Jun-Zhi Wu, Caimei Miao, Fenfang Mu, Xiaoyan Wang, J. Bai, Hong Wang
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引用次数: 0
摘要
在保持高催化活性的前提下提高抗积碳和抗烧结能力是镍基催化剂在CO甲烷化反应中应用的核心问题。为了解决这一问题,采用柠檬酸络合法制备了La0.75A0.25NiO3/SiO2 (a = Ce, Sr, Sm, Ca)催化剂。XRD结果表明,取代元素(Sr、Sm和Ca)进入LaNiO3晶格,部分取代了a位元素La。还原后的Ni0有利于提高催化剂的中温活性。不同元素的取代会产生不同的电子效应,显著影响Ni颗粒的尺寸以及Ni与La2O3的相互作用。掺杂Ca2+作为a位取代元素的催化剂由于晶格畸变容易产生氧空位,表现出更好的氧吸附、储存和迁移能力。掺杂Sr、Sm、Ca作为a位取代元素的催化剂在反应后产生La2O2CO3,起到消除积碳的作用。
Structure–activity relationship of an A-site-doped LaNiO3/SiO2 catalyst
Improving the anti-carbon deposition and anti-sintering ability under the premise of maintaining high catalytic activity is the core issue of Ni-based catalysts applied in CO methanation reactions. To address this issue, a La0.75A0.25NiO3/SiO2 (A = Ce, Sr, Sm, and Ca) catalyst is prepared via a citric acid complexation method. XRD results show that the substituted elements (Sr, Sm, and Ca) enter the LaNiO3 lattice and partially replace the A-site element La. The reduced Ni0 is beneficial to improve the medium temperature activity of the catalyst. The substitution of different elements produces different electronic effects that significantly affect the size of the Ni particles and the interaction between Ni and La2O3. The catalyst with doped Ca2+ as the A-site substituted element demonstrates better adsorption, storage, and migration capabilities for oxygen due to the lattice distortion that easily produces oxygen vacancies. Catalysts doped with Sr, Sm, and Ca as the A-site substituted element produce La2O2CO3 after the reactions, which plays a role in eliminating carbon deposits.
期刊介绍:
The Journal of Chemical Research is a peer reviewed journal that publishes full-length review and research papers in all branches of experimental chemistry. The journal fills a niche by also publishing short papers, a format which favours particular types of work, e.g. the scope of new reagents or methodology, and the elucidation of the structure of novel compounds. Though welcome, short papers should not result in fragmentation of publication, they should describe a completed piece of work. The Journal is not intended as a vehicle for preliminary publications. The work must meet all the normal criteria for acceptance as regards scientific standards. Papers that contain extensive biological results or material relating to other areas of science may be diverted to more appropriate specialist journals. Areas of coverage include: Organic Chemistry; Inorganic Chemistry; Materials Chemistry; Crystallography; Computational Chemistry.