To reach industrially relevant current densities in the electrochemical reduction of carbon dioxide, this process must be performed in continuous-flow electrolyzer cells, applying gas diffusion electrodes. Beyond the chemical composition of the catalyst, both its morphology and the overall structure of the catalyst layer are decisive in terms of reaction rate and product selectivity. We present an electrodeposition method for preparing coherent copper nanocube catalyst layers on hydrophobic carbon paper, hence forming gas diffusion electrodes with high coverage in a single step. This was enabled by the appropriate wetting of the carbon paper (controlled by the composition of the electrodeposition solution) and the use of a custom-designed 3D-printed electrolyzer cell, which allowed the deposition of copper nanocubes selectively on the microporous side of the carbon paper substrate. Furthermore, a polymeric binder (Capstone ST-110) was successfully incorporated into the catalyst layer during electrodeposition. The high electrode coverage and the binder content together result in an increased ethylene production rate during CO reduction, compared to catalyst layers prepared from simple aqueous solutions.
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http://dx.doi.org/10.1039/d3nr03834c | DOI Listing |
Nat Commun
December 2024
School of Chemistry and Chemical Engineering, Frontiers Science Center for Transformative Molecules, Shanghai Jiao Tong University, Shanghai, 200240, P. R. China.
Electrochemical nitrate reduction reaction offers a sustainable and efficient pathway for ammonia synthesis. Maintaining satisfactory Faradaic efficiency for long-term nitrate reduction under ampere-level current density remains challenging due to the inevitable hydrogen evolution, particularly in pure nitrate solutions. Herein, we present the application of electron deficiency of Ru metals to boost the repelling effect of counter K ions via the electric-field-dependent synergy of interfacial water and cations, and thus largely promote nitrate reduction reaction with a high yield and well-maintained Faradaic efficiency under ampere-level current density.
View Article and Find Full Text PDFSci Rep
December 2024
Department of Mechanical Engineering, Carnegie Mellon University, Pittsburgh, PA, USA.
Polymer electrolyte membrane water electrolyzers (PEMWEs) are a critical technology for efficient hydrogen production to decarbonize fuels and industrial feedstocks. To make hydrogen cost-effective, the overpotentials across the cell need to be decreased and platinum-group metal loading reduced. One overpotential that needs to be better understood is due to mass transport limitations from bubble formation within the porous transport layer (PTL) and anode catalyst layer (ACL), which can lead to a reduction in performance at typical operating current densities.
View Article and Find Full Text PDFNat Commun
December 2024
Jiangsu Co-Innovation Center of Efficient Processing and Utilization of Forest Resources, Nanjing Forestry University, Nanjing, 210037, China.
Carbon nanomaterials show outstanding promise as electrocatalysts for hydrogen peroxide (HO) synthesis via the two-electron oxygen reduction reaction. However, carbon-based electrocatalysts that are capable of generating HO at industrial-level current densities (>300 mA cm) with high selectivity and long-term stability remain to be discovered. Herein, few-layer boron nanosheets are in-situ introduced into a porous carbon matrix, creating a metal-free electrocatalyst (B-C) with HO production rates of industrial relevance in neutral or alkaline media.
View Article and Find Full Text PDFAdv Mater
December 2024
State Key Lab of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, Shanghai, 200050, P. R. China.
Nickel-iron layered double hydroxides (NiFe LDHs) are considered as promising substitutes for precious metals in oxygen evolution reaction (OER). However, most of the reported NiFe LDHs suffer from poor long-term stability because of the Fe loss during OER resulting in severe inactivation. Herein, a dynamically stable chelating interface through in situ transformation of asymmetric aldehyde-ligand (THB, 1,3,5-Tris(3'-hydroxy-4'-formylphenyl)-benzene) modified NiFe LDHs to anchor Fe and significantly enhance the OER stability is reported.
View Article and Find Full Text PDFFront Chem
December 2024
Research Center for Macromolecules and Biomaterials, National Institute for Materials Science (NIMS), Tsukuba, Japan.
Although the Diels-Alder reaction (DA) has garnered significant attention due to its numerous advantages, its long reaction time is a drawback. Herein, we investigated the effects of polarity difference on DA using Layer-by-Layer (LbL) films comprising polycationic polyallylamine hydrochloride and polyanionic poly (styrenesulfonic acid-co-furfuryl methacrylate) [poly (SS--FMA)] as the reaction environment. First, furan composition in poly (SS--FMA) was adjusted to be 19 mol% to achieve good water solubility and layer deposition.
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