Interface engineering of Ni and CeO2 catalysts for ethane dry reforming

被引:1
作者
Chen, Xinglong [1 ,2 ]
Li, Shuqing [1 ]
Xu, Zhenchao [1 ,2 ]
Li, Hongyu [3 ]
Li, Jiong [4 ]
Fu, Yu [1 ,2 ]
Zhang, Jun [1 ,2 ]
机构
[1] Chinese Acad Sci, CAS Key Lab Low Carbon Convers Sci & Engn, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Gaolu Air Prod & Chem Shanghai Energy Technol Co L, Shanghai 201620, Peoples R China
[4] Chinese Acad Sci, Shanghai Synchrotron Radiat Facil, Shanghai Adv Res Inst, Shanghai 201210, Peoples R China
基金
中国国家自然科学基金;
关键词
Dry reforming of ethane; Ni-O-Ce interface; Dual active site; Mars-van krevelen mechanism; Ni-Si@Ce; METHANE; CO2; DEHYDROGENATION; RESISTANCE; REDUCTION;
D O I
10.1016/j.ijhydene.2025.01.288
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The dry reforming of ethane (DRE) provides an efficient route for converting CO2 into syngas. Ni-based catalysts are highly regarded for their activity and cost-effectiveness; however, issues such as metal sintering and carbon deposition remain significant challenges. In this study, we developed a shell-structured Ni-Si@Ce catalyst for DRE, aimed at enhancing catalytic activity and stability by optimizing Ni-O-Ce interfaces. Comprehensive characterization using XRD, XPS, EXAFS, and H-2-TPR revealed the geometric and electronic structures of the catalyst, while TEM confirmed the confinement of similar to 4 nm Ni particles between the SiO2 core and CeO2 shell. Performance evaluation demonstrated C2H6 and CO2 conversion rates of 70% and 71% at 650 degrees C and 24,000 mL<middle dot>h(-1)g(cat) (-1), with minimal carbon deposition and excellent stability over 24 h of reaction. The activation energies for C2H6 and CO2 activation were determined to be 120.9 and 105.5 kJ/mol, respectively. A dual active site mechanism is proposed, where the CeO2 shell provides spatial confinement of Ni particles, suppresses carbon deposition, and facilitates the activation of C2H6 and CO2 via the Mars-van Krevelen mechanism, thereby enhancing catalytic performance and addressing competitive adsorption challenges.
引用
收藏
页码:501 / 512
页数:12
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