CAREER: SusChEM: Electrocatalytic Valorization of Biomass Intermediates via 1st-Row Transition Metal Electrocatalysts

如果能够开发适当的化学转化方法，从废弃的农业材料或高效种植的植物中获得的生物质有可能成为一种重要的、可再生的清洁能源和化学原料来源。犹他州州立大学的孙玉杰博士受到化学系化学催化计划的支持，致力于利用一种新的电催化过程进行生物质转化的研究。电催化使用电流提供的电子在受控和有效的催化过程中驱动化学反应，这是一种提高化学对话速度和效率的化学途径。孙博士的研究阐明了生物质分子电催化氧化的化学反应途径或机理步骤，并建立了第一排过渡金属基电催化剂的催化剂组成与其催化活性之间的关系。由于具有良好的导电性和高效的催化活性，过渡金属被制备成非常薄的薄膜，称为二维超薄纳米片。这项研究的更广泛影响来自开发一种有效的生物质转化过程，以利用可再生的生物质资源生产燃料和其他化学品。孙先生还在教育和外联活动中与学生一起工作，创造了更广泛的影响机会。他积极参与外展项目，专注于吸引和指导STEM领域中代表性不足的群体的学生，如美洲原住民本科生和经济困难的高中生，并在犹他州立大学的本科生实验课程中创造尖端的研究机会。尽管生物质价化已被认为是生产非化石化工产品的一种有吸引力的策略，但传统的升级方法往往需要苛刻的条件、有毒的试剂和/或昂贵的催化剂。在化学系化学催化项目的这一职业奖项的支持下，犹他州州立大学的孙玉杰博士正在开发一种替代电催化方法，利用第一排过渡金属基电催化剂进行生物质升级。特别是，本项目阐明了环境条件下5-羟甲基呋喃甲醛(HMF)的电催化氧化的机理步骤，并建立了用于HMF价态的第一排过渡金属氧化物(TMO)的组成-活性关系。利用这些信息，制备了最有希望的超薄二维TMO，并对其进行了研究，以获得其对HMF氧化的本征电催化活性。超薄的电催化剂厚度旨在绕过电阻率问题。实验活动得到与实验平行进行的密度泛函理论(DFT)计算的支持，并被用来帮助解释所测量的活性趋势和组成-活性关系中的其他变量。这项研究的更广泛影响来自开发一种有效的生物质转化过程，以利用可再生的生物质资源生产燃料和其他化学品。孙先生还在他的教育和外展活动中创造机会，在学生培训和指导方面产生更广泛的影响。他积极参与以STEM领域代表性不足的学生为重点的外展计划，如美洲原住民本科生和经济困难的高中生，并在犹他州的本科生实验课程中创造尖端的研究机会。

Biomass, obtained from waste agricultural materials or efficiently - grown plants, has the potential to be a significant, renewable source of clean energy and chemical feedstocks if appropriate methods of chemical conversion can be developed. Dr. Yujie Sun of Utah State University is supported by the Chemical Catalysis Program of the Chemistry Division to pursue research into the investigation of biomass conversion using a novel electrocatalytic process. Electrocatalysis uses electrons provided by an electric current to drive chemical reactions in the controlled and efficient process of catalysis, a chemical pathway that increases the speed and efficiency of the chemical converstion. Dr. Sun's research elucidates the chemical reaction pathways, or mechanistic steps, of the electrocatalytic oxidation of biomass molecules and establishes the relationship between the catalyst composition and its catalytic activity for 1st-row transition metal-based electrocatalysts. For good conductivity and efficient catalytic activity, the transition metals are fabricated as very thin films known as two-dimensional ultrathin "nanosheets". Broader impacts of the research result from the development of an efficient biomass conversion process to produce fuels and other chemicals from renewable biomoass resources. Dr. Sun also creates broader impact opportunities in his work with students in education and outreach activities. He is actively engaged in outreach programs focusing on attracting and mentoring students from groups that are under - represented in the STEM fields, such as Native American undergraduates and economically disadvantaged high school students, as well as creating cutting - edge research-based opportunities in experimental courses for undergraduate students at Utah State University. Even though biomass valorization has been recognized as an attractive strategy in producing nonfossil- based chemical products, the conventional upgrading approaches often require harsh conditions, toxic regents, and/or expensive catalysts. With the support of this CAREER award from the Chemical Catalysis Program of the Chemistry Division, Dr. Yujie Sun of Utah State University is developing an alternative electrocatalytic approach for biomass upgrading utilizing 1st row transition metal-based electrocatalysts. In particular, this project elucidates the mechanistic steps of the electrocatalytic oxidation of 5-hydroxymethyl furfural (HMF, one of the top biomass-derived platform chemicals) under ambient conditions and establishes a composition - activity relationship of 1st-row transition metal oxides (TMOs) for HMF valorization. Using this information, ultrathin two-dimensional (2D) TMOs of the most promising compositions are prepared and interrogated to obtain their intrinsic electrocatalytic activities for HMF oxidation. The ultrathin electocatalyst thickness is designed to circumvent electric resistivity problems. The experimental activities are supported with density functional theory (DFT) calculations, conducted in parallel with the experiments, and are used to aid the interpretation of measured activity trends and other variables in the composition-activity relationship. Broader impacts of the research result from the development of an efficient biomass conversion process to produce fuels and other chemicals from renewable biomoass resources. Dr. Sun also creates opportunities for broader impacts in student training and mentorship in his education and outreach activities. He is actively engaged in outreach programs that are focused on students from groups under - represented in the STEM fields, such as Native American undergraduates and economically disadvantaged high school students, as well as creating cutting - edge research-based opportunities in experimental courses for undergraduate students in Utah.