{"title":"掺氮多孔碳上富含缺陷的 α-MoC 支持喹啉向芳烃的转化","authors":"Zegang Qiu, Yuanzhe Wang, Zhiqin Li, Bo Ma, Chaoqiu Chen, Shuai Chen, Junqing Wen","doi":"10.1016/j.cej.2024.158728","DOIUrl":null,"url":null,"abstract":"The challenge for the conversion of alternative crude sources to aromatics is to retain aromatic rings in the hydrotreating process. The design of unique catalyst with low damage to the aromatic rings but with high ability to break C-N and C-C bonds is essential. Herein, defect-rich α-MoC supported on nitrogen-doped carbon (NC) was constructed to transform quinoline-like N-heterocyclic compounds to aromatics. The incorporation of NC increased the content of highly active coordination unsaturated Mo sites related to C or O defects and promoted the desorption and spillover of H<sub>2</sub>. Moreover, the introduction of NC strengthened the electron donating ability of Mo and enhanced the adsorption strength of quinoline on catalyst surface. Consequently, the ability of molybdenum carbide to break C-N and C-C bonds was enhanced. The selectivity of products from C-N bonds breaking reached to 99.5%, and the selectivity of aromatic products from C-C bonds breaking reached to 58.1%. Meanwhile, the aromatic ring was highly preserved. The selectivity of aromatics achieved an impressive level of 85.1% over α-MoC/NC-0.2. The processing capacity of α-MoC/NC-0.2 was 1.3 times that of α-MoC. The stability of α-MoC/NC remained exceptional even when subjected to high liquid hourly space velocity.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"52 1","pages":""},"PeriodicalIF":13.3000,"publicationDate":"2024-12-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Defect-rich α-MoC supported on nitrogen doped porous carbon for transformation of quinoline to aromatics\",\"authors\":\"Zegang Qiu, Yuanzhe Wang, Zhiqin Li, Bo Ma, Chaoqiu Chen, Shuai Chen, Junqing Wen\",\"doi\":\"10.1016/j.cej.2024.158728\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"The challenge for the conversion of alternative crude sources to aromatics is to retain aromatic rings in the hydrotreating process. The design of unique catalyst with low damage to the aromatic rings but with high ability to break C-N and C-C bonds is essential. Herein, defect-rich α-MoC supported on nitrogen-doped carbon (NC) was constructed to transform quinoline-like N-heterocyclic compounds to aromatics. The incorporation of NC increased the content of highly active coordination unsaturated Mo sites related to C or O defects and promoted the desorption and spillover of H<sub>2</sub>. Moreover, the introduction of NC strengthened the electron donating ability of Mo and enhanced the adsorption strength of quinoline on catalyst surface. Consequently, the ability of molybdenum carbide to break C-N and C-C bonds was enhanced. The selectivity of products from C-N bonds breaking reached to 99.5%, and the selectivity of aromatic products from C-C bonds breaking reached to 58.1%. Meanwhile, the aromatic ring was highly preserved. The selectivity of aromatics achieved an impressive level of 85.1% over α-MoC/NC-0.2. The processing capacity of α-MoC/NC-0.2 was 1.3 times that of α-MoC. The stability of α-MoC/NC remained exceptional even when subjected to high liquid hourly space velocity.\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"52 1\",\"pages\":\"\"},\"PeriodicalIF\":13.3000,\"publicationDate\":\"2024-12-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.cej.2024.158728\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://doi.org/10.1016/j.cej.2024.158728","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
引用次数: 0
摘要
在加氢处理过程中保留芳香环是将替代原油转化为芳烃所面临的挑战。设计一种独特的催化剂,既能降低对芳香环的破坏,又能提高断裂 C-N 和 C-C 键的能力,这一点至关重要。在此,我们构建了以掺氮碳 (NC) 为载体的富缺陷 α-MoC 催化剂,用于将喹啉类 N-杂环化合物转化为芳烃。NC 的加入增加了与 C 或 O 缺陷相关的高活性配位不饱和 Mo 位点的含量,促进了 H2 的解吸和溢出。此外,NC 的引入还增强了 Mo 的电子捐赠能力,提高了喹啉在催化剂表面的吸附强度。因此,碳化钼断裂 C-N 和 C-C 键的能力得到了增强。C-N 键断裂产物的选择性达到 99.5%,C-C 键断裂芳香产物的选择性达到 58.1%。同时,芳香环得到了很好的保留。与 α-MoC/NC-0.2 相比,芳烃的选择性达到了 85.1%的惊人水平。α-MoC/NC-0.2 的加工能力是 α-MoC 的 1.3 倍。即使在液体时空速度很高的情况下,α-MoC/NC 的稳定性仍然非常出色。
Defect-rich α-MoC supported on nitrogen doped porous carbon for transformation of quinoline to aromatics
The challenge for the conversion of alternative crude sources to aromatics is to retain aromatic rings in the hydrotreating process. The design of unique catalyst with low damage to the aromatic rings but with high ability to break C-N and C-C bonds is essential. Herein, defect-rich α-MoC supported on nitrogen-doped carbon (NC) was constructed to transform quinoline-like N-heterocyclic compounds to aromatics. The incorporation of NC increased the content of highly active coordination unsaturated Mo sites related to C or O defects and promoted the desorption and spillover of H2. Moreover, the introduction of NC strengthened the electron donating ability of Mo and enhanced the adsorption strength of quinoline on catalyst surface. Consequently, the ability of molybdenum carbide to break C-N and C-C bonds was enhanced. The selectivity of products from C-N bonds breaking reached to 99.5%, and the selectivity of aromatic products from C-C bonds breaking reached to 58.1%. Meanwhile, the aromatic ring was highly preserved. The selectivity of aromatics achieved an impressive level of 85.1% over α-MoC/NC-0.2. The processing capacity of α-MoC/NC-0.2 was 1.3 times that of α-MoC. The stability of α-MoC/NC remained exceptional even when subjected to high liquid hourly space velocity.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.