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Bimetallic Ni-Co/γ-Al2O3 catalyst for vapour phase production of γ-valerolactone: Deactivation studies and feedstock selection
Fuel ( IF 7.4 ) Pub Date : 2021-02-01 , DOI: 10.1016/j.fuel.2020.119094
Murali Kondeboina , Siva Sankar Enumula , K. Saidulu Reddy , Prathap Challa , David Raju Burri , Seetha Rama Rao Kamaraju

Abstract With an aim to establish supported non-noble Co metal catalysts for production of a promising fuel and fuel additive γ-valerolactone (GVL) at ambient pressure in continuous mode, Co/γ-Al2O3 and bimetallic Ni-Co/γ-Al2O3 catalysts were prepared and their catalytic activities vs. catalytic features were correlated. Ni-Co/γ-Al2O3 catalyst exhibited GVL productivity of 1.125 kgGVL.kgcatalyst−1h−1 which is relatively higher than Co/γ-Al2O3 catalyst. Ni-Co/γ-Al2O3 catalyst is stable during 12 h time-on-stream studies while Co/γ-Al2O3 catalyst suffers from deactivation. The addition of Ni to Co/γ-Al2O3 augments the resultant bimetallic catalyst activity and coke resistance capacity. As evidenced from XRD, H2-TPR, XPS analyses the addition of Ni to Co/γ-Al2O3 results in formation of Ni-Co alloy in the bimetallic catalysts. H2-pulse chemisorption studies and TEM analyses illustrate formation of smaller particles in bimetallic Ni-Co/γ-Al2O3 catalyst which in turn influenced the rate of formation of GVL. From TGA of spent catalysts, the carbon deposition rate is found to be decreased in the case of Ni-Co/γ-Al2O3 catalyst (0.43 mmol.gcat−1.h−1) than Co/γ-Al2O3 catalyst (1.014 mmol.gcat−1.h−1). Among the feedstocks of GVL i.e. levulinic acid, methyl levulinate, ethyl levulinate, ethyl levulinate is found to be prominent in constantly yielding GVL during 24 h study over bimetallic Ni-Co/γ-Al2O3 catalyst.

中文翻译:

用于气相生产 γ-戊内酯的双金属 Ni-Co/γ-Al2O3 催化剂:失活研究和原料选择

摘要 为了建立负载型非贵金属 Co 催化剂,用于在常压下连续生产有前景的燃料和燃料添加剂 γ-戊内酯 (GVL),Co/γ-Al2O3 和双金属 Ni-Co/γ-Al2O3 催化剂制备并且它们的催化活性与催化特征相关联。Ni-Co/γ-Al2O3 催化剂的 GVL 生产率为 1.125 kgGVL.kgcatalyst-1h-1,相对高于 Co/γ-Al2O3 催化剂。Ni-Co/γ-Al2O3 催化剂在 12 小时的运行时间研究中是稳定的,而 Co/γ-Al2O3 催化剂会失活。将 Ni 添加到 Co/γ-Al2O3 中提高了所得的双金属催化剂活性和抗焦炭能力。XRD、H2-TPR、XPS 分析表明,将 Ni 添加到 Co/γ-Al2O3 中导致在双金属催化剂中形成 Ni-Co 合金。H2 脉冲化学吸附研究和 TEM 分析表明,在双金属 Ni-Co/γ-Al2O3 催化剂中形成了较小的颗粒,这反过来影响了 GVL 的形成速率。从废催化剂的 TGA 中,发现在 Ni-Co/γ-Al2O3 催化剂(0.43 mmol.gcat-1.h-1)的情况下,碳沉积速率比 Co/γ-Al2O3 催化剂(1.014 mmol)降低。 gcat-1.h-1)。在 GVL 的原料中,即乙酰丙酸、乙酰丙酸甲酯、乙酰丙酸乙酯、乙酰丙酸乙酯在双金属 Ni-Co/γ-Al2O3 催化剂的 24 小时研究中在持续产生 GVL 方面表现突出。发现在 Ni-Co/γ-Al2O3 催化剂(0.43 mmol.gcat-1.h-1)的情况下,碳沉积速率比 Co/γ-Al2O3 催化剂(1.014 mmol.gcat-1.h-)降低1)。在 GVL 的原料中,即乙酰丙酸、乙酰丙酸甲酯、乙酰丙酸乙酯、乙酰丙酸乙酯在双金属 Ni-Co/γ-Al2O3 催化剂的 24 小时研究中在持续产生 GVL 方面表现突出。发现在 Ni-Co/γ-Al2O3 催化剂(0.43 mmol.gcat-1.h-1)的情况下,碳沉积速率比 Co/γ-Al2O3 催化剂(1.014 mmol.gcat-1.h-)降低1)。在 GVL 的原料中,即乙酰丙酸、乙酰丙酸甲酯、乙酰丙酸乙酯、乙酰丙酸乙酯在双金属 Ni-Co/γ-Al2O3 催化剂的 24 小时研究中在持续产生 GVL 方面表现突出。
更新日期:2021-02-01
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