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Boosting Propane Dehydrogenation by the Regioselective Distribution of Subnanometric CoO Clusters in MFI Zeolite Nanosheets
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-03-10 , DOI: 10.1021/acsami.2c21076 Xintong Lv 1 , Min Yang 1 , Shaojia Song 1 , Mingji Xia 1 , Jun Li 2 , Yuechang Wei 1 , Chunming Xu 1 , Weiyu Song 1 , Jian Liu 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-03-10 , DOI: 10.1021/acsami.2c21076 Xintong Lv 1 , Min Yang 1 , Shaojia Song 1 , Mingji Xia 1 , Jun Li 2 , Yuechang Wei 1 , Chunming Xu 1 , Weiyu Song 1 , Jian Liu 1
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Direct dehydrogenation of propane (PDH) has already been implemented worldwide in industrial processes to produce value-added propylene. The discovery of earth-abundant and environmentally friendly metal with high activity in C–H cleavage is of great importance. Co species encapsulated within zeolite are highly efficient for catalyzing direct dehydrogenation. However, exploring a promising Co catalyst remains a nontrivial target. Direct control of the regioselective distribution of Co species in the zeolite framework through altering their crystal morphology gives opportunities to modify the metallic Lewis acidic features, thus providing an active and appealing catalyst. Herein, we achieved the regioselective localization of highly active subnanometric CoO clusters in straight channels of siliceous MFI zeolite nanosheets with controllable thickness and aspect ratio. The subnanometric CoO species were identified by different types of spectroscopies, probe measurements, and density functional theory calculations, as the coordination site for the electron-donating propane molecules. The catalyst showed promising catalytic activity for the industrially important PDH with propane conversion of 41.8% and propylene selectivity higher than 95% and was durable during 10 successive regeneration cycles. These findings highlight a green and facile method to synthesize metal-containing zeolitic materials with regioselective metal distribution and also to open up a future perspectives for designing advanced catalysts with integrated advantages of the zeolitic matrix and metal structures.
中文翻译：
通过 MFI 沸石纳米片中亚纳米级 CoO 簇的区域选择性分布促进丙烷脱氢
丙烷直接脱氢 (PDH) 已在全球工业过程中实施，以生产增值丙烯。发现地球上储量丰富且对环境友好且具有高 C-H 裂解活性的金属具有重要意义。包封在沸石中的 Co 物质对于催化直接脱氢非常有效。然而，探索一种有前途的 Co 催化剂仍然是一个重要的目标。通过改变其晶体形态直接控制 Co 物种在沸石骨架中的区域选择性分布，为改变金属路易斯酸性特征提供了机会，从而提供了一种具有活性和吸引力的催化剂。在此处，我们在硅质 MFI 沸石纳米片的直通道中实现了高活性亚纳米 CoO 簇的区域选择性定位，厚度和纵横比可控。通过不同类型的光谱学、探针测量和密度泛函理论计算确定亚纳米级 CoO 物种作为给电子丙烷分子的配位点。该催化剂对工业上重要的 PDH 显示出良好的催化活性，丙烷转化率为 41.8%，丙烯选择性高于 95%，并且在 10 个连续的再生循环中经久耐用。
更新日期：2023-03-10
中文翻译：
通过 MFI 沸石纳米片中亚纳米级 CoO 簇的区域选择性分布促进丙烷脱氢
丙烷直接脱氢 (PDH) 已在全球工业过程中实施，以生产增值丙烯。发现地球上储量丰富且对环境友好且具有高 C-H 裂解活性的金属具有重要意义。包封在沸石中的 Co 物质对于催化直接脱氢非常有效。然而，探索一种有前途的 Co 催化剂仍然是一个重要的目标。通过改变其晶体形态直接控制 Co 物种在沸石骨架中的区域选择性分布，为改变金属路易斯酸性特征提供了机会，从而提供了一种具有活性和吸引力的催化剂。在此处，我们在硅质 MFI 沸石纳米片的直通道中实现了高活性亚纳米 CoO 簇的区域选择性定位，厚度和纵横比可控。通过不同类型的光谱学、探针测量和密度泛函理论计算确定亚纳米级 CoO 物种作为给电子丙烷分子的配位点。该催化剂对工业上重要的 PDH 显示出良好的催化活性，丙烷转化率为 41.8%，丙烯选择性高于 95%，并且在 10 个连续的再生循环中经久耐用。
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