Enhancing ionic conductivity of quasi‐solid‐state electrolytes (QSSEs) is one of the top priorities, while conventional metal–organic frameworks (MOFs) severely impede ion migration due to their abundant grain boundaries. Herein, ZIF‐4 glass, a subset of MOFs, is reported as QSSEs (LGZ) for lithium‐metal batteries. With lean Li content (0.12 wt%) and solvent amount (19.4 wt%), LGZ can achieve a remarkable ion conductivity of 1.61 × 10−4 S cm−1 at 30 °C, higher than those of crystalline ZIF‐4‐based QSSEs (LCZ, 8.21 × 10−5 S cm−1) and the reported QSSEs containing high Li contents (0.32–5.4 wt%) and huge plasticizer (30–70 wt%). Even at −56.6 °C, LGZ can still deliver a conductivity of 5.96 × 10−6 S cm−1 (vs 4.51 × 10−7 S cm−1 for LCZ). Owing to the grain boundary‐free and isotropic properties of glassy ZIF‐4, the facilitated ion conduction enables a homogeneous ion flux, suppressing Li dendrites. When paired with LiFePO4 cathode, LGZ cell demonstrates a prominent cycling capacity of 101 mAh g−1 for 500 cycles at 1 C with the near‐utility retention, outperforming LCZ (30.7 mAh g−1) and the explored MOF‐/covalent–organic frameworks (COF)‐based QSSEs. Hence, MOF glasses will be a potential platform for practical quasi‐solid‐state batteries in the future.

Constructing robust nucleation sites with an ultrafine size in a confined environment is essential toward simultaneously achieving superior utilization, high capacity, and long-term durability in Na metal-based energy storage, yet remains largely unexplored. Here, we report a previously unexplored design of spatially confined atomic Sn in hollow carbon spheres for homogeneous nucleation and dendrite-free growth. The designed architecture maximizes Sn utilization, prevents agglomeration, mitigates volume variation, and allows complete alloying-dealloying with high-affinity Sn as persistent nucleation sites, contrary to conventional spatially exposed large-size ones without dealloying. Thus, conformal deposition is achieved, rendering an exceptional capacity of 16 mAh cm −2 in half-cells and long cycling over 7000 hours in symmetric cells. Moreover, the well-known paradox is surmounted, delivering record-high Na utilization (e.g., 85%) and large capacity (e.g., 8 mAh cm −2 ) while maintaining extraordinary durability over 5000 hours, representing an important breakthrough for stabilizing Na anode.

The semiconductor–liquid junction (SCLJ), the dominant place in photoelectrochemical (PEC) catalysis, determines the interfacial activity and stability of photoelectrodes, whcih directly affects the viability of PEC hydrogen generation. Though efforts dedicated in past decades, a challenge remains regarding creating a synchronously active and stable SCLJ, owing to the technical hurdles of simultaneously overlaying the two advantages. The present work demonstrates that creating an SCLJ with a unique configuration of the dual interfacial layers can yield BiVO4 photoanodes with synchronously boosted photoelectrochemical activity and operational stability, with values located at the top in the records of such photoelectrodes. The bespoke dual interfacial layers, accessed via grafting laser‐generated carbon dots with phenolic hydroxyl groups (LGCDs‐PHGs), are experimentally verified effective, not only in generating the uniform layer of LGCDs with covalent anchoring for inhibited photocorrosion, but also in activating, respectively, the charge separation and transfer in each layer for boosted charge‐carrier kinetics, resulting in FeNiOOH–LGCDs‐PHGs–MBVO photoanodes with a dual configuration with the photocurrent density of 6.08 mA cm−2 @ 1.23 VRHE, and operational stability up to 120 h @ 1.23 VRHE. Further work exploring LGCDs‐PHGs from catecholic molecules warrants the proposed strategy as being a universal alternative for addressing the interfacial charge‐carrier kinetics and operational stability of semiconductor photoelectrodes.

Robust anchoring of high-capacity nanocrystals (NCs) on porous conductive substrates is of paramount importance but it is challenging for highly efficient energy storage to prevent the weak interfacial interactions, inevitable aggregation, and sluggish charge transfer, due to the technical hurdles of constructing heterostructures with firm electron/ion bridging. Herein, a facile and highefficiency liquid-phase laser manufacturing strategy to guarantee the covalent bonding of ultrafine NCs on conductive substrates by predesigning metastable supranano (<10 nm) particles is proposed. The manufacturing of supranano SnO 2 (≈3.4 nm) is demonstrated to tightly anchor on mesoporous walls of graphene with high loading (≈81.3%) and homogenous dispersion. Such a optimized heterostructure with unimpeded electron/ion transfer delivers extraordinary long-term cycling stability (1132 mAh g -1 at 1.0 A g -1 after 1250 cycles) and impressive rate capability (275 mAh g -1 at 30.0 A g -1 ) as the anode for Li-storage, which are some of the highest values among the reported SnO 2 -based anodes. The study provides an important avenue for addressing the interfacial bridging in-between heterostructures via creating active metastable supranano particles for intriguing electrochemical applications or even beyond, based on laser-matter interactions.

Potassium-ion batteries (PIBs) hold great promise as alternatives to lithium ion batteries in post-lithium age, while face challenges of slow reaction kinetics induced by the inherent characteristics of large-size K +. We herein show that creating sufficient exposed edges in MoS 2 via constructing ordered mesoporous architecture greatly favors for improved kinetics as well as increased reactive sites for K storage. The engineered MoS 2 with edge-enriched planes (EE-MoS 2) is featured by three-dimensional bicontinuous frameworks with ordered mesopores of ~ 5.0 nm surrounded by thin wall of ~ 9.0 nm. Importantly, EE-MoS 2 permits exposure of enormous edge planes at pore walls, renders its intrinsic layer spacing more accessible for K + and accelerates conversion kinetics, thus realizing enhanced capacity and high rate capability. Impressively, EE-MoS 2 displays a high reversible charge capacity of 506 mAh•g −1 at 0.05 A•g −1 , superior cycling capacities of 321 mAh•g −1 at 1.0 A•g −1 after 200 cycles and a capacity of 250 mAh•g −1 at 2.0 A•g −1 , outperforming edge-deficient MoS 2 with nonporous bulk structure. This work enlightens the nanoarchitecture design with abundant edges for improving electrochemical properties and provides a paradigm for exploring high-performance PIBs.