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Effect of Zeolitic Hydroxyl Nests on the Acidity and Propane Aromatization Performance of Zinc Nitrate Impregnation-Modified HZSM-5 Zeolite
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-09-01 , DOI: 10.1021/acs.iecr.0c02596 Long Lin 1 , Jiaxu Liu 1 , Xiaotong Zhang 1 , Jilei Wang 1 , Chunyan Liu 1 , Guang Xiong 1 , Hongchen Guo 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-09-01 , DOI: 10.1021/acs.iecr.0c02596 Long Lin 1 , Jiaxu Liu 1 , Xiaotong Zhang 1 , Jilei Wang 1 , Chunyan Liu 1 , Guang Xiong 1 , Hongchen Guo 1
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A defective HZSM-5 zeolite (SiO2/Al2O3 = 55, crystal size = 300 nm) with a high density of hydroxyl nests and its patched-up counterpart obtained by pretreating the defective zeolite with (NH4)2SiF6 were employed to investigate the effect of zeolitic hydroxyl nests on the acidity and propane aromatization performance of zinc nitrate-impregnated HZSM-5 zeolite. Catalyst characterizations show that, in the case of impregnating the defective HZSM-5 zeolite, zinc ions were preferentially introduced into the zeolitic hydroxyl nests, forming subnanomeric ZnO clusters as Lewis acid sites (showed 1451 cm–1 infrared (IR) adsorption feature when adsorbed by pyridine). By contrast, when the hydroxyl nests of the defective zeolite were patched by (NH4)2SiF6 pretreatment, the zinc ions were mainly ushered in as isolated Zn2+ and bulky ZnO particles, the former species were the known Lewis acid sites (showed 1455 cm–1 IR adsorption feature when adsorbed by pyridine) located at the counter-cation positions of zeolitic bridging hydroxyls. Propane aromatization operando infrared spectroscopic study and pulse microreactor evaluation indicated that the zeolitic hydroxyl nests-stabilized subnanomeric ZnO clusters had clear advantage over the known isolated Zn2+ Lewis acid sites in the dehydroaromatization of propane.
中文翻译：
沸石羟基巢对硝酸锌浸渍改性HZSM-5沸石酸度和丙烷芳构化性能的影响
具有高密度羟基巢的缺陷型HZSM-5分子筛（SiO 2 / Al 2 O 3 = 55，晶体尺寸= 300 nm）及其修补的对应物，该缺陷分子用（NH 4）2 SiF 6预处理分别研究了沸石羟基巢对硝酸锌浸渍的HZSM-5沸石的酸度和丙烷芳构化性能的影响。催化剂表征表明，在浸渍有缺陷的HZSM-5沸石的情况下，锌离子优先引入沸石的羟基巢中，形成亚纳米的ZnO团簇，作为路易斯酸位点（显示1451 cm –1）。被吡啶吸附时具有红外（IR）吸附特征）。相比之下，当通过（NH 4）2 SiF 6预处理修补缺陷沸石的羟基巢穴时，锌离子主要作为分离的Zn 2+和块状ZnO颗粒进入，前者是已知的路易斯酸位点（在吡啶桥键合羟基的反阳离子位置显示出1455 cm –1的IR吸附特征（被吡啶吸附）。丙烷芳构化操作红外光谱研究和脉冲微反应器评估表明，沸石羟基巢稳定的亚纳米ZnO团簇比已知的分离的Zn 2+具有明显的优势。 丙烷脱氢芳构化中的路易斯酸位点。
更新日期：2020-09-16
中文翻译：
沸石羟基巢对硝酸锌浸渍改性HZSM-5沸石酸度和丙烷芳构化性能的影响
具有高密度羟基巢的缺陷型HZSM-5分子筛（SiO 2 / Al 2 O 3 = 55，晶体尺寸= 300 nm）及其修补的对应物，该缺陷分子用（NH 4）2 SiF 6预处理分别研究了沸石羟基巢对硝酸锌浸渍的HZSM-5沸石的酸度和丙烷芳构化性能的影响。催化剂表征表明，在浸渍有缺陷的HZSM-5沸石的情况下，锌离子优先引入沸石的羟基巢中，形成亚纳米的ZnO团簇，作为路易斯酸位点（显示1451 cm –1）。被吡啶吸附时具有红外（IR）吸附特征）。相比之下，当通过（NH 4）2 SiF 6预处理修补缺陷沸石的羟基巢穴时，锌离子主要作为分离的Zn 2+和块状ZnO颗粒进入，前者是已知的路易斯酸位点（在吡啶桥键合羟基的反阳离子位置显示出1455 cm –1的IR吸附特征（被吡啶吸附）。丙烷芳构化操作红外光谱研究和脉冲微反应器评估表明，沸石羟基巢稳定的亚纳米ZnO团簇比已知的分离的Zn 2+具有明显的优势。 丙烷脱氢芳构化中的路易斯酸位点。
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