• 文献检索
  • 文档翻译
  • 深度研究
  • 学术资讯
  • Suppr Zotero 插件Zotero 插件
  • 邀请有礼
  • 套餐&价格
  • 历史记录
应用&插件
Suppr Zotero 插件Zotero 插件浏览器插件Mac 客户端Windows 客户端微信小程序
定价
高级版会员购买积分包购买API积分包
服务
文献检索文档翻译深度研究API 文档MCP 服务
关于我们
关于 Suppr公司介绍联系我们用户协议隐私条款
关注我们

Suppr 超能文献

核心技术专利：CN118964589B侵权必究
粤ICP备2023148730 号-1Suppr @ 2026

文献检索

告别复杂PubMed语法，用中文像聊天一样搜索，搜遍4000万医学文献。AI智能推荐，让科研检索更轻松。

立即免费搜索

文件翻译

保留排版，准确专业，支持PDF/Word/PPT等文件格式，支持 12+语言互译。

免费翻译文档

深度研究

AI帮你快速写综述，25分钟生成高质量综述，智能提取关键信息，辅助科研写作。

立即免费体验

一种具有质子响应性氮供体配体的铱配合物在CO加氢生成甲酸盐反应中的催化活性。

Catalytic reactivity of an iridium complex with a proton responsive N-donor ligand in CO hydrogenation to formate.

作者信息

Gunasekar Gunniya Hariyanandam, Yoon Yeahsel, Baek Il-Hyun, Yoon Sungho

机构信息

Department of Applied Chemistry, Kookmin University 77 Jeongneung-ro, Seongbuk-gu Seoul 136-702 Republic of Korea

Korea Institute of Energy Research 152 Gajeong-ro, Yuseong-gu Daejeon 305-343 Republic of Korea.

出版信息

RSC Adv. 2018 Jan 3;8(3):1346-1350. doi: 10.1039/c7ra12343d. eCollection 2018 Jan 2.

DOI:10.1039/c7ra12343d
PMID:35540928
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9077040/
Abstract

Catalytic hydrogenation of CO into formic acid/formate is an attractive conversion in the utilization of CO. Although various catalysts with high catalytic efficiency are reported, a very few studies have been carried out to correlate/understand the efficacy and stability of the hydrogenation catalysts, which could be helpful to direct the future design strategy of corresponding catalysts. Herein, a half-sandwich iridium complex containing bibenzimidazole as a proton responsive N-donor ligand, [CpIr(BiBzImH)Cl]Cl, has been synthesized and fully characterized. The generation of an N anion by the deprotonation of a bibenzimidazole group resulted in a significant enhancement of activity. The Ir complex showed about 20 times higher catalytic efficiency in the hydrogenation of CO into formate than that of its bipyridine counterpart [CpIr(Bpy)Cl]Cl. The time dependent catalytic activity studies revealed that the initial excellent activity of [CpIr(BiBzImH)Cl]Cl was reduced when catalytic cycle proceeds; which was found to be the structural instability of the catalyst caused by steric hindrance between the bibenzimidazole and Cp ligands.

摘要

将CO催化氢化为甲酸/甲酸盐是CO利用中一种有吸引力的转化方式。尽管已报道了各种具有高催化效率的催化剂，但针对氢化催化剂的功效和稳定性进行关联/理解的研究却很少，而这有助于指导相应催化剂未来的设计策略。在此，合成并全面表征了一种含联苯并咪唑作为质子响应性氮供体配体的半夹心铱配合物[CpIr(BiBzImH)Cl]Cl。联苯并咪唑基团去质子化生成N阴离子导致活性显著增强。该铱配合物在将CO氢化为甲酸盐的反应中显示出比其联吡啶类似物[CpIr(Bpy)Cl]Cl高约20倍的催化效率。随时间变化的催化活性研究表明，当催化循环进行时，[CpIr(BiBzImH)Cl]Cl最初优异的活性会降低；这被发现是由联苯并咪唑和Cp配体之间的空间位阻导致的催化剂结构不稳定性所致。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/f3c2139c85e2/c7ra12343d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/fcc05fbf7e57/c7ra12343d-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/9b7d28ac3ce4/c7ra12343d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/2ecff07cc81f/c7ra12343d-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/6fa8c65e4423/c7ra12343d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/f3c2139c85e2/c7ra12343d-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/fcc05fbf7e57/c7ra12343d-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/9b7d28ac3ce4/c7ra12343d-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/2ecff07cc81f/c7ra12343d-s2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/6fa8c65e4423/c7ra12343d-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/90b9/9077040/f3c2139c85e2/c7ra12343d-f3.jpg

