Multi-functional yolk-shell structured materials and their applications for high-performance lithium ion battery and lithium sulfur battery

Due to its high theoretical capacity, silicon is the most promising anode candidate for future lithium-ion batteries with high energy density and large power. Yet the low conductivity and poor structural stability resulting from huge volume expansion after full lithiation are still the critical issues impacting practical applications of silicon anodes. This review unveils how structural designs address these challenges and outlines the structural evolution of silicon anodes. Up to now, six generations of structural designs have been proposed for silicon anodes, encompassing solid nanostructures, porous structures, core-shell structures, yolk-shell structures, high-tap-density packed yolk-shell structures, and carbon-nanotube-improved yolk-shell structures. The evolution of structural improvement principles deployed for silicon anodes can provide valuable guidance for the rational structural design of other electrode materials that undergo large volume changes. In this review, Zhang et al. summarized the typical structural evolution of six silicon-based anode materials. Furthermore, the current limitations of fabrication methods and some promising future directions for the structural design of silicon anodes are also discussed. 

The typical structural evolution of silicon anode

Due to the increasingly serious energy consumption and demand worldwide, the development of advanced, flexible, and versatile advanced batteries and related materials has become an important research topic in the modern world. Copper-based metal–organic frameworks (Cu-MOFs) have large specific surface areas, high porosities, adjustable structures, simple preparation methods, and low cost. In recent years, the research on the chemical composition, structure, preparation methods, and application of Cu-MOFs and their derivatives has undergone continuous changes and growth, resulting in excellent candidate materials for electrochemical energy storage. Herein, this article reviews the application status and development of Cu-MOFs and their derivative materials in various rechargeable batteries, including lithium-ion batteries, sodium-ion batteries, lithium–sulfur batteries, and other rechargeable batteries. First, we have summarized and compared the synthesis methods of Cu-MOFs, then the research progress in the synthesis strategy, structure, and electrochemical performance of Cu-MOFs and their derivative materials is emphasized. Finally, a comprehensive summary of the research results of the applications of Cu-MOFs and their derivatives in the field of advanced batteries is given in order to provide various ideas and suggestions for their further development. 

Recent Advances in Cu-Based Metal–Organic Frameworks and Their Derivatives for Battery Applications

Transition metal selenides are considered as hopeful anode materials for sodium-ion battery (SIB) due to the high specific capacity and rich reserves in nature. However, the inherent low conductivity of these anode materials, as well as the inevitable volume expansion and structural collapse during cycling, result in their poor rate performance and cycling stability. Herein, a universal selenization-co-carbonization strategy is proposed to synthesize Cu2-xSe nanoparticles in-situ confined in highly defective nitrogen-doped carbon (Cu2-xSe@NC) with superior architectural features, which involves simultaneous selenization and carbonization procedure of octahedral metal–organic framework (Cu-BTC) precursor. The nitrogen-doped carbon matrix stabilizes/confines the Cu2-xSe nanoparticles to prevent their agglomeration and volume expansion during cycling while endowing high electrical conductivity to the hybrid materials. As anode for SIBs, the Cu2-xSe@NC exhibits a high reversible capacity of 340 mAh/g at 0.1 A/g with a high initial coulombic efficiency of 70 %, superior rate performance (capacity retention of 82.4 % from 0.02 to 5 A/g), and long-cycle durability. The ex-situ XRD and HRTEM techniques confirmed that Cu2-xSe undergoes complex intercalation and crystal evolution accompanied by reversible intermediate phases (NaCuSe and Na2Se) transformation during charge/discharge cycle. First-principles calculations and in-situ EIS confirmed that the intercalation of Na+ can greatly reducing the energy band gap and improving the electrical conductivity of Cu2-xSe@NC, thereby achieving excellent rate performance. Moreover, the Cu2-xSe@NC anode is also evaluated by matching with Na3V2(PO4)3 cathode to assemble a full SIB, which can provide high initial capacity and capacity retention, revealing its potential for practical application. 

In situ confined growth of Cu2-xSe nanoparticles in highly defective nitrogen-doped carbon for high-rate sodium-ion battery anodes

Nitrogen and phosphorus Co-doped non stoichiometric cobalt selenides (Co0.85Se) ultrathin nanosheets as highly efficient electrocatalysts for the hydrogen evolution reaction

Constructing nanostructures with multi-components and delicate architecture exhibits huge potential to improve the lithium storage performance of electrodes. Herein, we report a novel yolk-double-shell structure with complex chemical compositions. Starting with a core-shell structured Co-ZIF@ZnCo-ZIF as a precursor via a simple selenization process, yolk-double-shell polyhedra that assembled by nanosized Co0.85Se@N-doped carbon as the yolk and the first shell and nanosized Co0.85Se@N-doped carbon and ZnSe@N-doped carbon hetero-components as the second shell (marked as Co0.85Se@NC/ZnSe@NC-YDS) are synthesized. Benefiting from their multiple structural advantages, such as high surface area, large pore volume, uniform carbon coating, and intimate heterostructures, Co0.85Se@NC/ZnSe@NC-YDS exhibits high reversible capacity (1047 mA h g-1) and good rate capability for lithium storage. More importantly, even after 3000 cycles at 5.0 A g-1, an impressive reversible capacity of 468 mA h g-1 is retained with no capacity decay. After repeated discharge/charge processes, the integrated yolk-double-shell structure is still reserved, due to its structural and compositional advantages, which contribute to the enhanced rate and cycling performance.

A hierarchical structure of a Co0.85Se@NC/ZnSe@NC yolk-double-shell polyhedron for long-term lithium storage.

Controlling the microstructure and composition of electrodes is crucial to enhance their rate capability and cycling stability for lithium storage. Inspired by the highly interconnected network and good mechanical integrity of an ant-nest architecture, herein, a biomimetic strategy is proposed to enhance the electrochemical performance of Cu2-xSe. After facile carbonization and selenization treatments, the 3D Cu-MOF is successfully transformed into the final ant-nest-like Cu2-xSe@C (AN-Cu2-xSe@C). The AN-Cu2-xSe@C is composed of interconnected Cu2-xSe channels with amorphous carbon coated on the outer surface. The 3D interconnected channels within the AN-Cu2-xSe@C provide fast charge transport pathways and enhanced structural integrity to tolerate the large volume fluctuations of Cu2-xSe during cycling. When applied as the anode for lithium storage, the AN-Cu2-xSe@C shows remarkable electrochemical performance with a high capacity of 1452 mA h g-1 after 1200 cycles at 1.0 A g-1 and 879 mA h g-1 after 2500 cycles at 10.0 A g-1, respectively. Mechanism investigations demonstrate that the AN-Cu2-xSe@C experiences complicated conversion-intercalation co-existence reactions upon cycling. The existence of capacitive behaviour (74%) also contributes to the extended cycling performance. Our work offers a new avenue for designing a high performance electrode using the biomimetic concept.

Ant-nest-like Cu2-xSe@C with biomimetic channels boosts the cycling performance for lithium storage.

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A hierarchical structure of a Co0.85Se@NC/ZnSe@NC yolk-double-shell polyhedron for long-term lithium storage.

Ant-nest-like Cu2-xSe@C with biomimetic channels boosts the cycling performance for lithium storage.