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Pyrolysis of nickel salt@cellulose to prepare Ni/C catalyst with tunable hydrogenation and acid site for the selective hydrogenation of furfuryl alcohol
Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2023-04-25 , DOI: 10.1016/j.jece.2023.110013 Mengjiao Fan , Hongli Tian , Yuewen Shao , Lijun Zhang , Shu Zhang , Guangzhi Hu , Xun Hu
Journal of Environmental Chemical Engineering ( IF 7.4 ) Pub Date : 2023-04-25 , DOI: 10.1016/j.jece.2023.110013 Mengjiao Fan , Hongli Tian , Yuewen Shao , Lijun Zhang , Shu Zhang , Guangzhi Hu , Xun Hu
Ni/C catalysts could be prepared via pyrolysis of biomass impregnated with nickel salts, while varied anions of nickel salt impact not only catalytic behaviors of Ni/C catalyst, but also property/composition of resulting biochar/bio-oil. In this work, pyrolysis of the cellulose with Ni(NO3 )2 or NiCl2 was investigated, and the resulting pyrolysis products were analyzed while the Ni/C catalysts were evaluated in hydrogenation of furfuryl alcohol (FA) in water. The results indicated that the nitrate in Ni(NO3 )2 catalyzed cracking reactions to form less biochar, less heavy organics with π-conjugated structures but more light ones. It also resulted in the Ni/C with high nickel dispersion and hence superior activity for hydrogenation of FA, producing dominantly tetrahydrofurfuryl alcohol (THFA). In comparison, the chloride in NiCl2 enhanced dehydration of sugars to furans and condensation of heavy organics in the pyrolysis, which also created abundant Brønsted and Lewis acid sites, developed pore structures, but resulted in aggregation of metallic nickel. This decreased its capability for full hydrogenation of FA, but rendered the selective conversion of FA to cyclopentanone (CPO) and cyclopentanol (CPL) (sum yield: 91.0 %) with the aid of the acidic sites.
中文翻译:
镍salt@cellulose热解制备具有可调加氢和酸位的 Ni/C 催化剂,用于糠醇的选择性加氢
Ni/C 催化剂可以通过对浸渍镍盐的生物质进行热解来制备,而镍盐的不同阴离子不仅影响 Ni/C 催化剂的催化行为,还影响所得生物炭/生物油的性质/组成。在这项工作中,研究了纤维素与 Ni(NO3)2 或 NiCl2 的热解,并分析了所得的热解产物,同时评估了糠醇 (FA) 在水中加氢的 Ni/C 催化剂。结果表明,Ni(NO3)2 中的硝酸盐催化裂解反应形成较少的生物炭、较少的重有机物,具有π共轭结构但较轻的有机物。它还导致 Ni/C 具有高镍分散性,因此对 FA 的氢化具有优异的活性,主要产生四氢糠醇 (THFA)。相比之下,NiCl2 中的氯化物增强了糖脱水为呋喃和热解中重有机物的缩合,这也产生了丰富的 Brønsted 和 Lewis 酸位点,形成了孔隙结构,但导致金属镍的聚集。这降低了其 FA 完全氢化的能力,但在酸性位点的帮助下,FA 选择性地转化为环戊酮 (CPO) 和环戊醇 (CPL)(总产率:91.0%)。
更新日期:2023-04-25
中文翻译:
镍salt@cellulose热解制备具有可调加氢和酸位的 Ni/C 催化剂,用于糠醇的选择性加氢
Ni/C 催化剂可以通过对浸渍镍盐的生物质进行热解来制备,而镍盐的不同阴离子不仅影响 Ni/C 催化剂的催化行为,还影响所得生物炭/生物油的性质/组成。在这项工作中,研究了纤维素与 Ni(NO3)2 或 NiCl2 的热解,并分析了所得的热解产物,同时评估了糠醇 (FA) 在水中加氢的 Ni/C 催化剂。结果表明,Ni(NO3)2 中的硝酸盐催化裂解反应形成较少的生物炭、较少的重有机物,具有π共轭结构但较轻的有机物。它还导致 Ni/C 具有高镍分散性,因此对 FA 的氢化具有优异的活性,主要产生四氢糠醇 (THFA)。相比之下,NiCl2 中的氯化物增强了糖脱水为呋喃和热解中重有机物的缩合,这也产生了丰富的 Brønsted 和 Lewis 酸位点,形成了孔隙结构,但导致金属镍的聚集。这降低了其 FA 完全氢化的能力,但在酸性位点的帮助下,FA 选择性地转化为环戊酮 (CPO) 和环戊醇 (CPL)(总产率:91.0%)。