生物质化学工程 ›› 2023, Vol. 57 ›› Issue (1): 62-72.doi: 10.3969/j.issn.1673-5854.2023.01.008
收稿日期:
2021-11-17
出版日期:
2023-01-30
发布日期:
2023-02-03
通讯作者:
徐琼
E-mail:1650685779@qq.com;xuqiong@hunnu.edu.cn
作者简介:
徐琼, 教授, 硕士生导师, 研究领域: 生物质转化; E-mail: xuqiong@hunnu.edu.cn基金资助:
Jianhua WANG(), Sisi ZHANG, Yuting ZHUANG, Qiong XU(), Dulin YIN
Received:
2021-11-17
Online:
2023-01-30
Published:
2023-02-03
Contact:
Qiong XU
E-mail:1650685779@qq.com;xuqiong@hunnu.edu.cn
摘要:
γ-戊内酯(GVL)是一种重要的生物质平台化合物, 可以用作绿色溶剂、聚合物前体、燃料和燃料添加剂等, 催化转化生物质制备GVL是资源化利用生物质和缓解资源、能源危机的重要途径之一。糠醛经麦尓外因-彭多夫-沃莱(MPV)还原一锅制备GVL具有操作简单、经济环保、安全可靠等优点, 是GVL合成研究领域极具工业化潜质的路线, 受到学术界和工业界的广泛关注。本文阐述了糠醛转化为GVL各步所需Brønsted酸(B酸)和Lewis酸(L酸)催化活性中心, 从催化剂构筑方法、载体结构等方面总结了糠醛一锅法制备GVL的高效固体催化剂。发现水热稳定且具有良好传质效果的分子筛(如beta分子筛、ZSM-5分子筛等)是该反应中常用的载体, 以及通过分子筛脱Al改性, 或引入具有L酸位的Zr、Hf化合物、具有B酸位的磷钨酸(HPW)等活性中心是构筑该反应的高效双功能催化剂的常用手段。并对催化剂失活的原因和再生方法进行了总结, 分析了溶剂、温度等催化反应条件对反应活性的影响, 同时还对设计该反应的新型高效催化提出了建议。
中图分类号:
王建华, 张思思, 庄雨婷, 徐琼, 尹笃林. 糠醛一锅法制备γ-戊内酯的多相催化研究进展[J]. 生物质化学工程, 2023, 57(1): 62-72.
Jianhua WANG, Sisi ZHANG, Yuting ZHUANG, Qiong XU, Dulin YIN. Research Progress on Heterogenous Catalytic Conversion of Furfural to γ-Valerolactone by One-pot Reaction[J]. Biomass Chemical Engineering, 2023, 57(1): 62-72.
表1
物理混合催化剂催化糠醛制GVL1)"
催化剂 catalyst | 催化剂比例 ratio of catalysts | m(糠醛)/m(催化剂) m(FAL)/m(catalyst) | 最优条件 optimum conditions | GVL产率/% GVL yield | 文献 ref. |
Zr-beta分子筛+Al-MFI-ns分子筛 Zr-beta molecular sieve and Al-MFI nanosheets | n(Zr)∶ n(Al)=16 | — | 120 ℃,24 h, V(2-丁醇)/V(水)=95/5 12-butanol, 2-butanol to water volume ratio of 95/5 | 62 | [ |
Zr-HY分子筛+Al-HY分子筛 Zr-HY molecular sieve and Al-HY molecular sieve | m(Zr-HY)∶ m(Al-HY)=2 | 2 | 120 ℃,5 h,2-戊醇2-pentanol | 85 | [ |
Hf-MOF-808+Al-beta分子筛 Hf-MOF-808 and Al-beta molecular sieve | — | — | 120 ℃,10 h,2-丁醇2-butanol | 51 | [ |
Au/ZrO2+H-ZSM-5分子筛 Au/ZrO2+H-ZSM-5 molecular sieve | m(Au/ZrO2)∶ m(H-ZSM-5)=1 | 0.12 | 120 ℃,30 h,2-丙醇2-propanol | 80.4 | [ |
壳聚糖-Ru/PPh3+H-ZSM-5分子筛 chitosan-loaded Ru, PPh3 and H-ZSM-5 molecular sieves | — | — | 160 ℃,30 h, V(乙醇)/V(甲酸)=95/5 ethanol and formic acid volume ratio of 95/5 | 79 | [ |
