Heterostructured WOx /W2 C Nanocatalyst for Li2 S Oxidation in Lithium-Sulfur Batteries with High-Areal-Capacity.

Lithium-sulfur (Li-S) batteries show extraordinary promise as a next-generation battery technology due to their high theoretical energy density and the cost efficiency of sulfur. However, the sluggish reaction kinetics, uncontrolled growth of lithium sulfide (Li2 S), and substantial Li2 S oxidation barrier cause low sulfur utilization and limited cycle life. Moreover, these drawbacks get exacerbated at high current densities and high sulfur loadings. Here, a heterostructured WOx /W2 C nanocatalyst synthesized via ultrafast Joule heating is reported, and the resulting heterointerfaces contribute to enhance electrocatalytic activity for Li2 S oxidation, as well as controlled Li2 S deposition. The densely distributed nanoparticles provide abundant binding sites for uniform deposition of Li2 S. The continuous heterointerfaces favor efficient adsorption and promote charge transfer, thereby reducing the activation barrier for the delithiation of Li2 S. These attributes enable Li-S cells to deliver high-rate performance and high areal capacity. This study provides insights into efficient catalyst design for Li2 S oxidation under practical cell conditions.

Graphene and MOF Assembly: Enhanced Fabrication and Functional Derivative via MOF Amorphization.

The integration of graphene and metal-organic frameworks (MOFs) has numerous implications across various domains, but fabricating such assemblies is often complicated and time-consuming. Herein, a one-step preparation of graphene-MOF assembly is presented by directly impregnating vertical graphene (VG) arrays into the zeolitic imidazolate framework (ZIF) precursors under ambient conditions. This approach can effectively assemble multiple ZIFs, including ZIF-7, ZIF-8, and ZIF-67, resulting in their uniform dispersion on the VG with adjustable sizes and shapes. Hydrogen defects on the VG surface are critical in inducing such high-efficiency ZIF assembly, acting as the reactive sites to interact with the ZIF precursors and facilitate their crystallisation. The versatility of VG-ZIF-67 assembly is further demonstrated by exploring the process of MOF amorphization. Surprisingly, this process leads to an amorphous thin-film coating formed on VG (named VG-IL-amZIF-67), which preserves the short-range molecular bonds of crystalline ZIF-67 while sacrificing the long-range order. Such a unique film-on-graphene architecture maintains the essential characteristics and functionalities of ZIF-67 within a disordered arrangement, making it well-suited for electrocatalysis. In electrochemical oxygen reduction, VG-IL-amZIF-67 exhibits exceptional activity, selectivity, and stability to produce H2O2 in acid media.

Recent Progress on Electrode Design for Efficient Electrochemical Valorisation of CO2 , O2 , and N2.

CO2 reduction, two-electron O2 reduction, and N2 reduction are sustainable technologies to valorise common molecules. Their further development requires working electrode design to promote the multistep electrochemical processes from gas reactants to value-added products at the device level. This review proposes critical features of a desirable electrode based on the fundamental electrochemical processes and the development of scalable devices. A detailed discussion is made to approach such a desirable electrode, addressing the recent progress on critical electrode components, assembly strategies, and reaction interface engineering. Further, we highlight the electrode design tailored to reaction properties (e.g., its thermodynamics and kinetics) for performance optimisation. Finally, the opportunities and remaining challenges are presented, providing a framework for rational electrode design to push these gas reduction reactions towards an improved technology readiness level (TRL).