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
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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 |
DOI | 10.1021/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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来源:高能物理研究所
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