Hollow Carbon Nanospheres with Developed Porous Structure and Retained N Doping for Facilitated Electrochemical Energy Storage.

Development of highly porous carbons with abundant surface functionalities and well-defined nanostructure is of significance for many important electrochemical energy storage systems. However, porous carbons suffer from a compromise between porosity, doped functionality, and nanostructure that have thus far restricted their performances. Here, we report the design of highly porous, nitrogen-enriched hollow carbon nanospheres (PN-HCNs) by an interfacial copolymerization strategy followed by NH3-assisted carbonization, and further demonstrate their significance and effectiveness in enhancing the electrochemical performances. The PN-HCN simultaneously delivers a large surface area (1237 m2 g-1) and high N functionalities (6.25 atom %) with a remarkable efficiency of the surface area increase to N loss ratio enabled by NH3 treatment while inheriting the hollow nanospherical structure. Accordingly, owing to the enhanced surface area and retained N doping, the prepared PN-HCN demonstrates outstanding electrochemical performances as a cathode host in lithium-sulfur batteries, including a near-to-theoretical capacity of 1620 mAh g-1, high rate capability and good cycling stability (789 mAh g-1 at 0.5C after 200 cycles). These results are superior to those of HCN without NH3 treatment. Also, PN-HCN exhibits superior capacitances (203 F g-1) and fast ion transport ability in supercapacitors. Our finding shows the simultaneous achievement of both highly porous structures and sufficient N functionalities for high-performance applications.

Unraveling the Correlation between Structures of Carbon Nanospheres Derived from Polymeric Spheres and Their Electrochemical Performance to Achieve High-Rate Supercapacitors.

Understanding correlation between the nanostructure of porous carbons and their ion transport behavior is critical for achieving high-performance supercapacitors. Herein, the relationship between size and shell thickness of carbon nanospheres (CNSs) and capacitive electrochemical performance is clarified. Structural uniform CNSs with controlled diameters, prepared via template-free interfacial copolymerization, are emerging as an ideal platform for investigating the ion transport behavior. It is found that ionic transport is significantly enhanced while the introduction of hollow cores with thinner shell, by virtue of the hollow nanopore-accelerated mass transport to reduce ion diffusion length. The proof-of-concept supercapacitors, constituted of carbons with diameter and shell thickness of 91 and 28 nm, respectively, can maintain highest capacitance retention ratio of 86% at a high sweep rate of 300 mVs-1 , also far outperforming the commercial activated carbon in terms of capacitance, rate capability, and surface efficiency, promising a brilliant application.

Revisiting the Roles of Natural Graphite in Ongoing Lithium-Ion Batteries.

Graphite, commonly including artificial graphite and natural graphite (NG), possesses a relatively high theoretical capacity of 372 mA h g-1 and appropriate lithiation/de-lithiation potential, and has been extensively used as the anode of lithium-ion batteries (LIBs). With the requirements of reducing CO2 emission to achieve carbon neutral, the market share of NG anode will continue to grow due to its excellent processability and low production energy consumption. NG, which is abundant in China, can be divided into flake graphite (FG) and microcrystalline graphite (MG). In the past 30 years, many researchers have focused on developing modified NG and its derivatives with superior electrochemical performance, promoting their wide applications in LIBs. Here, a comprehensive overview of the origin, roles, and research progress of NG-based materials in ongoing LIBs is provided, including their structure, properties, electrochemical performance, modification methods, derivatives, composites, and applications, especially the strategies to improve their high-rate and low-temperature charging performance. Prospects regarding the development orientation as well as future applications of NG-based materials are also considered, which will provide significant guidance for the current and future research of high-energy-density LIBs.

Atomic Sn-enabled high-utilization, large-capacity, and long-life Na anode.

Constructing robust nucleation sites with an ultrafine size in a confined environment is essential toward simultaneously achieving superior utilization, high capacity, and long-term durability in Na metal-based energy storage, yet remains largely unexplored. Here, we report a previously unexplored design of spatially confined atomic Sn in hollow carbon spheres for homogeneous nucleation and dendrite-free growth. The designed architecture maximizes Sn utilization, prevents agglomeration, mitigates volume variation, and allows complete alloying-dealloying with high-affinity Sn as persistent nucleation sites, contrary to conventional spatially exposed large-size ones without dealloying. Thus, conformal deposition is achieved, rendering an exceptional capacity of 16 mAh cm-2 in half-cells and long cycling over 7000 hours in symmetric cells. Moreover, the well-known paradox is surmounted, delivering record-high Na utilization (e.g., 85%) and large capacity (e.g., 8 mAh cm-2) while maintaining extraordinary durability over 5000 hours, representing an important breakthrough for stabilizing Na anode.

A self-crosslinking procedure to construct yolk-shell Au@microporous carbon nanospheres for lithium-sulfur batteries.

An efficient self-crosslinking procedure to reasonably construct porous shells is reported for the synthesis of yolk-shell Au@microporous carbon nanospheres.