文献类型：期刊文献

英文题名：Direct Transformation of Glycerol to Propanal using Zirconium Phosphate-Supported Bimetallic Catalysts

作者：Gong, Honghui[1];Zhou, Chuan[1];Cui, Yan[2,3];Dai, Sheng[2,3];Zhao, Xiuge[1];Luo, Ruihan[1];An, Pengfei[4];Li, Huan[5];Wang, Haifeng[1];Hou, Zhenshan[1]

机构：[1]East China Univ Sci & Technol, Key Lab Adv Mat, Res Inst Ind Catalysis, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[2]East China Univ Sci & Technol, Key Lab Adv Mat, Shanghai 200237, Peoples R China;[3]East China Univ Sci & Technol, Feringa Nobel Prize Scientist Joint Res Ctr, Inst Fine Chem, Sch Chem & Mol Engn, Shanghai 200237, Peoples R China;[4]Chinese Acad Sci, Inst High Energy Phys, Beijing Synchrotron Radiat Facil BSRF, Beijing 100049, Peoples R China;[5]Shanxi Univ, Inst Crystalline Mat, Taiyuan 030006, Shanxi, Peoples R China

年份：2020

卷号：13

期号：18

起止页码：4954

外文期刊名：CHEMSUSCHEM

收录：;EI(收录号：20203409078161);WOS:【SCI-EXPANDED(收录号:WOS:000562030800001)】；

基金：The authors are grateful for support from the National Natural Science Foundation of China (21773061, 21978095), the innovation Program of Shanghai Municipal Education Commission (15ZZ031). S. D. acknowledges the support by Shanghai Risingstar Program (20QA1402400). Additional support was provided by Feringa Nobel Prize Scientist Joint Research Center.

语种：英文

外文关键词：cobalt; glycerol hydrogenolysis; propanal; ruthenium; zirconium phosphate

摘要：Selective transformation of glycerol to propanal (PA) provides a feasible route towards the sustainable synthesis of high value-added chemicals. In this work, zirconium phosphate (ZrP) was studied as support and Ru and Co as metal sites for glycerol hydrogenolysis in a continuous-flow reactor. It was found that ZrP-supported Co-O species had a moderate selectivity to PA (49.5 %) in glycerol hydrogenolysis. Notably, once Ru species were doped into CoO/ZrP, the resulting catalyst exhibited not only an outstanding catalytic performance for glycerol hydrogenolysis to PA (a selectivity of 80.2 % at full conversion), but also a high stability at least a 50 h long-term performance. The spent catalyst could be regenerated by calcining in air to remove carbonaceous deposits. Characterization indicated that the acid sites on ZrP played a very critical role in the dehydration of glycerol into acrolein (AE), that the distribution of Co was uniform, basically consistent with that of Zr, P and Ru, and that an especially close contact between Co-O and Ru species was formed on Ru/CoO/ZrP catalyst. The further activity tests and characterizations confirmed that there was a strong interaction between the dispersed Co-O species and Ru(0)nanoparticles, which endowed Ru sites with high electronic density. This effect could play a role in facilitating the dissociation of H-2, and thus in promoting the hydrogenation reaction. Besides, DFT calculations suggested that the Co-O species can adsorb more strongly the C=C bond of the intermediate AE on a highly coordinatively unsaturated Co (Co-cus) site and thus lead to preferential hydrogenation at the C=C bond of AE to PA.