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Abstract Sodium–oxygen (Na–O₂) batteries are considered a promising energy storage alternative to current state‐of‐the‐art technologies owing to their high theoretical energy density, along with the natural abundance and low price of Na metal. The chemistry of these batteries depends on sodium superoxide (NaO₂) or peroxide (Na₂O₂) being formed/decomposed. Most Na–O₂batteries form NaO₂, but reversibility is usually quite limited due to side reactions at interfaces. By using new materials, including a highly active catalyst based on vanadium phosphide (VP) nanoparticles, an ether/ionic liquid‐based electrolyte, and an effective sodium bromide (NaBr) anode protection layer, the sources of interface reactivity can be reduced to achieve a Na–O₂battery cell that is rechargeable for 1070 cycles with a high energy efficiency of more than 83%. Density functional theory calculations, along with experimental characterization confirm the three factors leading to the long cycle life, including the effectiveness of the NaBr protective layer on the anode, a tetraglyme/EMIM‐BF₄based electrolyte that prevents oxidation of the VP cathode catalyst surface, and the EMIM‐BF₄ionic liquid aiding in avoiding electrolyte decomposition on NaO₂. 

Abstract 1D materials, such as nanofibers or nanoribbons are considered as the future ultimate limit of downscaling for modern electrical and electrochemical devices. Here, for the first time, nanofibers of a solid solution transition metal trichalcogenide (TMTC), Nb_1‐xTa_xS₃, are successfully synthesized with outstanding electrical, thermal, and electrochemical characteristics rivaling the performance of the‐state‐of‐the art materials for each application. This material shows nearly unchanged sheet resistance (≈740 Ω sq⁻¹) versus bending cycles tested up to 90 cycles, stable sheet resistance in ambient conditions tested up to 60 days, remarkably high electrical breakdown current density of ≈30 MA cm⁻², strong evidence of successive charge density wave transitions, and outstanding thermal stability up to ≈800 K. Additionally, this material demonstrates excellent activity and selectivity for CO₂conversion to CO reaching ≈350 mA cm⁻²at −0.8 V versus RHE with a turnover frequency number of 25. It also exhibits an excellent performance in a high‐rate Li–air battery with the specific capacity of 3000 mAh g⁻¹at a current density of 0.3 mA cm⁻². This study uncovers the multifunctionality in 1D TMTC alloys for a wide range of applications and opens a new direction for the design of the next generation low‐dimensional materials. 

Abstract Redox meditators (RMs) are soluble catalysts located in an electrolyte that can improve the energy efficiency (reduced overpotential) and cyclability of Li–oxygen (Li–O₂) batteries. In this work, 20 RMs within a Li–O₂system with dimethyl sulfoxide and tetraethylene glycol dimethyl ether electrolytes are studied and their electrochemical features such as redox potential, the separation of cathodic and anodic peaks, and their current intensities are measured using cyclic voltammetry (CV) experiments. Six RMs are selected as “primary” choices based on their electrochemical performance, and stability tests are then performed to examine their electrochemical responses after consecutive cycles. Moreover, galvanostatic cycling tests are performed within a Li–O₂battery system assembled with selected six RMs for real case consistency investigations. It is found that results from CV to galvanostatic cycling tests are consistent for halides and organometallic RMs, where the former exhibit much higher stability. However, the organic RMs show high reversibility in CV but low in battery cycling results. Density functional theory calculations are carried out to gain more understanding of the stability and redox potentials of the RMs. This study provides comparative information to select the most reliable RMs for Li–O₂batteries along with new fundamental understanding of their electrochemical activity and stability. 

