Artificial Enzymes: Development of Biomimetic Catalysts in Metal-Organic Frameworks
人工酶:金属有机框架仿生催化剂的开发
基本信息
- 批准号:9397216
- 负责人:
- 金额:$ 5.63万
- 依托单位:
- 依托单位国家:美国
- 项目类别:
- 财政年份:2017
- 资助国家:美国
- 起止时间:2017-12-01 至 2020-11-30
- 项目状态:已结题
- 来源:
- 关键词:AcetyleneAcidsAmmoniaAnabolismBindingBiological MarkersBiomimetic MaterialsBiomimeticsCatalysisCatalytic DomainComplexDevelopmentElectronsEnzymesEthylenesHealthHumanHydrogenHydrogenaseIndustrializationLigandsMetalloproteinsMetalsMethodsModelingNatural GasNitrogenaseOutcomePhotosensitizationPhotosensitizing AgentsPlanet EarthProductionProteinsProtonsReactionReducing AgentsReportingResearchSamplingSchemeSiteTechnologyTestingWorkbiological systemsbiomaterial compatibilitycatalystdesigninsightmolecular hydrogenoxidationsmall molecule
项目摘要
PROJECT SUMMARY/ABSTRACT
This research aims to create new metal-organic frameworks with FeS clusters modeled from
metalloproteins. Using earth-abundant, biocompatible metals such as Fe in the biomimetic catalysts will
enhance health by contributing to the development of materials that may be used on human samples for
applications such as sensing biological markers. More specifically, successful synthesis of the proposed
materials will allow for the catalysis of more complex and wide-ranging reactions in artificial enzymes.
Two related projects are proposed. First, a biomimetic MOF containing [2Fe:2S] clusters and
photosensitizers that can efficiently catalyzes the reduction of protons to molecular hydrogen will be
constructed. A few examples of [2Fe:2S]-MOFs are reported; however, they have not been optimized for
efficient catalysis. Using a recently presented MOF called PCN-700, a linker containing a [2Fe:2S] cluster and
another containing a photosensitizer will be postsynthetically installed in the PCN-700 framework to yield a
catalytic MOF. These [2Fe:2S]-MOFs can then be easily tuned for catalytic efficiency by installing a third linker
that is functionalized to control polar contacts within the MOF.
Second, MOFs containing [4Fe:4S] clusters will be synthesized and assessed for catalytic activity.
Successful inclusion of [4Fe:4S] clusters in a MOF would expand the catalytic and/or biomimetic potential of
MOFs by utilizing the additional available oxidation states afforded by the four Fe sites compared to smaller
FeS clusters. For example, more complex reactions could be carried out, such as those requiring four or more
electrons. Also, since [4Fe:4S] clusters can bind reaction intermediates (which has not been demonstrated with
[2Fe:2S] clusters in a protein), the [4Fe:4S]-MOFs may be used to study reaction intermediates that have not
been successfully characterized using the biological system or small molecules. Two approaches are proposed
for synthesizing [4Fe:4S]-MOFs. First, free [4Fe:4S] clusters will be synthesized with -SCH3 groups on each
Fe. These SCH3 ligands will be exchanged with the bifunctional linker 4,4’-biphenyldithiol to yield a framework,
in the presence of reductant and acid. The second synthetic approach involves assembling the FeS clusters
and the framework simultaneously by using 4,4’-biphenyldithiol instead of HSCH3 in the scheme originally
designed for synthesizing free [4Fe:4S] clusters.
Overall, the results of this work will advance the field of biomimetic catalysts using FeS clusters. The
proposed [2Fe:2S]-MOFs will be optimized for catalytic activity, and the proposed [4Fe:4S]-MOFs would be the
first of their kind, thereby introducing a new class of biomimetic catalysts.
项目总结/文摘
项目成果
期刊论文数量(0)
专著数量(0)
科研奖励数量(0)
会议论文数量(0)
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Christine N Morrison其他文献
Christine N Morrison的其他文献
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{{ truncateString('Christine N Morrison', 18)}}的其他基金
Artificial Enzymes: Development of Biomimetic Catalysts in Metal-Organic Frameworks
人工酶:金属有机框架仿生催化剂的开发
- 批准号:
9568338 - 财政年份:2017
- 资助金额:
$ 5.63万 - 项目类别:
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