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As the most promising anodic candidate for alkali ion batteries, red phosphorus (P) still faces big challenges, such as the poor rate and cycling performance, which are caused by the insulative nature and the large volume change throughout the alloy/dealloy process. To ameliorate above issues, the traditional way is confining P into the carbon host. However, investigations on maximizing P utilization are inadequate; in other words, how to achieve entire confinement with a high loading amount is still a problem. Additionally, the application of P in potassium-ion batteries (PIBs) is in its infant stage, and the corresponding potassiation product is controversial. Herein, a nitrogen-doped stripped-graphene CNT (N-SGCNT) as carbon framework is prepared to exclusively confine ultrafine P to construct P@N-SGCNT composites. Benefitting from the in situ cross-linked structure, N-SGCNT loaded with 41.2 wt % P (P2@N-SGCNT) shows outstanding Na+/K+ storage performance. For instance, P2@N-SGCNT exhibits high reversible capacities of 2480 mAh g-1 for sodium-ion batteries (SIBs) and 762 mAh g-1 for PIBs, excellent rate capabilities of 1770 mAh g-1 for SIBs and 354 mAh g-1 for PIBs at 2.0 A g-1, and long cycling stability (a capacity of 1936 mAh g-1 after 2000 cycles for SIBs and 319 mAh g-1 after 1000 cycles for PIBs). Furthermore, due to this exclusively confined P structure, the K+ storage mechanism with the end product of K4P3 has been identified by experimental and theoretical results.

Magnesium-based hydrides are promising hydrogen storage materials; however, little progress has been achieved in improving hydrogen storage performance under ambient conditions, consequently impeding further commercial application. Herein, a lithium rich transition metal oxide, Li3VO4 has been employed to catalyze the hydrogen storage reaction of magnesium-based hydrides, enabling a fast and full hydrogenation of Mg at lower temperatures. The structural stability of Li3VO4 upon de/rehydrogenation reactions has been confirmed by neutron diffraction and transmission electron microscope observations. The synergistic catalytic role of Li3VO4 has elucidated that the existence of Li stimulates the catalytic activity of V and simultaneously suppresses the activity of O. V is the key catalytically active site, while O can react with active Mg to generate MgO which is a passivation layer and could prevent the diffusion of H. These findings will give an opportunity for the use of other lithium rich transition metal oxides in the field of catalyzing hydrogen storage systems.

The hexagonal sheet shaped Fe3O4/Fe7S8 heterojunction with lateral size of 1.5 μm has been controllably synthesized by gas sulfuration process. The most fascinating performance of this Fe3O4/Fe7S8 heterojunction structure is that the capacity attenuation is rather small of only 18%, from 818 mAh·g−1 to 670 mAh·g−1, when the current density increases ten-fold from 0.2 A·g−1 to 2.0 A·g−1. This high capacity retention upon current density shifting, is attributed to pseudocapacitance contribution, which is related to the two-dimensional hexagonal structure, faster electron/ion transfer and synergistic effect for the stepwise lithiation of Fe3O4 and Fe7S8 at different voltage in Fe3O4/Fe7S8 heterojunction. This rational design on heterojunction structure sheds light on further constructing novel anode material for secondary ion batteries.

Developing cheap and efficient transition metal-based catalysts for the oxygen evolution reaction (OER) plays the key role in large-scale implementation of hydrogen production. However, there is still a lack of effective ways to tune the catalysts performance for the OER reaction from the aspect of structure design and element modulation simultaneously. Herein, a novel Cu0.33Co0.67S2 hexagonal nanosheet has been synthesized through the coprecipitation reaction followed by subsequent vapor sulfidation. Simply mixed with carbon nanotubes (CNTs) during electrode preparation, this Cu0.33Co0.67S2 exhibits an overpotential of 284 mV vs. RHE at a current density of 10 mA cm−2 in 1.0 M KOH. The improved OER performance of the Cu0.33Co0.67S2 electrode can be attributed to the electrocatalytically active sites involved in octahedral coordination structures and further activated by Cu substitution. The encouraging results provide insight into further rational design of transition metal-based electrochemical catalysts towards OER applications.

