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Stimulating Methods for Promoting Catalytic Resonance doi.org/10.26434/chemrxiv.12818174.v1 The Catalytic Mechanics of Dynamic Surfaces: Stimulating Methods for Promoting Catalytic Resonance Manish Shetty, Amber Walton, Sallye R. Gathmann, M. Alexander Ardagh, Joshua Gopeesingh, Joaquin Resasco, Turan Birol, Qi Zhang, Michael Tsapatsis, Dionisios Vlachos, Phillip Christopher, C. Daniel Frisbie, Omar Abdelrahman, Paul Dauenhauer Submitted date: 17/08/2020 • Posted date: 24/08/2020 Licence: CC BY-NC-ND 4.0 Citation information: Shetty, Manish; Walton, Amber; Gathmann, Sallye R.; Ardagh, M. Alexander; Gopeesingh, Joshua; Resasco, Joaquin; et al. (2020): The Catalytic Mechanics of Dynamic Surfaces: Stimulating Methods for Promoting Catalytic Resonance. ChemRxiv. Preprint. https://doi.org/10.26434/chemrxiv.12818174.v1 Transformational catalytic performance in rate and selectivity is obtainable through catalysts that change on the time scale of catalytic turnover frequency. In this work, dynamic catalysts are defined in the context and history of forced and passive dynamic chemical systems, with classification of unique catalyst behaviors based on temporally-relevant linear scaling parameters. The conditions leading to catalytic rate and selectivity enhancement are described as modifying the local electronic or steric environment of the active site to independently accelerate sequential elementary steps of an overall catalytic cycle. These concepts are related to physical systems and devices that stimulate a catalyst using light, vibrations, strain, and electronic manipulations including electrocatalysis, back-gating of catalyst surfaces, and introduction of surface electric fields via solid electrolytes and ferroelectrics. These catalytic stimuli are then compared for capability to improve catalysis across some of the most important chemical challenges for energy, materials, and sustainability. File list (2) Perspective_Manuscript_ChemRxiv.pdf (3.88 MiB) view on ChemRxiv download file Perspective_Supporting_Information_ChemRxiv.pdf (149.75 KiB) view on ChemRxiv download file The Catalytic Mechanics of Dynamic Surfaces: Stimulating Methods for Promoting Catalytic Resonance Manish Shetty1,2†, Amber Walton1†, Sallye R. Gathmann1†, M. Alexander Ardagh1,2, Joshua Gopeesingh4, Joaquin Resasco3, Turan Birol1, Qi Zhang1, Michael Tsapatsis2,6,7, Dionisios G. Vlachos2,5, Phillip Christopher2,3, C. Daniel Frisbie1, Omar A. Abdelrahman2,4, Paul J. Dauenhauer1,2* 1 University of Minnesota, Department of Chemical Engineering and Materials Science, 421 Washington Ave. SE, Minneapolis, MN 55455, USA 2 Catalysis Center for Energy Innovation, 150 Academy Street, Newark, DE 19716, USA 3 University of California Santa Barbara, Engineering II Building, University of California, Santa Barbara, CA 93106, USA 4 University of Massachusetts Amherst, 686 N. Pleasant Street, Amherst, MA 01003, USA 5 University of Delaware, Department of Chemical and Biomolecular Engineering, 150 Academy Street, Newark, DE 19716, USA 6 Applied Physics Laboratory, Johns Hopkins University, Laurel, MD 20723, USA 7 Department of Chemical and Biomolecular Engineering & Institute for NanoBioTechnology, Johns Hopkins University, Baltimore, MD, 21218, USA * Corresponding author: [email protected] † Authors contributed equally Abstract. Transformational catalytic performance in rate and selectivity is obtainable through catalysts that change on the time scale of catalytic turnover frequency. In this work, dynamic catalysts are defined in the context and history of forced and passive dynamic chemical systems, with classification of unique catalyst behaviors based on temporally-relevant linear scaling parameters. The conditions leading to catalytic rate and selectivity enhancement are described as modifying the local electronic or steric environment of the active site to independently accelerate sequential elementary steps of an overall catalytic cycle. These concepts are related to physical systems and devices that stimulate a catalyst using light, vibrations, strain, and electronic manipulations including electrocatalysis, back-gating of catalyst surfaces, and introduction of surface electric fields via solid electrolytes and ferroelectrics. These catalytic stimuli are then compared for capability to improve catalysis across some of the most important chemical challenges for energy, materials, and sustainability. 