相似文献

1
Catalytic reactivity of an iridium complex with a proton responsive N-donor ligand in CO hydrogenation to formate.一种具有质子响应性氮供体配体的铱配合物在CO加氢生成甲酸盐反应中的催化活性。
RSC Adv. 2018 Jan 3;8(3):1346-1350. doi: 10.1039/c7ra12343d. eCollection 2018 Jan 2.
2
Chiral-at-Metal: Iridium(III) Tetrazole Complexes With Proton-Responsive P-OH Groups for CO Hydrogenation.金属手性：含质子响应性P-OH基团的铱（III）四唑配合物用于CO加氢反应
Front Chem. 2020 Nov 13;8:591353. doi: 10.3389/fchem.2020.591353. eCollection 2020.
3
Cp*Co(III) catalysts with proton-responsive ligands for carbon dioxide hydrogenation in aqueous media.具有质子响应配体的Cp*Co(III)催化剂用于水相二氧化碳加氢反应。
Inorg Chem. 2013 Nov 4;52(21):12576-86. doi: 10.1021/ic401707u. Epub 2013 Oct 16.
4
CO2 Hydrogenation Catalyzed by Iridium Complexes with a Proton-Responsive Ligand.质子响应配体铱配合物催化的二氧化碳加氢反应
Inorg Chem. 2015 Jun 1;54(11):5114-23. doi: 10.1021/ic502904q. Epub 2015 Feb 18.
5
Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO Hydrogenation.具有质子响应型唑类配体的铱配合物作为 CO 加氢的有效催化剂。
ChemSusChem. 2017 Nov 23;10(22):4535-4543. doi: 10.1002/cssc.201701676. Epub 2017 Nov 7.
6
Iridium and Ruthenium Complexes of -Heterocyclic Carbene- and Pyridinol-Derived Chelates as Catalysts for Aqueous Carbon Dioxide Hydrogenation and Formic Acid Dehydrogenation: The Role of the Alkali Metal.- 杂环卡宾和吡啶醇衍生螯合物的铱和钌配合物作为二氧化碳水相加氢和甲酸脱氢的催化剂：碱金属的作用
Organometallics. 2017 Mar 27;36(6):1091-1106. doi: 10.1021/acs.organomet.6b00806. Epub 2017 Mar 3.
7
Versatile Rh- and Ir-Based Catalysts for CO Hydrogenation, Formic Acid Dehydrogenation, and Transfer Hydrogenation of Quinolines.多功能 Rh 和 Ir 基催化剂在 CO 加氢、甲酸脱氢和喹啉转移加氢中的应用。
Inorg Chem. 2018 Nov 19;57(22):14186-14198. doi: 10.1021/acs.inorgchem.8b02164. Epub 2018 Nov 5.
8
Metal-Ligand Cooperation in Cp*Ir-Pyridylpyrrole Complexes: Rational Design and Catalytic Activity in Formic Acid Dehydrogenation and CO Hydrogenation under Ambient Conditions.Cp*Ir-吡啶基吡咯配合物中的金属-配体协同作用：常温条件下甲酸脱氢和CO加氢反应中的合理设计与催化活性
Inorg Chem. 2021 Nov 1;60(21):16584-16592. doi: 10.1021/acs.inorgchem.1c02487. Epub 2021 Oct 12.
9
Precisely Controlling Ancillary Ligands to Improve Catalysis of Cp*Ir Complexes for CO Hydrogenation.精确控制辅助配体以提高 Cp*Ir 配合物对 CO 加氢反应的催化性能。
Inorg Chem. 2023 Jul 17;62(28):11225-11232. doi: 10.1021/acs.inorgchem.3c01466. Epub 2023 Jul 4.
10
Half-sandwich rhodium(III) transfer hydrogenation catalysts: Reduction of NAD(+) and pyruvate, and antiproliferative activity.半三明治型铑（III）转移氢化催化剂：NAD（+）和丙酮酸的还原以及抗增殖活性。
J Inorg Biochem. 2015 Dec;153:322-333. doi: 10.1016/j.jinorgbio.2015.10.008. Epub 2015 Oct 19.

