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One-dimensional Ga2O3-Al2O3 nanofibers with unsaturated coordination Ga: Catalytic dehydrogenation of propane under CO2 atmosphere with excellent stability
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2024-03-27 , DOI: 10.1016/j.jcis.2024.03.171
Xue Han 1 , Yun Yang 2 , Rui Chen 2 , Jiaqi Zhou 2 , Xupeng Yang 2 , Xuyu Wang 2 , Hongbing Ji 3
Journal of Colloid and Interface Science ( IF 9.4 ) Pub Date : 2024-03-27 , DOI: 10.1016/j.jcis.2024.03.171
Xue Han 1 , Yun Yang 2 , Rui Chen 2 , Jiaqi Zhou 2 , Xupeng Yang 2 , Xuyu Wang 2 , Hongbing Ji 3
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The pressing demand for propylene has spurred intensive research on the catalytic dehydrogenation of propane to produce propylene. Gallium-based catalysts are regarded as highly promising due to their exceptional dehydrogenation activity in the presence of CO. However, the inherent coking issue associated with high temperature reactions poses a constraint on the stability development of this process. In this study, we employed the electrospinning method to prepare a range of GaO-AlO mixed oxide one-dimensional nanofiber catalysts with varying molar ratios for CO oxidative dehydrogenation of propane (CO-OPDH). The propane conversion was up to 48.4 % and the propylene selectivity was high as 96.8 % at 500 °C, the ratio of propane to carbon dioxide is 1:2. After 100 h of reaction, the catalyst still maintains approximately 10 % conversion and exhibits a propylene selectivity of around 98 %. The electrospinning method produces one-dimensional nanostructures with a larger specific surface area, unique multi-stage pore structure and low-coordinated Ga, which enhances mass transfer and accelerates reaction intermediates. This results in less coking and improved catalyst stability. The high activity of the catalyst is attributed to an abundance of low-coordinated Ga ions associated with weak/medium-strong Lewis acid centers. In situ infrared analysis reveals that the reaction mechanism involves a two-step dehydrogenation via propane isocleavage, with the second dehydrogenation of Ga-OR at the metal–oxygen bond being the decisive speed step.
中文翻译：
具有不饱和配位Ga的一维Ga2O3-Al2O3纳米纤维：CO2气氛下催化丙烷脱氢具有优异的稳定性
对丙烯的迫切需求促使人们对丙烷催化脱氢生产丙烯进行深入研究。镓基催化剂由于在CO存在下具有出色的脱氢活性而被认为是非常有前途的。然而，与高温反应相关的固有焦化问题限制了该过程的稳定性发展。在这项研究中，我们采用静电纺丝方法制备了一系列不同摩尔比的GaO-Al2O混合氧化物一维纳米纤维催化剂，用于丙烷CO氧化脱氢（CO-OPDH）。 500℃时丙烷转化率高达48.4%，丙烯选择性高达96.8%，丙烷与二氧化碳的比例为1:2。反应100小时后，催化剂仍保持约10%的转化率，丙烯选择性约为98%。静电纺丝方法产生具有较大比表面积、独特的多级孔隙结构和低配位Ga的一维纳米结构，增强了传质并加速反应中间体。这会减少结焦并提高催化剂稳定性。该催化剂的高活性归因于大量与弱/中强路易斯酸中心相关的低配位Ga离子。原位红外分析表明，反应机理涉及通过丙烷等裂解进行的两步脱氢，其中Ga-OR在金属-氧键处的第二次脱氢是决定性的速度步骤。
更新日期：2024-03-27
中文翻译：
具有不饱和配位Ga的一维Ga2O3-Al2O3纳米纤维：CO2气氛下催化丙烷脱氢具有优异的稳定性
对丙烯的迫切需求促使人们对丙烷催化脱氢生产丙烯进行深入研究。镓基催化剂由于在CO存在下具有出色的脱氢活性而被认为是非常有前途的。然而，与高温反应相关的固有焦化问题限制了该过程的稳定性发展。在这项研究中，我们采用静电纺丝方法制备了一系列不同摩尔比的GaO-Al2O混合氧化物一维纳米纤维催化剂，用于丙烷CO氧化脱氢（CO-OPDH）。 500℃时丙烷转化率高达48.4%，丙烯选择性高达96.8%，丙烷与二氧化碳的比例为1:2。反应100小时后，催化剂仍保持约10%的转化率，丙烯选择性约为98%。静电纺丝方法产生具有较大比表面积、独特的多级孔隙结构和低配位Ga的一维纳米结构，增强了传质并加速反应中间体。这会减少结焦并提高催化剂稳定性。该催化剂的高活性归因于大量与弱/中强路易斯酸中心相关的低配位Ga离子。原位红外分析表明，反应机理涉及通过丙烷等裂解进行的两步脱氢，其中Ga-OR在金属-氧键处的第二次脱氢是决定性的速度步骤。
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