Carbon-Boosted and Nitrogen-Stabilized Isolated Single-Atom Sites for Direct Dehydrogenation of Lower Alkanes

Li, Yang1,2; Xu, Cong-Qiao3; Chen, Chen1; Zhang, Yu1; Liu, Shoujie1; Zhuang, Zewen1; Zhang, Yaoyuan4; Zhang, Qiyang4; Li, Zhi1; Chen, Zheng1; Zheng, Lirong5; Cheong, Weng-Chon1; Wu, Konglin1; Jiang, Guiyuan4; Xiao, Hai1; Lian, Chao2; Wang, Dingsheng1; Peng, Qing1; Li, Jun1,3; Li, Yadong1

2024-07-01

10.1021/jacs.4c03048

JOURNAL OF THE AMERICAN CHEMICAL SOCIETY   影响因子和分区

0002-7863

1520-5126

Lower olefins are widely used in the chemical industry as basic carbon-based feedstocks. Here, we report the catalytic system featuring isolated single-atom sites of iridium (Ir-1) that can function within the entire temperature range of 300-600 degrees C and transform alkanes with conversions close to thermodynamics-dictated levels. The high turnover frequency values of the Ir-1 system are comparable to those of homogeneous catalytic reactions. Experimental data and theoretical calculations both indicate that Ir-1 is the primary catalytic site, while the coordinating C and N atoms help to enhance the activity and stability, respectively; all three kinds of elements cooperatively contribute to the high performance of this novel active site. We have further immobilized this catalyst on particulate Al2O3, and we found that the resulting composite system under mimicked industrial conditions could still give high catalytic performances; in addition, we have also developed and established a new scheme of periodical in situ regeneration specifically for this composite particulate catalyst.

SCI ; EI

英语

通讯

National Key R&D Program of China["2018YFA0702003","2021YFF0500503","2023YFA1506600","2022YFA1503900"] ; National Natural Science Foundation of China["21925202","U22B2071","22033005","22103035"] ; Fundamental Research Center of Single-Atom Catalysis by the National Natural Science Foundation of China[22388102] ; Yunnan Provincial Science and Technology Project at Southwest United Graduate School[202302AO370017] ; Shenzhen Science and Technology Program[RCYX20231211090357078] ; NSFC Center for Single-Atom Catalysis[22388102]

Chemistry

Chemistry, Multidisciplinary

WOS:001273640200001

AMER CHEMICAL SOC

20243016741933

Alumina ; Aluminum oxide ; Atoms ; Carbon ; Catalysis ; Catalysts ; Chemical industry ; Nitrogen ; Thermodynamics

Thermodynamics:641.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Inorganic Compounds:804.2 ; Chemical Engineering, General:805 ; Atomic and Molecular Physics:931.3

Web of Science

1.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
2.Beijing Single Atom Catalysis Technol Co Ltd, Beijing 100094, Peoples R China
3.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
4.China Univ Petr, State Key Lab Heavy Oil Proc, Beijing 102249, Peoples R China
5.Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil, Beijing 100049, Peoples R China

Li, Yang,Xu, Cong-Qiao,Chen, Chen,et al. Carbon-Boosted and Nitrogen-Stabilized Isolated Single-Atom Sites for Direct Dehydrogenation of Lower Alkanes[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2024,146:20668-20677.

Li, Yang.,Xu, Cong-Qiao.,Chen, Chen.,Zhang, Yu.,Liu, Shoujie.,...&Li, Yadong.(2024).Carbon-Boosted and Nitrogen-Stabilized Isolated Single-Atom Sites for Direct Dehydrogenation of Lower Alkanes.JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,146,20668-20677.

Li, Yang,et al."Carbon-Boosted and Nitrogen-Stabilized Isolated Single-Atom Sites for Direct Dehydrogenation of Lower Alkanes".JOURNAL OF THE AMERICAN CHEMICAL SOCIETY 146(2024):20668-20677.