Owing to high specific energy, low cost, and environmental friendliness, lithium–sulfur (Li–S) batteries hold great promise to meet the increasing demand for advanced energy storage beyond portable electronics, and to mitigate environmental problems. However, the application of Li–S batteries is challenged by several obstacles, including their short life and low sulfur utilization, which become more serious when sulfur loading is increased to the practically accepted level above 3–5 mg cm−2. More and more efforts have been made recently to overcome the barriers toward commercially viable Li–S batteries with a high sulfur loading. This review highlights the recent progress in high-sulfur-loading Li–S batteries enabled by hierarchical design principles at multiscale. Particularly, basic insights into the interfacial reactions, strategies for mesoscale assembly, unique architectures, and configurational innovation in the cathode, anode, and separator are under specific concerns. Hierarchy in the multiscale design is proposed to guide the future development of high-sulfur-loading Li–S batteries.

Review on High-Loading and High-Energy Lithium–Sulfur Batteries

As one important component of sulfur cathodes, the carbon host plays a key role in the electrochemical performance of lithium-sulfur (Li-S) batteries. In this paper, a mesoporous nitrogen-doped carbon (MPNC)-sulfur nanocomposite is reported as a novel cathode for advanced Li-S batteries. The nitrogen doping in the MPNC material can effectively promote chemical adsorption between sulfur atoms and oxygen functional groups on the carbon, as verifi ed by X-ray absorption near edge structure spectroscopy, and the mechanism by which nitrogen enables the behavior is further revealed by density functional theory calculations. Based on the advantages of the porous structure and nitrogen doping, the MPNC-sulfur cathodes show excellent cycling stability (95% retention within 100 cycles) at a high current density of 0.7 mAh cm −2 with a high sulfur loading (4.2 mg S cm −2 ) and a sulfur content (70 wt%). A high areal capacity (≈3.3 mAh cm −2 ) is demonstrated by using the novel cathode, which is crucial for the practical application of Li-S batteries. It is believed that the important role of nitrogen doping promoted chemical adsorption can be extended for development of other high performance carbon-sulfur composite cathodes for Li-S batteries.

Nitrogen-Doped Mesoporous Carbon Promoted Chemical Adsorption of Sulfur and Fabrication of High-Areal-Capacity Sulfur Cathode with Exceptional Cycling Stability for Lithium-Sulfur Batteries

High temperature (HT) polymer electrolyte membrane fuel cells (PEMFC) – A review

Intermediate polysulfides (Sn , where n = 2-8) play a critical role in both mechanistic understanding and performance improvement of lithium-sulfur batteries. The rational management of polysulfides is of profound significance for high-efficiency sulfur electrochemistry. Here, the key roles of polysulfides are discussed, with regard to their status, behavior, and their correspondingimpact on the lithium-sulfur system. Two schools of thoughts for polysulfide management are proposed, their advantages and disadvantages are compared, and future developments are discussed.

Revisiting the Role of Polysulfides in Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have arousing interest because of their high theoretical energy density. However, they often suffer from sluggish conversion of lithium polysulfides (LiPS) during the charge/discharge process. Single nickel (Ni) atoms on nitrogen-doped graphene (Ni@NG) with Ni-N4 structure are prepared and introduced to modify the separators of Li-S batteries. The oxidized Ni sites of the Ni-N4 structure act as polysulfide traps, efficiently accommodating polysulfide ion electrons by forming strong Sx 2- ⋅⋅⋅NiN bonding. Additionally, charge transfer between the LiPS and oxidized Ni sites endows the LiPS on Ni@NG with low free energy and decomposition energy barrier in an electrochemical process, accelerating the kinetic conversion of LiPS during the charge/discharge process. Furthermore, the large binding energy of LiPS on Ni@NG also shows its ability to immobilize the LiPS and further suppresses the undesirable shuttle effect. Therefore, a Li-S battery based on a Ni@NG modified separator exhibits excellent rate performance and stable cycling life with only 0.06% capacity decay per cycle. It affords fresh insights for developing single-atom catalysts to accelerate the kinetic conversion of LiPS for highly stable Li-S batteries.

