文献类型：期刊文献

中文题名：不同晶型Al_(2)O_(3)负载Ru催化剂对聚乙烯氢解的影响

英文题名：Effect of alumina support crystal structure of Ru-based catalysts on polyethylene hydrogenolysis performance

作者：高姣姣[1];颜诗宇[1];杨太顺[1];谢尚志[1];杨艳娟[1];徐晶[1,2]

机构：[1]广西大学化学化工学院广西石化资源加工与过程强化技术重点实验室,广西南宁530004;[2]华东理工大学绿色化工与工业催化全国重点实验室,化工学院,上海200237

年份：2025

卷号：44

期号：7

起止页码：3917

中文期刊名：化工进展

外文期刊名：Chemical Industry and Engineering Progress

收录：;EI(收录号：20253218946255);北大核心:【北大核心2023】；

基金：广西科技重大专项(桂科AA23062018);广西科技基地和人才专项(桂科AD23026311)。

语种：中文

中文关键词：Ru/Al_(2)O_(3)催化剂;加氢;甲烷;氧化铝;吸附

外文关键词：Ru/Al_(2)O_(3)catalyst;hydrogenation;methane;alumina;adsorption

摘要：废聚乙烯(PE)通过催化氢解制取燃料产品是实现塑料绿色循环的重要途径之一。本文探究了Al_(2)O_(3)晶型对负载型Ru基催化剂在PE催化氢解中反应性能的影响。通过浸渍法制备4种不同晶型的Ru/Al_(2)O_(3)催化剂,采用TEM、H_(2)-TPR和XPS对Ru/Al_(2)O_(3)催化剂进行表征,以揭示活性金属Ru与Al_(2)O_(3)载体之间的相互作用差异。PE氢解实验的结果表明,Al_(2)O_(3)晶型的差异对Ru/Al_(2)O_(3)催化剂催化氢解性能产生显著影响。在相同条件下进行PE氢解反应时,Ru/(δ+α)-Al_(2)O_(3)上产物总产率低于10%,甲烷的产率低于5%;而其他3种催化剂的产物总产率均高于90%,其中Ru/(θ+α)-Al_(2)O_(3)的甲烷产率(>90%)和选择性(>95%)最高。调控氢气反应压力,发现不同的*H覆盖率导致Ru/Al_(2)O_(3)催化剂上不同的反应行为。采用H_(2)-TPD和CO-DRIFTS对Ru/Al_(2)O_(3)催化剂进行表征,发现Ru/γ-Al_(2)O_(3)上活性位点Ru^(0)上的*H的过量吸附,导致了氢中毒;在Ru/(θ+α)-Al_(2)O_(3)上,活性位点Ru^(0)上的*H吸附和C-C长链吸附达到了平衡;在Ru/(δ+α)-Al_(2)O_(3)上,由于Run+的含量过高,导致*H在金属Ru上的吸附较弱,从而Ru/(δ+α)-Al_(2)O_(3)上产物总产率低于10%。
The production of fuel from polyethylene(PE)by catalytic hydrogen hydrolysis is an important approach to realize green recycle of PE.In this work,the effect of crystal structure of Al_(2)O_(3)on the performance of Ru-based catalyst for PE hydrogenolysis was investigated.Four kinds of Ru/Al_(2)O_(3)catalysts were prepared by impregnation method,and characterized by TEM,H_(2)-TPR and XPS to reveal the interaction between active metal Ru and Al_(2)O_(3)support.The experimental results of PE hydrolysis showed that the difference in Al_(2)O_(3)crystal structure led to a significant effect on the catalytic performance.Under the same reaction conditions,the total yield of products by Ru/(δ+α)-Al_(2)O_(3)catalystwas less than 10%,and the methane yield was less than 5%,while the total yield for the other three catalysts was all higher than 90%.Among them,Ru/(θ+α)-Al_(2)O_(3)exhibited the highest methane yield and selectivity,with methane yield higher than 90%and methane selectivity over 95%.By adjusting the hydrogen pressure,it was found that the different coverage of*H led to different reaction behaviors.With the combination of H_(2)-TPD and CO-DRIFTS characterization methods,it was found that the excess adsorption of*H at the active site Ru^(0)of Ru/γ-Al_(2)O_(3)could result in hydrogen poisoning.For Ru/(θ+α)-Al_(2)O_(3),the adsorption of*H at the active site Ru^(0)and the C—C intermediate could reach adsorption equilibrium.On Ru/(δ+α)-Al_(2)O_(3)catalyst,no*H adsorption on the active site Ru^(0)was detected,hence the total product yield for Ru/(δ+α)-Al_(2)O_(3)was below 10%.