Ru/AC和Ru-NPs/AC催化剂对乙炔氢氯化反应催化活性的比较OA北大核心CSTPCD
Comparison of catalytic activity of Ru/AC and Ru-NPs/AC catalysts for acetylene hydrochlorination
针对乙炔氢氯化反应无汞催化剂的开发,Ru基催化剂是最具工业潜力的催化剂之一.结合表面积分析仪(BET)、程序升温还原(TPR)、透射电镜(TEM)和程序升温脱附(TPD),以及动力学实验探究了导致Ru/AC(AC为活性炭)和高温H2处理后Ru-NPs/AC催化性能差异的原因.在排除内、外扩散的条件下,通过动力学实验判断了反应级数,初步推测了基元反应步骤和决速步骤.结果表明,Ru-NPs/AC相对于Ru/AC总反应速率更低,表观活化能更高,这是由于高温H2处理后活性组分的分散度降低、Ru物种被还原,并且导致活性中心对C2H2的吸附性能降低.
Ru-based catalysts are one of the most applicable catalysts in industry for the development of mercury-free acetylene hydrochlorination catalysts.The difference of catalytic performance between Ru/AC and Ru-NPS/AC after the high-temperature H2 treatment was investigated by Brunauer-Emmett-Teller(BET),temperature programmed reduction(TPR),transmission electron microscopy(TEM),temperature programmed desorption(TPD)and kinetic experiments.By exclusion of internal and external diffusion,the reaction orders were investigated by kinetic experiments,and the elementary reaction steps and velocity determination steps were preliminarily proposed.The results show that Ru-NPS/AC demonstrates lower catalytic activity than Ru/AC for acetylene hydrochlorination with a higher apparent activation energy,which is due to the decrease of active center dispersion and the reduction of Ru species after high-temperature H2 treatment.It results in the decrease of C2H2 adsorption capacity of active center.
徐达;王赛赛;马腾云;万立祺;赵佳;蔡海婷;李小年
浙江工业大学 化学工程学院,浙江 杭州 310014
化学
乙炔氢氯化Ru基催化剂反应级数表观活化能活性中心
acetylene hydrochlorinationRu-based catalystreaction orderapparent activation energyactive center
《高校化学工程学报》 2024 (004)
578-585 / 8
国家自然科学基金(22208299);国家重点研发计划(2021YFA1501801).
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