Zirconium Carbide Mediates Coke-Resistant Methane Dry Reforming on Nickel-Zirconium Catalysts

被引:20
|
作者
Haug, Leander [1 ]
Thurner, Christoph [1 ]
Bekheet, Maged F. [2 ]
Bischoff, Benjamin [2 ]
Gurlo, Aleksander [2 ]
Kunz, Martin [3 ]
Sartory, Bernhard [4 ]
Penner, Simon [1 ]
Kloetzer, Bernhard [1 ]
机构
[1] Univ Innsbruck, Inst Phys Chem, Innrain 52 C, A-6020 Innsbruck, Austria
[2] Tech Univ Berlin, Inst Werkstoffwissensch & Technol, Fachgebiet Keram Werkstoffe, Str 17 Juni 135, D-10623 Berlin, Germany
[3] Lawrence Berkeley Natl Lab, Adv Light Source, Berkeley, CA 94720 USA
[4] Mat Ctr Leoben Forsch GmbH, Roseggerstr 12, A-8700 Leoben, Austria
关键词
Carbon Spillover; Methane Dry Reforming; Near Ambient Pressure XPS; NiZr Intermetallic Catalyst; Zirconium Carbide; SYNTHESIS GAS; CARBON; STEAM; MECHANISM; DYNAMICS; COKING; GROWTH;
D O I
10.1002/anie.202213249
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Graphitic deposits anti-segregate into Ni-0 nanoparticles to provide restored CH4 adsorption sites and near-surface/dissolved C atoms, which migrate to the Ni-0/ZrO2 interface and induce local ZrxCy formation. The resulting oxygen-deficient carbidic phase boundary sites assist in the kinetically enhanced CO2 activation toward CO(g). This interface carbide mechanism allows for enhanced spillover of carbon to the ZrO2 support, and represents an alternative catalyst regeneration pathway with respect to the reverse oxygen spillover on Ni-CeZrxOy catalysts. It is therefore rather likely on supports with limited oxygen storage/exchange kinetics but significant carbothermal reducibility.
引用
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页数:7
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