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Tuning selectivity of acetic acid and alcohols by Brønsted and Lewis acid sites in plasma-catalytic CH4/CO2 conversion over zeolites
Applied Catalysis B: Environment and Energy ( IF 22.1 ) Pub Date : 2024-03-11 , DOI: 10.1016/j.apcatb.2024.123938
Li Wang , Linhui Fan , Yuezhao Wang , Qian Chen , Yimin Zhu , Yanhui Yi

Plasma catalysis enables CH/CO direct conversion to oxygenates under mild conditions. However, addressing complexity of oxygenate products is the main scientific challenge. Herein, the roles of Brønsted and Lewis acid site (i.e., BAS and LAS) in tuning the selectivity of acetic acid and alcohols have been comparatively investigated for the first time. BAS and LAS are provided by HZSM-5 and 13X zeolites, respectively, and their amounts are adjusted by steam treatment. Results reveal that BAS significantly promotes acetic acid formation, while LAS favors alcohols generation. In addition, Au supported zeolites show that Au-BAS synergy exhibits potential for acetic acid. FTIR spectra identify the bicarbonate (HCO) and formate (HCOO) to be the primary surface species on BAS and LAS, respectively. Correspondingly, the pathways for acetic acid and methanol production are proposed based on catalyst characterizations and plasma diagnosis. This work opens up zeolite-based catalysts for selective CH/CO conversion to oxygenates.

中文翻译:

通过沸石等离子体催化 CH4/CO2 转化中的 Brønsted 和 Lewis 酸位调节乙酸和醇的选择性

等离子体催化使 CH/CO 在温和条件下直接转化为含氧化合物。然而,解决含氧化合物产品的复杂性是主要的科学挑战。在此,首次对布朗斯台德酸位点和路易斯酸位点(即BAS和LAS)在调节乙酸和醇的选择性中的作用进行了比较研究。 BAS和LAS分别由HZSM-5和13X沸石提供,其用量通过蒸汽处理进行调节。结果表明,BAS 显着促进乙酸的形成,而 LAS 有利于醇的生成。此外,Au 负载的沸石表明 Au-BAS 协同作用对乙酸具有潜力。 FTIR 光谱确定碳酸氢盐 (HCO) 和甲酸盐 (HCOO) 分别是 BAS 和 LAS 上的主要表面物质。相应地,基于催化剂表征和等离子体诊断提出了乙酸和甲醇生产的途径。这项工作开辟了基于沸石的催化剂用于选择性 CH/CO 转化为含氧化合物。
更新日期:2024-03-11
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