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dc.contributor.advisorHuang, Kuo-Wei
dc.contributor.authorGuan, Chao
dc.date.accessioned2019-10-02T12:56:41Z
dc.date.available2019-10-02T12:56:41Z
dc.date.issued2019-09
dc.identifier.doi10.25781/KAUST-4W71Z
dc.identifier.urihttp://hdl.handle.net/10754/656843
dc.description.abstractFormic acid (FA) has been considered as one of the most promising materials for hydrogen storage today. The catalytic decarboxylation of formic acid ideally leads to the formation of CO2 and H2, and such CO2/H2 mixtures can be successfully applied in fuel cells. A large number of transition-metal based homogeneous catalysts with high activity and selectivity have been reported for the formic acid decarboxylation. In this presentation, we report ruthenium and rhodium complexes containing an N, N′-diimine ligand for the selective decomposition of formic acid to H2 and CO2 in water in the absence of any organic additives. Among them, the Ru complex could provide a TOF (turnover frequency) of 12 000 h–1 and a TON (turnover number) of 350 000 at 90 °C in the HCOOH/HCOONa aqueous solution. In addition to that, efficient production of high-pressure H2 and CO2 (24.0 MPa (3480 psi)) was achieved through the decomposition of formic acid with no formation of CO by this Ru complex. Moreover, well-defined ruthenium (II) PN3P pincer complexes were also developed for the reversible reaction-hydrogenation of carbon dioxide. Excellent product selectivity and catalytic activity with TOF and TON up to 13,000 h-1 and 33,000, respectively, in a THF/H2O biphasic system were achieved. Notably, effective conversion of carbon dioxide from the air into formate was conducted in the presence of an amine, allowing easy product separation and catalyst recycling.
dc.language.isoen
dc.subjecthomogeneous catalysis, Formic acid dehydrogenation, Hydrogen storage. CO2 Utilization
dc.titleReversible Formic Acid Dehydrogenation to Hydrogen and CO2 Catalyzed by Ruthenium and Rhodium Complexes
dc.typeDissertation
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.rights.embargodate2020-09-26
thesis.degree.grantorKing Abdullah University of Science and Technology
dc.contributor.committeememberHan, Yu
dc.contributor.committeememberLai, Zhiping
dc.contributor.committeememberZheng, Junrong
thesis.degree.disciplineChemical Science
thesis.degree.nameDoctor of Philosophy
dc.rights.accessrightsAt the time of archiving, the student author of this dissertation opted to temporarily restrict access to it. The full text of this dissertation will become available to the public after the expiration of the embargo on 2020-09-26.
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