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Catalytic Activity of Pt Loaded Zeolites for Hydroisomerization of n-Hexane Using Supercritical CO2
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-12-10 , DOI: 10.1021/acs.iecr.0c05184 Usama A. Al-Rawi 1 , Farooq Sher 2 , Abu Hazafa 3, 4 , Tahir Rasheed 5 , Nawar K. Al-Shara 4, 6 , Eder C. Lima 7 , Jabir Shanshool 1
Industrial & Engineering Chemistry Research ( IF 3.8 ) Pub Date : 2020-12-10 , DOI: 10.1021/acs.iecr.0c05184 Usama A. Al-Rawi 1 , Farooq Sher 2 , Abu Hazafa 3, 4 , Tahir Rasheed 5 , Nawar K. Al-Shara 4, 6 , Eder C. Lima 7 , Jabir Shanshool 1
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The present study investigates the synthesis of novel strontium (Sr) and barium (Ba) modified crystalline zeolites including Zeolite Socony Mobil-5 (ZSM-5) and Mordenite (MOR) utilizing a batchwise ion-exchange method with an appropriate chloride solution of 3 N at pH 7.2 and 50 °C. Modified zeolites (Ba-ZSM-5 and Ba-MOR, Sr-ZSM-5 and Sr-MOR) were coated with an inert metal (Pt) by a novel supercritical CO2 method using PtMe2COD as a precursor for n-hexane hydroisomerization in a microreactor unit at different temperatures (250–325 °C), H2/HC ratios of 3, 6, and 9, and a pressure of 5 bar. The acidic and physical features of Pt loaded zeolites were systematically characterized using FT-IR, XRD, BET surface area measurements, TGA, and TEM techniques. It is found that the metal loading in scCO2 results in more uniform and very small metal nanoparticle (1.37 nm) dispersion with high stability after reduction. It is also revealed that high loading pressure in scCO2 (280–300 bar) results in higher catalytic activity and surface area. The maximum conversion and selectivity of about 80 and 90% were achieved for n-hexane isomerization at 275 °C and a H2/HC ratio of 6 for Pt/Sr-ZSM-5 catalyst. Results reported that Pt loaded over all zeolites (H-MOR, Sr-MOR, Ba-MOR, H-ZSM-5, Ba-ZSM-5, and Sr-ZSM-5) by the scCO2 method showed the minimum production of cracking products (C1–C5) and maximum isomeric products including iso-C6 isomers (2,2-DMB, 2,3-DMB, 2-MP, and 3-MP). Furthermore, the overall results of the rate of reaction revealed that Pt/Sr-ZSM-5 and Pt/Ba-ZSM-5 catalysts showed a better rate of isomerization (46.44%) and conversion (47%) for n-hexane at 300 °C and a H2/HC ratio of 9 with a minimum rate of cracking. However, it is concluded that the small, pored size Pt loaded ZSM-5 zeolite showed the highest catalytical activity compared to large pored MOR zeolite making it of great interest for diesel and gasoline formation in the oil refining industry.
中文翻译：
铂的催化活性加载沸石用于加氢异构化Ñ正己烷使用超临界二氧化碳2
本研究利用分批的离子交换法和适当的氯化物溶液3来研究新型锶（Sr）和钡（Ba）改性的结晶沸石，包括Socony Mobil-5（ZSM-5）和Mordenite（MOR）沸石。 N在pH 7.2和50°C下。改性沸石（BA-ZSM-5和Ba-MOR，SR-ZSM-5和Sr-MOR）用超临界新颖CO涂覆有惰性金属（Pt）的2使用PTME方法2 COD作为前体Ñ己烷微反应器单元在不同温度（250–325°C），H 2下的加氢异构化/ HC比为3、6和9，压力为5 bar。使用FT-IR，XRD，BET表面积测量，TGA和TEM技术系统地表征了载Pt沸石的酸性和物理特性。发现scCO 2中的金属负载导致还原后具有更高稳定性的更均匀和非常小的金属纳米颗粒（1.37 nm）分散体。还发现scCO 2（280–300 bar）中的高加载压力会导致更高的催化活性和表面积。的约80和90％的最大转化率和选择性分别为实现Ñ在275℃以及H -己烷异构化2Pt / Sr-ZSM-5催化剂的/ HC比为6。结果报告说，通过scCO 2方法在所有沸石（H-MOR，Sr-MOR，Ba-MOR，H-ZSM-5，Ba-ZSM-5和Sr-ZSM-5）上负载的Pt显示出裂解产物（C 1 –C 5）和最大异构产物，包括iso -C 6异构体（2,2-DMB，2,3-DMB，2-MP和3-MP）。此外，反应速率的总体结果显示了Pt / SR-ZSM-5和Pt / BA-ZSM-5催化剂显示异构化（46.44％）和转化率（47％）的一个更好的速率Ñ己烷在300 °C和H 2/ HC比为9，且最小裂化速率。然而，得出的结论是，与大孔径的MOR沸石相比，小孔径的负载Pt的Pt ZSM-5沸石显示出最高的催化活性，这使其在炼油工业中对柴油和汽油的形成产生了极大的兴趣。
更新日期：2020-12-23
中文翻译：
铂的催化活性加载沸石用于加氢异构化Ñ正己烷使用超临界二氧化碳2
本研究利用分批的离子交换法和适当的氯化物溶液3来研究新型锶（Sr）和钡（Ba）改性的结晶沸石，包括Socony Mobil-5（ZSM-5）和Mordenite（MOR）沸石。 N在pH 7.2和50°C下。改性沸石（BA-ZSM-5和Ba-MOR，SR-ZSM-5和Sr-MOR）用超临界新颖CO涂覆有惰性金属（Pt）的2使用PTME方法2 COD作为前体Ñ己烷微反应器单元在不同温度（250–325°C），H 2下的加氢异构化/ HC比为3、6和9，压力为5 bar。使用FT-IR，XRD，BET表面积测量，TGA和TEM技术系统地表征了载Pt沸石的酸性和物理特性。发现scCO 2中的金属负载导致还原后具有更高稳定性的更均匀和非常小的金属纳米颗粒（1.37 nm）分散体。还发现scCO 2（280–300 bar）中的高加载压力会导致更高的催化活性和表面积。的约80和90％的最大转化率和选择性分别为实现Ñ在275℃以及H -己烷异构化2Pt / Sr-ZSM-5催化剂的/ HC比为6。结果报告说，通过scCO 2方法在所有沸石（H-MOR，Sr-MOR，Ba-MOR，H-ZSM-5，Ba-ZSM-5和Sr-ZSM-5）上负载的Pt显示出裂解产物（C 1 –C 5）和最大异构产物，包括iso -C 6异构体（2,2-DMB，2,3-DMB，2-MP和3-MP）。此外，反应速率的总体结果显示了Pt / SR-ZSM-5和Pt / BA-ZSM-5催化剂显示异构化（46.44％）和转化率（47％）的一个更好的速率Ñ己烷在300 °C和H 2/ HC比为9，且最小裂化速率。然而，得出的结论是，与大孔径的MOR沸石相比，小孔径的负载Pt的Pt ZSM-5沸石显示出最高的催化活性，这使其在炼油工业中对柴油和汽油的形成产生了极大的兴趣。
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