mof衍生的PdCo和PdMn体系作为炔半加氢反应的多用途催化剂

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL
Jordan Santiago Martinez, Luigi Carpisassi, Gonzalo Egea, Jaime Mazarío*, Christian Wittee Lopes, Carmen Mora-Moreno, Susana Trasobares, Luigi Vaccaro, Jose Juan Calvino, Giovanni Agostini and Pascual Oña-Burgos*, 
{"title":"mof衍生的PdCo和PdMn体系作为炔半加氢反应的多用途催化剂","authors":"Jordan Santiago Martinez,&nbsp;Luigi Carpisassi,&nbsp;Gonzalo Egea,&nbsp;Jaime Mazarío*,&nbsp;Christian Wittee Lopes,&nbsp;Carmen Mora-Moreno,&nbsp;Susana Trasobares,&nbsp;Luigi Vaccaro,&nbsp;Jose Juan Calvino,&nbsp;Giovanni Agostini and Pascual Oña-Burgos*,&nbsp;","doi":"10.1021/acscatal.4c0714910.1021/acscatal.4c07149","DOIUrl":null,"url":null,"abstract":"<p >This study investigates the structure and catalytic properties of bimetallic nanocomposites derived from PdCo- and PdMn-based metal–organic frameworks. These materials, synthesized via chemical (Q) and thermal treatments (T), resulted in <b>PdCo-QT</b> and <b>PdMn-QT</b> catalysts containing Pd-based nanoparticles modified with Co or Mn and supported on N-doped carbon. Detailed characterization techniques confirm these complex structures, including high-resolution transmission electron microscopy, scanning transmission electron microscopy energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy. The catalytic performances of these materials were evaluated for the selective semihydrogenation of phenylacetylene and 4-octyne under soft conditions (1 H<sub>2</sub> bar, room temperature) in batch reactors, demonstrating very high selectivity (≥95 mol %) toward alkenes at high conversion levels (≥94 mol %). Moreover, they displayed significant stability after five catalytic cycles with minimal leaching and highly competitive values of alkyne productivity in the semihydrogenation of phenylacetylene. The study also explored the potential of these catalysts in continuous gas-phase reactions, where <b>PdCo-QT</b> demonstrated remarkable catalytic activity and selectivity with a high gas hourly space velocity.</p>","PeriodicalId":9,"journal":{"name":"ACS Catalysis ","volume":"15 9","pages":"7263–7282 7263–7282"},"PeriodicalIF":13.1000,"publicationDate":"2025-04-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscatal.4c07149","citationCount":"0","resultStr":"{\"title\":\"MOF-Derived PdCo and PdMn Systems as Versatile Catalysts in Alkyne Semihydrogenation\",\"authors\":\"Jordan Santiago Martinez,&nbsp;Luigi Carpisassi,&nbsp;Gonzalo Egea,&nbsp;Jaime Mazarío*,&nbsp;Christian Wittee Lopes,&nbsp;Carmen Mora-Moreno,&nbsp;Susana Trasobares,&nbsp;Luigi Vaccaro,&nbsp;Jose Juan Calvino,&nbsp;Giovanni Agostini and Pascual Oña-Burgos*,&nbsp;\",\"doi\":\"10.1021/acscatal.4c0714910.1021/acscatal.4c07149\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >This study investigates the structure and catalytic properties of bimetallic nanocomposites derived from PdCo- and PdMn-based metal–organic frameworks. These materials, synthesized via chemical (Q) and thermal treatments (T), resulted in <b>PdCo-QT</b> and <b>PdMn-QT</b> catalysts containing Pd-based nanoparticles modified with Co or Mn and supported on N-doped carbon. Detailed characterization techniques confirm these complex structures, including high-resolution transmission electron microscopy, scanning transmission electron microscopy energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy. The catalytic performances of these materials were evaluated for the selective semihydrogenation of phenylacetylene and 4-octyne under soft conditions (1 H<sub>2</sub> bar, room temperature) in batch reactors, demonstrating very high selectivity (≥95 mol %) toward alkenes at high conversion levels (≥94 mol %). Moreover, they displayed significant stability after five catalytic cycles with minimal leaching and highly competitive values of alkyne productivity in the semihydrogenation of phenylacetylene. The study also explored the potential of these catalysts in continuous gas-phase reactions, where <b>PdCo-QT</b> demonstrated remarkable catalytic activity and selectivity with a high gas hourly space velocity.</p>\",\"PeriodicalId\":9,\"journal\":{\"name\":\"ACS Catalysis \",\"volume\":\"15 9\",\"pages\":\"7263–7282 7263–7282\"},\"PeriodicalIF\":13.1000,\"publicationDate\":\"2025-04-18\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://pubs.acs.org/doi/epdf/10.1021/acscatal.4c07149\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Catalysis \",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://pubs.acs.org/doi/10.1021/acscatal.4c07149\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Catalysis ","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acscatal.4c07149","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0

