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Greenhouse gas emissions present a significant challenge to humanity, and utilizing renewable electricity to convert emitted CO2 into value-added products offers a promising solution; however, traditional CO2 capture and regeneration processes remain energy-intensive, restricting the overall system efficiency and decarbonization efficacy. In this study, an advanced direct reduction of captured CO2 with large current densities for formate electrosynthesis was demonstrated without the need for CO2 regeneration or compression. The bismuth nanosheet (DRM-BiNS) was synthesized by direct reduction of a Bi-based MOF, representing a new class of catalytic materials with a large surface area and interconnected pores, suitable for the direct reduction of captured CO₂. By seamlessly combining experimentation and simulation, insights into the structure-parameter-performance relation were acquired in a flow cell setting, including critical membrane-electrode distance, cell orientation, and pumping flow rate. Important flow-cell components, such as catholyte volume, electrode substrate, membrane choice, and ionomer type, were also carefully examined to enhance the cell performance. In sharp contrast to prior studies limited to current densities below 20 mA/cm² in bicarbonate-based captured CO2 solutions, this work demonstrates a remarkable current density of 300 mA/cm² with an FE to formate comparable to the case with gas-fed CO2 reduction. Moreover, the process sustained an FE above 50% at a high current density of 500 mA/cm². The DRM-BiNS catalyst exhibited outstanding selectivity, activity, and stability, significantly outperforming oxide-derived bismuth nanosheets (OD-BiNS) in captured CO2 reduction. These findings offer critical insights into the development of sustainable and scalable CO2 utilization technologies. 

Greenhouse gas emissions present a significant challenge to humanity, and utilizing renewable electricity to convert emitted CO2 into value-added products offers a promising solution; however, traditional CO2 capture and regeneration processes remain energy-intensive, restricting the overall system efficiency and decarbonization efficacy. In this study, an advanced direct reduction of captured CO2 with large current densities for formate electrosynthesis was demonstrated without the need for CO2 regeneration or compression. The bismuth nanosheet (DRM-BiNS) was synthesized by direct reduction of a Bi-based MOF, representing a new class of catalytic materials with a large surface area and interconnected pores, suitable for the direct reduction of captured CO₂. By seamlessly combining experimentation and simulation, insights into the structure-parameter-performance relation were acquired in a flow cell setting, including critical membrane-electrode distance, cell orientation, and pumping flow rate. Important flow-cell components, such as catholyte volume, electrode substrate, membrane choice, and ionomer type, were also carefully examined to enhance the cell performance. In sharp contrast to prior studies limited to current densities below 20 mA/cm² in bicarbonate-based captured CO2 solutions, this work demonstrates a remarkable current density of 300 mA/cm² with an FE to formate comparable to the case with gas-fed CO2 reduction. Moreover, the process sustained an FE above 50% at a high current density of 500 mA/cm². The DRM-BiNS catalyst exhibited outstanding selectivity, activity, and stability, significantly outperforming oxide-derived bismuth nanosheets (OD-BiNS) in captured CO2 reduction. These findings offer critical insights into the development of sustainable and scalable CO2 utilization technologies. 

Highly efficient capacitive deionization (CDI) relies on unimpeded transport of salt ions to the electrode surface. Graphene is an ideal candidate to provide superb conditions for ion adsorption as it possesses high theoretical surface area and electrical conductivity. When ions are stored solely within the electric double layers (EDLs), a hydrophilic graphene surface with hierarchical pores can maximize the accessible surface area and promote the ion transport. In the case of synergistic ion storage via electrostatic adsorption and faradaic redox reaction, graphene can act as both the electron highway and the reciprocal spacer to provide surface-confined effects. Substantially, structural and chemical engineering towards graphene can enhance the ion removal capacity and rate, and improve the charge efficiency and ion selectivity. In this review, we keep pace with the in-depth studies of CDI technologies and recent progress on graphene-based materials for CDI. Major challenges in the rational assembly of the desired material functionalities in terms of surface area, pore structure, and hydrophilicity are addressed. As electrode materials develop, the ultimate goal is to achieve highly efficient, energy-saving, and environment-friendly CDI.