ChemElectroChem最新文献

This review showcases crucial factors in mechanisms of electrochemical CO₂ reduction by taking Pd-based electrocatalysts (mainly, monometallic Pd and Pd-based alloy nanoparticles) as examples. There are dependencies of experimental conditions (e.g., applied potentials) and constituent elements of the electrocatalysts on the reduction products of electrochemical CO₂ reduction. Moreover, Pd-based electrocatalysts have unique characteristics in electrochemical CO₂ reduction: alteration in selectivities for CO and HCOOH formations by applied potentials, almost no overpotential for HCOOH formation, deactivation of their electrocatalyses by poisoning with CO formed through CO₂ reduction, and in situ formation of palladium hydride. Here, we survey the characteristics of Pd-based electrocatalysts in terms of experimental and theoretical insights. Then, it is described that formation energies of intermediates estimated by density functional theory calculations are understandable factors to explain experimental performances of Pd-based electrocatalysts. Considering the estimated factors, this review exhibits a perspective of utilization of the factors to advance the research activity of electrochemical CO₂ reduction to its new horizon by using data science and high-throughput experiments.

Aromatic nitriles are extensively produced chemicals with a wide variety of applications. The high demand of these compounds justifies the search for sustainable synthesis alternatives using renewable energy. Here, an electrochemical oxidation of toluene and xylene derivatives to aromatic nitriles using NH₃ and H₂O under ambient conditions in a one-pot, two-step protocol is reported. In a first step, the toluene derivative is oxidized in the absence of a catalyst to the aldehyde. In the second step, ammonia is added together with LiI as an electrocatalyst to obtain the nitrile. The reaction network and mechanism are investigated using control experiments and cyclic voltammetry.

This study introduces a novel quasi-solid-state battery system as a proof of concept. A 55-nm solid-state electrolyte layer of lithium phosphorous oxynitride (LiPON) is deposited on slurry-based graphite electrodes and assembled against lithium metal to evaluate interfacial compatibility and electrochemical performance under controlled conditions. In contrast to thin-film quasi-solid-state batteries, this approach leverages a realistic electrode architecture, where LiPON adjusts to the rough surface of the slurry-cast graphite. By utilizing LiPON's dual functionality as both a solid-state electrolyte and a separator, the system eliminates the need for a conventional separator, while requiring only 5–10% of the liquid electrolyte used in equivalent systems. This design significantly reduces internal resistance and prevents contact loss during cyclic volume changes. Electrochemical analyses, including cyclic voltammetry, galvanostatic cycling, and impedance spectroscopy, demonstrate lithium intercalation stages consistent with those in liquid electrolyte-based systems, stable cycling behavior at room temperature and reduced electrode impedance of a few 10 Ω cm². Furthermore, X-ray photoelectron spectroscopy and scanning transmission electron microscopy confirm the formation of a solid–liquid electrolyte interface and the structural integrity of LiPON, which enhances charge transfer and long-term stability. These findings highlight the potential of quasi-solid-state batteries for safer, more compact, and cost-effective energy storage solutions.

This cover artwork illustrates the development of emerging materials such as MOFs, 2D materials, SACs, HEAs, perovskites, and MXenes as highly efficient electrocatalysts for water splitting. It highlights the advances in synthesis and heterostructural engineering for judicious synchronization of the synthesis strategies with the emerging electrocatalysts for exploring the potentials and challenges of the next generation of high-performing advanced electrocatalysts for sustainable hydrogen production. Further information can be found in the Research Article by Thangjam Ibomcha Singh, Seunghyun Lee, and co-workers (DOI: 10.1002/celc.202500014).

This study presents the synthesis of biomass-derived carbon-metal organic framework (C-MOF) using modified sawdust as a sustainable precursor and elucidates its electrochemical performance as an anode material for sodium-ion batteries (SIBs). Optimization at a pyrolysis temperature of 1000 °C with 7.5% catalyst concentration, C-MOF achieves a high surface area of 312 m⁻²g⁻¹ and electrical conductivity of 28 S cm⁻¹, contributing to its long cycling electrochemical performance compared to commercial hard carbon (HC). The C-MOF delivers a maximum discharge capacity of 348.5 mAh g⁻¹ at 25 mA g⁻¹ and exhibits an outstanding cycling stability over 600 cycles with minimal degradation. Electrochemical techniques (cyclic voltammetry, impedance, and galvanostatic charge–discharge) reveal efficient sodium-ion intercalation and favorable ion diffusion characteristics within the porous C-MOF structure. These findings position C-MOF as a promising, sustainable, and long-standing anode material for advanced SIB applications, offering enhanced rate capability, durability, and effective sodium-ion kinetics.