Single Nickel Atoms on Nitrogen-Doped Graphene Enabling Enhanced Kinetics of Lithium-Sulfur Batteries.

Li-ion and Li-S batteries find enormous applications in different fields, such as electric vehicles and portable electronics. A separator is an indispensable part of the battery design, which functions as a physical barrier for the electrode as well as an electrolyte reservoir for ionic transport. The properties of the separators directly influence the performance of the batteries. Traditional polyolefin separators showed low thermal stability, poor wettability toward the electrolyte, and inadequate barrier properties to polysulfides. To improve the performance and durability of Li-ion and Li-S batteries, development of advanced separators is required. In this review, we summarize recent progress on the fabrication and application of novel separators, including the functionalized polyolefin separator, polymeric separator, and ceramic separator, for Li-ion and Li-S batteries. The characteristics, advantages, and limitations of these separators are discussed. A brief outlook for the future directions of the research in the separators is also provided.

Advanced Separators for Lithium-Ion and Lithium-Sulfur Batteries: A Review of Recent Progress.

Self-assembled Nafion®/metal oxide nanoparticles hybrid proton exchange membranes

Toward dendrite-free and anti-corrosion Zn anodes by regulating a bismuth-based energizer

With the disruptive carbon cycle being blamed for global warming, the plausible electrocatalytic CO2 reduction reaction (CO2RR) to form valuable C2+ hydrocarbons and feedstock is becoming a hot topic. Cu-based electrocatalysts have been proven to be excellent CO2RR alternatives for high energy value-added products in this regard. However, the selectivity of CO2RR to form C2+ products via Cu-based catalysts suffers from a high overpotential, slow reaction kinetics, and low selectivity. This review attempts to discuss various cutting-edge strategies for understanding catalytic design such as Cu-based catalyst surface engineering, tuning Cu bandgap via alloying, nanocatalysis, and the effect of the electrolyte and pH on catalyst morphology. The most recent advances in in situ spectroscopy and computational techniques are summarized to fully comprehend reaction mechanisms, structural transformation/degradation mechanisms, and crystal facet loss with subsequent effects on catalyst activity. Furthermore, approaches for tuning Cu interactions are discussed from four key perspectives: single-atom catalysts, interfacial engineering, metal-organic frameworks, and polymer-incorporated materials, which provide new insights into the selectivity of C2+ products. Finally, major challenges are outlined, and potential prospects for the rational design of catalysts for robust CO2RR are proposed. The integration of catalytic design with mechanistic understanding is a step forward in the promising advancement of CO2RR technology for industrial applications.

Electrochemical CO
 2 Reduction to C
 2+ Products Using Cu-Based Electrocatalysts: A Review

The electrochemical reduction of CO2 to produce carbon-based fuels and chemicals possesses huge potentials to alleviate current environmental problems. However, it is confronted by great challenges in the design of active electrocatalysts with low overpotentials and high product selectivity. Here we report the atomic tuning of a single-Fe-atom catalyst with phosphorus (Fe-N/P-C) on commercial carbon black as a robust electrocatalyst for CO2 reduction. The Fe-N/P-C catalyst exhibits impressive performance in the electrochemical reduction of CO2 to CO, with a high Faradaic efficiency of 98% and a high mass-normalized turnover frequency of 508.8 h-1 at a low overpotential of 0.34 V. On the basis of ex-situ X-ray absorption spectroscopy measurements and DFT calculations, we reveal that the tuning of P in single-Fe-atom catalysts reduces the oxidation state of the Fe center and decreases the free-energy barrier of *CO intermediate formation, consequently maintaining the electrocatalytic activity and stability of single-Fe-atom catalysts.

Ke Li

Papers

Advanced Separators for Lithium-Ion and Lithium-Sulfur Batteries: A Review of Recent Progress.

Self-assembled Nafion®/metal oxide nanoparticles hybrid proton exchange membranes

Toward dendrite-free and anti-corrosion Zn anodes by regulating a bismuth-based energizer

Electrochemical CO 2 Reduction to C 2+ Products Using Cu-Based Electrocatalysts: A Review

Atomic Tuning of Single-Atom Fe-N-C Catalysts with Phosphorus for Robust Electrochemical CO2 Reduction.