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Achieving stable Zn anodes is essential for advancing high-performance Zn metal batteries. Here, we propose a Sabatier principle inspired bifunctional transition-metal (TM) interface to enable homogeneous Zn dissolution during discharging and dendrite-free Zn deposition during charging. Among various TM-coated Zn (TM@Zn) electrodes, Cu@Zn exhibits the highest reversibility and structural stability, attributed to the optimal interaction between Cu and Zn. The heteroatomic interaction-dependent electrochemical performance parallels the Sabatier principle. Morphological analyses reveal that bare Zn anodes display detrimental etching pits during stripping, which is different from the uniform dissolution for Cu@Zn electrodes. During subsequent plating, the conductive interface serves as a secondary current collector for uniform Zn deposition in Cu@Zn, thus demonstrating a bifunctional nature. Atomic observations disclose the working mechanisms of this interface as a gradual phase transition from Cu to CuZn5 during cycling. The Cu@Zn anodes exhibit an ultralong cycling lifespan of over 8000 h at a low current of 1 mA cm-2 and over 250 h at a high depth of discharge of 80%. They also demonstrate practical feasibility by maintaining 88.7% capacity retention after 1000 cycles in Cu@Zn||VO2 full cells. This work provides new insights into the Sabatier chemistry inspired bifunctional layers for Zn metal battery system., (© 2025 Wiley‐VCH GmbH.)

Aprotic Li-CO 2 batteries suffer from sluggish solid-solid co-oxidation kinetics of C and Li 2 CO 3 , requiring extremely high charging potentials and leading to serious side reactions and poor energy efficiency. Herein, we introduce a novel approach to address these challenges by modulating the reaction pathway with tailored Pt d-electrons and develop an aprotic Li-CO 2 battery with CO and Li 2 CO 3 as the main discharge products. Note that the gas-solid co-oxidation reaction between CO and Li 2 CO 3 is both kinetically and thermodynamically more favorable. Consequently, the Li-CO 2 batteries with CoPt alloy-supported on nitrogen-doped carbon nanofiber (CoPt@NCNF) cathode exhibit a charging potential of 2.89 V at 50 μA cm -2 , which is the lowest charging potential to date. Moreover, the CoPt@NCNF cathode also shows exceptional cycling stability (218 cycles at 50 μA cm -2 ) and high energy efficiency up to 74.6 %. Comprehensive experiments and theoretical calculations reveal that the lowered d-band center of CoPt alloy effectively promotes CO desorption and inhibits further CO reduction to C. This work provides promising insights into developing efficient and CO-selective Li-CO 2 batteries., (© 2024 Wiley-VCH GmbH.)

Single-atom catalysts with maximal atom-utilization have emerged as promising alternatives for chlorine evolution reaction (CER) toward valuable Cl 2 production. However, understanding their intrinsic CER activity has so far been plagued due to the lack of well-defined atomic structure controlling. Herein, we prepare and identify a series of atomically dispersed noble metals (e.g., Pt, Ir, Ru) in nitrogen-doped nanocarbons (M 1 -N-C) with an identical M-N 4 moiety, which allows objective activity evaluation. Electrochemical experiments, operando Raman spectroscopy, and quasi-in situ electron paramagnetic resonance spectroscopy analyses collectively reveal that all the three M 1 -N-C proceed the CER via a direct Cl-mediated Vomer-Heyrovský mechanism with reactivity following the trend of Pt 1 -N-C>Ir 1 -N-C>Ru 1 -N-C. Density functional theory (DFT) calculations reveal that this activity trend is governed by the binding strength of Cl*-Cl intermediate (ΔG Cl*-Cl ) on M-N 4 sites (Pt2 electrosynthesis., (© 2024 Wiley-VCH GmbH.)

Designing efficient catalysts for operating CO 2 electroreduction in membrane electrode assembly (MEA) faces significant obstacles. Herein, we propose an asymmetrically coordinated Ni single-atom catalyst featuring axial Br coordination at NiN 4 Br sites anchoring onto hollow Br/N co-doped carbon nanocages, achieved through a NaBr-assisted confined-pyrolysis strategy. The Ni-NBr-C catalyst exhibits a high CO Faradaic efficiency (FE CO >97 %) over the current density range of 50 to 350 mA cm -2 in the MEA device. Furthermore, Ni-NBr-C shows a stable cell voltage of 2.66±0.2 V while delivering a large current density of 350 mA cm -2 over an 85-hour long-term operation, demonstrating its potential for industrial-scale applications. Advanced characterization techniques and theoretical calculations reveal that the coordination and doping of Br not only enhance the intrinsic activity but also highlight that the unique pore structure improves mass transfer efficiency., (© 2024 Wiley-VCH GmbH.)

Electrocatalytic urea synthesis from carbon dioxide (CO 2 ) and nitrate (NO 3 - ) offers a promising alternative to traditional industrial methods. However, current catalysts face limitations in the supplies of CO* and N related * intermediates, and their coupling, resulting in unsatisfactory urea production efficiency and energy consumption. To overcome these challenges, we carried out tandem electrosynthesis approach using ruthenium dioxide-supported palladium-gold alloys (Pd 2 Au 1 /RuO 2 ). This catalyst system effectively catalyzes CO 2 -to-CO* conversion on Pd 2 Au 1 and NO 3 - -to-NH 2 * conversion on RuO 2 . Crucially, the minimized work function difference between two components promotes remote CO* spillover from Pd 2 Au 1 to RuO 2 , improving effective coupling of CO* and NH 2 * for urea production. Our catalyst demonstrated exceptional performance, achieving a record-high Faradaic efficiency for urea (FE urea ) of 75.6±0.5 % and a urea production rate (r urea ) of 73.5±0.8 mmol g cat -1  h -1 . Notably, this was accomplished with an ultralow energy consumption of 18.9 kWh kg urea -1 . We also successfully demonstrate the long-term stability of our catalyst in a flow cell, achieving over 160 h of uninterrupted urea and formate production with consistent profitability. This achievement represents a significant step towards the large-scale practical application of sustainable urea electrosynthesis., (© 2025 Wiley-VCH GmbH.)