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

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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.