Dongpei Zhang , Jiefeng Liu , Sicheng Shao , Quanxing Zhang , Mengyuan Liu , Yuangao Wang , Mingyu Ma , Ning Cao , Guangyu Zhang , Jinyao Wang , Junwei Yang , Wenjuan Yan , Xin Jin , Chaohe Yang
{"title":"在协同 Co/ZnO 催化剂上增强 2-庚酮向 2-庚醇的转移加氢反应","authors":"Dongpei Zhang , Jiefeng Liu , Sicheng Shao , Quanxing Zhang , Mengyuan Liu , Yuangao Wang , Mingyu Ma , Ning Cao , Guangyu Zhang , Jinyao Wang , Junwei Yang , Wenjuan Yan , Xin Jin , Chaohe Yang","doi":"10.1016/j.ccst.2024.100227","DOIUrl":null,"url":null,"abstract":"<div><p>2-Heptanol is an important secondary alcohol, applied in food, pharmaceutical and plastic industries. However, current industrial synthetic methods require energy intensive hydrogenation of 2-heptanone using homogeneous noble catalysts in alkaline medium. In this work, we presented a systematic study on enhanced transfer hydrogenation of 2-heptanone to 2-heptanol using non-noble Co/ZnO catalysts without alkaline promoters. The strong synergism of Co and ZnO contributes to formation of amorphous metallic Co species and electronically reconfigured CoO species, leading to a 20-fold activity enhancement at 180 °C and a TOF of 89.4 h<sup>−1</sup> over Co<sub>0.09</sub>/ZnO-500 catalysts. Structure-dependency studies further revealed that, the lattice strain between Co and ZnO induced the generation of multi-phased Co/CoO/Co:ZnO interfaces, facilitating tandem H<sub>2</sub> generation, spillover and activation of C=O bond (of 2-heptanone molecule), respectively. The insights of molecular catalysis on interface of amorphous Co/ZnO for enhanced C=O bond activation, provide fundamental understanding for transfer hydrogenation of various other ketones into valuable alcohols.</p></div>","PeriodicalId":9387,"journal":{"name":"Carbon Capture Science & Technology","volume":"12 ","pages":"Article 100227"},"PeriodicalIF":0.0000,"publicationDate":"2024-05-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S2772656824000393/pdfft?md5=4b16e9ac069b6cc58c07afb18a42cb1a&pid=1-s2.0-S2772656824000393-main.pdf","citationCount":"0","resultStr":"{\"title\":\"Enhanced transfer hydrogenation of 2-heptanone to 2-heptanol over synergistic Co/ZnO catalysts\",\"authors\":\"Dongpei Zhang , Jiefeng Liu , Sicheng Shao , Quanxing Zhang , Mengyuan Liu , Yuangao Wang , Mingyu Ma , Ning Cao , Guangyu Zhang , Jinyao Wang , Junwei Yang , Wenjuan Yan , Xin Jin , Chaohe Yang\",\"doi\":\"10.1016/j.ccst.2024.100227\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>2-Heptanol is an important secondary alcohol, applied in food, pharmaceutical and plastic industries. However, current industrial synthetic methods require energy intensive hydrogenation of 2-heptanone using homogeneous noble catalysts in alkaline medium. In this work, we presented a systematic study on enhanced transfer hydrogenation of 2-heptanone to 2-heptanol using non-noble Co/ZnO catalysts without alkaline promoters. The strong synergism of Co and ZnO contributes to formation of amorphous metallic Co species and electronically reconfigured CoO species, leading to a 20-fold activity enhancement at 180 °C and a TOF of 89.4 h<sup>−1</sup> over Co<sub>0.09</sub>/ZnO-500 catalysts. Structure-dependency studies further revealed that, the lattice strain between Co and ZnO induced the generation of multi-phased Co/CoO/Co:ZnO interfaces, facilitating tandem H<sub>2</sub> generation, spillover and activation of C=O bond (of 2-heptanone molecule), respectively. The insights of molecular catalysis on interface of amorphous Co/ZnO for enhanced C=O bond activation, provide fundamental understanding for transfer hydrogenation of various other ketones into valuable alcohols.</p></div>\",\"PeriodicalId\":9387,\"journal\":{\"name\":\"Carbon Capture Science & Technology\",\"volume\":\"12 \",\"pages\":\"Article 100227\"},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2024-05-23\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.sciencedirect.com/science/article/pii/S2772656824000393/pdfft?md5=4b16e9ac069b6cc58c07afb18a42cb1a&pid=1-s2.0-S2772656824000393-main.pdf\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Carbon Capture Science & Technology\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S2772656824000393\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Carbon Capture Science & Technology","FirstCategoryId":"1085","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S2772656824000393","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
Enhanced transfer hydrogenation of 2-heptanone to 2-heptanol over synergistic Co/ZnO catalysts
2-Heptanol is an important secondary alcohol, applied in food, pharmaceutical and plastic industries. However, current industrial synthetic methods require energy intensive hydrogenation of 2-heptanone using homogeneous noble catalysts in alkaline medium. In this work, we presented a systematic study on enhanced transfer hydrogenation of 2-heptanone to 2-heptanol using non-noble Co/ZnO catalysts without alkaline promoters. The strong synergism of Co and ZnO contributes to formation of amorphous metallic Co species and electronically reconfigured CoO species, leading to a 20-fold activity enhancement at 180 °C and a TOF of 89.4 h−1 over Co0.09/ZnO-500 catalysts. Structure-dependency studies further revealed that, the lattice strain between Co and ZnO induced the generation of multi-phased Co/CoO/Co:ZnO interfaces, facilitating tandem H2 generation, spillover and activation of C=O bond (of 2-heptanone molecule), respectively. The insights of molecular catalysis on interface of amorphous Co/ZnO for enhanced C=O bond activation, provide fundamental understanding for transfer hydrogenation of various other ketones into valuable alcohols.