Employing Ag2Cu2O3, a mixed metal oxide, as a template catalyst material for electrochemical reduction of CO enables generation of multi-carbon products with a faradaic efficiency of close to 92%, at a current density of 600 mA cm−2.
The key to fully leveraging the potential of the electrochemical CO2 reduction reaction (CO2RR) to achieve a sustainable solar‐power‐based economy is the development of high‐performance electrocatalysts. The development process relies heavily on trial and error methods due to poor mechanistic understanding of the reaction. Demonstrated here is that ionic liquids (ILs) can be employed as a chemical trapping agent to probe CO2RR mechanistic pathways. This method is implemented by introducing a small amount of an IL ([BMIm][NTf2]) to a copper foam catalyst, on which a wide range of CO2RR products, including formate, CO, alcohols, and hydrocarbons, can be produced. The IL can selectively suppress the formation of ethylene, ethanol and n‐propanol while having little impact on others. Thus, reaction networks leading to various products can be disentangled. The results shed new light on the mechanistic understanding of the CO2RR, and provide guidelines for modulating the CO2RR properties. Chemical trapping using an IL adds to the toolbox to deduce the mechanistic understanding of electrocatalysis and could be applied to other reactions as well.
Supportinginformation and the ORCID identification number(s) for the author(s) of this article can be found under: https://doi. Figure 3. Ex situ XPS characterization of the surface chemical state in the Cu 2p 3/2 energy region:Pristine (blue), anodized (red), and anodized followed by areductive cyclic voltammetry scan in the CO 2 RR potential region (green). Cu 2p 3/2 peak binding energies are denoted in black lines for standard samples of Cu 0 ,Cu 2 O, CuO, and CuCO 3 ·Cu(OH) 2 .
Copper electrodes produce several industrially relevant chemicals and fuels during the electrochemical CO2 reduction reaction (CO2RR). Knowledge about the reaction pathways can help tune the reaction selectivity toward higher-value products....
The outstanding demonstration of quantum confinement in Si nanocrystals (Si NC) in a SiC matrix requires the fabrication of Si NC with a narrow size distribution. It is understood without controversy that this fabrication is a difficult exercise and that a multilayer (ML) structure is suitable for such fabrication only in a narrow parameter range. This parameter range is sought by varying both the stoichiometric SiC barrier thickness and the Si-rich SiC well thickness between 3 and 9 nm and comparing them to single layers (SL). The samples processed for this investigation were deposited by plasma-enhanced chemical vapor deposition (PECVD) and subsequently subjected to thermal annealing at 1000-1100 degrees C for crystal formation. Bulk information about the entire sample area and depth were obtained by structural and optical characterization methods: information about the mean Si NC size was determined from grazing incidence X-ray diffraction (GIXRD) measurements. Fourier-transform infrared spectroscopy (FTIR) was applied to gain insight into the structure of the Si-C network, and spectrophotometry measurements were performed to investigate the absorption coefficient and to estimate the bandgap E-04. All measurements showed that the influence of the ML structure on the Si NC size, on the Si-C network and on the absorption properties is subordinate to the influence of the overall Si content in the samples, which we identified as the key parameter for the structural and optical properties. We attribute this behavior to interdiffusion of the barrier and well layers. Because the produced Si NC are within the target size range of 2-4 nm for all layer thickness variations, we propose to use the Si content to adjust the Si NC size in future experiments
Silicon nanocrystals formed in the annealed SiNx/Si3N4 superlattices are attractive for research due to the smaller band offsets of Si3N4 matrix to Si in comparison with commonly used SiOx/SiO2 superlattices. However, the annealed SiNx/Si3N4 structures contain an increased number of nanocrystal interface defects, which completely suppress nanocrystal emission spectrum. In this work, we study a novel SiOxNy/Si3N4 hetero multilayer combination, which compromises the major issues of SiOx/SiO2 and SiNx/Si3N4 superlattices. The annealed SiOxNy/Si3N4 superlattices are investigated by TEM, demonstrating a precise sublayer thicknesses control. The PL spectra of the annealed SiOxNy/Si3N4 superlattices are centered at 845–950 nm with an expected PL peak shift for silicon nanocrystals of different sizes albeit the PL intensity is drastically reduced as compared to SiO2 separation barriers. The comparison of PL spectra of annealed SiOxNy/Si3N4 superlattice with those of SiOxNy/SiO2 superlattice enables the analysis of the interface quality of silicon nanocrystals. Using the literature data, the number of the interface defects and their distribution on the nanocrystal facets are estimated. Finally, it is shown that the increase of the Si3N4 barrier thickness leads to the increased energy transfer from the Si nanocrystals into the Si3N4 matrix, which explains an additional drop of the nanocrystal PL intensity
The key to fully leveraging the potential of the electrochemical CO2 reduction reaction (CO2RR) to achieve a sustainable solar‐power‐based economy is the development of high‐performance electrocatalysts. The development process relies heavily on trial and error methods due to poor mechanistic understanding of the reaction. Demonstrated here is that ionic liquids (ILs) can be employed as a chemical trapping agent to probe CO2RR mechanistic pathways. This method is implemented by introducing a small amount of an IL ([BMIm][NTf2]) to a copper foam catalyst, on which a wide range of CO2RR products, including formate, CO, alcohols, and hydrocarbons, can be produced. The IL can selectively suppress the formation of ethylene, ethanol and n‐propanol while having little impact on others. Thus, reaction networks leading to various products can be disentangled. The results shed new light on the mechanistic understanding of the CO2RR, and provide guidelines for modulating the CO2RR properties. Chemical trapping using an IL adds to the toolbox to deduce the mechanistic understanding of electrocatalysis and could be applied to other reactions as well.
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