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Hydrodeoxygenation of guaiacol over Ni2P/SiO2–reaction mechanism and catalyst deactivation
Applied Catalysis A: General ( IF 5.5 ) Pub Date : 2017-10-28 , DOI: 10.1016/j.apcata.2017.10.018
Xuefang Lan , Emiel J.M. Hensen , Thomas Weber

The catalytic hydrodeoxygenation of guaiacol, a phenolic model compound of biomass lignin pyrolysis products, has been investigated under atmospheric pressure in H2 utilizing a Ni2P/SiO2 catalyst. Reaction networks are proposed based on the product distribution as a function of contact time and the temperature programmed surface reaction of adsorbed guaiacol and anisole. Guaiacol is mainly converted to benzene through demethoxylation and dehydroxylation via phenol and anisole as intermediates. Demethylation of guaiacol is a side-reaction, which produces small amounts of catechol. Spent catalyst samples were characterized by means of XRD, XPS, TEM, and temperature programmed oxidation to gain understanding the observed slight deactivation. Coke deposition, sintering, and the altering properties of Ni and P species on catalyst surface all contribute to deactivation, while there is no indication of surface oxidation after reaction. The increase of Niδ+ or Ni0 on the Ni2P surface and the decrease of Brønsted acid sites (i.e. POH) are considered to be the major reasons of product distribution changes.



中文翻译:

Ni 2 P / SiO 2上愈创木酚的加氢脱氧反应机理和催化剂失活

已经在大气压下于H 2中利用Ni 2 P / SiO 2研究了生物质木质素热解产物的酚类模型化合物guaiacol的催化加氢脱氧。催化剂。根据产物分布随接触时间和已编程的愈创木酚和苯甲醚的程序升温表面反应,提出了反应网络。愈创木酚主要通过脱甲氧基化和经由苯酚和苯甲醚作为中间体的脱羟基化而转化为苯。愈创木酚的去甲基化是一种副反应,会产生少量的儿茶酚。用XRD,XPS,TEM和程序升温氧化对用过的催化剂样品进行表征,以了解所观察到的轻微失活。焦炭的沉积,烧结以及催化剂表面Ni和P物种的变化性质均会导致失活,而反应后没有表面氧化的迹象。Ni的增加δ+或Ni 0在Ni2 P表面和布朗斯台德酸位(即P OH)的减少被认为是产品分布变化的主要原因。

更新日期:2017-10-28
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