引用本文的文献

1
Chiral-at-Metal: Iridium(III) Tetrazole Complexes With Proton-Responsive P-OH Groups for CO Hydrogenation.金属手性：含质子响应性P-OH基团的铱（III）四唑配合物用于CO加氢反应
Front Chem. 2020 Nov 13;8:591353. doi: 10.3389/fchem.2020.591353. eCollection 2020.

本文引用的文献

1
N-Methylation of Amines with Methanol Catalyzed by a Cp*Ir Complex Bearing a Functional 2,2'-Bibenzimidazole Ligand.Cp*Ir 配合物负载功能化 2,2'-联苯并咪唑配体催化胺的 N-甲基化反应：甲醇作为甲基供体。
Org Lett. 2017 Nov 3;19(21):5790-5793. doi: 10.1021/acs.orglett.7b02723.
2
Iridium Complexes with Proton-Responsive Azole-Type Ligands as Effective Catalysts for CO Hydrogenation.具有质子响应型唑类配体的铱配合物作为 CO 加氢的有效催化剂。
ChemSusChem. 2017 Nov 23;10(22):4535-4543. doi: 10.1002/cssc.201701676. Epub 2017 Nov 7.
3
Efficient Hydrogen Storage and Production Using a Catalyst with an Imidazoline-Based, Proton-Responsive Ligand.
使用具有基于咪唑啉的质子响应配体的催化剂进行高效储氢和制氢
ChemSusChem. 2017 Mar 22;10(6):1071-1075. doi: 10.1002/cssc.201601437. Epub 2016 Dec 28.
4
A Highly Efficient Heterogenized Iridium Complex for the Catalytic Hydrogenation of Carbon Dioxide to Formate.一种用于二氧化碳催化加氢生成甲酸盐的高效非均相铱配合物。
ChemSusChem. 2015 Oct 26;8(20):3410-3. doi: 10.1002/cssc.201500436. Epub 2015 Aug 25.
5
CO2 Hydrogenation to Formate and Methanol as an Alternative to Photo- and Electrochemical CO2 Reduction.将二氧化碳加氢生成甲酸盐和甲醇作为光催化和电化学二氧化碳还原的替代方法
Chem Rev. 2015 Dec 9;115(23):12936-73. doi: 10.1021/acs.chemrev.5b00197. Epub 2015 Sep 3.
6
CO2 Hydrogenation Catalyzed by Iridium Complexes with a Proton-Responsive Ligand.质子响应配体铱配合物催化的二氧化碳加氢反应
Inorg Chem. 2015 Jun 1;54(11):5114-23. doi: 10.1021/ic502904q. Epub 2015 Feb 18.
7
Cp*Co(III) catalysts with proton-responsive ligands for carbon dioxide hydrogenation in aqueous media.具有质子响应配体的Cp*Co(III)催化剂用于水相二氧化碳加氢反应。
Inorg Chem. 2013 Nov 4;52(21):12576-86. doi: 10.1021/ic401707u. Epub 2013 Oct 16.
8
Interconversion of CO2 and formic acid by bio-inspired Ir complexes with pendent bases.通过带有侧基碱的仿生铱配合物实现二氧化碳与甲酸的相互转化。
Biochim Biophys Acta. 2013 Aug-Sep;1827(8-9):1031-8. doi: 10.1016/j.bbabio.2012.11.004. Epub 2012 Nov 19.
9
A well-defined iron catalyst for the reduction of bicarbonates and carbon dioxide to formates, alkyl formates, and formamides.一种用于将碳酸氢盐和二氧化碳还原为甲酸盐、甲酸烷基酯和甲酰胺的明确的铁催化剂。
Angew Chem Int Ed Engl. 2010 Dec 10;49(50):9777-80. doi: 10.1002/anie.201004263.
10
Ruthenium-catalyzed hydrogenation of bicarbonate in water.钌催化水中碳酸氢盐的氢化反应。
ChemSusChem. 2010 Sep 24;3(9):1048-50. doi: 10.1002/cssc.201000151.