With the ever-increasing adaption of large-scale energy storage systems and electric devices, the energy storage capability of batteries and supercapacitors has faced increased demand and challenges. The electrodes of these devices have experienced radical change with the introduction of nano-scale materials. As new generation materials, heterostructure materials have attracted increasing attention due to their unique interfaces, robust architectures, and synergistic effects, and thus, the ability to enhance the energy/power outputs as well as the lifespan of batteries. In this review, the recent progress in heterostructure from energy storage fields is summarized. Specifically, the fundamental natures of heterostructures, including charge redistribution, built-in electric field, and associated energy storage mechanisms, are summarized and discussed in detail. Furthermore, various synthesis routes for heterostructures in energy storage fields are roundly reviewed, and their advantages and drawbacks are analyzed. The superiorities and current achievements of heterostructure materials in lithium-ion batteries (LIBs), sodium-ion batteries (SIBs), lithium-sulfur batteries (Li-S batteries), supercapacitors, and other energy storage devices are discussed. Finally, the authors conclude with the current challenges and perspectives of the heterostructure materials for the fields of energy storage.

Emerging of Heterostructure Materials in Energy Storage: A Review.

Engineering novel electrode materials with unique architectures has a significant impact on tuning the structural/electrochemical properties for boosting the performance of secondary battery systems. Herein, starting from well-organized WS2 nanorods, an ingenious design of a one-step method is proposed to prepare a bimetallic sulfide composite with a coaxial carbon coating layer, simply enabled by ZIF-8 introduction. Rich sulfur vacancies and WS2 /ZnS heterojunctions can be simultaneously developed, that significantly improve ionic and electronic diffusion kinetics. In addition, a homogeneous carbon protective layer around the surface of the composite guarantees an outstanding structural stability, a reversible capacity of 170.8 mAh g-1 after 5000 cycles at a high rate of 5 A g-1 . A great potential in practical application is also exhibited, where a full cell based on the WS2- x /ZnS@C anode and the P2-Na2/3 Ni1/3 Mn1/3 O2 cathode can maintain a reversible capacity of 89.4 mAh g-1 after 500 cycles at 1 A g-1 . Moreover, the underlying electrochemical Na storage mechanisms are illustrated in detail by theoretical calculations, electrochemical kinetic analysis, and operando X-ray diffraction characterization.

Co-Construction of Sulfur Vacancies and Heterojunctions in Tungsten Disulfide to Induce Fast Electronic/Ionic Diffusion Kinetics for Sodium-Ion Batteries

Challenges and future perspectives on sodium and potassium ion batteries for grid-scale energy storage

Heterostructure construction is an efficient method for reinforcing K+ storage of transition metal selenides. The spontaneously developed internal electric fields give a strong boost to charge transport and significantly reduce the activation energy. Nevertheless, perfection of the interfacial region based on the energy level gradient and lattice matching degree is still a great challenge. Herein, rich vacancies and ultrafine CoSe2 -FeSe2 heterojunctions with semicoherent phase boundary are simultaneously obtained, which possess unique electronic structures and abundant active sites. When employed as anodes for potassium-ion batteries (PIBs), CoSe2 -FeSe2 @C composites display a reversible potassium storage of 401.1 mAh g-1 at 100 mA g-1 and even 275 mAh g-1 at 2 A g-1 . Theoretical calculation also reveals that the potassium-ion diffusion can be dramatically promoted by the controllable CoSe2 -FeSe2 heterojunction.

Controllable Heterojunctions with a Semicoherent Phase Boundary Boosting the Potassium Storage of CoSe2 /FeSe2.

Metal sulfides, such as MoS2, are widely investigated in lithium-sulfur (Li-S) batteries to suppress the shuttling of lithium polysulfides (LiPSs) due to their chemical adsorption ability and catalytic activity. However, their relatively low conductivity and activity limit the LiPS conversion kinetics. Herein, the Co-doped MoS2 is proposed to accelerate the catalytic conversion of LiPS as the Co doping can promote the transition from semiconducting 2H phase to metallic 1T phase and introduce the sulfur vacancies in MoS2. A one-step hydrothermal process is used to prepare such a Co-doped MoS2 with more 1T phase and rich sulfur vacancies, which enhances the electron transfer and catalytic activity, thus effectively improving the LiPS adsorption and conversion kinetics. The cathode using the three-dimensional graphene monolith loaded with Co-doped MoS2 catalyst as the sulfur host shows a high rate capability and long cycling stability. A high capacity of 941 mAh g-1 at 2 C and a low capacity fading of 0.029% per cycle at 1 C over 1000 cycles are achieved, suggesting the effectively suppressed LiPS shuttling and improved sulfur utilization. Good cyclic stability is also maintained under a high sulfur loading indicating the doping is an effective way to optimize the metal sulfide catalysts in Li-S batteries.

