Anirudha Shekhawat

Targeting the electrocatalytic CO ₂ reduction reaction (eCO ₂ RR) using complex multimetal catalysts is a relatively new approach in electrocatalyst design. We explored the eCO ₂ RR performance for lanthanoids and similar rare‐earth elements such as Gd, Sc, Tb, Nd, Sm, and Y as components in CuAgAl catalyst mixtures. Product selectivity is highly sensitive to the complexity of the catalysts (i.e. the number and identity of constituting elements) and the potential (activity) controlled by the compositions. Particularly, most of the Gd‐containing catalysts showed high Faradaic efficiency (FE) for C ₂₊ products (FE _C2+ ), >60%, at a current density of −400 mA cm ⁻² . Using mean absolute error analysis, we investigated the correlation between multimetal composition, product selectivity, and required potential at a defined current density. The modulation in product distribution is likely promoted by the distinct properties of the multimetal catalysts. Operando Raman measurements of two multimetal catalysts (Cu ₈₀ Ag ₅ Al ₅ Gd ₅ Sm ₅ and Cu ₈₀ Ag ₅ Al ₅ Nd ₅ Sm ₅ ) revealed different mechanisms shown by the variations in the local alkalinity of the microenvironments and catalyst reconstruction, despite both catalysts exhibit an FE _C2+ of 65%. Exploring multimetal catalysts expands the design space for elemental selection, allowing for distinct mechanisms that expand the understanding of selectivity modulation.

Electrochemical CO ₂ reduction is a promising approach for a sustainable economy, as it converts CO ₂ into valuable products. However, converting CO ₂ into multicarbon products specifically, toward acetate as the major product, is challenging due to high energy barriers and low CO* coverage on the catalyst surface. This leads to the primary products being ethylene and ethanol instead. While electrochemical approaches for converting CO to acetate are gaining attention, accomplishing this directly through CO ₂ reduction remains a substantial challenge. This mini review summarizes recent advancements in catalyst design and experimental strategies to convert CO ₂ into acetate. We discuss various strategies, innovations in catalyst design, and electrochemical setups to enhance selectivity and efficiencies.

Operando Raman spectroscopy captures the gradual transition from CO ₂ reduction to hydrogen evolution under increasingly cathodic potentials, revealing the pivotal role of interfacial water reorientation in initiating HER.

Metal–organic frameworks (MOFs) are considered promising electrocatalytic materials due to their adjustable coordination bonds between metal ions and organic ligands. The abundance of metal centers within MOFs offers potential active sites. However, the limited availability of adsorption sites in the case of fully coordinated metal ions might lead to insufficient electrocatalytic activity. The selectivity is tuned during the electrochemical CO ₂ reduction reaction (eCO ₂ RR) using Cu‐1H‐1,2,3‐triazole MOF from C ₁ products to C ₂₊ products by generating defects to enable a local increase in CO ^* coverage, thus improving eCO ₂ RR performance. The catalyst exhibits ≈78.4% of total Faradaic efficiency for C ₂₊ products at −200 mA cm ⁻² current density in 1.0 m KOH as electrolyte.