The electroreduction of nitrate offers a promising, sustainable, and decentralized route to generate valuable ammonia. However, a key challenge in the nitrate reduction reaction is the energy efficiency of the reaction, which requires both a high ammonia yield rate and a high Faradaic efficiency of ammonia at a low working potential (≥-0.2 V versus reversible hydrogen electrode).
View Article and Find Full Text PDFElectrochemical epoxidation of olefins using water as an oxygen atom source is emerging as an alternative approach for an atom economic and sustainable method towards a highly selective synthesis of epoxides. We report an electrochemical procedure for epoxidation of cyclooctene using water as the sole oxygen atom source over a sodium dodecyl sulfonate (SDS) modified nickel hydroxide Ni(OH) catalyst directly grown on Ni foam. The SDS modification facilitates the mass transfer of cyclooctene towards the anode, thus achieving a 2.
View Article and Find Full Text PDFRenewable electricity-powered nitrate (NO ) reduction reaction (NO RR) offers a net-zero carbon route to the realization of high ammonia (NH ) productivity. However, this route suffers from low energy efficiency (EE, with a half-cell EE commonly <36%), since high overpotentials are required to overcome the weak NO binding affinity and sluggish NO RR kinetics. To alleviate this, a rational catalyst design strategy that involves the linear assembly of sub-5 nm Cu/Co nanophases into sub-20 nm thick nanoribbons is suggested.
View Article and Find Full Text PDFBi-based electrocatalysts have been widely investigated in the CO reduction reaction (CO RR) for the formation of formate. However, it remains a challenge to achieve high Faradaic efficiency (FE) and industrial current densities at low overpotentials for obtaining both high formate productivity and energy efficiency (EE). Herein, we report an Ag-Bi O hybrid nanofiber (Ag-Bi O ) for highly efficient electrochemical reduction of CO to formate.
View Article and Find Full Text PDFElectrocatalytic recycling of waste nitrate (NO) to valuable ammonia (NH) at ambient conditions is a green and appealing alternative to the Haber-Bosch process. However, the reaction requires multi-step electron and proton transfer, making it a grand challenge to drive high-rate NH synthesis in an energy-efficient way. Herein, we present a design concept of tandem catalysts, which involves coupling intermediate phases of different transition metals, existing at low applied overpotentials, as cooperative active sites that enable cascade NO-to-NH conversion, in turn avoiding the generally encountered scaling relations.
View Article and Find Full Text PDFBimetallic tandem catalysts have emerged as a promising strategy to locally increase the CO flux during electrochemical CO reduction, so as to maximize the rate of conversion to C-C-coupled products. Considering this, a novel Cu/C-Ag nanostructured catalyst has been prepared by a redox replacement process, in which the ratio of the two metals can be tuned by the replacement time. An optimum Cu/Ag composition with similarly sized particles showed the highest CO conversion to C products compared to non-Ag-modified gas-diffusion electrodes.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
October 2021
Developing highly efficient and selective electrocatalysts for the CO reduction reaction to produce value-added chemicals has been intensively pursued. We report a series of Cu O C nanostructured electrocatalysts derived from a Cu-based MOF as porous self-sacrificial template. Blending catalysts with polytetrafluoroethylene (PTFE) on gas diffusion electrodes (GDEs) suppressed the competitive hydrogen evolution reaction.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
April 2021
Electroreduction of CO to multi-carbon products has attracted considerable attention as it provides an avenue to high-density renewable energy storage. However, the selectivity and stability under high current densities are rarely reported. Herein, B-doped Cu (B-Cu) and B-Cu-Zn gas diffusion electrodes (GDE) were developed for highly selective and stable CO conversion to C products at industrially relevant current densities.
View Article and Find Full Text PDFAlthough the use of bioresorbable materials in stent production is thought to improve long-term safety compared to their durable counterparts, a recent FDA report on the 2-year follow-up of the first FDA-approved bioresorbable vascular stent showed an increased occurrence of major adverse cardiac events and thrombosis in comparison to the metallic control. In order to overcome the issues of first generation bioresorbable polymers, a series of polyethylene glycol-functionalized poly-L-lactide-co-ε-caprolactone copolymers with varying lactide-to-caprolactone content is developed using a novel one-step PEG-functionalization and copolymerization strategy. This approach represents a new facile way toward surface enhancement for cellular interaction, which is shown by screening these materials regarding their cyto- and hemocompatibility in terms of cytotoxicity, hemolysis, platelet adhesion, leucocyte activation and endothelial cell adhesion.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
January 2020
Carbon corrosion at high anodic potentials is a major source of instability, especially in acidic electrolytes and impairs the long-term functionality of electrodes. In-depth investigation of carbon corrosion in alkaline environment by means of differential electrochemical mass spectrometry (DEMS) is prevented by the conversion of CO into CO . We report the adaptation of a DEMS system for online CO detection as the product of carbon corrosion in alkaline electrolytes.
View Article and Find Full Text PDFNiFe layered double hydroxide (LDH) is inarguably the most active contemporary catalyst for the oxygen evolution reaction under alkaline conditions. However, the ability to sustain unattenuated performance under challenging industrial conditions entailing high corrosivity of the electrolyte (≈30 wt. % KOH), high temperature (>80 °C) and high current densities (>500 mA cm ) is the ultimate criterion for practical viability.
View Article and Find Full Text PDFChemphyschem
September 2014
The oxygen evolution reaction (OER) is an enabling process for technologies in the area of energy conversion and storage, but its slow kinetics limits its efficiency. We performed an electrochemical evaluation of 14 different perovskites of variable composition and stoichiometry as OER electrocatalysts in alkaline media. We particularly focused on improved methods for a reliable comparison of catalyst activity.
View Article and Find Full Text PDFScanning electrochemical microscopy (SECM) has been used to detect and visualize the local electrocatalytic activity of dimensionally stable anodes (DSA) for Cl(2) evolution from brine. The sample generation-tip collection (SG-TC) mode of SECM shows limitations arising from complications connected with the reduction of Cl(2) at the SECM tip due to the presence of a significant amount of nondissolved Cl(2) gas. Because only dissolved Cl(2) can be electrochemically reduced at the tip, a large amount of the Cl(2) gas which is produced at active spots of the DSA is not detected.
View Article and Find Full Text PDFFaraday Discuss
October 2005
The interaction of water vapour with mineral dust and soot surfaces has been studied in the temperature range 203 K < T < 298 K using a Knudsen cell reactor. For the uptake of water on mineral dust an initial uptake coefficient of gamma(ini) = (6.3 +/- 0.
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