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Application of silica-supported Ir and Ir-M (M = Pt, Pd, Au) catalysts for low-temperature hydrodechlorination of tetrachloromethane

机译:二氧化硅负载的Ir和Ir-M(M = Pt,Pd,Au)催化剂在四氯甲烷低温加氢脱氯中的应用

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Herein, it is presented a catalytic system for gas-phase hydrodechlorination of tetrachloromethane at low temperature and atmospheric pressure, using iridium supported on silica as parent catalyst. Iridium electronic configuration is suitable to catalyse the hydrodechlorination reactions, however, it has been rarely used in this reaction to date. The catalytic abilities were significantly improved when a second transition metal was added. Catalysts' stability and selectivity to the desired products (i.e. C-1-C-4 hydrocarbons) improved compared to conventional activation in hydrogen when catalysts were activated shortly with microwave irradiation. Microwave irradiation of catalysts favourably influences the homogeneity of the metallic active phase, both in terms of the size of metal crystals and the homogeneity of bimetallic systems. Addition of platinumto the 'parent' iridium catalyst improved its catalytic properties and decreased deactivation. Fresh and spent catalysts were comprehensively characterized using several techniques (BET, CO-chemisorption, XRD, XPS, electron microscopy and mass spectrometry) to determine structure-activity relationships and potential causes for catalyst deactivation. No significant changes in crystalline size or bimetallic phase composition were observed for spent catalysts (with the exception of Ir-Pd catalysts which underwent bulk carbide during the reaction). (C) 2018 Elsevier B.V. All rights reserved.
机译:在此,提出了使用负载在二氧化硅上的铱作为母体催化剂在低温和大气压下对四氯甲烷进行气相加氢脱氯的催化体系。铱电子构型适合于催化加氢脱氯反应,然而,迄今为止该反应中很少使用铱。当添加第二过渡金属时,催化能力显着提高。当用微波辐射不久将催化剂活化时,与常规的氢活化相比,催化剂对所需产物(即C-1-C-4烃)的稳定性和选择性得到改善。催化剂的微波辐射在金属晶体的大小和双金属体系的均质性方面均有利地影响金属活性相的均质性。将铂添加到“母体”铱催化剂中可改善其催化性能并减少失活。使用几种技术(BET,CO化学吸附,XRD,XPS,电子显微镜和质谱法)对新鲜和用过的催化剂进行了全面表征,以确定其结构活性关系和催化剂失活的潜在原因。对于用过的催化剂(在反应过程中经历块状碳化物的Ir-Pd催化剂除外),没有观察到晶体尺寸或双金属相组成的显着变化。 (C)2018 Elsevier B.V.保留所有权利。

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