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Electrolyte engineering is considered as an effective strategy to establish stable solid electrolyte interface (SEI), and thus to suppress the growth of lithium dendrites. In a recent study reported in Advanced Functional Materials by Ma group, discovered that strong coordination force could be founded between 15-Crown-5 ether (15-C-5) and Li+, which facilitates the crown ether (15-C-1) to participate in the solvation structure of Li+ in the electrolyte for the same purpose. Such a novel strategy might impact the design of high-performance and safe lithium metal batteries (LMBs). [ABSTRACT FROM AUTHOR]

Electrolyte engineering is considered as an effective strategy to establish stable solid electrolyte interface (SEI), and thus to suppress the growth of lithium dendrites. In a recent study reported in Advanced Functional Materials by Ma group, discovered that strong coordination force could be founded between 15-Crown-5 ether (15-C-5) and Li+, which facilitates the crown ether (15-C-1) to participate in the solvation structure of Li+ in the electrolyte for the same purpose. Such a novel strategy might impact the design of high-performance and safe lithium metal batteries (LMBs). [ABSTRACT FROM AUTHOR]

Highlights: The state-of-the-art development in electrochemical H2O2 production via the two-electron oxygen reduction reaction is reviewed with emphasis on material science, reaction mechanisms, and fundamental factors that govern the reaction route. General principles and strategies for catalyst design are summarized to understand the inherent relationships between the catalyst properties and electrocatalytic performances. Perspectives and challenges are presented to get insights into the large-scale manufacturing of H2O2 via the electrochemical routes. An environmentally benign, sustainable, and cost-effective supply of H2O2 as a rapidly expanding consumption raw material is highly desired for chemical industries, medical treatment, and household disinfection. The electrocatalytic production route via electrochemical oxygen reduction reaction (ORR) offers a sustainable avenue for the on-site production of H2O2 from O2 and H2O. The most crucial and innovative part of such technology lies in the availability of suitable electrocatalysts that promote two-electron (2e–) ORR. In recent years, tremendous progress has been achieved in designing efficient, robust, and cost-effective catalyst materials, including noble metals and their alloys, metal-free carbon-based materials, single-atom catalysts, and molecular catalysts. Meanwhile, innovative cell designs have significantly advanced electrochemical applications at the industrial level. This review summarizes fundamental basics and recent advances in H2O2 production via 2e–-ORR, including catalyst design, mechanistic explorations, theoretical computations, experimental evaluations, and electrochemical cell designs. Perspectives on addressing remaining challenges are also presented with an emphasis on the large-scale synthesis of H2O2 via the electrochemical route. [ABSTRACT FROM AUTHOR]

Highlights: Cyclohexanedodecol (CHD) could facilitate the Zn dendrite-free plating/stripping at a nanoscale. The CHD molecules could effectively modify the hydrated Zn(H2O)62+ structure in aqueous Zn ion batteries. The addition of CHD could establish robust protection layers on the Zn electrode surface. The CHD-modified electrolytes exhibit long-term cycling stability. Aqueous zinc-ion batteries (AZIBs) can be one of the most promising electrochemical energy storage devices for being non-flammable, low-cost, and sustainable. However, the challenges of AZIBs, including dendrite growth, hydrogen evolution, corrosion, and passivation of zinc anode during charging and discharging processes, must be overcome to achieve high cycling performance and stability in practical applications. In this work, we utilize a dual-functional organic additive cyclohexanedodecol (CHD) to firstly establish [Zn(H2O)5(CHD)]2+ complex ion in an aqueous Zn electrolyte and secondly build a robust protection layer on the Zn surface to overcome these dilemmas. Systematic experiments and theoretical calculations are carried out to interpret the working mechanism of CHD. At a very low concentration of 0.1 mg mL−1 CHD, long-term reversible Zn plating/stripping could be achieved up to 2200 h at 2 mA cm−2, 1000 h at 5 mA cm−2, and 650 h at 10 mA cm−2 at the fixed capacity of 1 mAh cm−2. When matched with V2O5 cathode, the resultant AZIBs full cell with the CHD-modified electrolyte presents a high capacity of 175 mAh g−1 with the capacity retention of 92% after 2000 cycles under 2 A g−1. Such a performance could enable the commercialization of AZIBs for applications in grid energy storage and industrial energy storage. [ABSTRACT FROM AUTHOR]

