Zhou Shu-Zhen, Li Wen-Cui, He Bowen, Xie Ya-Dong, Wang Haowei, Liu Xi, Chen Liwei, Wei Jiake, Lu An-Hui
State Key Laboratory of Fine Chemicals, Liaoning Key Laboratory for Catalytic Conversion of Carbon Resources, School of Chemical Engineering, Dalian University of Technology, Dalian, 116024, P. R. China.
School of Chemistry and Chemical Engineering, In situ Center for Physical Sciences, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Angew Chem Int Ed Engl. 2024 Oct 21;63(43):e202410835. doi: 10.1002/anie.202410835. Epub 2024 Sep 12.
Propane dehydrogenation (PDH) is crucial for propylene production, but commercially employed Pt-based catalysts face susceptibility to deactivation due to the Pt sintering during reaction and regeneration steps. Here, we report a SiO supported nanometric (MnCoCuZnPt) high-entropy PDH catalyst with high activity and stability. The catalyst exhibited a super high propane conversion of 56.6 % with 94 % selectivity of propylene at 600 °C. The propylene productivity reached 68.5 mol ⋅ g ⋅ h, nearly three times that of Pt/SiO (23.5 mol ⋅ g ⋅ h) under a weight hourly space velocity of 60 h. In a high-entropy nanoparticle, Pt atoms were atomically dispersed through coordination with other metals and exhibited a positive charge, thereby showcasing remarkable catalytic activity. The high-entropy effect contributes to the catalyst a superior stability with a low deactivation constant of 0.0004 h during 200 hours of reaction under the industrial gas composition at 550 °C. Such high-entropy PDH catalyst is easy regenerated through simple air combustion of deposited coke. After the fourth consecutive regeneration cycle, satisfactory catalytic stability was observed, and the element distribution of spent catalysts almost returned to their initial state, with no detectable Pt sintering. This work provides new insights into designing active, stable, and regenerable novel PDH catalysts.
丙烷脱氢(PDH)对于丙烯生产至关重要,但商业上使用的铂基催化剂在反应和再生步骤中由于铂烧结而容易失活。在此,我们报道了一种具有高活性和稳定性的SiO负载的纳米级(MnCoCuZnPt)高熵PDH催化剂。该催化剂在600°C时表现出56.6%的超高丙烷转化率和94%的丙烯选择性。在60 h-1的重量时空速下,丙烯生产率达到68.5 mol⋅g-1⋅h,几乎是Pt/SiO(23.5 mol⋅g-1⋅h)的三倍。在高熵纳米颗粒中,铂原子通过与其他金属配位而原子级分散,并呈现正电荷,从而展现出显著的催化活性。高熵效应赋予催化剂优异的稳定性,在550°C的工业气体组成下反应200小时期间失活常数低至0.0004 h-1。这种高熵PDH催化剂通过对沉积焦炭进行简单的空气燃烧即可轻松再生。在连续第四个再生循环后,观察到令人满意的催化稳定性,并且失活催化剂的元素分布几乎恢复到初始状态,未检测到铂烧结。这项工作为设计活性、稳定且可再生的新型PDH催化剂提供了新的见解。