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Surfactant-Assisted Preparation of Nanorod La2O3 Catalysts for Oxidative Coupling of Methane
Energy & Fuels ( IF 5.2 ) Pub Date : 2023-09-28 , DOI: 10.1021/acs.energyfuels.3c02246 Junrong Yue 1, 2, 3 , Qingyue Xiao 1, 3 , Dawei Zhao 1 , Yu Guan 3 , Jiao Liu 3 , Guangwen Xu 1, 2, 3
Energy & Fuels ( IF 5.2 ) Pub Date : 2023-09-28 , DOI: 10.1021/acs.energyfuels.3c02246 Junrong Yue 1, 2, 3 , Qingyue Xiao 1, 3 , Dawei Zhao 1 , Yu Guan 3 , Jiao Liu 3 , Guangwen Xu 1, 2, 3
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It is generally agreed upon that oxidative coupling of methane is structure-sensitive over the La2O3 catalysts and that morphology such as nanowire or nanorod exhibited the highest activity. Therefore, three crystalline La2O3 catalysts were synthesized by the hydrothermal method without (denoted as La-NS) or with polyvinylpyrrolidone (PVP) (denoted as La-PVP) or cetyltrimethylammonium bromide (denoted as La-CTAB) as the surfactant. The HRTEM results suggested (110) and (101) planes were both exposed in La-PVP, while only the (101) facet in La-NS and the (002) facet in La-CTAB were exposed. CO2-TPD characterization showed that La-PVP exhibited a larger capacity of CO2 adsorption and more amounts of moderate basic sites than La-NS and La-CTAB. Then, the formation of the chemisorbed oxygen species O2– was facilitated. In situ DRIFT spectra revealed that surface O2– species are the activated oxygen species which would convert methane to a methyl radical and then couple to C2+ hydrocarbons during the OCM reaction over the nanorod La2O3 catalysts. Therefore, the La-PVP catalyst outperformed its peers in both activity and selectivity.
中文翻译：
表面活性剂辅助制备甲烷氧化偶联纳米棒La2O3催化剂
人们普遍认为，甲烷的氧化偶联对La 2 O 3催化剂具有结构敏感性，并且纳米线或纳米棒等形态表现出最高的活性。因此，采用水热法合成了三种结晶La 2 O 3 催化剂，分别不使用表面活性剂（记为La-NS）或使用聚乙烯吡咯烷酮（PVP）（记为La-PVP）或十六烷基三甲基溴化铵（记为La-CTAB）作为表面活性剂。HRTEM结果表明La-PVP中的(110)和(101)面均暴露，而La-NS中仅暴露了(101)面和La-CTAB中的(002)面。CO 2 -TPD表征表明，La-PVP比La-NS和La-CTAB表现出更大的CO 2吸附容量和更多的中等碱性位点。然后，促进了化学吸附氧O 2 –的形成。原位 DRIFT 光谱显示，表面 O 2 -物质是活化的氧物质，在纳米棒 La 2 O 3催化剂上的 OCM 反应过程中，它会将甲烷转化为甲基自由基，然后与 C2+ 碳氢化合物偶联。因此，La-PVP催化剂在活性和选择性方面均优于同类催化剂。
更新日期：2023-09-28
中文翻译：
表面活性剂辅助制备甲烷氧化偶联纳米棒La2O3催化剂
人们普遍认为，甲烷的氧化偶联对La 2 O 3催化剂具有结构敏感性，并且纳米线或纳米棒等形态表现出最高的活性。因此，采用水热法合成了三种结晶La 2 O 3 催化剂，分别不使用表面活性剂（记为La-NS）或使用聚乙烯吡咯烷酮（PVP）（记为La-PVP）或十六烷基三甲基溴化铵（记为La-CTAB）作为表面活性剂。HRTEM结果表明La-PVP中的(110)和(101)面均暴露，而La-NS中仅暴露了(101)面和La-CTAB中的(002)面。CO 2 -TPD表征表明，La-PVP比La-NS和La-CTAB表现出更大的CO 2吸附容量和更多的中等碱性位点。然后，促进了化学吸附氧O 2 –的形成。原位 DRIFT 光谱显示，表面 O 2 -物质是活化的氧物质，在纳米棒 La 2 O 3催化剂上的 OCM 反应过程中，它会将甲烷转化为甲基自由基，然后与 C2+ 碳氢化合物偶联。因此，La-PVP催化剂在活性和选择性方面均优于同类催化剂。
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