CO2 electroreduction reaction (CO2RR) to fuels and feedstocks is an attractive route to close the anthropogenic carbon cycle and store renewable energy. The generation of more reduced chemicals, especially multicarbon oxygenate and hydrocarbon products (C2+) with higher energy density is highly desirable for industrial applications. However, selective conversion of CO2 to C2+ suffers from high overpotential, low reaction rate and low selectivity, and the process is extremely sensitive to the catalyst structure and electrolyte. Here we discuss strategies to achieve high C2+ selectivity through rational design of the catalyst and electrolyte. Current state-of-the-art catalysts, including Cu and Cu-bimetallic catalysts as well as alternative materials are considered. The importance of taking into consideration the dynamic evolution of the catalyst structure and composition are highlighted, focusing on findings extracted from in situ and operando characterizations. Additional theoretical insight into the reaction mechanisms underlying the improved C2+ selectivity of specific catalyst geometries/compositions in synergy with a well-chosen electrolyte are also provided.

Rational Catalyst and Electrolyte Design for Co2 Electroreduction Towards Multicarbon Products

The carbon dioxide (CO2) methanation reaction not only provides a solution for mitigating the excessive carbon dioxide emissions but also can potentially be employed for the storage and transportat...

Essential Role of the Support for Nickel-Based CO2 Methanation Catalysts

Atomically dispersed metal catalysts maximize atom efficiency and display unique catalytic properties compared with regular metal nanoparticles. However, achieving high reactivity while preserving high stability at appreciable loadings remains challenging. Here we solve the challenge by synergizing metal–support interactions and spatial confinement, which enables the fabrication of highly loaded atomic nickel (3.1 wt%) along with dense atomic copper grippers (8.1 wt%) on a graphitic carbon nitride support. For the semi-hydrogenation of acetylene in excess ethylene, the fabricated catalyst shows extraordinary catalytic performance in terms of activity, selectivity and stability—far superior to supported atomic nickel alone in the absence of a synergizing effect. Comprehensive characterization and theoretical calculations reveal that the active nickel site confined in two stable hydroxylated copper grippers dynamically changes by breaking the interfacial nickel–support bonds on reactant adsorption and making these bonds on product desorption. Such a dynamic effect confers high catalytic performance, providing an avenue to rationally design efficient, stable and highly loaded, yet atomically dispersed, catalysts. Synergizing metal–support interactions and spatial confinement through atomic copper grippers boost the dynamics of highly loaded atomic nickel for high activity, high thermal/chemical stability and unprecedented coke inhibition in hydrogenation reactions.

Synergizing metal–support interactions and spatial confinement boosts dynamics of atomic nickel for hydrogenations

Recent advances in CO2 hydrogenation to value-added products — Current challenges and future directions

Ceria-Based Materials for Thermocatalytic and Photocatalytic Organic Synthesis

It is challenging to elucidate the mechanism of CO2 methanation reaction over nickel-based catalysts and precisely tune the kinetics of rate-determining-step. In this work, we propose a strategy to engineer the oxygen vacancies of nickel-based catalysts for enhanced CO2 methanation. A Y2O3-promoted NiO-CeO2 catalyst is prepared and found to exhibit an outstanding methanation activity that is up to three folds higher than NiO-CeO2 and six folds higher than NiO-Y2O3 at mild reaction temperatures (

Vacancy engineering of the nickel-based catalysts for enhanced CO2 methanation

Ceria has been used as a hydrogenation catalyst especially in selective alkyne hydrogenation, but the reaction mechanism regarding the role of different surface hydrogen species remains unclear. In...

Jisue Moon

Papers

Vacancy engineering of the nickel-based catalysts for enhanced CO2 methanation

Discriminating the Role of Surface Hydride and Hydroxyl for Acetylene Semihydrogenation over Ceria through In Situ Neutron and Infrared Spectroscopy