Single-atom Fe–N–C electrocatalysts have demonstrated exceptional selectivity toward CO during CO₂ reduction, yet their practical application is severely hindered by the intrinsic activity–stability trade-off. Herein, we report a straightforward in-situ sulfidation of Fe-doped zeolitic imidazolate frameworks to construct ZnS nanoparticle-modified S-doped Fe–N–C catalysts (ZnS@Fe–NSC). This approach causes the concurrent formation of Fe–N₄ active sites, S doping, and ZnS nanoparticles. Operando characterizations and density functional theory (DFT) calculations reveal that ZnS nanoparticles donate electrons to Fe centers with a 0.5 eV negative shift in Fe 2p binding energy and strengthen Fe–N bonds with an increased integrated crystal orbital Hamiltonian population value from −0.94 to −1.30 eV. This electronic modulation accelerates the formation of the key *COOH intermediate and suppresses the hydrogen-induced Fe leaching by over 20-fold. The ZnS@Fe–NSC exhibits a CO Faradaic efficiency of 98.5% at −0.58 V versus reversible hydrogen electrode and maintains over 90% selectivity for 30 h. When integrated into a Zn–CO₂ battery, it delivers a peak power density of 6.2 mW·cm⁻² and operates stably for 125 h. This work opens an avenue for the rational design of robust single-atom electrocatalysts toward practical CO₂ conversion and beyond.

Two-dimensional (2D) mesoporous carbon materials demonstrate attractive potential in advanced energy storage applications due to their dual advantages of combing mesoporous carbon and 2D structure. However, achieving efficient and controllable synthesis of these materials while precisely regulating their pore architecture remains a significant challenge. Herein, a soft-hard template directed co-assembly strategy has been proposed for synthesis of two kinds of mesoporous carbon materials (DMC and AMC) using copolymer P123 as the soft template and MWW-type zeolite as the 2D hard template. The obtained two composites both show unique maze-like morphology, open 2D structure, and high nitrogen doping of above 14.0 at.%. Compared to the AMC electrode, the achieved DMC electrode demonstrates a better lithium-ion storage performance owing to its faster electron/ion transfer dynamics and stronger structural stability. As a result, it shows an outstanding cycling stability, delivering a high reversible capacity of 827.5 mAh·g⁻¹ at 2000 mA·g⁻¹ after 600 cycles. This work not only provides a new design concept for the synthesis of 2D materials, but also offers a good reference for the energy storage applications of mesoporous carbon electrode materials.

Exploring cost-effective and highly-active oxygen evolution reaction (OER) electrocatalysts is a pressing task to propel water electrolysis for green hydrogen production. Herein, we constructed a class of Fe-doped and S-enriched Ni₃S₂ nanowires electrocatalysts for optimizing the target intermediates adsorption to decrease the OER overpotentials at various current densities. The optimal Ni₃S₂-1.4%Fe electrocatalyst possesses the most active sites and exhibits an ultralow overpotential of 190 mV at 10 mA cm⁻² with an excellent stability of > 60 h, exceeding the majority of recently-reported Ni₃S₂-based electrocatalysts. The trivalence Fe-doping not only reduces the electron density of the Ni center, but also enables the sulfur enrichment on the Ni₃S₂ surface, which greatly improves the intrinsic activity and the number of target intermediates (^*OOH). A novel methanol-assisted electrochemical evaluation further reveals that the Ni₃S₂-1.4%Fe electrocatalyst demonstrates a weaker binding ability to ^*OH with the rapid generation of ^*OOH species, and thus gives a lower apparent activation energy compared with the surface sulfur reduced ones. This work provides a new perspective for regulating the adsorption of intermediates through doping strategy.

The low specific capacity and sluggish electrochemical reaction kinetics greatly block the development of sodium-ion batteries (SIBs). New high-performance electrode materials will enhance development and are urgently required for SIBs. Herein, we report the preparation of supersaturated bridge-sulfur and vanadium co-doped MoS₂ nanosheet arrays on carbon cloth (denoted as V-MoS_2+x/CC). The bridge-sulfur in MoS₂ has been created as a new active site for greater Na⁺ storage. The vanadium doping increases the density of carriers and facilitates accelerated electron transfer. The synergistic dual-doping effects endow the V-MoS_2+x/CC anodes with high sodium storage performance. The optimized V-MoS_2.49/CC gives superhigh capacities of 370 and 214 mAh·g^-1 at 0.1 and 10 A·g^-1 within 0.4-3.0 V, respectively. After cycling 3,000 times at 2 A·g^-1, almost 83% of the reversible capacity is maintained. The findings indicate that the electrochemical performances of metal sulfides can be further improved by edge-engineering and lattice-doping co-modification concept.