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The synthesis of cathode materials plays an important role in determining the production efficiency, cost, and performance of lithium-ion batteries. However, conventional synthesis methods always experience a slow heating rate and involve a complicated multistep reaction process and sluggish reaction dynamics, leading to high energy and long time consumption. Herein, a high-temperature shock (HTS) strategy is reported for the ultrafast synthesis of cathode materials in seconds. The HTS process experiences an ultrahigh heating rate, leading to a non-equilibrium reaction and fast reaction kinetics, and avoids high energy and long time consumption. Mainstream cathode materials (such as LiMn

Metal-organic framework (MOF) derivatives promise great potential in energy storage and conversion because of their excellent tunability in both the active metal sites, organic links, and the overall structures down to atomic and up to mesoscale. Nevertheless, a big challenge is to precisely control and thoroughly understand the actual MOF-to-derivative conversion process to realize the template-free synthesis of the MOF-derived ordered mesoporous materials. Here, a class of ordered mesoporous N-doped carbon nanoflakes is presented with slit-shaped pores synthesized by one-step pyrolysis of Zn

CO2 electroreduction (CO2 RR) to CO is promising for the carbon cycle but still remains challenging. Au is regarded as the most selective catalyst for CO2 RR, but its high cost significantly hinders its industrial application. Herein, the bimetallic CuInSe2 is found to exhibit an Au-like catalytic feature: i) the interaction of Cu and In orbitals induces a moderate adsorption strength of CO2 RR intermediates and favors the reaction pathway; and ii) the hydrogen evolution is energetically unfavorable on CuInSe2 , as a surface reconstruction along with high energy change will occur after hydrogen adsorption. Furthermore, the Se vacancy is found to induce an electron redistribution, slightly tune the band structure, and optimize the CO2 RR route of bimetallic selenide. Consequently, the Se-defective CuInSe2 (V-CuInSe2 ) achieves a highly selective CO production ability that is comparable to noble metals in aqueous electrolyte, and the V-CuInSe2 cathode shows a satisfactory performance in an aqueous Zn-CO2 cell. This work demonstrates that designing cost-effective catalysts with noble-metal-like properties is an ideal strategy for developing efficient electrocatalysts. Moreover, the class of transition bimetallic selenides has shown promising prospects as active and cost-effective electrocatalysts owing to their unique structural, electronic, and catalytic properties.

Crystal structure engineering of nanomaterials is crucial for the design of electrocatalysts. Inducing dislocations is an efficient approach to generate strain effects in nanomaterials to optimize the crystal and electronic structures and improve the catalytic properties. However, it is almost impossible to produce and retain dislocations in commercial mainstream catalysts, such as single metal platinum (Pt) catalysts. In this work, a non-equilibrium high-temperature (>1400 K) thermal-shock method is reported to induce rich dislocations in Pt nanocrystals (Dr-Pt). The method is performed in an extreme environment (≈77 K) created by liquid nitrogen. The dislocations induced within milliseconds by thermal and structural stress during the crystallization process are kinetically frozen at an ultrafast cooling rate. The high-energy surface structures with dislocation-induced strain effects can prevent surface restructuring during catalysis. The findings indicate that a novel extreme environmental high-temperature thermal-shock method can successfully introduce rich dislocations in Pt nanoparticles and significantly boost its hydrogen evolution reaction performance.

Designing high-performance and low-cost electrocatalysts is crucial for the electrochemical production of hydrogen. Dislocation-strained IrNi nanoparticles loaded on a carbon nanotube sponge (DSIrNi@CNTS) driven by unsteady thermal shock in an extreme environment are reported here as a highly efficient hydrogen evolution reaction (HER) catalyst. Experimental results demonstrate that numerous dislocations are kinetically trapped in self-assembled IrNi nanoparticles due to the ultrafast quenching and different atomic radii, which can induce strain effects into the IrNi nanoparticles. Such strain-induced high-energy surface structures arising from bulk defects (dislocations), are more likely to be resistant to surface restructuring during catalysis. The catalyst exhibits outstanding HER activity with only 17 mV overpotential to achieve 10 mA cm-2 in an alkaline electrolyte with fabulous stability, exceeding state-of-the-art Pt/C catalysts. These density functional theory results demonstrate that the electronic structure of as-synthesized IrNi nanostructure can be optimized by the strain effects induced by the dislocations, and the free energy of HER can be tuned toward the optimal region.

