Harnessing Redox-Active Ligands and Cofactors to Facilitate Multi-electron Reactivity

有了这个奖项，化学系的化学催化计划正在资助加州大学欧文分校化学系的Alan Heyduk教授开发新的分子催化剂，用于将水分解为氢和氧。利用间歇性替代能源，如风能和太阳能，需要制定有效的转换战略，以产生化学燃料。水分解以提供氢和氧是用于该目标的有吸引力的能量储存反应，并且为了广泛应用，这些催化剂必须由廉价且地球丰富的元素制成。该项目还为本科生和研究生两级的学生培训提供了途径，并包括来自科学领域历来代表性不足的群体的强有力的代表性。Heyduk教授正在开发新的三齿氧化还原活性配体，这些配体可以在与金属结合时在三种氧化态之间穿梭，作为向金属络合物引入多电子氧化还原功能的一种方式。PI正在探索这些配合物在重要的多电子反应催化中的应用，如水氧化和质子还原。 该项目的最终目标是为水裂解反应的两个部分产生分子电催化剂，并基于地球丰富的第一行过渡金属。 用于质子电化学还原成氢和水电化学氧化成氧的新分子催化剂的开发提供了对有效水裂解的机理和动力学障碍的深入了解。为了广泛应用，这些催化剂必须由廉价且地球上丰富的元素制成，其中控制多电子反应性的因素尚未阐明。这一奋进的成功将影响替代能源战略，为将瞬时能源转化为可储存、便携式化学燃料提供新的途径。

With this award, the Chemical Catalysis Program of the Division of Chemistry is funding Professor Alan Heyduk of the Department of Chemistry at the University of California, Irvine to develop new molecular catalysts for splitting water into hydrogen and oxygen. The utilization of intermittent alternative energy sources such as wind and solar requires that efficient conversion strategies be developed to generate chemical fuels. Water-splitting to afford hydrogen and oxygen is an attractive energy-storing reaction for this goal, and for widespread applicability, these catalysts must be made from inexpensive and earth-abundant elements. This project is also providing avenues for the training of students at both the undergraduate and graduate levels and includes strong representation from groups that are historically underrepresented in the sciences. Professor Heyduk is developing new tridentate, redox active ligands that can be shuttled among three oxidation states while bound to a metal, as a way to introduce multi-electron redox functionality to the metal complex. The PI is exploring the use of these complexes in the catalysis of important multi-electron reactions, such as water oxidation and proton reduction. The ultimate goal of the project is to generate molecular electrocatalysts for both halves of the water-splitting reaction and based upon earth abundant first row transition metals. The development of new molecular catalysts for the electrochemical reduction of protons to hydrogen and the electrochemical oxidation of water to oxygen provide insights into the mechanistic and kinetic barriers to efficient water splitting. For widespread applicability, these catalysts must be made from inexpensive and earth-abundant elements, where the factors governing multi-electron reactivity are yet to be elucidated. Success in this endeavor will impact alternative energy strategies by providing new avenues for the conversion of transient energy sources into storable, portable, chemical fuels.