摘要
CO_(2)过量排放导致全球气候异常,通过CO_(2)催化加氢将CO_(2)转化为具有高附加值的基础化学品或燃料是实现碳循环的有效方式,同时也有助于实现我国的“碳中和”目标。本文报道了基于稻谷壳前体制备具有多层次、相互贯通的介孔及大孔结构的bio-SAPO-34分子筛,该结构有利于反应过程中反应中间体的传质。本文系统地研究了分子筛前体液浓度、微孔导向剂种类及浓度、生物模板加入量等因素对bio-SAPO-34合成过程中维持生物模板分级结构的影响规律。将bio-SAPO-34与ZnZrOx固溶体氧化物组装构筑ZnZrO_(x)&bio-SAPO-34双功能催化剂用于催化CO_(2)加氢制备低碳烯烃反应。在380℃、3MPa的反应条件下,双功能催化剂的CO_(2)转化率为11.8%,低碳烯烃的选择性为66.4%(占烃类产物),且经过连续反应60h后未发现催化剂明显失活。
The excessive emission of greenhouse gas CO_(2) has caused global climate change.Catalytic conversion of CO_(2) via hydrogenation is a promising route for the achievement of carbon circular economy and carbon neutralization target.In this study,the bio-SAPO-34 with multiple meso-and macro-structures was synthesized by using rice husk as the bio-template.The hierarchical structure of bio-SAPO-34 facilitated the diffusion of reaction intermediates and improved the catalytic activity.The effect of synthesis parameters such as precursor concentration,structure-directing agent and the amount of rice husks on the replication the architecture of rice husks biotemplate have been systematically studied.Moreover,the ZnZrO_(x) was composited with bio-SAPO-34 to form ZnZrOx&bio-SAPO-34 bifunctional catalyst for CO_(2) hydrogenation to light olefins.Under reaction conditions of 380℃and 3MPa,the selectivity of low olefins was 66.4%(in hydrocarbon products)with a CO_(2) conversion of 11.8%.Furthermore,the obtained ZnZrOx&bio-SAPO-34 bifunctional catalysts showed excellent stability in a 60h long-term test.
作者
李雯
詹国武
黄加乐
李清彪
LI Wen;ZHAN Guowu;HUANG Jiale;LI Qingbiao(College of Advanced Manufacturing,Fuzhou University,Jinjiang 362200,Fujian,China;College of Chemical Engineering,Huaqiao University,Xiamen 361021,Fujian,China;College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,Fujian,China)
出处
《化工进展》
EI
CAS
CSCD
北大核心
2022年第3期1298-1308,共11页
Chemical Industry and Engineering Progress
基金
福州大学贵重仪器设备开放测试基金(2022T027)
国家自然科学基金(21908073,22038012)。
关键词
二氧化碳
生物模板
分子筛
催化
还原
carbon dioxide
biotemplating
molecular sieves
catalysis
reduction
