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).

Electroreduction of carbon dioxide into value-added fuels or chemicals using renewable energy helps to effectively reduce carbon dioxide emission and alleviate the greenhouse effect while storing intermittent energies. Due to the existing infrastructure of global natural gas utilization and distribution, methane produced in such a green route attracts wide interests. However, limited success has been witnessed in the practical application of catalysts imparting satisfactory methane activity and selectivity. Herein, we report the fabrication of an atomically dispersed Co-Cu alloy through the reconstruction of trace-Co doped Cu metal-organic framework. This catalyst exhibits a methane Faradaic efficiency of 60% ± 1% with the corresponding partial current density of 303 ± 5 mA·cm⁻². Operando X-ray adsorption spectroscopy and attenuated-total-reflection surface enhanced infrared spectroscopy unravel that the introduction of atomically dispersed Co in Cu favors *CO protonation via enhancing surface water activation, and suppresses C−C coupling by reducing *CO coverage, thereby leading to high methane selectivity.

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.