CAS-SC: Understanding Synergistic Effects of Organic Mixtures for Electrocatalytic Hydrogenation for Fuel Production

该项目旨在提高生物油电催化加氢（ECH）的知识。废弃生物质（例如，生物质来源与用于食物的生物质来源分开）可以在高温下加热形成生物油，生物油含有许多重要的燃料化合物，但能量密度低。使用可再生电力，这种生物油的ECH可以形成具有更高能量密度的化学品，并可用作燃料。因此，该项目将研究一种方法，以提供高能量密度的运输燃料，净零二氧化碳排放作为石油的替代品。该项目的目标是从根本上了解如何通过电催化同时升级与生物油混合物相关的多种有机分子。特别是，该团队将研究不同有机分子可以相互帮助转化为所需产物的条件。这项研究将使可持续的生物基产品，更有效地使用可再生能源来驱动化学过程，帮助开发碳中性燃料生产过程，并使用预测建模来了解电催化反应。拟议的教育和宣传活动将使代表性不足的高中生参与研究，并帮助四年级和五年级的学生更多地了解化学，以及为什么它是重要和有趣的，帮助培养下一代STEM专业人员。该项目的目标是了解模型生物的ECH，衍生的有机混合物，以确定多个有机分子如何可以同时以高效率进行电化学升级。这个联合实验和计算项目将研究有机分子的ECH（即，酚类化合物和萜烯的混合物），并研究这些分子在混合物中的反应如何不同于每个分子单独的反应。该项目将确定协同增强彼此转化的有机分子，并了解这种协同增强金属和合金电催化剂的起源，以便电化学反应器设计可用于降低生物衍生有机物的ECH生产的燃料成本。这项工作的三个主要任务是：（1）了解模型有机分子的ECH隔离;（2）阐明模型有机混合物如何增强或减缓ECH;（3）设计系统，同时氢化的有机混合物。本研究将阐明ECH的生物油混合物的反应机制，并产生知识的作用，所施加的电化学电位和水溶剂ECH使用量子力学建模和实验动力学测量和光谱。还有，这项工作将阐明共吸附有机物对电催化加氢速率和选择性的作用，并确定电化学转化速率，以评估与最新技术相比的商业可行性。这项研究将产生可用于提高生物催化加氢效率的基础知识。该奖项反映了NSF的法定使命，并被认为值得通过使用基金会的智力价值和更广泛的影响审查标准。

This project aims to advance knowledge of electrocatalytic hydrogenation (ECH) of bio-oil. Waste biomass (e.g., biomass sources separate from those that are used for food) can be heated at high temperatures to form bio-oil, which contains many of the important compounds for fuels, but with low energy density. Using renewable electricity, ECH of this bio-oil can form chemicals that have higher energy density and can be used as fuels. Thus, this project will study a method to provide high energy density transportation fuels with net-zero carbon dioxide emissions as an alternative to petroleum. The goal of this project is to fundamentally understand how to simultaneously upgrade multiple organic molecules relevant to bio-oil mixtures via electrocatalysis. Particularly, the team will investigate conditions where the different organic molecules can help one another in converting to the desired products. This research would enable sustainable bio-based products, use renewable energy more efficiently to drive chemical processes, help develop carbon-neutral processes for fuel production, and use predictive modeling to understand electrocatalytic reactions. The proposed education and outreach activities will engage underrepresented high-school students in research and help 4th and 5th grade students understand more about chemistry and why it is important and interesting, helping to foster the next generation of STEM professionals.The project goal is to understand the ECH of model bio-derived organic mixtures to determine how multiple organic molecules can be simultaneously electrochemically upgraded with high efficiency. This joint experimental and computational project will investigate ECH of organic molecules (i.e., mixtures of phenolics and terpenes) that are present in biomass-based feedstocks and investigate how the reaction of these molecules in mixtures differs from that of each molecule individually. This project will identify organic molecules that synergistically enhance one another’s conversion and understand the origin of this synergistic enhancement on metal and alloy electrocatalysts, such that electrochemical reactor design can be used to decrease the cost of fuels produced by ECH of bio-derived organics. The three major tasks of this work are to: (1) Understand ECH of model organic molecules in isolation; (2) Elucidate how model organic mixtures enhance or slow ECH; and (3) Design systems for simultaneous hydrogenation of organic mixtures. This research will elucidate reaction mechanisms for ECH of bio-oil mixtures and generate knowledge about the role of the applied electrochemical potential and water solvent for ECH using quantum mechanical modeling and experimental kinetics measurements and spectroscopy. Also, this work will clarify the role of co-adsorbed organics on the rate and selectivity of electrocatalytic hydrogenation and identify rates of electrochemical conversion to evaluate commercial feasibility compared to the state-of-the-art. This research will generate fundamental knowledge that can be used to enhance the efficiencies for bio-based fuel manufacturing processes at scale using renewable energy.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.