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>Highly efficient CO-assisted conversion of methane to acetic acid over Rh-encapsulated MFI zeolite prepared using RhCl3 molten salt
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Highly efficient CO-assisted conversion of methane to acetic acid over Rh-encapsulated MFI zeolite prepared using RhCl3 molten salt
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机译：Highly efficient CO-assisted conversion of methane to acetic acid over Rh-encapsulated MFI zeolite prepared using RhCl3 molten salt
Direct catalytic conversion of methane to value-added chemicals with a high reaction rate and selectivity under mild conditions remains a great challenge. Rh-supported zeolite is one of the promising heterogeneous catalysts capable of selectively oxidizing methane to acetic acid using carbon monoxide and oxygen at low temperatures. However, the difficulty in the preparation of the catalytically active species, i.e., zeolite-confined RhI single-atom sites, has limited the mass activity. Here, we successfully prepared a highly-active Rh-containing zeolite using RhCl3 molten salt. By high-temperature treatment of the physically-mixed H+-MFI zeolite and bulk RhCl3, the RhCl3 molten salt was formed under in situ conditions and then diffused into the zeolite pores, resulting in being trapped within the zeolite cavity via host–guest interaction and ion-exchange with H+. The encapsulated RhCl3 species are efficiently dispersed with the formation of RhI single-atom species as the active sites in the catalytic reaction, boosting the direct conversion of methane to acetic acid with a record turnover frequency (592 mol molRh−1 h−1) and yield (14.6 mmol gcat−1 h−1) with high selectivity (76.9%).
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机译：直接催化甲烷转化附加值高的化学反应速率和仍然是一个温和条件下选择性巨大的挑战。有前途的异构催化剂的能力选择性氧化甲烷醋酸使用在低一氧化碳和氧气温度。制备催化地活跃的物种,也就是说,单原子站点,zeolite-confined奥镁有限的质量活动。准备了一个高度活跃Rh-containing沸石使用RhCl3熔盐。治疗physically-mixed H + mfi沸石和散装RhCl3 RhCl3熔盐成立在原位条件下,然后扩散到沸石的毛孔,导致被困通过主-客体沸石内腔交互和H +离子交换。封装RhCl3物种都是有效的分散与奥镁单原子的形成催化物种活动网站反应,提高的直接转换甲烷与营业额记录醋酸频率(592摩尔molRh−1 h−1)和产量(14.6更易gcat−1 h−1)高选择性(76.9%)。
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