NiCo/Al2O3 nanocatalysts for the synthesis of 5-amino-1-pentanol and 1,5-pentanediol from biomass-derived 2-hydroxytetrahydropyran

IF 9.1 Q1 ENGINEERING, CHEMICAL Green Chemical Engineering Pub Date : 2023-02-02 DOI:10.1016/j.gce.2023.01.003
Jian Yang , Jia Zhang , Enrico Benassi , Xuemei Li , Hailong Liu , Weiguo Fang , Junying Tian , Chungu Xia , Zhiwei Huang
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Abstract

Al2O3-supported monometallic Ni, Co, and bimetallic Ni–Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method, and used for the synthesis of useful 5-amino-1-pentanol (5-AP) and 1,5-pentanediol (1,5-PD) by reductive amination (RA) or direct hydrogenation of biofurfural-derived 2-hydroxytetrahydropyran (2-HTHP), respectively. In both reactions, the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al2O3 catalysts, owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60 °C. However, the incorporation of Co could improve the reducibility of the NiCo/Al2O3 bimetallic catalysts and promote the reaction stability of the catalysts, especially for Ni2Co1/Al2O3, in both reactions with over 180 h time-on-stream. Characterization of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni0 species, thanks to the formation of Ni–Co alloy in the bimetallic catalysts. DFT-based modeling of the reaction mechanisms is also performed, supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.

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NiCo/Al2O3纳米催化剂用于生物质衍生的2-羟基四氢吡喃合成5-氨基-1-戊醇和1,5-戊二醇
采用共沉淀法合成了以层状双氢氧化物为前驱体的 Al2O3 支承单金属 Ni、Co 和双金属 Ni-Co 纳米催化剂,并分别用于还原胺化 (RA) 或直接氢化生物糠醛衍生的 2-hydroxytetrahydropyran (2-HTHP) 合成有用的 5-amino-1-pentanol (5-AP) 和 1,5-pentanediol (1,5-PD)。在这两种反应中,目标产物的产率随着 NiCo/Al2O3 催化剂中 Co 含量的增加而单调下降,这可能是由于在 60 °C 的低反应温度下,Co 取代了氢化活性较低的高活性 Ni。然而,掺入 Co 可以改善 NiCo/Al2O3 双金属催化剂的还原性,并提高催化剂的反应稳定性,尤其是 Ni2Co1/Al2O3 催化剂在两个反应中的反应时间都超过 180 小时。反应前后催化剂的表征表明,由于双金属催化剂中形成了镍钴合金,钴的加入可以抑制金属颗粒的烧结,并阻碍活性更高的 Ni0 物种的表面氧化。此外,还对反应机理进行了基于 DFT 的建模,支持了之前提出的反应途径,并证明在 2-HTHP 的 RA 反应中,镍的活性远高于钴。
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来源期刊
Green Chemical Engineering
Green Chemical Engineering Process Chemistry and Technology, Catalysis, Filtration and Separation
CiteScore
11.60
自引率
0.00%
发文量
58
审稿时长
51 days
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