-zH catalysts via enhanced reducibility of CuO, and peak shift of Cu to a lower binding energy. The difference in the efficient utilization of hydrogen spillover effect of Pd promoter over two CZA supports resulted in the different performances for methanol synthesis under mild reaction conditions.

Abstract Image

含混相前驱体钯改性CuO-ZnO-Al2O3催化剂温和条件下CO2加氢合成甲醇
采用湿浸渍法制备了钯改性(Pd改性)CuO-ZnO-Al2O3 (CZA)催化剂,催化剂的Pd负载量在0.3 wt% ~ 2.4 wt%之间。CZA载体为两种不同结构的CZA载体,分别是由锌-孔雀石和类水滑石相混合组成的CZA- zh前驱体和CuO-ZnO-Al2O3金属氧化物纳米颗粒(CZA- mo)。在180 ~ 240℃的温度范围内,pd修饰的CZA催化剂对CO2加氢合成甲醇的催化活性均有增强。Pd/CZA-zH催化剂在180℃的较低反应温度下,反应时间为100小时,制备甲醇的效率更高、更稳定。活性的提高主要是由于CZA-zH载体具有更高的表面积和丰富的含氧官能团(如-OH),有利于Pd促进剂更好的吸附和分布。氢温度程序还原和x射线光电子能谱结果表明,Pd和Cu在Pd/CZA-zH催化剂上通过增强CuO的还原性和Cu的峰移到更低的结合能而更好地相互作用。钯促进剂在两种CZA载体上的氢溢出效应利用率不同,导致两种CZA载体在温和反应条件下的甲醇合成性能不同。
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来源期刊
Carbon Resources Conversion
Carbon Resources Conversion Materials Science-Materials Science (miscellaneous)
CiteScore
9.90
自引率
11.70%
发文量
36
审稿时长
10 weeks
期刊介绍: Carbon Resources Conversion (CRC) publishes fundamental studies and industrial developments regarding relevant technologies aiming for the clean, efficient, value-added, and low-carbon utilization of carbon-containing resources as fuel for energy and as feedstock for materials or chemicals from, for example, fossil fuels, biomass, syngas, CO2, hydrocarbons, and organic wastes via physical, thermal, chemical, biological, and other technical methods. CRC also publishes scientific and engineering studies on resource characterization and pretreatment, carbon material innovation and production, clean technologies related to carbon resource conversion and utilization, and various process-supporting technologies, including on-line or off-line measurement and monitoring, modeling, simulations focused on safe and efficient process operation and control, and process and equipment optimization.
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