摘要

本文研究了由PdCo和pdmn基金属有机骨架制备的双金属纳米复合材料的结构和催化性能。这些材料通过化学(Q)和热处理(T)合成,得到了PdCo-QT和PdMn-QT催化剂,这些催化剂含有以Co或Mn修饰的pd基纳米颗粒,并负载在n掺杂的碳上。详细的表征技术证实了这些复杂的结构,包括高分辨率透射电子显微镜、扫描透射电子显微镜能量色散x射线能谱、x射线衍射、x射线光电子能谱和x射线吸收能谱。在间歇反应器中,在软条件下(1 H2 bar,室温)对苯乙炔和4-辛烷的选择性半加氢性能进行了评价,结果表明,在高转化率(≥94 mol %)下,这些材料对烯烃具有很高的选择性(≥95 mol %)。此外,它们在五次催化循环后表现出显著的稳定性,在苯乙炔半加氢过程中浸出最小,炔产率具有高度竞争性。该研究还探索了这些催化剂在连续气相反应中的潜力,其中PdCo-QT在高气时空速下表现出了卓越的催化活性和选择性。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
MOF-Derived PdCo and PdMn Systems as Versatile Catalysts in Alkyne Semihydrogenation

This study investigates the structure and catalytic properties of bimetallic nanocomposites derived from PdCo- and PdMn-based metal–organic frameworks. These materials, synthesized via chemical (Q) and thermal treatments (T), resulted in PdCo-QT and PdMn-QT catalysts containing Pd-based nanoparticles modified with Co or Mn and supported on N-doped carbon. Detailed characterization techniques confirm these complex structures, including high-resolution transmission electron microscopy, scanning transmission electron microscopy energy-dispersive X-ray spectroscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and X-ray absorption spectroscopy. The catalytic performances of these materials were evaluated for the selective semihydrogenation of phenylacetylene and 4-octyne under soft conditions (1 H2 bar, room temperature) in batch reactors, demonstrating very high selectivity (≥95 mol %) toward alkenes at high conversion levels (≥94 mol %). Moreover, they displayed significant stability after five catalytic cycles with minimal leaching and highly competitive values of alkyne productivity in the semihydrogenation of phenylacetylene. The study also explored the potential of these catalysts in continuous gas-phase reactions, where PdCo-QT demonstrated remarkable catalytic activity and selectivity with a high gas hourly space velocity.

求助全文
通过发布文献求助,成功后即可免费获取论文全文。 去求助
来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
×
引用
GB/T 7714-2015
复制
MLA
复制
APA
复制
导出至
BibTeX EndNote RefMan NoteFirst NoteExpress
×
提示
您的信息不完整,为了账户安全,请先补充。
现在去补充
×
提示
您因"违规操作"
具体请查看互助需知
我知道了
×
提示
确定
请完成安全验证×
copy
已复制链接
快去分享给好友吧!
我知道了
右上角分享
点击右上角分享
0
联系我们:info@booksci.cn Book学术提供免费学术资源搜索服务,方便国内外学者检索中英文文献。致力于提供最便捷和优质的服务体验。 Copyright © 2023 布克学术 All rights reserved.
京ICP备2023020795号-1
ghs 京公网安备 11010802042870号
Book学术文献互助
Book学术文献互助群
群 号:604180095
Book学术官方微信