Investigating the Role of Solvents Toward the Targeted Reduction of Aldehydes to Alcohols
EMSL Project ID
51171
Abstract
Tackling climate change and environmental protection is one of the chief Sustainable Development Goals identified by United Nation at the nexus of social and economic factors across the globe. Lignocellulosic biomass has been recognized as the sustainable alternative that has the ability to the impact our future energy resources. Owing to its abundance, biomass has always been part of human history to provide energy generally via direct burning. However, we need to go beyond the conventional methods to efficiently utilize its potential, where catalysis can play a central role to accelerate the production of energy, commodity chemicals and value-added products from these sources. Moreover, catalytic biomass conversion to fuels could produce energy in carbon-neutral and even carbon negative ways minimizing the overall carbon footprint in the atmosphere. One of the grand challenges in the design of catalysts for the direct upgrading of biomass is the presence of an insurmountable and diverse array of hydrocarbons along with the mixture of oxygenated compounds produced during its thermochemical treatment. The high oxygen content of functional groups like aldehydes, ketones, acids that require catalytic upgrading, in the form of selective hydrogenation in order to produce sustainable biofuels and bioproducts, further complicates the design of effective hydrogenating catalysts due to the complexity and heterogeneity of the biomass feedstocks. The design of hydrogenation catalysts must be able to selectively target the C-O bonds in these compounds, while minimizing its hydrogen consumption and thus upgrading cost. The transfer of hydrogen to bio-based oxygen functional groups at the catalyst surface can be significantly enhanced through solvent effects at the liquid-solid interface but at the cost of increased design variables for catalysis. To fully optimize the catalyst performance, there is a critical need to gain fundamental insight into the atomistic-scale elementary reduction reactions occurring at the liquid-solid interface.For competitive fuel generation from sustainable biomass-derived sources, we aim at probing the scientific questions related to the atomistic-scale interplay between polar protic solvents and metal surfaces during elementary hydrogen transport, C-H and O-H formation reactions under realistic hydrogenation conditions. Within our research scope, we will be demonstrating that the rate and dominant pathway for the reduction of aldehydes can be systematically tuned by the presence of water and provide an atomistic understanding of the formation of reactive surface hydrogen species under liquid phase hydrogenation conditions leading to targeted reduction of C-O bonds. The working hypothesis is that the hydrogen addition to carbonyl functionality in aldehydes or ketones can be selectively tuned with the charge of H, stabilization of the transition state, hydrogen bonding and barriers along the elementary reaction. We propose to use the computational resources available at EMSL to understand the atomistic interactions that are associated with the catalytic conversion of biomass. We will be closely collaborate with experimentalists to model catalysts so as to reduce both the computational expense and experimental efforts in characterizing such complex systems. We have a team with rich experience in application and science of heterogeneous catalysis along with record of collaborating with EMSL staff in producing high impact science, particularly related to the catalytic upgrading of bio-oils, and an outstanding expertise in the tools required to accomplish the objectives of the proposed studies in stipulated time.
Project Details
Start Date
2019-10-01
End Date
2020-09-30
Status
Closed
Released Data Link
Team
Principal Investigator
Co-Investigator(s)
Team Members