您好，欢迎访问江苏省农业科学院 机构知识库！
江苏省农业科学院机构知识库

全部

  • 全部
  • 标题
  • 学者
  • 机构
  • 关键词

Highly enhanced direct catalytic oxidation of cyclohexane to adipic acid with molecular oxygen: Dynamic collaboration between zeolite channel micro-environment and Au clusters

文献类型： 外文期刊

作者： Zhang, Zhiyang 1 ; Hu, Mi 1 ; Gui, Qingfeng 4 ; Gu, Jing 3 ; Xu, Wenlong 1 ; Xiao, Qingbo 1 ; Huang, Wei 5 ;

作者机构： 1.Jiangsu Acad Agr Sci, Inst Agr Resources & Environm, Nanjing 210014, Peoples R China

2.Minist Agr & Rural Affairs, Key Lab Agroenvironm Downstream Yangtze Plain, Nanjing 210014, Peoples R China

3.Anhui Univ Technol, Sch Chem & Chem Engn, 59 Hudong Rd, MAAnshan 243002, Peoples R China

4.Jiangsu Maritime Inst, Coll Naval Architecture & Ocean Engn, Nanjing 211170, Peoples R China

5.Northwestern Polytech Univ, Frontiers Sci Ctr Flexible Elect, Xian 710072, Peoples R China

6.Northwestern Polytech Univ, Inst Flexible Elect IFE, Xian 710072, Peoples R China

关键词： Cyclohexane oxidation; Adipic acid; Zeolite; Superior performance; Au clusters; Dynamic collaboration

期刊名称：CHEMICAL ENGINEERING JOURNAL （ 影响因子：15.1； 五年影响因子：14.3 ）

ISSN： 1385-8947

年卷期： 2023 年 467 卷

页码：

收录情况： SCI

摘要： Adipic acid is a valuable chemical used to product Nylon-66, and one of the greenest ways to synthesize it is catalyzing the oxidation of cyclohexane by molecular oxygen in the absence of any other chemicals. However, it is challenging to convert cyclohexane effectively with high selectivity to adipic acid using the available catalysts. In response to the dilemma of achieving satisfactory conversion and selectivity at the same time, a remarkable Au@NaX catalyst is proposed using an improved in-situ crystallization method that exhibits Au clusters sur-rounded by X-zeolite channels. A 29.5% conversion of cyclohexane and an 85.6% selectivity to adipic acid can be obtained in a one-pot oxidation of cyclohexane at 140 degrees C, 20 bar O2, far exceeding most published results. Since determined by detailed characterizations and DFT calculations, the effective dynamic collaboration between Au clusters and zeolite inner micro-environment is the decisive role for superior catalytic performance. Specifically, the surrounding zeolite channel encourages the adsorption and activation of cyclohexane over the confined Au clusters, resulting in an unprecedented activity. The continuous oxidation of cyclohexanol and cyclohexanone to adipic acid is also vulnerable on the enclosed Au clusters, and the subsequent adipic acid can be further stabilized as a result of the strong interaction of -COOH with Na +/- in zeolite channels surrounding enclosed Au clusters. It prevents AA from poisoning active sites and generates a higher selectivity for the desired adipic acid. Our study highlighted the critical significance of the dynamic interaction between metal clusters and the zeolite channel microenvironment. It would shed light on the further high-performance catalysts designs for selective oxidation.

  • 相关文献
作者其他论文 更多>>
置顶
购物车
反馈

© 京ICP备09089781号-29 主办单位：江苏省农业科学院

学术资源： 中国农业科学院 农业专业知识服务系统 农科联盟资源共建共享平台 中国农业科技文献与信息服务平台 中国农业期刊集成服务平台