Developing sodium ion battery (SIB) anode materials of a low-cost and high-capacity nature for future large-scale applications still involves challenges. Herein, we have reported gallium sulfide (Ga2S3) as a novel SIB anode material for the first time. Ga2S3 nanorods have been synthesized via the facile hydrothermal preparation of a GaOOH precursor with subsequent H2S annealing. Mixed with graphene upon electrode preparation, this Ga2S3 electrode maintains a reversible specific capacity of 476 mA h g−1 after 100 cycles at a current density of 0.4 A g−1, with a coulombic efficiency of over 99%. Ex situ XRD analysis and theoretical calculations are employed to comprehensively elucidate the detailed sodium ion storage mechanism of Ga2S3, which is composed of initial Na+ intercalation, a subsequent multi-step conversion reaction between S and Na+, and an eventual alloying reaction between Ga and Na+ with the end product of Na7Ga13. Further kinetics analysis has demonstrated that the conversion reaction is the rate-limiting step due to a multi-step reaction with the intermediate phase of GaS. Moreover, the appearance of liquid metal Ga, as confirmed via TEM observations and theoretical calculations, can serve as a self-healing agent that repairs cracks in the electrode. Our findings shed light on the further design of Ga-based materials, and they also can be extended to solid-state-battery systems.

Developing sodium ion battery (SIB) anode materials of a low-cost and high-capacity nature for future large-scale applications still involves challenges. Herein, we have reported gallium sulfide (Ga2S3) as a novel SIB anode material for the first time. Ga2S3 nanorods have been synthesized via the facile hydrothermal preparation of a GaOOH precursor with subsequent H2S annealing. Mixed with graphene upon electrode preparation, this Ga2S3 electrode maintains a reversible specific capacity of 476 mA h g-1 after 100 cycles at a current density of 0.4 A g-1, with a coulombic efficiency of over 99%. Ex situ XRD analysis and theoretical calculations are employed to comprehensively elucidate the detailed sodium ion storage mechanism of Ga2S3, which is composed of initial Na+ intercalation, a subsequent multi-step conversion reaction between S and Na+, and an eventual alloying reaction between Ga and Na+ with the end product of Na7Ga13. Further kinetics analysis has demonstrated that the conversion reaction is the rate-limiting step due to a multi-step reaction with the intermediate phase of GaS. Moreover, the appearance of liquid metal Ga, as confirmed via TEM observations and theoretical calculations, can serve as a self-healing agent that repairs cracks in the electrode. Our findings shed light on the further design of Ga-based materials, and they also can be extended to solid-state-battery systems.

A three-dimensional porous copper film is directly deposited on Cu foam by an electrodeposition method using hydrogen bubbles as dynamic template (denoted as Cu/Cu foam). Its electrocatalytic activity toward hydrazine electrooxidation is tested by linear sweep voltammetry, chronoamperometry and electrochemical impedance spectroscopy. Compared with Cu foam, hydrazine electrooxidation on the Cu/Cu foam electrode shows that the onset oxidation potential displays a ~100 mV negative shift, the current density at −0.6 V raises about 14 times, the apparent activation energy and the charge transfer resistance reduce significantly. The increasing electrocatalytic performance for hydrazine electrooxidation is mainly caused by the highly porous structure of the Cu/Cu foam electrode which can provide a large surface area and make electrolyte access the electrocatalyst surfaces more easily. Hydrazine electrooxidation on the Cu/Cu foam electrode proceeds through a near 4-electron process.

Germanium-based materials possess high theoretical capacity of approximately 1000 mAh·g−1, nevertheless, the practical electrochemical performance is severely hampered by poor cyclability due to volumetric expansion of Ge upon cycling. Herein, novel hydrangea-like CoGeO2(OH)2 constructed by 2D nanoplates has been facilely synthesized with the assistance of ethylene glycol and further applied to anode materials for lithium ion storage. The hydrangea-like CoGeO2(OH)2 anode exhibits an enhanced specific capacity of 1174 mAh·g−1 at a current density of 0.5 A g−1 after 100 cycles. Such outstanding electrochemical performance could be accredited to the rationally designed hydrangea-like structure, which can relieve the interval stress aroused by lithiation/de-lithiation, shorten the pathway of electron/ion transportation and take advantage of the pseudocapacitive nature of two dimensional nanosheets that could improve the reaction kinetics and endow the material with remarkable rate capability. Moreover, the inherent Co-bonded hydroxyl groups facilitate the pseudocapacitive effect, and Ge-based component contributes to the capacity. These advantages help CoGeO2(OH)2 hydrangeas gain a competitive edge over other candidates of anode materials for lithium-ion batteries.