1.0 Introduction. The history of synthetic catalyst structure has led to an open question in heterogeneous catalysts has been a quest to find the catalysis; do undiscovered catalysts still exist that optimal material to accelerate and control surface can provide transformational control of surface reactions. The best catalytic site for any chemistry chemistry? More importantly, is the pursuit solely has specific physical and electronic structure, of optimal catalytic structure via materials which has frequently been found through discovery or optimization even the right approach exploratory research, high throughput screening, to further improve catalyst design? directed evolution, and experimental The pursuit of ‘better’ catalysts relies on the serendipity(1,2,3,4,5). This search has led to entirely design philosophy that refined structures will new classes of inorganic materials for catalytic always provide faster and more selective applications including single metal atoms and catalysts(18,19,20,21); however, this strategy eventually alloys(6,7,8,9), metal-organic frameworks(10,11), approaches the fundamental limitations on static hierarchical zeolites(12,13), multi-metallic(14,15) and catalytic sites. The most restrictive catalytic intermetallic surfaces(16,17), all of which provide limitation is the Sabatier principle, which posits that structural and electronic control in the design of optimal catalysts exhibit intermediate surface catalytic active sites. However, the challenge of binding energies to balance the kinetic rates of two improving catalytic performance for some more or more reaction phenomena including surface mature applications by continued optimization of reactions, desorption, or adsorption(22). Since first ____________________________________________________________________________ Shetty, et al. Page 1 40 a A B b 20 A ] ] 0 1 1 B - - ] ] 1 1 - - -20 ΔHA ΔHB -40 TS State 2 E -60 A B* A* B* -80 -100 Enthalpy mol mol [kJ[kJ Enthalpy Enthalpy Enthalpy molmol [kJ[kJ Enthalpy Enthalpy Oscillation Oscillation Frequency -120 Frequency B* A* -140 State 1 -160 Figure 1. Dynamic heterogeneous catalysis. (a) A catalytic surface reaction is comprised of independent steps of adsorption, surface reaction(s), and desorption. (b) Forced variation of the energetic surface states including intermediates (e.g., A*, B*) and the transition state (TS) yields conditions favorable to adsorption and surface reaction (state 1) and desorption (state 2). proposed by Sabatier that the optimal catalyst forms hundreds of potential catalytic technologies such as (42) a ‘surface complex’ that readily forms and direct methane oxidation to methanol , CO2 desorbs(23), the principle was demonstrated decades conversion to methanol or ethylene(43,44), and later as kinetic plots referred to as ‘Sabatier hydrogen peroxide formation from oxygen and volcanoes’ with the optimal catalyst existing at the hydrogen(45,46,47) that are not yet sufficiently conditions of peak turnover frequency(24,25,26). selective for economic feasibility. Increasing the Lower catalytic rate on either side of the volcano kinetic ratio of desirable-to-side-reaction rates by derives from the catalyst favoring one elementary orders of magnitude to achieve nearly perfect step over the others, resulting in lower overall product selectivity (>99%) for most chemicals will turnover frequency through the whole sequence of require a completely different approach to catalyst steps. This concept has since been demonstrated design. across a broad range of chemistries and even A complementary catalysis strategy to active extended into ‘volcano surfaces’ or ‘maps’ for site design derives from the nature of catalytic multicomponent reactions(27,28,29,30,31,32,33,34,35) and mechanisms. Surface reactions are multiple dual site catalysts(36,37). sequential steps each with unique energetic and The selective capability of static catalysts for temporal characteristics.(48) From this perspective, many important chemistries has also achieved a an effective static catalytic active site is designed to performance status quo. Though a theoretical balance the needs of two-or-more elementary limitation does not exist for catalytic selectivity in phenomena. The ideal active site for product parallel, series, or more complicated network desorption is unlikely to also be ideal for surface reaction mechanisms, many commercial chemical reaction and reactant adsorption. However, a processes with the best available static catalysts dynamic catalytic active site that changes on the only achieve ~80-90% selectivity to desired time scale of the turnover frequency of the reaction products, including large-scale reactions such as could evolve over the catalytic cycle, providing an ethylene epoxidation(38) and propane optimal energetic environment for each step and the dehydrogenation,(39) in addition to technologies overall progression of the reaction sequence(49). A such as methanol-to-olefins that produce a single active site can be modulated to alternate distribution of products(40,41). For catalysts under between ideal characteristics for product kinetic control, 80% selectivity indicates that the desorption,
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