Activity Origin of the Nickel Cluster on TiC Support for Nonoxidative Methane Conversion

Harrath, Karim1,2; Yao, Zhen1,2; Jiang, Ya-Fei1,2; Wang, Yang-Gang1,2; Li, Jun1,2,3,4

2023-05-04

10.1021/acs.jpclett.3c00375

JOURNAL OF PHYSICAL CHEMISTRY LETTERS   影响因子和分区

1948-7185

Designing an active and selective catalyst for nonoxidative conversion of methane under mild conditions is critical for natural gas utilization as a chemical feedstock. Here, we demonstrate that the origin of the selective nonoxidative conversion of methane by the titanium carbide supported nickel cluster arises from the formation of a nickel carbide site under the reaction conditions, which could stabilize the CHx intermediate to facilitate the C- C coupling, but further coking is rather limited. The reaction mechanism reveals that the C2 products can be formed via a key -CHx-CH3 intermediate. In addition, we demonstrate that boration of the nickel cluster site can improve the methane conversion toward C2 products. That higher activity and selectivity from the moderate rise in d orbital energy levels can therefore be considered as a descriptor of the catalyst effectiveness. These findings provide an understanding of the dynamic behavior of the single nickel cluster toward methane conversion to C2 products and guidance for their future rational design.

SCI ; EI

英语

NI论文

第一 ; 通讯

NSFC of China["22022504","22033005","92261111"] ; Guangdong Provincial Key Laboratory of Catalysis[2019QN01L353] ; null[2020B121201002]

Chemistry ; Science & Technology - Other Topics ; Materials Science ; Physics

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary ; Physics, Atomic, Molecular & Chemical

WOS:000980733800001

AMER CHEMICAL SOC

20231914060941

Catalyst selectivity ; Methane ; Nickel compounds ; Product design ; Reaction intermediates

Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Inorganic Compounds:804.2 ; Production Engineering:913.1

Web of Science

1.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China
2.Southern Univ Sci & Technol, Guangdong Prov Key Lab Catalysis, Shenzhen 518055, Peoples R China
3.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
4.Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China

Harrath, Karim,Yao, Zhen,Jiang, Ya-Fei,et al. Activity Origin of the Nickel Cluster on TiC Support for Nonoxidative Methane Conversion[J]. JOURNAL OF PHYSICAL CHEMISTRY LETTERS,2023,14(17):4033-4041.

Harrath, Karim,Yao, Zhen,Jiang, Ya-Fei,Wang, Yang-Gang,&Li, Jun.(2023).Activity Origin of the Nickel Cluster on TiC Support for Nonoxidative Methane Conversion.JOURNAL OF PHYSICAL CHEMISTRY LETTERS,14(17),4033-4041.

Harrath, Karim,et al."Activity Origin of the Nickel Cluster on TiC Support for Nonoxidative Methane Conversion".JOURNAL OF PHYSICAL CHEMISTRY LETTERS 14.17(2023):4033-4041.