Highlights: Interface engineering of heterogeneous CoS/CoO nanocrystals and N-doped graphene composite facilitates high-performance oxygen reduction reaction and oxygen evolution reaction. Density functional theory calculations and experimental results confirm the enhanced electrocatalytic performances via the proposed interface engineering. The bifunctional oxygen electrocatalyst exhibits excellent performances in rechargeable Zn–air batteries. Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are crucial for the large-scale application of rechargeable Zn–air batteries (ZABs). In this work, our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution, improve the electronic conductivity and enhance the catalyst stability. In order to realize such a structure, we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst (CoS/CoO@NGNs). The optimization of the composition, interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER. The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm−2, a specific capacity of 723.9 mAh g−1 and excellent cycling stability (continuous operating for 100 h) with a high round-trip efficiency. In addition, the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances, showing great potential for applications in flexible and wearable electronic devices. [ABSTRACT FROM AUTHOR]

In the original publication, the label text. [ABSTRACT FROM AUTHOR]

Highlights: Interface engineering of heterogeneous CoS/CoO nanocrystals and N-doped graphene composite facilitates high-performance oxygen reduction reaction and oxygen evolution reaction. Density functional theory calculations and experimental results confirm the enhanced electrocatalytic performances via the proposed interface engineering. The bifunctional oxygen electrocatalyst exhibits excellent performances in rechargeable Zn–air batteries. Low cost and green fabrication of high-performance electrocatalysts with earth-abundant resources for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) are crucial for the large-scale application of rechargeable Zn–air batteries (ZABs). In this work, our density functional theory calculations on the electrocatalyst suggest that the rational construction of interfacial structure can induce local charge redistribution, improve the electronic conductivity and enhance the catalyst stability. In order to realize such a structure, we spatially immobilize heterogeneous CoS/CoO nanocrystals onto N-doped graphene to synthesize a bifunctional electrocatalyst (CoS/CoO@NGNs). The optimization of the composition, interfacial structure and conductivity of the electrocatalyst is conducted to achieve bifunctional catalytic activity and deliver outstanding efficiency and stability for both ORR and OER. The aqueous ZAB with the as-prepared CoS/CoO@NGNs cathode displays a high maximum power density of 137.8 mW cm−2, a specific capacity of 723.9 mAh g−1 and excellent cycling stability (continuous operating for 100 h) with a high round-trip efficiency. In addition, the assembled quasi-solid-state ZAB also exhibits outstanding mechanical flexibility besides high battery performances, showing great potential for applications in flexible and wearable electronic devices. [ABSTRACT FROM AUTHOR]

Highlights: Comprehensive summary of crystalline structures and morphologies of carbon nitride-based materials (CNBMs). Density functional theory computation for the design of functional CNBMs for rechargeable battery applications. The experimental synthesis strategies of CNBMs for rechargeable battery application. Carbon nitrides (including CN, C2N, C3N, C3N4, C4N, and C5N) are a unique family of nitrogen-rich carbon materials with multiple beneficial properties in crystalline structures, morphologies, and electronic configurations. In this review, we provide a comprehensive review on these materials properties, theoretical advantages, the synthesis and modification strategies of different carbon nitride-based materials (CNBMs) and their application in existing and emerging rechargeable battery systems, such as lithium-ion batteries, sodium and potassium-ion batteries, lithium sulfur batteries, lithium oxygen batteries, lithium metal batteries, zinc-ion batteries, and solid-state batteries. The central theme of this review is to apply the theoretical and computational design to guide the experimental synthesis of CNBMs for energy storage, i.e., facilitate the application of first-principle studies and density functional theory for electrode material design, synthesis, and characterization of different CNBMs for the aforementioned rechargeable batteries. At last, we conclude with the challenges, and prospects of CNBMs, and propose future perspectives and strategies for further advancement of CNBMs for rechargeable batteries. [ABSTRACT FROM AUTHOR]