(326j) Reactivity Vs. Durability: Building Physics-Driven, Quantitative Blueprints of Catalytic Interfaces for Decarbonization

Catalytic interfaces lie at the center of sustainable energy technologies that reduce carbon emissions, generate renewable electricity, and produce green chemicals and fuels. However, the implementation of these clean energy technologies is currently constrained by the lack of catalysts that work efficiently (i.e., high activity) without degrading (i.e., high stability). Notably, state-of-the-art catalysts still have intrinsic activity orders of magnitude lower than their biological counterparts, resulting in low efficiency. Moreover, the degradation of catalytic interfaces over short timescales has severely hampered their commercial viability. Given such performance gaps, unfortunately, the optimization of catalytic activity and stability has been severely limited by traditional research paradigms that largely rely on chemical intuition and serendipity [1], lacking physics-driven, quantitative design principles to grapple with balancing the reactivity and durability of catalytic interfaces and elucidating their intricate nature.

My research addresses this scientific question—how to physically elucidate and quantitatively engineer catalysts on the atomic scale to have optimal activity and stability for diverse renewable technologies. To this end, I have identified one of the first-ever sets of stability design principles for inhibiting catalyst dissolution in acid, where modulating the electronic structure of transition metal oxides and nitrides stabilizes these catalysts against decomposition in acidic electrolytes by controlling the bonding character and dissolution barrier. [2,3]. Moreover, I have shown that rationally tuning the electron-withdrawing capability of heterometal substituents in transition metal oxides optimizes their bonding properties, reaction barrier, and catalytic activity for electrochemical water splitting to generate clean hydrogen fuels [4,5]. These design principles provide new, physics-driven blueprints with quantitative predictive power for activity−stability optimization in catalyst development to combat the most recalcitrant, urgent societal challenges in sustainability and decarbonization, including climate change, environmental pollution, and energy and food insecurity. Such design principles can also motivate future work to rationalize, control, and balance the reactivity and durability of other key reactive interfaces for clean energy conversion and storage, e.g., in batteries and photovoltaics, and bring qualitative changes to the world.

References:

[1] Peng, et al. Nat. Rev. Mater. 7, 991–1009 (2022).

[2] Peng, et al. Joule 7, 150–167 (2023).

[3] Peng, et al. Chem. Mater. 34, 7774–7787 (2022).

[4] Yuan†, Peng†, Cai†, et al. Nat. Mater. 21, 673–680 (2022). († denotes equal contribution)

[5] Kuznetsov†, Peng†, et al. J. Phys. Chem. C 124, 6562–6570 (2020). († denotes equal contribution)