Journal
ACS CATALYSIS
Volume 9, Issue 10, Pages 9072-9080Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acscatal.9b00968
Keywords
surface spatial confinement; dendritic mesoporous silica; coking resistance; sintering resistance; dry reforming of methane
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Funding
- National Key R&D Program of China [2016YFCO205900]
- National Natural Science Foundation of China [21503106, 21566022, 21773106]
- Natural Science Foundation of Jiangxi Province [20171BCB23016, 20171BAB203024, 20181BCD4004]
- Foundation of State Key Laboratory of High -efficiency Utilization of Coal and Green Chemical Engineering [2018-K04]
- U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
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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 degrees C). More importantly, the prepared catalyst remained stable after 145 h time-on-stream at 700 degrees 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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