有序介孔炭负载Pt-MoO_(x)催化剂的制备及其催化甲基环己烷脱氢性能  

SYNTHESIZE OF ORDERED MESOPOROUS CARBON SUPPORTED Pt-MoO_(x) CATALYST AND ITS CATALYTIC PERFORMANCE FOR METHYLCYCLOHEXANE DEHYDROGENATION

作　　者：王森[1,2] 孟繁春 李卓 杨慧敏 代晓敏[3] 白靖 许云华 覃勇 张斌[1] Wang Sen;Meng Fanchun;Li Zhuo;Yang Huimin;Dai Xiaomin;Bai Jing;Xu Yunhua;Qin Yong;Zhang Bin(Chinese Academy of Sciences,Taiyuan 030001;University of Chinese Academy of Sciences;Yulin University)

机构地区：[1]中国科学院山西煤炭化学研究所,太原030001 [2]中国科学院大学 [3]榆林学院

出　　处：《石油炼制与化工》2024年第9期33-41,共9页Petroleum Processing and Petrochemicals

基　　金：国家自然科学基金资助项目(22072172);国家杰出青年科学基金资助项目(21825204);中国科学院青年创新促进会资助项目(Y2021056);榆林学院与大连清洁能源国家实验室合作基金资助项目(YLU-DNL Fund 2022007);山西省科技创新团队专项资金资助项目(202304051001007)。

摘　　要：以有序介孔炭(CMK-3)作为载体,采用原子层沉积技术制备出催化剂y Pt CMK-3及MoO_(x)助剂调控催化剂y Pt-z MoO_(x)CMK-3(y、z分别为Pt和MoO_(x)的沉积循环次数),研究了沉积循环次数对Pt金属分散度和催化剂甲基环己烷脱氢性能的影响。结果表明,适中的Pt分散度和适量原子级分散的MoO_(x)助剂能显著提升Pt基催化剂的性能。与10Pt CMK-3相比,10Pt-1MoO_(x)CMK-3催化剂上的脱氢速率(单位时间内单位质量Pt产生H_(2)的物质的量)从79.02 mol(g·h)提高至97.88 mol(g·h),甲基环己烷转化率由71%提高到91%。MoO_(x)助剂加入对Pt颗粒分散度影响较小,主要提高了Pt表面电子密度,降低了催化剂的起活温度。此外,MoO_(x)助剂还通过氢溢流促进H_(2)在催化剂表面的脱附,从而提高H_(2)产率。Using ordered mesoporous carbon(CMK-3)as a carrier,y Pt CMK-3 and MoO_(x) additive-modulated catalyst y Pt-z MoO_(x) CMK-3(y and z are the number of deposition cycles of Pt and MoO_(x),respectively)were prepared by atomic layer deposition technology.The impact of the number of deposition cycles on the dispersion of the Pt metal and the catalytic performance for the dehydrogenation of methylcyclohexane was studied.The results showed that optimal Pt dispersion and an appropriate amount of atomically dispersed MoO_(x) additives could significantly improved the performance of Pt-based catalysts.Compared with 10Pt CMK-3,the dehydrogenation rate(amount of H_(2) produced per unit mass of Pt per unit time)on the catalyst 10Pt-1MoO_(x) CMK-3 increased from 79.02 mol(g·h)to 97.88 mol(g·h),and the methylcyclohexane conversion rate increased from 71%to 91%.The addition of MoO_(x) additive had little effect on the dispersion of Pt nanoparticles,mainly increased the electron density on the Pt surface and decreased the activation temperature of catalyst.In addition,the MoO_(x) additives can promote the desorption of H_(2) on the catalyst surface through hydrogen overflow,thus increasing the yield of H_(2).

关 键 词：甲基环己烷 有机液态储氢载体 脱氢催化剂 助剂 有序介孔炭 

分 类 号：TQ116.2[化学工程—无机化工] TQ426