Catalysts in Coronas: A Surface Spatial Confinement Strategy for High-Performance Catalysts in Methane Dry Reforming

Peng, Honggen; Zhang, Xianhua; Han, Xue; You, Xiaojuan; Lin, Sixue; Chen, Hao; Liu, Wenming; Wang, Xiang; Zhang, Ning; Wang, Zheng; Wu, Peng; Zhu, Huiyuan; Dai, Sheng

doi:10.1021/acscatal.9b00968

Title: Catalysts in Coronas: A Surface Spatial Confinement Strategy for High-Performance Catalysts in Methane Dry Reforming

Journal Article · Fri Jun 21 00:00:00 EDT 2019 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.9b00968· OSTI ID:1785619

^[1]; Zhang, Xianhua ^[2]; Han, Xue ^[3]; You, Xiaojuan ^[2]; Lin, Sixue ^[2];

^[4]; Liu, Wenming ^[2];

^[2]; Zhang, Ning ^[2]; Wang, Zheng ^[5];

^[6];

^[7];

^[7]

Nanchang Univ., Jiangxi (China). College of Chemistry. Key Lab. of Jaingxi Province for Environment and Energy Catalysis; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division
Nanchang Univ., Jiangxi (China). College of Chemistry. Key Lab. of Jaingxi Province for Environment and Energy Catalysis
Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemical Engineering
Univ. of Tennessee, Knoxville, TN (United States). Dept. of Chemistry
Ningxia Univ., Yinchuan (China). State Key Lab. of High-efficiency Utilization of Coal & Green Chemical Engineering
East China Normal Univ., Shanghai (China). Dept. of Chemistry and Molecular Engineering. Shanghai Key Lab. of Green Chemistry and Chemical Processes
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Sciences Division; Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States). Dept. of Chemical Engineering

One of the grand challenges in industrial catalytic processes is the inevitable sintering and aggregation of conventional supported catalysts to large particles, leading to the decrease of activity and even deactivation with time. Herein, a surface spatial confinement strategy was employed to design high-performing catalysts for the dry reforming of methane (DRM). Specifically, active nickel (Ni) nanoparticles (NPs) were confined on the surface of a dendritic mesoporous silica (DMS) in the form of the “catalysts in coronas”. The Ni/DMS catalyst exhibited a high catalytic performance close to its equilibrium conversion (76% conversion for CH4 at 700 °C). More importantly, the prepared catalyst remained stable after 145 h time-on-stream at 700 °C without noticeable carbon deposition. This sintering and coking resistance was found to arise from the surface spatial confinement effect in which the three-dimensional dendritic layers in the corona posted a steric barrier against migration and aggregation of Ni NPs and size of Ni NPs was controlled below 5 nm, hence against sintering and coking. Meanwhile, the mesoporous feature of the layered wall facilitated mass transport of reactants to Ni species and further boosted catalysis. This strategy should be broadly applicable to a range of metal- and metal oxide-supported catalysts in high-temperature heterogeneous reactions, such as DRM, water gas shift reaction, and vehicle emission control related reactions.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

DOE Contract Number:: AC05-00OR22725; 2016YFC0205900; 21773106; 21566022; 21503106; 20181BCD4004; 20171BCB23016; 20171BAB203024; 2018-K04

OSTI ID:: 1785619

Journal Information:: ACS Catalysis, Vol. 9, Issue 10; ISSN 2155-5435

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
surface spatial confinement
dendritic mesoporous silica
coking resistance
sintering resistance
dry reforming of methane

Title: Catalysts in Coronas: A Surface Spatial Confinement Strategy for High-Performance Catalysts in Methane Dry Reforming

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