Developing highly-efficient non-noble-metal electrocatalysts for water splitting is crucial for the development of clean and reversible hydrogen energy. Introducing lattice strain is an effective strategy to develop efficient electrocatalysts. However, lattice strain is typically co-created with heterostructure, vacancy, or substrate effects, which complicate the identification of the strain-activity correlation. Herein, a series of lattice-strained homogeneous NiSx Se1-x nanosheets@nanorods hybrids are designed and synthesized by a facile strategy. The NiS0.5 Se0.5 with ≈2.7% lattice strain exhibits outstanding activity for hydrogen and oxygen evolution reaction (HER/OER), affording low overpotentials of 70 and 257 mV at 10 mA cm-2 , respectively, as well as excellent long-term durability even at a large current density of 100 mA cm-2 (300 h), significantly superior to other benchmarks and the precious metal catalysts. Experimental and theoretical calculation results reveal that the generated lattice strain decreases the metal d-orbital overlap, leading to a narrower bandwidth and a closer d-band center toward the Fermi level. Thus, NiS0.5 Se0.5 possesses favorable H* adsorption kinetics for HER and lower energy barriers for OER. This work provides a new insight to regulate the lattice strain of advanced catalyst materials and further improve the performance of energy conversion technologies.

Exploring earth-abundant and highly efficient electrocatalysts is critical for further development of water electrolyzer systems. Integrating bifunctional catalytically active sites into one multi-component might greatly improve the overall water-splitting performance. In this work, amorphous NiO nanosheets coupled with ultrafine Ni and MoO3 nanoparticles (MoO3 /Ni-NiO), which contains two heterostructures (i.e., Ni-NiO and MoO3 -NiO), is fabricated via a novel sequential electrodeposition strategy. The as-synthesized MoO3 /Ni-NiO composite exhibits superior electrocatalytic properties, affording low overpotentials of 62 mV at 10 mA cm-2 and 347 mV at 100 mA cm-2 for catalyzing the hydrogen and the oxygen evolution reaction (HER/OER), respectively. Moreover, the MoO3 /Ni-NiO hybrid enables the overall alkaline water-splitting at a low cell voltage of 1.55 V to achieve 10 mA cm-2 with outstanding catalytic durability, significantly outperforming the noble-metal catalysts and many materials previously reported. Experimental and theoretical investigations collectively demonstrate the generated Ni-NiO and MoO3 -NiO heterostructures significantly reduce the energetic barrier and act as catalytically active centers for selective HER and OER, synergistically accelerating the overall water-splitting process. This work helps to fundamentally understand the heterostructure-dependent mechanism, providing guidance for the rational design and oriented construction of hybrid nanomaterials for diverse catalytic processes.

Constructing heterostructures with abundant interfaces is essential for integrating the multiple functionalities in single entities. Herein, the synthesis of NiSe2 /CoSe2 heterostructures with different interfacial densities via an innovative strategy of successive ion injection is reported. The resulting hybrid electrocatalyst with dense heterointerfaces exhibits superior electrocatalytic properties in an alkaline electrolyte, superior to other benchmarks and precious metal catalysts. Advanced synchrotron techniques, post structural characterizations, and density functional theory (DFT) simulations reveal that the introduction of atomic-level interfaces can lower the oxidation overpotential of bimetallic Ni and Co active sites (whereas Ni2+ can be more easily activated than Co2+ ) and induce the electronic interaction between the core selenides and surface in situ generated oxides/hydroxides, which play a critical role in synergistically reducing energetic barriers and accelerating reaction kinetics for catalyzing the oxygen evolution. Hence, the heterointerface structure facilitates the catalytic performance enhancement via increasing the intrinsic reactivity of metallic atoms and enhancing the synergistic effect between the inner selenides and surface oxidation species. This work not only complements the understanding on the origins of the activity of electrocatalysts based on metal selenides, but also sheds light on further surface and interfacial engineering of advanced hybrid materials.

Tremendous effort have recently been made in optimizing the air catalysts of flexible zinc-air batteries (ZABs). Unfortunately, the bottleneck factors in electrolytes that largely limit the working life and energy efficiency of ZABs have long been relatively neglected. Herein, an alkaline gel polymer electrolyte (GPE) is fabricated through multiple crosslinking reactions among poly(vinyl alcohol) (PVA), poly(acrylic acid), and graphene oxide followed by intense uptake of an alkali and the KI reaction modifier. The prepared GPE exhibits essentially improved properties compared to traditional PVA gel electrolyte in terms of mechanical strength, ionic conductivity, and water retention capability. In addition, the introduced reaction modifier I- in the GPE changes the path of the conventional oxygen evolution reaction, leading to a more thermodynamically favorable path. The optimized GPE enables flexible ZABs exhibiting an exceptionally low charge potential of 1.69 V, a long cycling time of 200 h, a high energy efficiency of 73%, and rugged reliability under different extreme working conditions. Moreover, the successful integration of ZABs in a variety of real wearable electronic devices demonstrates their excellent practicability as flexible power sources.

