{"title":"使用 MOF 衍生碳支撑的双金属 NiMo 催化剂促进月桂酸与烷烃的反应","authors":"Jiang Tao Li, Shuqian Xia","doi":"10.1007/s10563-024-09425-2","DOIUrl":null,"url":null,"abstract":"<div><p>Hydrodeoxygenation (HDO) is a promising way to produce the second generation biodiesel from aliphatic acid based biomass. In this study, Ni<sub>x</sub>Mo<sub>y</sub>@NC bimetallic catalysts with varying molar ratios were prepared using ZIF-8 as a representative MOF precursor. Lauric acid was chosen as the model compound, the catalytic performance of these catalysts with different metal ratios, reaction temperatures, and pressures was investigated. In addition, the reaction of lauric acid, lauric alcohol, and lauric aldehyde at different reaction times were investigated to explore the pathways of lauric acid. The influence of Mo doping on the catalyst structure, reducibility, and electronic properties was investigated through a series of characterizations, including SEM, TEM, XPS, H<sub>2</sub>-TPR, and NH<sub>3</sub>-TPD. This study revealed that the ZIF-8 support with incorporated Ni and Mo maintained a stable structure. Compared to Ni-based catalysts, the addition of Mo in the bimetallic catalyst can bring the electron transfer between Ni and Mo and increased the active sites and acid sites. An appropriate amount of Mo can lower the reduction temperature and enhance the catalytic activity for hydrogenation and deoxygenation reactions. Based on the catalytic experimental results, it can be observed that liquid alkanes, such as undecane and dodecane, are primarily formed through decarbonylation of lauric aldehyde and hydrodeoxygenation of lauric alcohol. Additionally, under high-temperature conditions, the hydrodeoxygenation reaction is favored over the decarbonylation reaction, promoting the production of dodecane. This indicates that Mo exhibits better activation for the C–OH reaction, leading to these observations. Under repeated use, the catalyst still has good catalytic activity and stability.</p></div>","PeriodicalId":509,"journal":{"name":"Catalysis Surveys from Asia","volume":"28 3","pages":"269 - 282"},"PeriodicalIF":2.1000,"publicationDate":"2024-04-26","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Bimetallic NiMo Using MOF-Derived Carbon-Supported Catalysts for the Reaction of Lauric Acid to Alkane\",\"authors\":\"Jiang Tao Li, Shuqian Xia\",\"doi\":\"10.1007/s10563-024-09425-2\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><p>Hydrodeoxygenation (HDO) is a promising way to produce the second generation biodiesel from aliphatic acid based biomass. In this study, Ni<sub>x</sub>Mo<sub>y</sub>@NC bimetallic catalysts with varying molar ratios were prepared using ZIF-8 as a representative MOF precursor. Lauric acid was chosen as the model compound, the catalytic performance of these catalysts with different metal ratios, reaction temperatures, and pressures was investigated. In addition, the reaction of lauric acid, lauric alcohol, and lauric aldehyde at different reaction times were investigated to explore the pathways of lauric acid. The influence of Mo doping on the catalyst structure, reducibility, and electronic properties was investigated through a series of characterizations, including SEM, TEM, XPS, H<sub>2</sub>-TPR, and NH<sub>3</sub>-TPD. This study revealed that the ZIF-8 support with incorporated Ni and Mo maintained a stable structure. Compared to Ni-based catalysts, the addition of Mo in the bimetallic catalyst can bring the electron transfer between Ni and Mo and increased the active sites and acid sites. An appropriate amount of Mo can lower the reduction temperature and enhance the catalytic activity for hydrogenation and deoxygenation reactions. Based on the catalytic experimental results, it can be observed that liquid alkanes, such as undecane and dodecane, are primarily formed through decarbonylation of lauric aldehyde and hydrodeoxygenation of lauric alcohol. Additionally, under high-temperature conditions, the hydrodeoxygenation reaction is favored over the decarbonylation reaction, promoting the production of dodecane. This indicates that Mo exhibits better activation for the C–OH reaction, leading to these observations. Under repeated use, the catalyst still has good catalytic activity and stability.