Investigation of the promotion effect of metal oxides on the water-gas shift reaction activity over Pt-MOx/CeO2 catalysts for aqueous phase reforming

Q3 Energy 燃料化学学报 Pub Date : 2023-12-01 DOI:10.1016/S1872-5813(23)60363-9

Wei-jie ZHANG , Zhi-peng TIAN , Jia-hao HUANG , Jun-yao WANG , Xiang-long LUO , Chao WANG , Ri-yang SHU , Jian-ping LIU , Ying CHEN

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Abstract

Aqueous phase reforming (APR) of methanol is a potential pathway for the effective hydrogen production under relatively mild conditions. The Pt/CeO₂ and a series of Pt-MO_x/CeO₂ (M = Fe, Cr, Mg, Mn) catalysts were prepared by sequential impregnation method and their APR reaction performances were studied. The catalyst properties including valence state of the promoters, the amount of oxygen vacancies, the metal distributions, the adsorption properties of CO and the acidity/basicity of catalysts were characterized and analyzed by XPS, XRD, TEM, CO-TPD, NH₃-TPD, CO₂-TPD, etc. It was found that the addition of MO_x weakened the Pt-CeO₂ interaction and promoted the generation of Pt^δ+ species with lower valence state, which contribute to the C–H bond cleavage and facilitate methanol conversion. The highest hydrogen production (164.78 mmol) and relatively low CO and CH₄ selectivities were obtained over the Pt-MgO/CeO₂, while the highest CH₄ selectivity was obtained over the Pt-CrO_x/CeO₂ (2.21%). Over the Pt/CeO₂ and Pt-MO_x/CeO₂ (M = Fe, Cr, Mg, Mn) catalysts, CO₂/CH₄ ratio correlated well with the catalyst basicity, indicating that the basicity promotes the dissociation adsorption of H₂O as well as the water-gas shift (WGS) reaction activity and decreases the methanation activity.

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金属氧化物对用于水相转化的 Pt-MOx/CeO2 催化剂上水气转化反应活性的促进作用研究

甲醇水相重整（APR）是在相对温和的条件下有效制氢的潜在途径。通过顺序浸渍法制备了 Pt/CeO2 和一系列 Pt-MOx/CeO2（M = Fe、Cr、Mg、Mn）催化剂，并研究了它们的 APR 反应性能。通过 XPS、XRD、TEM、CO-TPD、NH3-TPD、CO2-TPD 等方法表征和分析了催化剂的性质，包括促进剂的价态、氧空位量、金属分布、对 CO 的吸附性以及催化剂的酸碱性。研究发现，MOx 的加入削弱了 Pt-CeO2 的相互作用，促进了价态较低的 Ptδ+ 物种的生成，从而有助于 C-H 键的裂解，促进甲醇的转化。Pt-MgO/CeO2 的产氢量最高（164.78 mmol），CO 和 CH4 选择性相对较低，而 Pt-CrOx/CeO2 的 CH4 选择性最高（2.21%）。在 Pt/CeO2 和 Pt-MOx/CeO2（M = Fe、Cr、Mg、Mn）催化剂上，CO2/CH4 比率与催化剂碱性有很好的相关性，这表明碱性会促进 H2O 的解离吸附以及水气变换（WGS）反应活性，降低甲烷化活性。

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来源期刊

燃料化学学报 Chemical Engineering-Chemical Engineering (all)

CiteScore

2.80

自引率

0.00%

发文量

5825

期刊介绍： Journal of Fuel Chemistry and Technology (Ranliao Huaxue Xuebao) is a Chinese Academy of Sciences(CAS) journal started in 1956, sponsored by the Chinese Chemical Society and the Institute of Coal Chemistry, Chinese Academy of Sciences(CAS). The journal is published bimonthly by Science Press in China and widely distributed in about 20 countries. Journal of Fuel Chemistry and Technology publishes reports of both basic and applied research in the chemistry and chemical engineering of many energy sources, including that involved in the nature, processing and utilization of coal, petroleum, oil shale, natural gas, biomass and synfuels, as well as related subjects of increasing interest such as C1 chemistry, pollutions control and new catalytic materials. Types of publications include original research articles, short communications, research notes and reviews. Both domestic and international contributors are welcome. Manuscripts written in Chinese or English will be accepted. Additional English titles, abstracts and key words should be included in Chinese manuscripts. All manuscripts are subject to critical review by the editorial committee, which is composed of about 10 foreign and 50 Chinese experts in fuel science. Journal of Fuel Chemistry and Technology has been a source of primary research work in fuel chemistry as a Chinese core scientific periodical.