摘要
合成了含硝酸根离子的脱水Ni-Fe类水滑石(Ni-Fe HTLCs)并将其应用于室温下的糠醛缩醛化反应。脱水Ni-Fe HTLCs对糠醛缩醛化反应显示出高选择性并基本实现糠醛的完全转化。作为耐水的路易斯酸和脱水剂,脱水Ni-Fe HTLCs被证明是适用于糠醛缩醛化反应的高效双功能催化剂。通过研究发现,脱除Ni-Fe HTLCs中水分导致颗粒收缩并增强层板间硝酸根离子间的电荷互斥,Ni-Fe HTLCs中弱酸性位点在糠醛缩醛化中发挥重要作用,脱水可改变酸性位点结构并增强其活性。脱水Ni-Fe HTLCs可吸收缩醛化反应中产生的大部分水分,但吸水后Ni-Fe HTLCs的结构并不能完全恢复,这可能是由扩散进入HTLCs层板间的有机分子导致。
The dehydrated Ni-Fe hydrotalcite-like compounds(Ni-Fe HTLCs) containing nitrate anions were synthesized and applied in furfural acetalization at room temperature.The dehydrated Ni-Fe HTLCs showed good selectivity for furfural acetalization and achieved almost complete conversion of furfural.The dehydrated Ni-Fe HTLCs as water-tolerant Lewis acids and water scavengers was proved to be an efficient bifunctional catalyst for furfural acetalization.The removal of interlayer water leads to shrinkage of Ni-Fe HTLCs particles and increase in electronic repulsion among NO;ions in the interlayer.The weak acid sites in Ni-Fe HTLCs play an important role in furfural acetalization.The dehydration changes structure of the acid sites and thus improves activity of the weak acid sites.The dehydrated Ni-Fe HTLCs can absorb the most of the resulting water during furfural acetalization,but the structure of Ni-Fe HTLCs cannot completely recover after rehydration possibly due to hindering effect of organic molecules diffusing into interlayer space.
作者
程淑艳
寇佳伟
程芳琴
CHENG Shu-Yan;KOU Jia-Wei;CHENG Fang-Qin(State Key Laboratory of Clean and Efficient Coal Utilization,Taiyuan University of Technology,Taiyuan 030024,China;College of Environmental&Resource Science,Shanxi University,Taiyuan 030013,China;Shanxi Laboratory for Yellow River,Shanxi University,Taiyuan 030013,China)
出处
《无机化学学报》
SCIE
CAS
CSCD
北大核心
2021年第11期2092-2100,共9页
Chinese Journal of Inorganic Chemistry
基金
国家自然科学基金(No.22108161)
山西省青年科学基金(No.201901D211297)资助。
关键词
类水滑石
糠醛
缩醛
双功能催化剂
生物油
hydrotalcite-like compound
furfural
acetal
bifunctional catalyst
bio-oil
