CAREER SusChEM: Recyclable transfer hydrogenation catalysts by tuning non-innocent catalytic supports

Career SusChEM：可回收的转移加氢催化剂通过调整非无害催化支持可持续催化过程的开发需要最大限度地减少催化中稀有、昂贵和有毒金属的使用，从而增加对可应用于工业过程的富含地球和无害的催化材料的依赖。与此同时，需要找到建设性地利用工业废物的新方法，例如燃烧过程中产生的二氧化碳和生物柴油生产中产生的甘油。在化学催化项目的资助下，Voutchkova-Kostal博士正在通过开发基于地球上丰富的金属的可回收催化剂来应对这些挑战，这些催化剂有助于将二氧化碳和甘油转化为甲酸和二羟丙酮，从而将两股废物流转化为有用的工业化学品。她正在通过跨学科的绿色化学、环境健康和科学政策论坛以及强调探究性学习的新的研究型有机化学实验室模块，将她的工作的更广泛影响扩展到大学和更大的华盛顿特区社区。这些活动通过吸引研究生和本科生跨越这些学科，在绿色化学、政策和公共卫生领域架起了一座桥梁。开发能够与均相类似物的活性和选择性相匹配的负载型单位多相催化剂(SSHC)需要对载体和固定化金属络合物之间的相互作用和潜在的协同作用有基本的了解。在化学催化项目的资助下，Voutchkova-Kostal博士正在探索结构-性质-活性关系，这些关系是为挑战转移加氢反应而设计活性、选择性和长寿命SSHC所需的。具体地说，通过磺酸盐连接物将Ir和Rh有机金属络合物固定在电子可调的层状双氢氧化物载体上。使用表面敏感和体光谱技术的补充来探索影响催化活性和稳定性的电子效应。这些研究成果被应用于甘油二氧化碳转移加氢催化剂和不对称转移加氢催化剂的活性、选择性和稳定性的优化。为了将这项工作和其他绿色化学发展的更广泛影响转化为大学和更大的DC社区，Voutchkova-Kostal博士正在共同组织一个跨学科的绿色化学、环境健康和科学政策论坛，以促进科学家和公众就热门科学问题进行对话。为了让学生参与研究，她还实施了新的以研究为基础的有机化学实验室模块，强调基于探究的学习。

CAREER SusChEM: Recyclable transfer hydrogenation catalysts by tuning of non-innocent catalytic supports The development of sustainable catalytic processes requires minimizing the use of rare, expensive, and toxic metals in catalysis, thus increasing reliance on earth-abundant and benign catalytic materials that are applicable to industrial processes. Concurrently, there is a need for finding new ways of constructively using industrial waste products, such as carbon dioxide generated in combustion processes and glycerol generated in biodiesel production. With funding from the Chemical Catalysis program, Dr. Voutchkova-Kostal is addressing these challenges by developing recyclable catalysts based on earth-abundant metals that are useful for converting carbon dioxide and glycerol into formic acid and dihydroxyacetone, thus turning two waste streams into useful industrial chemicals. She is extending the broader impacts of her work to the University and greater DC communities via an interdisciplinary Green Chemistry, Environmental Health and Science Policy Forum and new research-based organic chemistry laboratory modules that emphasize inquiry-based learning. These activities bridge the fields of green chemistry, policy and public health by engaging graduate and undergraduate students across these disciplines.The development of supported single-site heterogeneous catalysts (SSHCs) that can match the activity and selectivity of homogeneous analogs requires fundamental understanding of the interactions and potential synergies between supports and immobilized metal complexes. With funding from the Chemical Catalysis program, Dr. Voutchkova-Kostal is probing the structure-property-activity relationships that are needed to predictably design active, selective and long-lived SSHCs for challenging transfer hydrogenation reactions. Specifically, iridium and rhodium organometallic complexes are immobilized onto electronically-tunable layered double-hydroxide supports via sulfonate linkers. A complement of surface-sensitive and bulk spectroscopic techniques is used to probe the electronic effects that impact catalytic activity and stability. The insights developed are applied to optimizing the activity, selectivity and stability of a recyclable heterogeneous catalyst for transfer hydrogenation CO2 from glycerol, as well as recyclable catalysts for asymmetric transfer hydrogenation. To translate the broader impacts of this work and other developments in green chemistry to the university and greater DC communities, Dr. Voutchkova-Kostal is co-organizing an interdisciplinary Green Chemistry, Environmental Health and Science Policy Forum that facilitates dialogue on topical scientific issues across scientists and the public. To engage students in research she is also implementing new research-based organic chemistry laboratory modules that emphasize inquiry-based learning.