Sr-Promoted Co/CN Catalyst with Enhanced Oxygen Vacancy and Carbon Removal Capability for Pressurized Dry Reforming of Methane
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更新:2026-08-30 21:35:42 浏览:1次
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摘要
Rapid catalyst deactivation caused by severe coking and active-phase reconstruction fundamentally hinders the application of high-pressure dry reforming of methane (DRM). To address this challenge, we developed a robust strontium-promoted, defect-rich N-doped carbon-supported cobalt catalyst (Co-Sr/CN). The catalysts were systematically evaluated under variable-pressure conditions (0.5-1.4 MPa) and a rigorous high-pressure "ultimate lifetime test" (780 oC, 1.1 MPa), combined with surface and in-situ mechanistic characterizations. The optimized Co-3Sr/CN catalyst significantly shortened the reaction induction period, achieving stable CH4 and CO2 conversions of 75.5% and 84.8%, respectively, at 0.5 MPa. Mechanistic studies, including in-situ DRIFTS and CO2-TPSR, revealed that Sr promotion enriches oxygen-vacancy sites and strengthens the surface oxygen cycle, thereby accelerating intermediate CO2 activation and oxygen-assisted carbon removal. Consequently, Co-3Sr/CN extended the high-pressure lifetime to 1046 h, vastly outperforming the unpromoted Co/C catalyst (482 h). However, post-reaction analyses revealed that both catalysts ultimately succumbed to catastrophic coking and aggregation. These findings demonstrate that while Sr-mediated oxygen cycles effectively delay deactivation, runaway carbon accumulation dictates late-stage failure in pressurized DRM, providing crucial insights for future industrial catalyst design.
关键词
Pressurized dry reforming of methane; Surface oxygen cycling; Extreme lifetime evaluation; Coking
稿件作者
Kai-Rui Luan
China University of Mining & Technology
Wen Tang
Huangshan University
Jing-Pei Cao
China University of Mining and Technology
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