Impact of Macroporosity on Catalytic Upgrading of Fast Pyrolysis Bio-Oil by Esterification over Silica Sulfonic Acids.
Impact of Macroporosity on Catalytic Upgrading of Fast Pyrolysis Bio-Oil by Esterification over Silica Sulfonic Acids.
复制标题
DOI：
10.1002/cssc.201700959
复制
发表时间：
2017-09-11
期刊：
影响因子：
8.4
通讯作者：
Wilson K
中科院分区：
文献类型：
--
作者：
Manayil JC;Osatiashtiani A;Mendoza A;Parlett CMA;Isaacs MA;Durndell LJ;Michailof C;Heracleous E;Lappas A;Lee AF;Wilson K
快速热解生物油具有不利的理化性质和稳定性差，这在很大程度上是由于羧酸的存在，这阻碍了它们作为生物燃料的使用。催化酯化提供了一种原子效率和能量效率高的途径来升级热解生物油。丙基磺酸 (PrSO3H) 二氧化硅对羧酸酯化具有活性，但对于大体积基材存在传质限制。大孔（200 nm）的加入增强了介孔SBA-15结构（通过热液盐水促进的接枝进行后功能化）对直链羧酸酯化的活性，随着羧酸链长度从5 %（C3）到110 %（C12），周转频率（TOF）增强的幅度增加。大孔-介孔 PrSO3H/SBA-15 还比其介孔类似物提供两倍的 TOF 增强，用于从木片中提取的真正的热快速热解生物油的酯化。通过GC×GC-飞行时间质谱（GC×GC-ToFMS）测定，总酸值降低了57％，这表明随着酸、酚、醛和酮组分的损失，酯和醚形成。
Fast pyrolysis bio‐oils possess unfavorable physicochemical properties and poor stability, in large part, owing to the presence of carboxylic acids, which hinders their use as biofuels. Catalytic esterification offers an atom‐ and energy‐efficient route to upgrade pyrolysis bio‐oils. Propyl sulfonic acid (PrSO3H) silicas are active for carboxylic acid esterification but suffer mass‐transport limitations for bulky substrates. The incorporation of macropores (200 nm) enhances the activity of mesoporous SBA‐15 architectures (post‐functionalized by hydrothermal saline‐promoted grafting) for the esterification of linear carboxylic acids, with the magnitude of the turnover frequency (TOF) enhancement increasing with carboxylic acid chain length from 5 % (C3) to 110 % (C12). Macroporous–mesoporous PrSO3H/SBA‐15 also provides a two‐fold TOF enhancement over its mesoporous analogue for the esterification of a real, thermal fast‐pyrolysis bio‐oil derived from woodchips. The total acid number was reduced by 57 %, as determined by GC×GC–time‐of‐flight mass spectrometry (GC×GC–ToFMS), which indicated ester and ether formation accompanying the loss of acid, phenolic, aldehyde, and ketone components.
登录
查看更多内容
影响因子：
8.4
作者：
Keller, Tobias C.;Rodrigues, Elodie G.;Perez-Ramirez, Javier
通讯作者：
Perez-Ramirez, Javier
影响因子：
7.4
作者：
Li, Xiang;Gunawan, Richard;Li, Chun-Zhu
通讯作者：
Li, Chun-Zhu
影响因子：
5.3
作者：
Czernik, S;Bridgwater, AV
通讯作者：
Bridgwater, AV
影响因子：
7.4
作者：
Alcala, A.;Bridgwater, A. V.
通讯作者：
Bridgwater, A. V.
影响因子：
3.9
作者：
Duan, Xixin;Liu, Yue;Li, Shiwu
通讯作者：
Li, Shiwu