In this study, the copper-nickel (Cu-Ni) bimetallic electrocatalysts for electrochemical CO reduction reaction(CORR) are fabricated by taking the finely designed poly(ionic liquids) (PIL) containing abundant Salen and imidazolium chelating sites as the surficial layer, wherein Cu-Ni, PIL-Cu and PIL-Ni interaction can be readily regulated by different synthetic scheme. As a proof of concept, Cu@Salen-PIL@Ni(NO) and Cu@Salen-PIL(Ni) hybrids differ significantly in the types and distribution of Ni species and Cu species at the surface, thereby delivering distinct Cu-Ni cooperation fashion for the CORR. Remarkably, Cu@Salen-PIL@Ni(NO) provides a C2+ faradaic efficiency (FE) of 80.
View Article and Find Full Text PDFThe electrocatalytic reduction of CO to CO with high efficiency is one of the most promising approaches for CO conversion due to its considerable economic feasibility and broad application prospects. In this study, three Ag@COF-R (R = -H, -OCH, -OH) hybrids were facilely fabricated by impregnating silver acetate (AgOAc) into respective covalent organic frameworks (COFs) prepared in advance. They differ significantly in the crystallinity, porosity, distribution, size, and electronic configuration of AgOAc species, which thereby influences both the activity and the selectivity of electrolytic CO-to-CO transformation.
View Article and Find Full Text PDFThe electrocatalytic transformation of carbon dioxide (CO ) to formate is a promising route for highly efficient conversion and utilization of CO gas, due to the low production cost and the ease of storage of formate. In this work, porous poly(ionic liquid) (PPIL)-based tin-silver (Sn-Ag) bimetallic hybrids (PPIL -Sn Ag ) are prepared for high-performance formate electrolytic generation. Under optimal conditions, an excellent formate Faradaic efficiency of 95.
View Article and Find Full Text PDFIn this study, a tungstated zirconia (WO/ZrO) catalyst was developed for the continuous synthesis of adiponitrile (ADN) by gas-phase nitrilation of dimethyl adipate (DMA) with NH. The highest TOF could be reached on WO/ZrO bearing ∼1D WO species (highly dispersed and discontinuous status) at the surface, which, however, delivered the poorest selectivity toward nitrilation (S). In comparison, both efficient and selective transformation of DMA to ADN was achieved by fabricating WO/ZrO with continuously distributed oligomeric WO species (∼2D) at the surface, either by varying the dosage of the W-reagent in the preparation of WO(m)/ZrO or by doping a proper amount of the Mn element into WO(5.
View Article and Find Full Text PDFElectrocatalytic reduction of CO (CORR) to multi-electron (> 2e) products provides a green and sustainable route for producing fuels and chemicals. Introducing the second metal element is a feasible strategy for "managing" the key intermediate on Cu-based materials to further improve the CORR catalytic performance. In this work, palladium, which promises the generation of CO, was introduced into the poly(ionic liquid)-based copper hybrid (Cu@PIL) to construct a novel Cu-Pd bimetallic electrocatalyst (Cu@PIL@Pd).
View Article and Find Full Text PDFThe reliable and accurate quantification of ammonia in electrochemical and photochemical experiments has been a technical challenge owing to the extremely low concentration of generated ammonia, interference from trace amounts of cations and organic compounds, and ammonia contamination from various sources. As a result, overestimation and significant errors may happen in many research works. Herein, accuracy and precision of ion chromatography (IC) are evaluated at different pH; excellent performance with a low detection limit (<2 μg L ) under acidic and neutral conditions is found, whereas the linearity is unsatisfactory in the low NH concentration range (0-100 μg L ) under alkaline conditions.
View Article and Find Full Text PDF