Publication date: 17th July 2025
(Photo)electrochemical transformations represent a promising route to convert waste into value-added chemicals and fuels. Among the various approaches, photoelectrochemical (PEC) CO₂ reduction is particularly attractive due to its potential for direct solar-to-chemical energy conversion. However, realizing such devices requires selective and stable multi-carbon (C₂⁺) product formation, which remains a key challenge in the field. In our recent work, we have focused on improving both the selectivity and stability of PEC systems by using novel photocathode materials and tailored interfaces.
Here, we explore the role of microenvironments in addressing reaction selectivity,1,2 and we couple this concept with integration of halide perovskite based photoelectrodes. We show that halide perovskite based photoelectrodes coupled with tailored catalytic interfaces enable enhanced CO₂ physisorption, leading to a substantial increase in ethylene production efficiency, while maintaining long-term stability.
We also propose a similar approach for the electrochemical nitrate (NO3−) reduction reaction (NO3RR), which is a promising route for NH3 production by utilizing NO3−, a ubiquitous pollutant commonly found in wastewater. The electrochemical NO3RR to NH3 is recognized as a tandem catalytic process, comprising two major steps: NO3− to NO2− and NO2− to NH3. Therefore, achieving high overall NH3 conversion efficiency requires effective catalysis in both steps. While many researchers have focused on developing novel electrocatalysts for NO3RR, the influence of the underlying microenvironment on selective NH3 production remains poorly understood. Herein, we investigate the use of organic modifiers, specifically ionomers, to enhance the electrochemical NO3RR to NH3 on pure Cu electrocatalysts, which inherently exhibit a large energy barrier for hydrogenation due to limited H* availability.
[1] A. K. Buckley, M. Lee, T. Cheng, R. V. Kazantsev, D. M. Larson, W. A. Goddard III, F. D. Toste, F. M. Toma, Electrocatalysis at Organic–Metal Interfaces: Identification of Structure–Reactivity Relationships for CO2 Reduction at Modified Cu Surfaces, JACS 2019, 141, 18, 7355–7364
[2] A. K. Buckley, T. Cheng, M. Hwan Oh, G. M. Su, J. Garrison, S. W. Utan, C. Zhu, F. D. Toste, W. A. Goddard III, Francesca M. Toma, Approaching 100% Selectivity at Low Potential on Ag for Electrochemical CO2 Reduction to CO Using a Surface Additive, ACS Catalysis 2021, 11, 15, 9034-9042
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