Abstract Metal–organic frameworks (MOFs) are promising materials for electrocatalysis; however, lack of electrical conductivity in the majority of existing MOFs limits their effective utilization in the field. Herein, an excellent catalytic activity of a 2D copper (Cu)‐based conductive MOF, copper tetrahydroxyquinone (CuTHQ), is reported for aqueous CO₂reduction reaction (CO₂RR) at low overpotentials. It is revealed that CuTHQ nanoflakes (NFs) with an average lateral size of 140 nm exhibit a negligible overpotential of 16 mV for the activation of this reaction, a high current density of ≈173 mA cm⁻²at −0.45 V versus RHE, an average Faradaic efficiency (F.E.) of ≈91% toward CO production, and a remarkable turnover frequency as high as ≈20.82 s⁻¹. In the low overpotential range, the obtained CO formation current density is more than 35 and 25 times higher compared to state‐of‐the‐art MOF and MOF‐derived catalysts, respectively. The operando Cu K‐edge X‐ray absorption near edge spectroscopy and density functional theory calculations reveal the existence of reduced Cu (Cu⁺) during CO₂RR which reversibly returns to Cu²⁺after the reaction. The outstanding CO₂catalytic functionality of conductive MOFs (c‐MOFs) can open a way toward high‐energy‐density electrochemical systems. 

Abstract Transition metal dichalcogenide (TMDCs) alloys could have a wide range of physical and chemical properties, ranging from charge density waves to superconductivity and electrochemical activities. While many exciting behaviors of unary TMDCs have been demonstrated, the vast compositional space of TMDC alloys has remained largely unexplored due to the lack of understanding regarding their stability when accommodating different cations or chalcogens in a single‐phase. Here, a theory‐guided synthesis approach is reported to achieve unexplored quasi‐binary TMDC alloys through computationally predicted stability maps. Equilibrium temperature–composition phase diagrams using first‐principles calculations are generated to identify the stability of 25 quasi‐binary TMDC alloys, including some involving non‐isovalent cations and are verified experimentally through the synthesis of a subset of 12 predicted alloys using a scalable chemical vapor transport method. It is demonstrated that the synthesized alloys can be exfoliated into 2D structures, and some of them exhibit: i) outstanding thermal stability tested up to 1230 K, ii) exceptionally high electrochemical activity for the CO₂reduction reaction in a kinetically limited regime with near zero overpotential for CO formation, iii) excellent energy efficiency in a high rate Li–air battery, and iv) high break‐down current density for interconnect applications. This framework can be extended to accelerate the discovery of other TMDC alloys for various applications. 

Abstract Conversion of CO₂to energy‐rich chemicals using renewable energy is of much interest to close the anthropogenic carbon cycle. However, the current photoelectrochemical systems are still far from being practically feasible. Here the successful demonstration of a continuous, energy efficient, and scalable solar‐driven CO₂reduction process based on earth‐abundant molybdenum disulfide (MoS₂) catalyst, which works in synergy with an inexpensive hybrid electrolyte of choline chloride (a common food additive for livestock) and potassium hydroxide (KOH) is reported. The CO₂saturated hybrid electrolyte utilized in this study also acts as a buffer solution (pH ≈ 7.6) to adjust pH during the reactions. This study reveals that this system can efficiently convert CO₂to CO with solar‐to‐fuel and catalytic conversion efficiencies of 23% and 83%, respectively. Using density functional theory calculations, a new reaction mechanism in which the water molecules near the MoS₂cathode act as proton donors to facilitate the CO₂reduction process by MoS₂catalyst is proposed. This demonstration of a continuous, cost‐effective, and energy efficient solar driven CO₂conversion process is a key step toward the industrialization of this technology. 

Abstract The optimization of traditional electrocatalysts has reached a point where progress is impeded by fundamental physical factors including inherent scaling relations among thermokinetic characteristics of different elementary reaction steps, non‐Nernstian behavior, and electronic structure of the catalyst. This indicates that the currently utilized classes of electrocatalysts may not be adequate for future needs. This study reports on synthesis and characterization of a new class of materials based on 2D transition metal dichalcogenides including sulfides, selenides, and tellurides of group V and VI transition metals that exhibit excellent catalytic performance for both oxygen reduction and evolution reactions in an aprotic medium with Li salts. The reaction rates are much higher for these materials than previously reported catalysts for these reactions. The reasons for the high activity are found to be the metal edges with adiabatic electron transfer capability and a cocatalyst effect involving an ionic‐liquid electrolyte. These new materials are expected to have high activity for other core electrocatalytic reactions and open the way for advances in energy storage and catalysis.