(451e) Dynamic Electrification Toward Sustainable and Enhanced Catalysis

Dynamic electrification, particularly employing high-frequency temperature pulses through Joule heating^1-3, can significantly improve performance and facilitate the decarbonization of chemical manufacturing processes. We start from comprehensive prototypical models⁴ and move up to full microkinetic models, toward applications like ammonia decomposition and synthesis on a ruthenium multisite catalyst⁵. We also validate the model experimentally using a millisecond pulse reactor, allowing for a rigorous examination of the dynamic pulse heating's efficacy in surpassing conventional steady-state and thermodynamic limits.

We elucidate a profound enhancement in ammonia decomposition rates through dynamic operation, notably exceeding equilibrium values, through our models and experiments. We provide a detailed mechanistic understanding of the reasons for the enhanced performance. We unveil interesting catalyst dynamics in turn affecting the chemistry during the pulsing operation and provide detailed analysis of energy requirements. We discuss metrics to compare continuous and pulsed Joule heating with conventional heating. This exploration elucidates the technical intricacies of dynamic electrification and underscores its potential to revolutionize catalytic processes toward the decarbonization of the chemical industry.

References

(1) Yu, K.; Wang, C.; Zheng, W.; Vlachos, D. G. ACS Energy Letters 2023, 8 (2), 1050-1057. DOI: 10.1021/acsenergylett.2c02666.

(2) Yu, K.; Sourav, S.; Zheng, W.; Vlachos, D. G. Chemical Engineering Journal 2024, 481, 148528. DOI: https://doi.org/10.1016/j.cej.2024.148528.

(3) Dong, Q.; Yao, Y.; Cheng, S.; Alexopoulos, K.; Gao, J.; Srinivas, S.; Wang, Y.; Pei, Y.; Zheng, C.; Brozena, A. H.; et al. Nature 2022, 605 (7910), 470-476. DOI: 10.1038/s41586-022-04568-6.

(4) Railkar, R.; Vlachos, D. Industrial & Engineering Chemistry Research 2024, 63 (1), 130-138. DOI: 10.1021/acs.iecr.3c03198.

(5) Wittreich, G. R.; Liu, S.; Dauenhauer, P. J.; Vlachos, D. G.Science Advances 2022, 8 (4), eabl6576. DOI: 10.1126/sciadv.abl6576.