Death and Life of Catalysts: A Theory-Guided Unified Approach for Non-Critical Metal Catalyst Development

ERC-2016-COG | Project no. 725686

Catalysis plays a pivotal role in all strategies towards sustainable chemical technologies of the future. To minimize the adverse effects due to the use of non-renewable hydrocarbon feedstocks, novel technologies have to be conceived and materialized shortly to enable the direct use of renewable feedstocks and to make the existing chemical processes more atom- and energy-efficient. Endeavors towards the sustainable use of feedstocks should be accompanied by the efforts to make the catalyst utilization also more sustainable. The current paradigm is that most developments in catalysis largely rely on empirical findings gained through laborious experimental efforts, in which potentially active systems can be overlooked simply because of the sub-optimal conditions of the initial activity assessment. Mechanistic and kinetic studies could provide a framework for a more adequate assessment of new catalysts, but such rigorous experiments are not practical for general catalyst discovery. Modern chemical theory and computations hold a promise to be employed in new efficient theory-guided approaches for rational catalyst and process development.

The main aim of DeLiCat is to develop an integrated computational and experimental strategy for the design and optimization of efficient catalytic systems based on non-critical metal-based catalysts for sustainable chemical transformations such as catalytic reduction of carbonyl-containing compounds. Besides their fundamental importance to synthetic organic chemistry as the sustainable alternatives to the conventional stoichiometric routes producing vast amounts of waste, these highly atom-efficient catalytic transformations can be employed in various processes ranging from biomass upgrading to hydrogen storage and fine organic synthesis. In addition, other important catalytic processes such as selective oxidation of methane, dehydrogenation of alkanes, CO2 hydrogenation, electroreduction and other other relevant systems are considered as representative model processes for the integration of computational and experimental catalyst development workflows.

The innovative workflow that we develop in the course of this project integrates advanced chemical theory and computational screening with an experimental chemical and chemical engineering approaches in an efficient knowledge exchange loop. An important goal of the theoretical program in this project is to develop new operando modeling approaches that would allow to better understand how variation in the reaction conditions affects the behaviour of the catalyst system.

These insights would help the experimentalist navigate through the highly complex and multidimensional condition space towards enhanced catalyst lifetime and overall process efficiency.

DeLiCat puts a special emphasis on understanding the undesirable side-reactions resulting in the deactivation of the catalyst and decreasing thus the efficiency of the overall project. Catalyst deactivation is inevitable. However, we propose that by optimizing the catalytic system, one can postpone the deactivation and, hence, improve substantially catalyst performance in terms of the catalyst use so that higher yield of desirable products could be produced with lower catalyst concentration, making the catalyst use more sustainable and contributing to the improved economics of the process. In this project we use computer simulations to understand the chemistry of the “death” and the “life” of catalyst systems and learn how to control the underlying chemical transformations. These insights are then used in the targeted design of novel multifunctional catalyst systems to direct the selectivity of the reaction network and to prevent deactivation paths.

DeLiCAT Publications