</p></div>\",\"PeriodicalId\":509,\"journal\":{\"name\":\"Catalysis Surveys from Asia\",\"volume\":\"28 3\",\"pages\":\"269 - 282\"},\"PeriodicalIF\":2.1000,\"publicationDate\":\"2024-04-26\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Catalysis Surveys from Asia\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://link.springer.com/article/10.1007/s10563-024-09425-2\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Catalysis Surveys from Asia","FirstCategoryId":"92","ListUrlMain":"https://link.springer.com/article/10.1007/s10563-024-09425-2","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
摘要
加氢脱氧(HDO)是利用脂肪族酸基生物质生产第二代生物柴油的一种可行方法。本研究以 ZIF-8 为代表性 MOF 前驱体,制备了不同摩尔比的 NixMoy@NC 双金属催化剂。以月桂酸为模型化合物,研究了这些催化剂在不同金属比、反应温度和压力下的催化性能。此外,还研究了不同反应时间下月桂酸、月桂醇和月桂醛的反应,以探索月桂酸的生成途径。通过一系列表征,包括 SEM、TEM、XPS、H2-TPR 和 NH3-TPD 等,研究了掺杂 Mo 对催化剂结构、还原性和电子特性的影响。研究结果表明,掺入镍和钼的 ZIF-8 载体保持了稳定的结构。与镍基催化剂相比,在双金属催化剂中添加 Mo 可以促进镍和 Mo 之间的电子转移,增加活性位点和酸性位点。适量的 Mo 可以降低还原温度,提高加氢和脱氧反应的催化活性。根据催化实验结果可知,液态烷烃(如十一烷和十二烷)主要是通过月桂醛的脱羰基反应和月桂醇的加氢脱氧反应生成的。此外,在高温条件下,加氢脱氧反应比脱羰基反应更有利,从而促进了十二烷的生成。这表明钼对 C-OH 反应具有更好的活化作用,从而导致了上述观察结果。在反复使用的情况下,催化剂仍然具有良好的催化活性和稳定性。
Bimetallic NiMo Using MOF-Derived Carbon-Supported Catalysts for the Reaction of Lauric Acid to Alkane
Hydrodeoxygenation (HDO) is a promising way to produce the second generation biodiesel from aliphatic acid based biomass. In this study, NixMoy@NC bimetallic catalysts with varying molar ratios were prepared using ZIF-8 as a representative MOF precursor. Lauric acid was chosen as the model compound, the catalytic performance of these catalysts with different metal ratios, reaction temperatures, and pressures was investigated. In addition, the reaction of lauric acid, lauric alcohol, and lauric aldehyde at different reaction times were investigated to explore the pathways of lauric acid. The influence of Mo doping on the catalyst structure, reducibility, and electronic properties was investigated through a series of characterizations, including SEM, TEM, XPS, H2-TPR, and NH3-TPD. This study revealed that the ZIF-8 support with incorporated Ni and Mo maintained a stable structure. Compared to Ni-based catalysts, the addition of Mo in the bimetallic catalyst can bring the electron transfer between Ni and Mo and increased the active sites and acid sites. An appropriate amount of Mo can lower the reduction temperature and enhance the catalytic activity for hydrogenation and deoxygenation reactions. Based on the catalytic experimental results, it can be observed that liquid alkanes, such as undecane and dodecane, are primarily formed through decarbonylation of lauric aldehyde and hydrodeoxygenation of lauric alcohol. Additionally, under high-temperature conditions, the hydrodeoxygenation reaction is favored over the decarbonylation reaction, promoting the production of dodecane. This indicates that Mo exhibits better activation for the C–OH reaction, leading to these observations. Under repeated use, the catalyst still has good catalytic activity and stability.
期刊介绍:
Early dissemination of important findings from Asia which may lead to new concepts in catalyst design is the main aim of this journal. Rapid, invited, short reviews and perspectives from academia and industry will constitute the major part of Catalysis Surveys from Asia . Surveys of recent progress and activities in catalytic science and technology and related areas in Asia will be covered regularly as well. We would appreciate critical comments from colleagues throughout the world about articles in Catalysis Surveys from Asia . If requested and thought appropriate, the comments will be included in the journal. We will be very happy if this journal stimulates global communication between scientists and engineers in the world of catalysis.