Synergistic effect of coordinating interface and promoter for enhancing ammonia synthesis activity of Ru@N-C catalyst

被引:1
|
作者
Wang, Dongwei [1 ,2 ]
Ma, Zhanwei [1 ]
Gou, Farong [1 ]
Hu, Bin [1 ]
机构
[1] Chinese Acad Sci, Lanzhou Inst Chem Phys, State Key Lab Oxo Synth & Select Oxidat, Lanzhou 730000, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
基金
中国国家自然科学基金;
关键词
RUTHENIUM CATALYSTS; NITROGEN; METAL; SENSITIVITY; ACTIVATION; REDUCTION; SUPPORT;
D O I
10.1039/d3ra04824a
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Triruthenium dodecacarbonyl (Ru3(CO)12) was applied to prepare the Ru-based ammonia synthesis catalysts. The catalyst obtained from this precursor exhibited higher activity than the other Ru salts owing to its unique atomic reorganization under mild temperatures. Herein, Ru3(CO)12 as a guest metal source incorporated into the pore of ZIF-8 formed the Ru@N-C catalysts. The results indicated that the Ru nanoparticle (1.7 nm) was dispersed in the confined N coordination environment, which can increase the electron density of the Ru nanoparticles to promote N0000000000000000000000000000000000000000000000000000111111111111111000000000000000000011111111111111100000000000000000001111111111111110000000000000000000000000000000000000000000000000000N bond cleavage. The promoters donate the basic sites for transferring the electrons to Ru nanoparticles, further enhancing ammonia synthesis activity. Ammonia synthesis investigations revealed that the obtained Ru@N-C catalysts exhibited obvious catalytic activity compared with the Ru/AC catalyst. After introducing the Ba promoter, the 2Ba-Ru@N-C(450) catalyst exhibited the highest ammonia synthesis activity among the catalysts. At 360 & DEG;C and 1 MPa, the activity of the 2Ba-Ru@N-C(450) is 16 817.3 & mu;mol h-1 gRu-1, which is 1.1, 1.6, and 2 times higher than those of 2Cs-Ru@N-C(450) (14 925.4 & mu;mol h-1 gRu-1), 2K-Ru@N-C(450) (10 736.7 & mu;mol h-1 gRu-1), and Ru@N-C(450) (8604.2 & mu;mol h-1 gRu-1), respectively. A series of characterizations were carried out to explore the 2Ba-Ru@N-C(450) catalysts, such as H2-TPR, XPS, and NH3-TPD. These results suggest that the Ba promoter played the role of an electronic and structural promoter; moreover, it can promote the NH3 desorption from the Ru nanoparticles. Ru3(CO)12, as a guest metal source, was incorporated into the pores of ZIF-8 to form the Ru@N-C catalysts. The Ba promoter acted as an electronic and structural promoter; it can also promote NH3 desorption from Ru nanoparticles.
引用
收藏
页码:28736 / 28742
页数:7
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