Lattice-embedded Ni single-atom catalyst on porous Al2O3 nanosheets derived from Ni-doped carbon dots for efficient propane dehydrogenation

被引:5
|
作者
Ma, Rui [1 ]
Dean, David P. [2 ]
Gao, Junxian [2 ]
Wang, Mingshan [1 ]
Liu, Yuan [1 ]
Liang, Kaijun [1 ]
Wang, Junbo [1 ]
Miller, Jeffrey T. [2 ]
Zhou, Bo [1 ]
Zou, Guojun [1 ]
Kou, Jiajing [3 ]
机构
[1] Guangdong Lab Chem & Chem Engn, Shantou 515031, Peoples R China
[2] Purdue Univ, Davidson Sch Chem Engn, 480 Stadium Mall Dr, W Lafayette, IN 47907 USA
[3] Yanshan Univ, Sch Vehicles & Energy, Qinhuangdao 066000, Peoples R China
来源
APPLIED CATALYSIS B-ENVIRONMENT AND ENERGY | 2024年 / 347卷
基金
美国国家科学基金会;
关键词
Propane dehydrogenation; Single-atom catalysts; Metal doped carbon dots; Alumina; Thermal stability; LIGHT ALKANE DEHYDROGENATION; TOTAL-ENERGY CALCULATIONS; DEACTIVATION; GAMMA-AL2O3; ACTIVATION; KINETICS; ALUMINA; POINTS; METALS; DESIGN;
D O I
10.1016/j.apcatb.2024.123798
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 controlled synthesis of highly durable single-atom catalysts (SACs) for high-temperature applications remains a great challenge. Herein, we develop a facile strategy to construct Al2O3 lattice-embedded Ni SAC via thermal treatment of aluminum oxide encapsulated Ni-doped carbon dots (Ni-CDs@Al2O3). Detailed studies reveal that the Ni atoms are released from carbon matrix and simultaneously captured by cation defects formed in situ within a phase transformation of aluminum oxide. Al2O3 stabilized Ni atoms via Ni-O-4 coordination are well illustrated by combined characterizations. For propane dehydrogenation, reactivity measurements show that the center of Ni-O ion pairs effectively activates C3H8 and the higher rate of C3H6 formation on Ni SAs than Ni NPs, by a factor of 12, is the result of inhibition of C-C bond cleavage involving side reactions, as identified by density functional calculations. Beyond that, this lattice-embedded Ni SAC exhibits superior stability and recyclability in long-term operation with little coke accumulation.
引用
收藏
页数:10
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