This is the first review on potassium-sulfur (K-S) batteries (KSBs), which are emerging metal battery (MB) systems. Since KSBs are quite new, there are fundamental questions regarding the electrochemistry of S-based cathode and of K metal anode, as well as the holistic aspects of full-cell performance. The manuscript begins with a critical discussion regarding the potassium-sulfur electrochemistry and on how it differs from the much better-known lithium-sulfur. Cathodes are discussed next, focusing on the role of sulfur structure, carbon host chemistry and porosity, and electrolytes in establishing the reversible potassium sulfide K2 Sn phase sequence, the parasitic polysulfide shuttle, pulverization-driven capacity fade, etc. Following is a discussion of solid-state electrolytes (SSEs), including of hybrid solid-liquid systems that show much promise. Potassium metal anodes are then critically reviewed, emphasizing electrolyte reactions to form stable versus unstable solid electrolyte interphase (SEI), covering the current understanding of potassium dendrites, and highlighting the deep-eutectic K-Na alloying approaches for room temperature liquid anodes. The manuscript concludes with K-S batteries, focusing on cell architectures and providing quantitative performance comparisons as master plots. Unanswered scientific/technological questions are identified, emerging research opportunities are discussed, and potential experimental and simulation-based studies that can unravel these unknowns are proposed.

Hybrid materials composed of transition-metal compounds and nitrogen-doped carbonaceous supports are promising electrocatalysts for various electrochemical energy conversion devices, whose activity enhancements can be attributed to the synergistic effect between metallic sites and N dopants. While the functionality of single-metal catalysts is relatively well-understood, the mechanism and synergy of bimetallic systems are less explored. Herein, the design and fabrication of an integrated flexible electrode based on NiCo2 S4 /graphitic carbon nitride/carbon nanotube (NiCo2 S4 @g-C3 N4 -CNT) are reported. Comparative studies evidence the electronic transfer from bimetallic Ni/Co active sites to abundant pyridinic-N in underlying g-C3 N4 and the synergistic effect with coupled conductive CNTs for promoting reversible oxygen electrocatalysis. Theoretical calculations demonstrate the unique coactivation of bimetallic Ni/Co atoms by pyridinic-N species (a Ni, Co-N2 moiety), which simultaneously downshifts their d-band center positions and benefits the adsorption/desorption features of oxygen intermediates, accelerating the reaction kinetics. The optimized NiCo2 S4 @g-C3 N4 -CNT hybrid manifests outstanding bifunctional performance for catalyzing oxygen reduction/evolution reactions, highly efficient for realistic zinc-air batteries featuring low overpotential, high efficiency, and long durability, superior to those of physical mixed counterparts and state-of-the-art noble metal catalysts. The identified bimetallic coactivation mechanism will shed light on the rational design and interfacial engineering of hybrid nanomaterials for diverse applications.

The practical scale-up of renewable energy technologies will require catalysts that are more efficient and durable than present ones. This is, however, a formidable challenge that will demand a new capability to tailor the electronic structure. Here, an original electronic structure tailoring of CoO by Ni and Zn dual doping is reported. This changes it from an inert material into one that is highly active for the hydrogen evolution reaction (HER). Based on combined density functional theory calculations and cutting-edge characterizations, it is shown that dual Ni and Zn doping is responsible for a highly significant increase in HER activity of the host oxide. That is, the Ni dopants cluster around surface oxygen vacancy of the host oxide and provide an ideal electronic surface structure for hydrogen intermediate binding, while the Zn dopants distribute inside the host oxide and modulate the bulk electronic structure to boost electrical conduction. As a result, the dual-doped Ni, Zn CoO nanorods achieve current densities of 10 and 20 mA cm-2 at overpotentials of, respectively, 53 and 79 mV. This outperforms reported state-of-the-art metal oxide, metal oxide/metal, metal sulfide, and metal phosphide catalysts.

Under development for next-generation wearable electronics are flexible, knittable, and wearable energy-storage devices with high energy density that can be integrated into textiles. Herein, knittable fiber-shaped zinc-air batteries with high volumetric energy density (36.1 mWh cm-3 ) are fabricated via a facile and continuous method with low-cost materials. Furthermore, a high-yield method is developed to prepare the key component of the fiber-shaped zinc-air battery, i.e., a bifunctional catalyst composed of atomically thin layer-by-layer mesoporous Co3 O4 /nitrogen-doped reduced graphene oxide (N-rGO) nanosheets. Benefiting from the high surface area, mesoporous structure, and strong synergetic effect between the Co3 O4 and N-rGO nanosheets, the bifunctional catalyst exhibits high activity and superior durability for oxygen reduction and evolution reactions. Compared to a fiber-shaped zinc-air battery using state-of-the-art Pt/C + RuO2 catalysts, the battery based on these Co3 O4 /N-rGO nanosheets demonstrates enhanced and stable electrochemical performance, even under severe deformation. Such batteries, for the first time, can be successfully knitted into clothes without short circuits under external forces and can power various electronic devices and even charge a cellphone.