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[資源]
Acc. Chem. Res綜述：除了活性位點，外部配位層對于電催化產(chǎn)氫以及氧化的影響
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題目為Beyond the Active Site: The Impact of the Outer Coordination Sphere on Electrocatalysts for Hydrogen Production and Oxidation 作者為Bojana Ginovska-Pangovska , Arnab Dutta , Matthew L. Reback , John C. Linehan , and Wendy J. Shaw * Wendy J. Shaw is a Senior Research Scientist at PNNL. She received her Ph.D. from the University of Washington. Her research interests emphasize learning from nature and include understanding the contribution of an enzyme like outer coordination sphere on molecular catalysts with relevance for renewable energies and understanding protein–surface interactions for biomineralization systems. 全文10頁，參考文獻45篇。 具有氧化還原活化能力的金屬酶在生物體系的能量轉(zhuǎn)移反應(yīng)中發(fā)揮著至關(guān)重要的作用。典型的例子是甲酸脫氫酶，固氮酶，一氧化碳脫氫酶以及氫化酶。這些反應(yīng)對于人體非常重要，可以作為潛在的儲存和使用能量反應(yīng)來用于光電化學(xué)，電催化以及燃料電池等應(yīng)用上。這些金屬酶由具有氧化還原活化能力的金屬中心構(gòu)成，在這些金屬點基質(zhì)被活化而轉(zhuǎn)化為相應(yīng)的產(chǎn)物，這個過程伴隨著電子和質(zhì)子轉(zhuǎn)移過程。 Redox active metalloenzymes play a major role in energy transformation reactions in biological systems. Examples include formate dehydrogenases, nitrogenases, CO dehydrogenase, and hydrogenases. Many of these reactions are also of interest to humans as potential energy storage or utilization reactions for photoelectrochemical, electrolytic, and fuel cell applications. These metalloenzymes consist of redox active metal centers where substrates are activated and undergo transformation to products accompanied by electron and proton transfer to or from the substrate. These active sites are typically buried deep within a protein matrix of the enzyme with channels for proton transport, electron transport, and substrate/product transport between the active site and the surface of the protein. In addition, there are amino acid residues that lie in close proximity to the active site that are thought to play important roles in regulating and enhancing enzyme activity. Directly studying the outer coordination sphere of enzymes can be challenging due to their complexity, and the use of modified molecular catalysts may allow us to provide some insight. There are two fundamentally different approaches to understand these important interactions. The “bottom-up” approach involves building an amino acid or peptide containing outer coordination sphere around a functional molecular catalyst, and the “top-down” approach involves attaching molecular catalyst to a structured protein. Both of these approaches have been undertaken for hydrogenase mimics and are the emphasis of this Account. Our focus has been to utilize amino acid or peptide based scaffolds on an active functional enzyme mimic for H2 oxidation and production, [Ni(PR2NR′2)2]2+. This “bottom-up” approach has allowed us to evaluate individual functional group and structural contributions to electrocatalysts for H2 oxidation and production. For instance, using amine, ether, and carboxylic acid functionalities in the outer coordination sphere enhances proton movement and results in lower catalytic overpotentials for H2 oxidation, while achieving water solubility in some cases. Amino acids with acidic and basic side chains concentrate substrate around catalysts for H2 production, resulting in up to 5-fold enhancements in rate. The addition of a structured peptide in an H2 production catalyst limited the structural freedom of the amino acids nearest the active site, while enhancing the overall rate. Enhanced stability to oxygen or extreme conditions such as strongly acidic or basic conditions has also resulted from an amino acid based outer coordination sphere. From the “top-down” approach, others have achieved water solubility and photocatalytic activity by associating this core complex with photosystem-I. Collectively, by use of this well understood core, the role of individual and combined features of the outer coordination sphere are starting to be understood at a mechanistic level. Common mechanisms have yet to be defined to predictably control these processes, but our growing knowledge in this area is essential for the eventual mimicry of enzymes by efficient molecular catalysts for practical use. 360軟件小助手截圖20140620084138.png |
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本內(nèi)容由用戶自主發(fā)布，如果其內(nèi)容涉及到知識產(chǎn)權(quán)問題，其責(zé)任在于用戶本人，如對版權(quán)有異議，請聯(lián)系郵箱：xiaomuchong@tal.com - 附件 1 : 2014-ar5001742Beyond_the_Active_Site_The_Impact_of_the_Outer_Coordination_Sphere_on_Electrocatalysts_for_Hydrogen_Production_and_Oxidation.pdf
2014-06-20 09:20:08, 4.27 M
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[考研] 291 求調(diào)劑 +4 | 化工2026屆畢業(yè)?/a> 2026-03-21 | 5/250 |
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[考研] 求調(diào)劑 +7 | Auroracx 2026-03-22 | 7/350 |
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[考研] 材料求調(diào)劑 +5 | @taotao 2026-03-21 | 5/250 |
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[考研] 297求調(diào)劑 +3 | 喜歡還是不甘心 2026-03-20 | 3/150 |
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[考研] 求調(diào)劑 +3 | 13341 2026-03-20 | 3/150 |
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[考研] 313求調(diào)劑 +4 | 肆叁貳壹22 2026-03-19 | 4/200 |
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