Tremendous efforts are being made to develop electrode materials, electrolytes, and separators for energy storage devices to meet the needs of emerging technologies such as electric vehicles, decarbonized electricity, and electrochemical energy storage. However, the sustainability concerns of lithium-ion batteries (LIBs) and next-generation rechargeable batteries have received little attention. Recycling plays an important role in the overall sustainability of future batteries and is affected by battery attributes including environmental hazards and the value of their constituent resources. Therefore, recycling should be considered when developing battery systems. Herein, we provide a systematic overview of rechargeable battery sustainability. With a particular focus on electric vehicles, we analyze the market competitiveness of batteries in terms of economy, environment, and policy. Considering the large volumes of batteries soon to be retired, we comprehensively evaluate battery utilization and recycling from the perspectives of economic feasibility, environmental impact, technology, and safety. Battery sustainability is discussed with respect to life-cycle assessment and analyzed from the perspectives of strategic resources and economic demand. Finally, we propose a 4H strategy for battery recycling with the aims of high efficiency, high economic return, high environmental benefit, and high safety. New challenges and future prospects for battery sustainability are also highlighted.

The authors' full names, academic degrees, and affiliations are listed in the Appendix. Address reprint requests to Dr. Kan at P.O. Box 249, 130 Dong-An Road, Shanghai 200032, China, or at kanh@ fudan . edu . cn.Drs. Liu and R. Chen and Drs. Gasparrini and Kan contributed equally to this article.

Ever-growing global energy needs and environmental damage have motivated the pursuit of sustainable energy sources and storage technologies. As attractive energy storage technologies to integrate renewable resources and electric transportation, rechargeable batteries, including lead-acid, nickel-metal hydride, nickel-cadmium, and lithium-ion batteries, are undergoing unprecedented rapid development. However, the intrinsic toxicity of rechargeable batteries arising from their use of toxic materials is potentially environmentally hazardous. Additionally, the massive production of batteries consumes numerous resources, some of which are scarce. It is therefore essential to consider battery recycling when developing battery systems. Here, we provide a systematic overview of rechargeable battery recycling from a sustainable perspective. We present state-of-the-art fundamental research and industrial technologies related to battery recycling, with a special focus on lithium-ion battery recycling. We introduce the concept of sustainability through a discussion of the life-cycle assessment of battery recycling. Considering the forecasted trend of a massive number of retired power batteries from the forecasted surge in electric vehicles, their repurposing and reuse are considered from economic, technical, environmental, and market perspectives. New opportunities, challenges, and future prospects for battery recycling are then summarized. A reinterpreted 3R strategy entailing redesign, reuse, and recycling is recommended for the future development of battery recycling.

This review systematically summarizes the limitations of solid electrolytes including inorganic solid electrolytes, solid polymer electrolytes, and composite solid electrolytes.

Novel sulfur/polythiophene composites with core/shell structure composites were synthesized via an in situ chemical oxidative polymerization method with chloroform as a solvent, thiophene as a reagent, and iron chloride as an oxidant at 0 °C. Different ratios of the sulfur/polythiophene composites were characterized by elemental analysis, FTIR, XRD, SEM, TEM, and electrochemical methods. A suitable ratio for the composites was found to be 71.9% sulfur and 18.1% polythiophene as determined by CV and EIS results. Conductive polythiophene acts as a conducting additive and a porous adsorbing agent. It was uniformly coated onto the surface of the sulfur powder to form a core/shell structure, which effectively enhances the electrochemical performance and cycle life of the sulfur cells. The initial discharge capacity of the active material was 1119.3 mA h g−1, sulfur and the remaining capacity was 830.2 mA h g−1 sulfur after 80 cycles. After a rate test from 100 to 1600 mA g−1 sulfur, the cell remained at 811 mA h g−1 sulfur after 60 cycles when the current density returned to 100 mA g−1 sulfur. The sulfur utilization, the cycle life, and the rate performance of the S−PTh core/shell electrode in a lithium−sulfur battery improved significantly compared to that of the pure sulfur electrode. The pore and thickness of the shell affected the battery performance of the lithium ion diffusion channels.

Owing to the high volumetric capacity and low redox potential, zinc (Zn) metal is considered to be a remarkably prospective anode for aqueous Zn‐ion batteries (AZIBs). However, dendrite growth severely destabilizes the electrode/electrolyte interface, and accelerates the generation of side reactions, which eventually degrade the electrochemical performance. Here, an artificial interface film of nitrogen (N)‐doped graphene oxide (NGO) is one‐step synthesized by a Langmuir–Blodgett method to achieve a parallel and ultrathin interface modification layer (≈120 nm) on Zn foil. The directional deposition of Zn crystal in the (002) planes is revealed because of the parallel graphene layer and beneficial zincophilic‐traits of the N‐doped groups. Meanwhile, through the in situ differential electrochemical mass spectrometry and in situ Raman tests, the directional plating morphology of metallic Zn at the interface effectively suppresses the hydrogen evolution reactions and passivation. Consequently, the pouch cells pairing this new anode with LiMn2O4 cathode maintain exceptional energy density (164 Wh kg−1 after 178 cycles) at a reasonable depth of discharge, 36%. This work provides an accessible synthesis method and in‐depth mechanistic analysis to accelerate the application of high‐specific‐energy AZIBs.

A multiwalled carbon nanotube/sulfur (MWCNT@S) composite with core-shell structure was successfully embedded into the interlay galleries of graphene sheets (GS) through a facile two-step assembly process. Scanning and transmission electron microscopy images reveal a 3D hierarchical sandwich-type architecture of the composite GS-MWCNT@S. The thickness of the S layer on the MWCNTs is ~20 nm. Raman spectroscopy, X-ray diffraction, thermogravimetric analysis, and energy-dispersive X-ray analysis confirm that the sulfur in the composite is highly crystalline with a mass loading up to 70% of the composite. This composite is evaluated as a cathode material for Li/S batteries. The GS-MWCNT@S composite exhibits a high initial capacity of 1396 mAh/g at a current density of 0.2C (1C = 1672 mA/g), corresponding to 83% usage of the sulfur active material. Much improved cycling stability and rate capability are achieved for the GS-MWCNT@S composite cathode compared with the composite lacking GS or MWCNT. The superior electrochemical performance of the GS-MWCNT@S composite is mainly attributed to the synergistic effects of GS and MWCNTs, which provide a 3D conductive network for electron transfer, open channels for ion diffusion, strong confinement of soluble polysulfides, and effective buffer for volume expansion of the S cathode during discharge.

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