CAREER: Low-Dimensional Reactive Hydrides for the Efficient Electro-hydrogenation of Aromatic and Aliphatic Hydrocarbons

化学和石油工业占美国工业部门年能源消耗的46%。这些工业的能源消耗的减少将对未来的能源供应产生重大影响。该研究项目研究了通过电化学氢化过程将有机分子与氢反应的电化学方法。电化学加氢有可能取代目前主导化工和石油工业的能源密集型热/化学加氢过程。电化学加氢技术为提高能源效率和使用可再生化学原料打开了大门，从而减少了碳排放。本研究项目的重点是催化剂在推进电化学系统设计中的作用，作为提高过程效率和降低系统运行成本的一种手段。该项目将为研究生和本科生提供电化学科学研究的基础。通过与德雷塞尔大学（Drexel University）林迪中心（Lindy Center）的合作，工程专业的大一学生将设计实验室模块，通过“周六科学”项目向当地6-12年级的学生教授电化学能量储存和转换的原理。与热/化学加氢相比，电化学加氢有几个优点，即：(1)水是氢的来源，(2)操作温度/压力低，(3)用应用电位控制活性/选择性。下一代电化学加氢催化剂的开发需要：(1)通过对反应性描述符的更基本的理解来控制大量氢化物的反应性；(2)更详细地了解电化学界面对芳香族/脂肪族反应物吸附、吸附中间溶剂化和近地表水直接加氢的影响。虽然过渡金属氢化物已被用于高温非均相加氢/脱氢催化，但其向电加氢的过渡很慢。限制这种转变的是缺乏对特定材料性质，特别是氢化物性质对活性和选择性的直接影响的分析。本研究项目将确定有机反应物的化学性质、本征催化剂性质和金属/电解质界面电场之间的相互关系，以指导特定有机反应物的选择性电化学加氢系统的设计。该项目还将为未来的研究奠定基础，重点是利用电化学界面作为解决限制过程的工具，包括吸附反应物溶剂化，中间结垢以及活性，选择性和耐久性之间的不平衡。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。

The chemical and petroleum industries account for 46% of the yearly energy consumption in the U.S. industrial sector. A reduction in energy consumption by these industries would have a significant impact on future energy supply. This research project investigates electrochemical methods for reacting organic molecules with hydrogen through a process known as electrochemical hydrogenation. Electrochemical hydrogenation has potential to replace the more energy intensive thermal/chemical hydrogenation processes that currently dominate the chemical and petroleum industries. Electrochemical hydrogenation technologies open the door to improvements in energy efficiencies and to the use of renewable chemical feedstocks, thereby decreasing carbon emissions. This research project focuses on the role that catalysts can play in advancing electrochemical system design as a means to improve process efficiency and lower the costs of running the system. The project will provide both graduate and undergraduate students a fundamental foundation in electrochemical science research. Through a partnership with the Lindy Center at Drexel University, freshman engineering students will design lab modules to teach the principles of electrochemical energy storage and conversion to local grade 6-12 students through a Science Saturdays program.Electrochemical hydrogenation has several advantages over thermal/chemical hydrogenation, namely: (1) water is the source of hydrogen, (2) low operational temperature/pressure, and (3) control of activity/selectivity with applied potential. The development of next-generation electrochemical hydrogenation catalysts requires (1) strategies to manipulate bulk hydride reactivity through a more fundamental understanding of their reactivity descriptors, and (2) more detailed insight into the effect of the electrochemical interface on aromatic/aliphatic reactant adsorption, adsorbed intermediate solvation, and direct hydrogenation by near surface water. While transition metal hydrides have been used for high temperature, heterogeneous hydrogenation/dehydrogenation catalysis, their transition to electro-hydrogenation has been slow. Limiting this transition has been an absence of analysis of the direct effect of specific material properties, particularly hydride properties, on both activity and selectivity. This research project will identify the interrelation between chemical properties of the organic reactant, intrinsic catalyst properties, and electric field established at the metal/electrolyte interface, to guide the design of systems for the selective electrochemical hydrogenation of specific organic reactants. The project also will build a base for future research centered on exploitation of electrochemical interfaces as a tool to address limiting processes including adsorbed reactant solvation, intermediate scaling, and imbalance between activity, selectivity, and durability.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.