The synthesis of peptide-based linkers for antibody-drug conjugates involves an oxidative decarboxylation step. Traditional Hofer–Moest electrolysis conditions are not suitable to achieve this transformation due to the presence of an oxidatively labile Fmoc-protecting group. Herein, a solvent-enabled electrochemical procedure has been established, whereby the solvent electrochemical window prevents degradation of the protecting group. The method has been demonstrated for several relevant peptides in good to very good yields (64–92%).

Physical and chemical parameters, such as temperature, water/hydrogen/oxygen partial pressures, are distributed inhomogeneous inside a polymer electrolyte fuel cell during the operation and have a large influence on its performance and durability. In this study, the oxygen partial pressure (p(O₂)) is visualized in real-time/space using an oxygen-sensitive dye on the surface of the gas diffusion layer (GDL) during power generation at temperatures of 80, 100, and 110 °C using a 20 mm × 20 mm single cell with ten straight gas flow channels. p(O₂) on the surface of the GDL is visualized for the first time at temperatures higher than 100 °C, desired especially for heavy-duty vehicle application, due to advantages such as less susceptibility to catalyst poisoning and the option to use smaller and lighter radiators. The oxygen partial pressure on the surface of the GDLs is monitored to be higher than the values expected from a simple model and decreased only slightly along the gas flow channel with increasing current densities. The work shows that high p(O₂) on the surface of the GDL is due to the short gas flow channels and accumulating water/vapor inside the GDL and the catalyst layer limiting the gas diffusion.

Lithium–sulfur batteries have attracted great research interest due to the high theoretical capacity of sulfur of 1672 mAh g⁻¹. However, they have various problems due to the shuttle current caused by molecular sulfur dissolving in the electrolyte. Hence, electrolyte design is a key focus when optimizing the batteries. This study investigates the relationship between cycling data and electrochemical properties measured with cyclovoltammetric measurements, shuttle current measurements, and impedance spectroscopy. Using the acquired data, a partial least squares model to screen solvent candidates in reference to these findings is introduced. This model is based on cycling data as well as density functional theory-calculated Conductor-like Screening Model for Real Solvents data of the solvents and (solvated) lithium–polysulfides. The usefulness of the converged method is demonstrated by using it to identify new possible electrolyte systems. A subset of ten selected electrolyte systems is evaluated experimentally and their performance is reported. One of those electrolytes, 1.4 M LiTFSI, in pimelonitrile solution and without any further additives, displays exceptional cycling stability already on the first attempt, reaching a state of health of 50% after 115 cycles and maintaining a Coulombic efficiency of close to 100% during the entire cycling procedure.

The surface oxide reduction method, a well-established technique for determining the electrochemically active surface area of Pd, is also widely used for Pd–Co alloys. However, comprehensive studies investigating the influence of the alloy composition on the determination of the surface area by the surface oxide reduction method are lacking for this alloy system. To fill this gap, a systematic investigation is conducted by applying the surface oxide reduction method to homogeneous Pd_100−xCo_x alloy samples with different compositions (x = 0−20). The results reveal that full monolayer coverage with surface oxide occurs at lower potentials than for pure Pd and that the surface area determined by this method systematically decreases with increasing Co content, indicating that only the Pd sites are accessible by this method. However, it is demonstrated that by taking the alloy composition into account, the surface area of the whole alloy can also be reliably determined.

The image depicts personifications of sulfur and lithium mirroring each other’s movements to illustrate the linear correlation observed in our study. They are surrounded by molecules of the solvents used in the research. The Research Article by Ingo Krossing and co-workers explores the correlation between the potentials of lithium and sulfur as influenced by the choice of electrolyte solvent (DOI: 10.1002/celc.202500109).