Cobalt-Doping of Molybdenum Disulfide for Enhanced Catalytic Polysulfide Conversion in Lithium-Sulfur Batteries.

Heterostructures are attractive for advanced energy storage devices due to their rapid charge transfer kinetics, which is of benefit to the rate performance. The rational and facile construction of heterostructures with satisfactory electrochemical performance, however, is still a great challenge. Herein, ultrafine hetero-CoO/ Co3S4 nanoparticles embedded in N-doped carbon frameworks (CoO/Co3S4@N-C) are successfully obtained by employing metal-organic frameworks as precursors. As anodes for sodium ion batteries, the CoO/Co3S4@N-C electrodes exhibit high specific capacity (1029.5 mA h g−1 at 100 mA g−1) and excellent rate capability (428.0 mA h g−1 at 5 A g−1), which may be attributed to their enhanced electric conductivity, facilitated Na+ transport, and intrinsic structural stability. Density functional theoretical calculations further confirm that the constructed heterostructures induce electric fields and promote fast reaction kinetics in Na+ transport. This work provides a feasible approach to construct metal oxide/sulfide heterostructures toward high-performance metal-ion batteries.

/pdf/constructing-coo-co3s4-heterostructures-embedded-in-n-doped-2sfu4hxrj0.pdf

Constructing CoO/Co3S4 Heterostructures Embedded in N-doped Carbon Frameworks for High-Performance Sodium-Ion Batteries

Pyrometallurgy technique is usually applied as a pretreatment to enhance the leaching efficiencies in the hydrometallurgy process for recovering valuable metals from spent lithium-ion batteries. However, traditional pyrometallurgy processes are energy and time consuming. Here, we report a carbothermal shock (CTS) method for reducing LiNi0.3Co0.2Mn0.5O2 (NCM325) cathode materials with uniform temperature distribution, high heating and cooling rates, high temperatures, and ultrafast reaction times. Li can be selectively leached through water leaching after CTS process with an efficiency of >90 %. Ni, Co, and Mn are recovered by dilute acid leaching with efficiencies >98 %. The CTS reduction strategy is feasible for various spent cathode materials, including NCM111, NCM523, NCM622, NCM811, LiCoO2, and LiMn2O4. The CTS process, with its low energy consumption and potential scale application, provides an efficient and environmentally friendly way for recovering spent lithium-ion batteries.

Recycling Valuable Metals from Spent Lithium-Ion Batteries Using Carbothermal Shock Method.

Zn-ion batteries are re-evaluated as a potential choice to address the safety issue and cost concerns of current energy storage systems. Unfortunately, further application is severely hindered by low coulombic efficiency and poor cycle life, which are caused by the undesirable dendrite growth and side reactions on metal Zn anode. Herein, ethylenediaminetetraacetic acid (EDTA) is employed as an electrolyte additive to solve the problem. The functional groups of EDTA adsorption layer on Zn foil results in refined grains by providing abundant nucleation sites for initial deposition and further induces uniform and flat Zn deposition without dendrites. Moreover, the chelation of EDTA with Zn2+ changes the coordination environment of hydrated Zn2+ and suppresses the side reactions. The smooth deposition of Zn endows the Zn anodes with super stability in both symmetric cells and Zn–V2O5 full cells. This work provides a simple and feasible approach for solving anode issues in high-performance and safe Zn-ion batteries. 

Toward Stable Zinc-Ion Batteries: Use of a Chelate Electrolyte Additive for Uniform Zinc Deposition

The coupling of photocatalysis and biodegradation (CPB) has shown great potential as a low-cost, environmental friendly and sustainable wastewater treatment technology. However, the photo-generated reactive oxidative species (ROS) could attack microorganisms in the CPB. Here, a photo-controlled reversible photocatalytic system was developed for protecting microorganisms from ROS attack in CPB. Thermal-responsive polymer (TRP) was coated on the surface of yolk-shell [email protected]2, and then [email protected]2 @TRP was attached to the surface of graphene (photo-thermal converter) to form the photo controlled reversible photocatalytic system (RPS). Without light irradiation, the soluble contaminants could be absorbed into the void space of [email protected]2 @TRP. And under light irradiation, the photo-generated ROS would be locked inside the silica shell to degrade the absorbed organic molecules, avoiding harming microorganisms in CPB. Batch results showed that this CPB system could simultaneously remove 97.24 % of phenol (model contaminant) and 91.12 % of TOC under intermittent light irradiation, which was superior to other control groups. This work provides a new strategy to protect microorganisms in CPB for effective wastewater treatment. 

Reversible Controlled Switching of Photocatalysis for Microorganism Protection in the Coupling of Photocatalysis and Biodegradation

Pomegranate-like mesoporous double carbon-coated Fe2P nanoparticles as advanced anode materials for sodium-ion batteries

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