A CaMnAl-hydrotalcite solid basic catalyst toward the aldol condensation reaction with a comparable level to liquid alkali catalysts

doi:10.1039/c8gc00851e

	A CaMnAl-hydrotalcite solid basic catalyst toward the aldol condensation reaction with a comparable level to liquid alkali catalysts
	Zheng, L; Bing, WH; Wang, HM; Zheng L(郑雷); Zheng LR(郑黎荣); Rao, DM; Yang, YS; Zheng, LR; Wang, B; Wang, YD
刊名	GREEN CHEMISTRY
	2018
卷号	20 期号:13 页码:3071-3080
ISSN号	1463-9262
DOI	10.1039/c8gc00851e
文献子类	Article
英文摘要	In a number of heterogeneous catalysis processes, the promotion effect toward active sites is of vital importance and remains a challenge to obtain largely-improved catalytic performance. Herein, rehydrated Ca4MnxAl-layered double hydroxides (denoted as re-Ca4MnxAl-LDH) were prepared based on a structure memory effect of LDH precursors, which exhibited extremely high heterogeneous catalytic performance for the aldol condensation reaction, with the assistance of the promotion effect of Mn. A combination study including XRD, EXAFS, XPS, CDCl3-FTIR and DFT calculations confirms that re-Ca4MnxAl-LDH samples with Ca-O-Mn-IV structure show a highly-exposed Ca2+ s-orbital and strengthened coordination between Ca2+ with 7-fold OH-, providing a weakened BrOnsted basic site compared with the reference sample re-Ca4Al-LDH. The optimized re-Ca4Mn0.5Al-LDH catalyst exhibits prominent catalytic performance toward the condensation of isobutyraldehyde (IBD) and formaldehyde (FA) to produce hydroxypivaldehyde (HPA), with a HPA yield of 70.3%. This is significantly higher than re-Ca4Al-LDHs (63.3%) and even comparable to the level of liquid alkali catalysts (73.2%). Studies on the structure-property correlation reveal that the weakened basic site originating from Ca-O-Mn-IV serves as a promoted active center, which accelerates the product desorption and thus largely improves HPA selectivity. This promoted re-Ca4Mn0.5Al-LDH catalyst can be potentially applied as a promising candidate in heterogeneous aldol condensation reactions.
电子版国际标准刊号	1463-9270
WOS关键词	BIRNESSITE-TYPE MNO2 ; OXIDATION ; TEMPERATURE ; ACETONE ; FORMALDEHYDE ; METHANOL ; COMPLEX ; VACANCY
WOS研究方向	Chemistry ; Science & Technology - Other Topics
语种	英语
WOS记录号	WOS:000437187500018
内容类型	期刊论文
源URL	[http://ir.ihep.ac.cn/handle/311005/286088]
专题	高能物理研究所_多学科研究中心
通讯作者	Zheng LR(郑黎荣)
作者单位	中国科学院高能物理研究所
推荐引用方式 GB/T 7714	Zheng, L,Bing, WH,Wang, HM,et al. A CaMnAl-hydrotalcite solid basic catalyst toward the aldol condensation reaction with a comparable level to liquid alkali catalysts[J]. GREEN CHEMISTRY,2018,20(13):3071-3080.
APA	Zheng, L.,Bing, WH.,Wang, HM.,郑雷.,郑黎荣.,...&Wei, M.(2018).A CaMnAl-hydrotalcite solid basic catalyst toward the aldol condensation reaction with a comparable level to liquid alkali catalysts.GREEN CHEMISTRY,20(13),3071-3080.
MLA	Zheng, L,et al."A CaMnAl-hydrotalcite solid basic catalyst toward the aldol condensation reaction with a comparable level to liquid alkali catalysts".GREEN CHEMISTRY 20.13(2018):3071-3080.