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Chinese Academy of Sciences Institutional Repositories Grid
Insights on active sites of caal-hydrotalcite as a high-performance solid base catalyst toward aldol condensation

文献类型:期刊论文

作者Bing, Weihan1; Zheng, Lei2; He, Shan1; Rao, Deming1; Xu, Ming1; Zheng, Lirong2; Wang, Bin3; Wang, Yangdong4; Wei, Min1
刊名Acs catalysis
出版日期2018
卷号8期号:1页码:656-664
关键词Caal-hydrotalcite Solid basic catalysts Aldol condensation Hydroxypivaldehyde Structure-activity correlation
ISSN号2155-5435
DOI10.1021/acscatal.7b03022
通讯作者Zheng, lirong(zhenglr@ihep.ac.cn) ; Wang, yangdong(wangyd.sshy@sinopec.com) ; Wei, min(weimin@mail.buct.edu.cn)
英文摘要Solid base catalysts are highly demanded in many heterogeneous catalysis processes, but insights on active sites and structure-property correlation have rarely been revealed and remain a challenge. herein, activated mxal-layered double hydroxides (denoted as re-mxal-ldh, m = ca, mg), as solid base catalysts toward the aldol condensation reaction, were prepared via a two-step procedure: calcination of the mxal-ldh precursor to produce mxal-mixed metal oxide (mxal-mmo), followed by a further rehydration treatment. structural characterizations confirm that re-caxal-ldh and re-mgxal-ldh show similar morphology, particle size, specific surface area, and pore size distribution. however, a combination study including xps, exafs, cdcl3-ftir, and dft calculations verifies that the host layer of re-caxal-ldh contains a distorted ca(oh)(6) octahedron with an additional ca-oh coordination that provides weak bronsted basic site; in contrast, re-mgxal-ldh consists of a mg(oh)(6) octahedron structure accompanied by surface adsorbed hydroxyl group via noncovalent interaction, resulting in a medium bronsted basic site. for the re-caxal-ldh samples, the concentration of weak bronsted basic sites can be enhanced by tuning the ca/al molar ratio in the ldh precursor. the optimized re-caxal-ldh catalyst (re-ca4al-ldh) exhibits prominent catalytic performance toward the condensation of isobutyraldehyde (ibd) and formaldehyde (fa) to produce hydroxypivaldehyde (hpa), with a hpa yield of 61.5%. this is much higher than that of re-mgxal-ldh (12.2%) and conventional solid base catalysts (4-33%), and even comparable to the level of liquid alkali (55-72%). studies on the structure-property correlation reveal that the weak bronsted basic site serves as active center to catalyze the aldol condensation, which accelerates the product desorption and largely promotes the hpa selectivity.
WOS关键词LAYERED DOUBLE HYDROXIDES ; ACETONE SELF-CONDENSATION ; FRIEDELS SALT ; MIXED-OXIDES ; WATER ; HYDROGENATION ; OXIDATION ; PHOSPHATE ; ALCOHOLS ; ALKANES
WOS研究方向Chemistry
WOS类目Chemistry, Physical
语种英语
WOS记录号WOS:000419751100067
出版者AMER CHEMICAL SOC
URI标识http://www.irgrid.ac.cn/handle/1471x/2177906
专题高能物理研究所
通讯作者Zheng, Lirong; Wang, Yangdong; Wei, Min
作者单位1.Beijing Univ Chem Technol, State Key Lab Chem Resource Engn, Beijing Adv Innovat Ctr Soft Matter Sci & Engn, Beijing 100029, Peoples R China
2.Chinese Acad Sci, Inst High Energy Phys, Beijing 100049, Peoples R China
3.Sinopec Grp, Beijing Res Inst Chem Ind, Beijing 100013, Peoples R China
4.SINOPEC Shanghai Res Inst Petrochem Technol, Shanghai 201208, Peoples R China
推荐引用方式
GB/T 7714
Bing, Weihan,Zheng, Lei,He, Shan,et al. Insights on active sites of caal-hydrotalcite as a high-performance solid base catalyst toward aldol condensation[J]. Acs catalysis,2018,8(1):656-664.
APA Bing, Weihan.,Zheng, Lei.,He, Shan.,Rao, Deming.,Xu, Ming.,...&Wei, Min.(2018).Insights on active sites of caal-hydrotalcite as a high-performance solid base catalyst toward aldol condensation.Acs catalysis,8(1),656-664.
MLA Bing, Weihan,et al."Insights on active sites of caal-hydrotalcite as a high-performance solid base catalyst toward aldol condensation".Acs catalysis 8.1(2018):656-664.

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