表2
双功能催化剂催化糠醛制GVL1)"
催化剂 catalyst | B与L酸量比 B and L acid content ratio | m(糠醛)/m(催化剂) m(FAL)/m(catalyst) | 反应条件 reaction conditions | GVL产率/% GVL yield | 文献 ref. |
ZrO2-[Al]MFI-ns分子筛 ZrO2[Al]MFI nanosponge | 0.035 | 2.5 | 170 ℃,36 h,2-丙醇2-propanol | 82.8 | [ |
Zr-Al-beta分子筛 (n(Al)∶n(Zr)=0.2) Zr-Al-beta molecular sieve | 0.05 | 1.2 | 170 ℃,4 h,2-丙醇2-propanol | 70 | [ |
介孔Zr-Al-beta分子筛 (n(Al)∶n(Zr)=0.77) mesoporous Zr-Al-beta molecular sieve | ~0.5 | 0.4 | 120 ℃,24 h,2-丙醇2-propanol,5%水5% water | 95 | [ |
Sn-Al-beta分子筛 (n(Al)∶n(Sn)=7.5) Sn-Al-beta molecular sieve | ~0.55 | 1.32 | 180 ℃,24 h,2-丁醇2-butanol | 60 | [ |
Zr-Al-beta分子筛 (n(Al)∶n(Zr)=0.22) Sn-Al-beta molecular sieve | — | 2.5 | 170 ℃,24 h,2-丙醇2-propanol | 22.6 | [ |
Zr-Al-SCM-1分子筛 Zr-Al-SCM-1 molecular sieve | 0.46 | 2.0 | 170 ℃,28 h,2-丙醇2-propanol | 47.3 | [ |
Zr-KIT-5(10) | 0.15 | 0.96 | 180 ℃,6 h,2-丙醇2-propanol | 40.1 | [ |
HPW/Zr-beta分子筛 HPW/Zr-beta molecular sieve | 0.31 | 2.5 | 160 ℃,24 h,2-丙醇2-propanol | 70 | [ |
ZrO2-HPW-beta分子筛 ZrO2-HPW-beta molecular sieve | 0.65 | 1.3 | 170 ℃,10 h,2-丙醇2-propanol | 90 | [ |
HPW/ZrO2-SBA-15 | ~0.49 | 1.31 | 170 ℃,11 h,2-丙醇2-propanol | 81 | [ |
Zr-CN/H-bate分子筛 Zr-CN/H-bate molecular sieve | — | 2.2 | 160 ℃,18 h,2-丙醇2-propanol | 76.5 | [ |
FM-Zr-ARS | ~1.89 | 0.48 | 160 ℃,8 h,2-丙醇2-propanol | 72.4 | [ |
Zr-MCM-41@Fe3O4 | — | 0.12 | 130 ℃,30 h,2-丙醇2-propanol | 85.7 | [ |
硫酸化DUT-67(Hf) sulfated DUT-67(Hf) | — | 0.4 | 180 ℃,24 h,2-丙醇2-propanol | 87.1 | [ |
ZrP/H-ZSM-5分子筛 ZrP/H-ZSM-5 molecular sieve | 0.15 | — | 180 ℃,10 h,2-丙醇2-propanol,0.5 MPa N2 | 64.2 | [ |
Zr-P/SAPO-34分子筛 Zr-P/SAPO-34 molecular sieve | ~0.12 | 0.5 | 150 ℃,18 h,2-丙醇2-propanol | 80.0 | [ |
ZrPO-1.50 | — | 1.9 | 210 ℃,5 h,2-丙醇2-propanol,1 MPa N2 | 54.8 | [ |
介孔Al2O3-SO3H+0.1g LiCl mesoporous Al2O3-SO3H and 0.1g LiCl | 4.35 | 1.33 | 120 ℃,4 h,2-丁醇2-butanol, 超声波功率90 W 90W ultrasonic power,占空比60% 60% duty cycle | 85.6 | [ |
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