Architectural design of lithium metal anodes (LMAs) is crucial for smooth Li plating/stripping with suppressed dendrites, which is paramount for high-performance lithium metal batteries (LMBs). In this study, to leverage the carbonaceous host with low gravimetric density for enhanced Li accommodation and reversible Li deposition, mesoporous carbon nanocages comprising dendritic nanochannels embedded with lithophilic Ni nanoparticles are fabricated and exploited to mitigate superficial Li deposition and promote fast and reversible Li plating/stripping within the three-dimensional (3D) host of LMA. Through guided Li⁺ infiltration, enhanced Li⁺ diffusivity, lowered nucleation barrier, and expedited redox kinetics, the optimal Li host exhibits a high Coulombic efficiency of Li plating/stripping in Li-Cu half cells with significantly reduced dendrite formation and superb cycling stability of symmetric cells over 2000 h at 1 mA·cm⁻². When paired with the LiFePO₄ cathode, the LMB full cell demonstrates a prolonged cycle life, retaining 82.2% of its initial capacity after 600 cycles. This work highlights the crafting of 3D Li hosts with desired structure and functionality for guiding and accommodating smooth Li deposition.

Assembly of two-dimensional (2D) metal–organic layers (MOLs) based on the hard and soft acid–base theorem represents an exquisite strategy for the construction of photocatalytic platforms in virtue of the highly exposed active sites, much improved mass transport, and greatly elevated stability. Herein, nanocages composed of MOLs are produced for the first time through a cosolvent approach utilizing zirconium-based UiO-66-(OH)₂ as the structural precursor. To endow the catalytic activity for CO₂ conversion, single atomic Co²⁺ sites are appended to the Zr-oxo nodes of the MOL cages, demonstrating a remarkable CO yield of 7.74 mmol·g⁻¹·h⁻¹ and operational stability of 97.1% product retention after five repeated cycles. Such an outstanding photocatalytic performance is mainly attributed to the unique nanocage morphology comprising enormous 2D nanosheets for augmented Co²⁺ exposure and the abundant surface hydroxyl groups for local CO₂ enrichment. This work underlines the tailoring of both metal–organic framework (MOF) morphology and functionality to boost the turnover rate of photocatalytic CO₂ reduction reaction (CO₂RR).

The development of deeply cyclable lithium metal batteries with fast-charging capability offers a promising solution to relieve the “range anxiety” in driving electric vehicles. Conventional lithium metal anodes suffered from low operating current densities and shallow charge/discharge depths, owing to the intrinsic dendrite growth governed by Sand’s law. Herein, we come up with a novel design of heavy-duty lithium metal anode fabricated by partially infusing the three-dimensional (3D) porous graphene aerogel with molten Li. Both electroanalytical measurements and simulations show that the unique electrode architecture brings notable advantages in mediating smooth Li plating/stripping, including reduced local current density, inhibited dendrite growth, buffered volume fluctuation, as well as more efficient Li utilization. Consequently, a remarkable cycling performance in symmetric cells for over 400 cycles (800 h) with an ultrahigh cycling capacity of 15 mAh·cm⁻² at 15 mA·cm⁻² is achieved, which, to our best knowledge, has been never seen in literature. LiFePO₄ full cells demonstrate a superb rate capability up to 10 C and a prolonged cycling of 1,600 cycles at 2 C with the per-cycle capacity decay of only 0.023%. This study paves the way for the ultimate deployment of lithium metal batteries in real-world applications that require fast charging and deep cycling.