Direct CH₄ to CH₃OH conversion is a long-standing grand challenge in catalysis. We present one-step steam reforming of methane to methanol (OSRMtM) by combining an atmospheric pressure CH₄/H₂O/Ar plasma with a Cu/Mordenite (Cu/MOR) catalyst at 170°C, achieving 77% CH₃OH selectivity with 3.0% CH₄ conversion. Catalyst characterization and plasma diagnostics, as well as D₂O and H₂¹⁸O-labeled isotope tracer experiments reveal that the excellent reaction performance is attributed to Cu-O active sites confined by MOR zeolite. During plasma-catalytic OSRMtM, both CH₄ and H₂O are activated in the plasma and dissociated to produce radicals (CH₃, OH, and H). These radicals drive the redox process between Cu²⁺ and Cu⁺, playing an important role in plasma-catalytic OSRMtM. Although a gradual reduction of Cu²⁺ to Cu⁺ leads to slow deactivation, the catalytic performance can be completely recovered through simple calcination, which enables a continuous plasma-catalytic OSRMtM process using a fluidized-bed reactor.

中文翻译：

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甲烷等离子体催化一步蒸汽重整制甲醇：揭示铜/丝光沸石的催化循环


CH ₄直接转化为CH ₃ OH 是催化领域长期存在的巨大挑战。我们提出了通过在 170°C 下将常压 CH ₄ /H ₂ O/Ar 等离子体与 Cu/丝光沸石 (Cu/MOR) 催化剂相结合，将甲烷一步蒸汽重整为甲醇 (OSRMtM)，实现了 77% CH ₃ OH选择性，CH ₄转化率为3.0%。催化剂表征和等离子体诊断以及D ₂ O和H ₂ ¹⁸ O标记同位素示踪实验表明，优异的反应性能归因于MOR沸石限制的Cu-O活性位点。在等离子体催化OSRMtM期间，CH ₄和H ₂ O在等离子体中被激活并解离产生自由基（CH ₃ 、OH和H）。这些自由基驱动Cu ²⁺和Cu ⁺之间的氧化还原过程，在等离子体催化OSRMtM中发挥重要作用。虽然Cu ²⁺逐渐还原为Cu ⁺会导致缓慢失活，但通过简单的煅烧可以完全恢复催化性能，这使得使用流化床反应器的连续等离子体催化OSRMtM过程成为可能。