In situ construction of thiol-silver interface for selectively electrocatalytic CO2 reduction

Abstract

Electrochemical CO 2 reduction (ECR) is one of the most effective methods to obtain carbonaceous chemicals and reduce greenhouse gases passingly under the ambient condition. However, efficient electrocatalysts featured with high selectivity and stability are still lacking. A novel molecule-mediated Ag electrocatalyst with capped thiols is rationally designed for high-performance ECR. The thiol-capped and carbon-supported Ag nanostructures (Ag-TC) are formed by in situ electrochemical reduction from three-dimentional (3D) Ag-thiol metal-organic compound with cysteine as the anchor agent and carbon source. Ag-TC exhibits high selectivity and stability for CO 2 conversion to CO (86.7%), which is more catalytically active than that of common Ag nanoparticles. The function of thiols for ECR is proved by replacing cysteine with alanine without thiol group. Meanwhile, alternatively replacing and removing the surface molecules on the Ag foil further demonstrate the effct of thiols. This work enlightens the promise of in situ construction method for molecule capped metal electrocatalyst towards selective and stable ECR.

Evolution of Electrocatalytic CO2 Reduction Activity Induced by Charge Segregation in Atomically Precise AuAg Nanoclusters Based on Icosahedral M13 Unit 3D Assembly

“…The Tafel slopes of the three NCs are lower than those usually obtained in Au/Ag-based catalysts (80-120 mV dec −1 ), suggesting the faster reaction kinetics and better CO 2 RR activity of NCs. [20][21][22][23][24][25] However, the three NCs show similar Tafel slopes with the value ranging from 72 to 75 mV dec −1 , indicating that the three NCs undergo same electrochemical kinetic process for CO 2 RR (Figure S9, Supporting Information). Therefore, the kinetics factor is excluded.…”

Ce4+-Doped CuO Mesoporous Nanosheets for CO2 Electroreduction to C2H6 with High Selectivity under a Wide Potential Window in a Flow Cell

“…CO 2 electrocatalytic reduction (CO 2 ER) to oxygenates or hydrocarbons provides an appealing route to reduce climate change and realize carbon neutrality. − Compared to C 1 products, C 2 products have gained ever-growing attention due to their higher energy densities, which can be expediently integrated with the existing infrastructure. − Among the C 2 products, C 2 H 6 is evoking increasing interest by its highest energy density and wide application as a commodity chemical. , At present, metal Cu materials are promising candidates for C 2 H 6 production, such as Cu mesopore electrodes, skeleton (sponge) Cu, oxide-derived Cu, ,, or iodide-derived Cu nanoarchitectures, ,, owing to their strong binding energies for *CO by the high overlap of the binding states between Cu 3d and C 2p that promotes subsequent C–C coupling. , However, the selectivity of ethane on various catalysts during CO 2 ER rarely exceeds 50% because of the poor controllability on C–C coupling and the hydrogenation process that generally leads to the competitive pathways toward methane, ethylene, or ethanol with higher selectivity. This situation also directly results in no report on CO 2 ER to ethane in a flow cell to obtain a large commercial current density (>200 mA cm –2 ).…”

Cu-Loaded NaNbO3 Three-Dimensional Networks for CO2 Photoreduction to C2 Species

“…To address these issues, it is necessary to develop new technology for carbon dioxide capture, storage, and utilization to realize carbon neutrality. 1,2 Solar energy is one of the potential renewable energies that can satisfy the future energy needs. Artificial photosynthesis using solar energy can split water into H 2 gas and reduce CO 2 to produce green fuels, such as methane and methanol, as well as high-valued compounds, such as ethane and ethylene, thereby converting solar energy into chemical energy.…”

“…In the past centuries, with the development of human society, the increase in energy demand has led to the massive consumption of fossil fuels in the world, resulting in critical energy and environmental problems. To address these issues, it is necessary to develop new technology for carbon dioxide capture, storage, and utilization to realize carbon neutrality. , Solar energy is one of the potential renewable energies that can satisfy the future energy needs. Artificial photosynthesis using solar energy can split water into H 2 gas and reduce CO 2 to produce green fuels, such as methane and methanol, as well as high-valued compounds, such as ethane and ethylene, thereby converting solar energy into chemical energy. , In recent years, the use of CO 2 photoreduction to produce carbon-based energy and high-valued compounds has attracted extensive attention of researchers because it can generate renewable green energy and useful chemicals. , …”