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，从废弃农业材料或高效生长的植物中获得的生物质具有成为清洁能源和化学原料的重要的可再生来源的潜力。 犹他州州立大学的孙宇杰博士得到化学系化学催化项目的支持，利用一种新型的电催化过程对生物质转化进行研究。 电催化使用电流提供的电子来驱动催化过程中的受控和有效的化学反应，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械步骤，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。 为了获得良好的导电性和有效的催化活性，过渡金属被制成非常薄的薄膜，称为二维纳米片。这项研究的更广泛影响来自于开发一种有效的生物质转化过程，从可再生生物质资源中生产燃料和其他化学品。孙博士还在教育和外展活动中与学生一起创造更广泛的影响机会。 他积极参与外展计划，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困难的高中生，以及为犹他州州立大学的本科生创造实验课程中的前沿研究机会。 尽管生物质价值稳定已被认为是生产非化石基化学产品的有吸引力的策略，但常规的升级方法通常需要苛刻的条件、有毒试剂和/或昂贵的催化剂。在化学部化学催化项目的支持下，犹他州州立大学的Yujie Sun博士正在开发一种利用第一排过渡金属基电催化剂进行生物质升级的替代电催化方法。特别是，该项目阐明了在环境条件下5-羟甲基糠醛（HMF，顶级生物质衍生平台化学品之一）的电催化氧化的机理步骤，并建立了用于HMF稳定化的第一行过渡金属氧化物（TMO）的组成-活性关系。使用这些信息，制备和询问最有前途的组合物的二维（2D）TMO，以获得其固有的HMF氧化的电催化活性。 电催化剂的厚度被设计成避免电阻率问题。实验活动的支持与密度泛函理论（DFT）的计算，在平行进行的实验，并用于帮助解释测得的活动趋势和其他变量的组合物-活性关系。这项研究的更广泛影响来自于开发一种有效的生物质转化过程，从可再生生物质资源中生产燃料和其他化学品。孙博士还在其教育和外展活动中为学生培训和导师提供更广泛的影响力。 他积极参与外展计划，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困难的高中生，以及为犹他州的本科生创造实验课程中的前沿研究机会。

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.