The incompatibility between the anode and the cathode chemistry limits the used of Mg as an anode. This issue may be addressed by separating the anolyte and the catholyte with a membrane that only allows for Mg2+ transport. Mg‐MOF‐74 thin films were used as the separator for this purpose. It was shown to meet the needs of low‐resistance, selective Mg2+ transport. The uniform MOF thin films supported on Au substrate with thicknesses down to ca. 202 nm showed an intrinsic resistance as low as 6.4 Ω cm2, with the normalized room‐temperature ionic conductivity of ca. 3.17×10−6 S cm−1. When synthesized directly onto a porous anodized aluminum oxide (AAO) support, the resulting films were used as a standalone membrane to permit stable, low‐overpotential Mg striping and plating for over 100 cycles at a current density of 0.05 mA cm−2. The film was effective in blocking solvent molecules and counterions from crossing over for extended period of time.
Significant optical absorption in the blue–green spectral range, high intralayer carrier mobility, and band alignment suitable for water splitting suggest tin disulfide (SnS2) as a candidate material for photo‐electrochemical applications. In this work, vertically aligned SnS2 nanoflakes are synthesized directly on transparent conductive substrates using a scalable close space sublimation (CSS) method. Detailed characterization by time‐resolved terahertz and time‐resolved photoluminescence spectroscopies reveals a high intrinsic carrier mobility of 330 cm2 V−1 s−1 and photoexcited carrier lifetimes of 1.3 ns in these nanoflakes, resulting in a long vertical diffusion length of ≈1 µm. The highest photo‐electrochemical performance is achieved by growing SnS2 nanoflakes with heights that are between this diffusion length and the optical absorption depth of ≈2 µm, which balances the competing requirements of charge transport and light absorption. Moreover, the unique stepped morphology of these CSS‐grown nanoflakes improves photocurrent by exposing multiple edge sites in every nanoflake. The optimized vertical SnS2 nanoflake photoanodes produce record photocurrents of 4.5 mA cm−2 for oxidation of a sulfite hole scavenger and 2.6 mA cm−2 for water oxidation without any hole scavenger, both at 1.23 VRHE in neutral electrolyte under simulated AM1.5G sunlight, and stable photocurrents for iodide oxidation in acidic electrolyte.
SUMMARYThe generalized model of di erential hysteresis contains 13 control parameters with which it can curveÿt practically any hysteretic trace. Three identiÿcation algorithms are developed to estimate the control parameters of hysteresis for di erent classes of inelastic structures. These algorithms are based upon the simplex, extended Kalman ÿlter, and generalized reduced gradient methods. Novel techniques such as global search and internal constraints are incorporated to facilitate convergence and stability. E ectiveness of the devised algorithms is demonstrated through simulations of two inelastic systems with both pinching and degradation characteristics in their hysteretic traces. Owing to very modest computing requirements, these identiÿcation algorithms may become acceptable as a design tool for mapping the hysteretic traces of inelastic structures.
Redox-switchable polymerization of lactide and epoxides were extended to the solid state by anchoring an iron-based polymerization catalyst to TiO2 nanoparticles. The reactivity of the molecular complexes and their redox-switching...
Multi‐elemental alloy (MEA) nanoparticles have recently received notable attention owing to their high activity and superior phase stability. Previous syntheses of MEA nanoparticles mainly used carbon as the support, owing to its high surface area, good electrical conductivity, and tunable defective sites. However, the interfacial stability issue, such as nanoparticle agglomeration, remains outstanding due to poor interfacial binding between MEA and carbon. Such a problem often causes performance decay when MEA nanoparticles are used as catalysts, hindering their practical applications. Herein, an interface engineering strategy is developed to synthesize MEA–oxide–carbon hierarchical catalysts, where the oxide on carbon helps disperse and stabilize the MEA nanoparticles toward superior thermal and electrochemical stability. Using several MEA compositions (PdRuRh, PtPdIrRuRh, and PdRuRhFeCoNi) and oxides (TiO2 and Cr2O3) as model systems, it is shown that adding the oxide renders superior interfacial stability and therefore excellent catalytic performance. Excellent thermal stability is demonstrated under transmission electron microscopy with in situ heating up to 1023 K, as well as via long‐term cycling (>370 hours) of a Li–O2 battery as a harsh electrochemical condition to challenge the catalyst stability. This work offers a new route toward constructing efficient and stable catalysts for various applications.
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