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Chloroform conversion into ethane and propane by catalytic hydrodechlorination with Pd supported on activated carbons from lignin†
Catalysis Science & Technology ( IF 5 ) Pub Date : 2018-07-04 00:00:00 , DOI: 10.1039/c8cy00461g
C. Fernandez-Ruiz 1, 2, 3, 4, 5 , J. Bedia 1, 2, 3, 4, 5 , P. Bonal 1, 2, 3, 4, 5 , J. J. Rodriguez 1, 2, 3, 4, 5 , L. M. Gómez-Sainero 1, 2, 3, 4, 5
Affiliation  

Conversion of chloroform (TCM) by gas-phase catalytic hydrodechlorination (HDC) has been addressed to maximize the selectivity to ethane and propane. Several own-made Pd (1 wt%) catalysts have been tested. The catalysts were prepared by incipient wetness impregnation of five different activated carbons. These carbons were obtained by chemical activation of lignin with different activating agents, namely, H3PO4, ZnCl2, FeCl3, NaOH and KOH. The catalysts were fully characterized by N2 adsorption–desorption at −196 °C, CO2 adsorption at 0 °C, TPR, NH3-TPD, XRD, XPS and TEM. The activating agents provided important differences in the characteristics of activated carbon supports, and hence in the resulting catalysts, in terms of their porous texture, surface acidity, Pd oxidation state and Pd particle size distribution. NaOH and KOH activation led to carbons with the highest surface areas (2158 and 2991 m2 g−1, respectively) and low Pd0/Pdn+ ratios, while ZnCl2- and H3PO4-activated carbons yielded the highest surface acidity and mean Pd particle sizes. The analysis of the TOF values revealed that the HDC of TCM on these catalysts is a structure-sensitive reaction, increasing TOF values with Pd particle size. The best results, in terms of selectivity to ethane and propane, were obtained with the catalysts supported on KOH- and NaOH-activated carbons. The former allowed 80% selectivity to the target compounds at almost complete dechlorination (>99%) at 300 °C. The KOH-based catalyst showed fairly good stability at a reaction temperature of 200 °C.

中文翻译:

氯仿转化成乙烷和丙烷通过用Pd催化加氢脱氯支撑在从木质素活性炭

已经解决了通过气相催化加氢脱氯(HDC)进行氯仿(TCM)的转化,以最大程度地提高对乙烷和丙烷的选择性。已测试了几种自制的Pd(1 wt%)催化剂。通过对五个不同的活性炭进行初湿浸渍来制备催化剂。这些碳是通过用不同的活化剂,即H 3 PO 4,ZnCl 2,FeCl 3,NaOH和KOH对木质素进行化学活化而获得的。催化剂具有以下特征:在-196°C下可进行N 2吸附-解吸,在0°C下可进行CO 2吸附,TPR,NH 3-TPD,XRD,XPS和TEM。活化剂在活性炭载体的特性上,因此在所得催化剂上,就其多孔质地,表面酸度,Pd氧化态和Pd粒度分布而言,提供了重要的差异。NaOH和KOH活化导致碳具有最高的表面积(分别为2158和2991 m 2 g -1)和低的Pd 0 / Pd n +比,而ZnCl 2-和H 3 PO 4活化的碳产生最高的表面酸度和平均Pd粒径。TOF值的分析表明,在这些催化剂上,TCM的HDC是结构敏感的反应,随着Pd粒径的增加,TOF值增加。就对乙烷和丙烷的选择性而言,用负载在KOH和NaOH活性炭上的催化剂可获得最佳结果。前者在300°C下几乎完全脱氯(> 99%)时,对目标化合物的选择性为80%。基于KOH的催化剂在200℃的反应温度下显示出相当好的稳定性。
更新日期:2018-07-04
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