Cooperative Catalysis by Multiple Active Centers in Nonoxidative Conversion of Methane

Li, Teng-Hao1; Yan, Ming1; Liu, Yuan2,3,4; Huang, Zheng-Qing1; Chang, Chun-Ran1; Li, Jun2,3,4

2020-06-25

10.1021/acs.jpcc.0c01422

Journal of Physical Chemistry C   影响因子和分区

1932-7447

1932-7455

A breakthrough in direct, nonoxidative conversion of methane was accomplished on a silica-confined single-atom iron catalyst (Fe (c) SiO2) in 2014. However, the formation mechanism of the identified active center (FeSiC2 (c) SiO2) remains mysterious and the catalytic reaction mechanism is still under debate. Here, we report a dynamic formation mechanism of FeSiC2 (c) SiO2 starting from FeO3 (c) SiO2 by combining density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations. It is found that FeSiC2 (c) SiO2 is formed under the reaction atmosphere of methane, which undergoes two periods: the removal of oxygen and the insertion of carbon species. The removal of oxygen by generating CO/CO2 is the dominant way, and the insertion of carbon species can be facilely achieved once oxygen is removed. Importantly, during the formation of FeSiC2 (c) SiO2, six other active centers, FeSiO2 (c) SiO2, FeCO2 (c) SiO2, FeSiCO (c) SiO2, FeC2O (c) SiO2, FeSi(CH2)(2)(c) SiO2 and FeSi(CH)(2)(c) SiO2, are revealed, which deliver different and cooperative catalytic behaviors on methane conversion and thus demonstrate a combined gas-phase and surface reaction mechanism.

SCI ; EI

英语

其他

National Natural Science Foundation of China[91645203][21603170] ; China Postdoctoral Science Foundation[2018T111034] ; Fundamental Research Funds for the Central Universities[xtr0218016][cxtd2017004] ; Shaanxi Creative Talents Promotion Plan-Technological Innovation Team[2019TD039] ; Guangdong Provincial Key Laboratory of Catalysis[2020B121201002]

Chemistry ; Science & Technology - Other Topics ; Materials Science

Chemistry, Physical ; Nanoscience & Nanotechnology ; Materials Science, Multidisciplinary

WOS:000545668100016

AMER CHEMICAL SOC

20202908939324

Methane ; Catalysts

Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1

Web of Science

1.Xi An Jiao Tong Univ, Sch Chem Engn & Technol, Shaanxi Key Lab Energy Chem Proc Intensificat, Xian 710049, Peoples R China
2.Tsinghua Univ, Dept Chem, Beijing 100084, Peoples R China
3.Tsinghua Univ, Key Lab Organ Optoelect & Mol Engn, Minist Educ, Beijing 100084, Peoples R China
4.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Li, Teng-Hao,Yan, Ming,Liu, Yuan,et al. Cooperative Catalysis by Multiple Active Centers in Nonoxidative Conversion of Methane[J]. Journal of Physical Chemistry C,2020,124(25):13656-13663.

Li, Teng-Hao,Yan, Ming,Liu, Yuan,Huang, Zheng-Qing,Chang, Chun-Ran,&Li, Jun.(2020).Cooperative Catalysis by Multiple Active Centers in Nonoxidative Conversion of Methane.Journal of Physical Chemistry C,124(25),13656-13663.

Li, Teng-Hao,et al."Cooperative Catalysis by Multiple Active Centers in Nonoxidative Conversion of Methane".Journal of Physical Chemistry C 124.25(2020):13656-13663.