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

如果能够开发出适当的化学转化方法，从废弃农业材料或有效种植的植物中获得的生物质有可能成为清洁能源和化学原料的重要可再生来源。犹他州立大学的孙玉杰博士得到了化学学部化学催化项目的支持，致力于研究利用新型电催化过程进行生物质转化的研究。电催化利用电流提供的电子在可控和有效的催化过程中驱动化学反应，这是一种提高化学转化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，并建立了第一行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，过渡金属被制成非常薄的薄膜，称为二维超薄“纳米片”。研究结果的更广泛影响来自于开发一种有效的生物质转化过程，以从可再生生物质资源中生产燃料和其他化学品。孙博士还在与学生的教育和外展活动中创造了更广泛的影响机会。他积极参与外展项目，专注于吸引和指导来自STEM领域代表性不足的群体的学生，如美国原住民本科生和经济上处于不利地位的高中生，以及为犹他州立大学本科生的实验课程创造前沿研究机会。尽管生物质增值已被认为是生产非化石基化学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。在化学部化学催化项目CAREER奖的支持下，犹他州立大学的孙玉杰博士正在开发一种利用第一排过渡金属基电催化剂的生物质升级替代电催化方法。特别地，本项目阐明了环境条件下5-羟甲基糠醛（HMF）电催化氧化的机理步骤，并建立了第一行过渡金属氧化物（TMOs）在HMF活化中的组成-活性关系。利用这些信息，制备了最有前途的组合物的超薄二维（2D） TMOs，并对其进行了研究，以获得其对HMF氧化的固有电催化活性。超薄的电催化剂厚度是为了避免电阻率问题而设计的。实验活动由密度泛函理论（DFT）计算支持，与实验并行进行，并用于帮助解释测量的活性趋势和成分-活性关系中的其他变量。研究结果的更广泛影响来自于开发一种有效的生物质转化过程，以从可再生生物质资源中生产燃料和其他化学品。孙博士还在他的教育和外展活动中为学生培训和指导创造了更广泛的影响机会。他积极参与外展项目，重点关注来自STEM领域代表性不足的群体的学生，如美国原住民本科生和经济上处于不利地位的高中生，以及为犹他州本科生的实验课程创造前沿研究机会。

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.