Ambient electrochemical N2 reduction is emerging as a highly promising alternative to the Haber–Bosch process but is typically hampered by a high reaction barrier and competing hydrogen evolution, leading to an extremely low Faradaic efficiency. Here, we demonstrate that under ambient conditions, a single-atom catalyst, iron on nitrogen-doped carbon, could positively shift the ammonia synthesis process to an onset potential of 0.193 V, enabling a dramatically enhanced Faradaic efficiency of 56.55%. The only doublet coupling representing 15NH4+ in an isotopic labeling experiment confirms reliable NH3 production data. Molecular dynamics simulations suggest efficient N2 access to the single-atom iron with only a small energy barrier, which benefits preferential N2 adsorption instead of H adsorption via a strong exothermic process, as further confirmed by first-principle calculations. The released energy helps promote the following process and the reaction bottleneck, which is widely considered to be the first hydrogenation step, is successfully overcome.

A new type of amino polar binder with 3D network flexibility structure for high energy Li-S batteries is synthesized and successfully used with commercial sulfur powder cathodes. The binder shows significant performance improvement in capacity retention and high potential for practical application, which arouse the battery community's interest in the commercial application of high energy Li-S battery.

Lithium metal, the ideal anode material for rechargeable batteries, suffers from the inherent limitations of sensitivity to the humid atmosphere and dendrite growth. Herein, low-cost fabrication of a metallic-lithium anode that is stable in air and plated dendrite-free from an organic-liquid electrolyte solves four key problems that have plagued the development of large-scale Li-ion batteries for storage of electric power. Replacing the low-capacity carbon anode with a safe, dendrite-free lithium anode provides a fast charge while reducing the cost of fabrication of a lithium battery, and increasing the cycle life of a rechargeable cell by eliminating the liquid-electrolyte ethylene-carbonate additive used to form a solid-electrolyte interphase passivation layer on the anode that is unstable during cycling. This solution is accomplished by formation of a hydrophobic solid-electrolyte interphase on a metallic-lithium anode that allows for handling of the treated lithium anode membrane in a standard dry room during cell fabrication.

For the first time a new strategy is reported to improve the volumetric capacity and Coulombic efficiency by selenium doping for lithium-organosulfur batteries. Selenium-doped cathodes with four sulfur atoms and one selenium atom (as the doped heteroatom) in the confined structure are designed and synthesized; this structure exhibits greatly improved volumetric/areal capacities, and a Coulombic efficiency of almost 100% for highly stable lithium-organosulfur batteries. The doping of Se significantly enhances the electronic conductivity of battery electrodes by a factor of 6.2 compared to pure sulfur electrodes, and completely restricts the production of long-chain lithium polysulfides. This allows achievement of a high gravimetric capacity of 700 mAh g close to its theoretical mass capacity, an exceptional volumetric capacity of 2457 mAh cm , and excellent capacity retention of 92% after 400 cycles. Shuttle effect is efficiently weakened since no long-chain polysulfides are detected from in situ UV/vis results throughout the entire cycling process arising from selenium doping, which is theoretically confirmed by density functional theory calculations.

Generally, self-healing research based on commercial rubber is of great significance in sustainable development by extending the lifetime of materials. However, it is still a great challenge so far to prepare recyclable rubber that combine excellent self-healing properties with good mechanical strength and is also recyclable. Herein, we report the use of epoxidized natural rubber (ENR), a reactive polymer presenting dual functional groups (unsaturated double bonds and epoxy sites) available for cross-linking, to prepare a dual cross-linked self-healing ENR based on dynamic disulfide metathesis and thermoreversible hydrogen bonding. Specifically, different structures of aromatic disulfide compounds are introduced into the same system to promote the disulfide metathesis and thus improving the self-healing efficiency of the material. As a result, the dual cross-linked ENR shows high mechanical strength (9.3 ± 0.3 MPa), high self-healing efficiency (up to 98%), and ideal recyclability. In addition, cyclic fatigue tensile test shows that the self-healing properties of the present material are not affected by the damage forms, whether it is complete fracture or cyclic fatigue damage. These outcomes are expected to promote the development of self-healing technology in the sustainable application of cross-linked rubber materials.

Lithium-metal batteries (LMB) are very attractive owing to their high theoretical energy density, but significant challenges such as low ionic conductivity and safety risks prevent their widespread application. Herein, we report a new design of high-safety all-solid-state LMB by using highionic-conductivity thermoresponsive solid-polymer electrolyte (TSPE), providing a smart and active approach to realize thermally induced autonomic shutdown of LMBs by efficiently inhibiting the ionic conduction between electrodes beyond an unsafe temperature. The as-obtained TSPE exhibits a high ionic conductivity (2 × 10 −4 S cm −1 at 30 °C), which enables a significantly improved capacity of 160 mA h g −1 at 0.2 C and outstanding high rate capability up to 5 C as well as a super-long cycle life of over 400 cycles for the constructed all-solid-state Li||LiFePO 4 batteries. The present study opens up a new avenue for the fabrication of self-protective all-solid-state batteries with inherent intelligent thermal management to ensure batteryseries safety.

Efficient bifunctional electrocatalysts with desirable oxygen activities are closely related to practical applications of renewable energy systems including metal-air batteries, fuel cells, and water splitting. Here a composite material derived from a combination of bimetallic zeolitic imidazolate frameworks (denoted as BMZIFs) and Fe/N/C framework was reported as an efficient bifunctional catalyst. Although BMZIF or Fe/N/C alone exhibits undesirable oxygen reaction activity, a combination of these materials shows unprecedented ORR (half-wave potential of 0.85 V as well as comparatively superior OER activities (potential@10 mA cm of 1.64 V), outperforming not only a commercial Pt/C electrocatalyst but also most reported bifunctional electrocatalysts. We then tested its practical application in Zn-air batteries. The primary batteries exhibit a high peak power density of 235 mW cm, and the batteries are able to be operated smoothly for 100 cycles at a curent density of 10 mA cm. The unprecedented catalytic activity can be attritued to chemical coupling effects between Fe/N/C and BMZIF and will aid the development of highly active electrocatalysts and applications for electrochemical energy devices.

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