Coupling N2 electroreduction with kinetically and/or thermodynamically favored oxidation reactions in one system can realize the co-production of NH3 and value-added oxygen-containing fine chemicals at lower energy consumption. Here, a new N2 electrolysis system based on nitrogen-doped carbon-supported Bi2O3 and NiO catalysts (Bi2O3/NC and NiO/NC) is demonstrated, in which the methanol oxidation reaction in the anode to make formic acid is coupled with N2 electroreduction for NH3. The optimal NH3 yield of 2.79 μ g_ NH_3 h^-1 cm^-2 is achieved at the voltage of 2.35 V with a high Faradaic efficiency of 5.04

A novel amorphous Cu-Co catalyst is developed and achieves a high faradaic efficiency of over 90% for electrochemical NO-to-NH3 conversion. Importantly, the structure of the catalyst remains unchanged under electroreduction conditions due to an intrinsically disordered, reconstruction-resistant framework that suppresses phase transformation and surface restructuring, delivering long-term stability over 20 h at 200 mA cm-2.

Lithium-sulfur (Li-S) batteries have been regarded as a promising high-energy-density secondary battery system since their inception in the 1960s. However, poor long-term cycling performance and reversibility arose from the shuttle effect remains a challenge. Two-dimensional transition metal borides (MBenes) are ideal conductive frameworks due to their layered structure, excellent electrical conductivity, adjustable chemical surface and abundant active sites, which will effectively mitigate the lithium polysulfides (LiPSs) shuttling effect and simultaneously enhance the redox kinetics in Li-S batteries, thereby demonstrating substantial potential for practical applications. In this study, the Mo4/3B2-MoS2 composite was synthesized for the first time using an in-situ vulcanization strategy. By combining the strong chemical adsorption ability of MoS2 toward LiPSs with the high conductivity and electrocatalytic activity of Mo4/3B2 MBene, the shuttle effect is effectively suppressed, and the conversion kinetics are significantly accelerated. The tight interface formed in situ enhances both charge transfer and adsorption capacity, while the MBene skeleton effectively mitigates volume expansion, thereby maintaining electrode stability. Benefiting from the above synergistic mechanism, the Li-S batteries demonstrate an initial discharge capacity of 1311.4 mAh g-1 at 0.2 C, and maintain an ultra-low decay rate of 0.035% per cycle after 500 cycles at 1 C. This study presents an efficient in-situ synthesis strategy for the development of MBene-based composite catalysts, which enhances the immobilization and conversion of LiPSs through interface regulation and a synergistic catalytic mechanism, thereby promoting the advancement of highly reversible Li-S batteries.

The escalating discharge of recalcitrant organic wastewater presents a significant threat to global water security. Electrochemical advanced oxidation processes (EAOPs) have emerged as a promising technology to address this challenge, leveraging the in-situ generation of highly reactive species for effective mineralization of organic pollutants. Central to the efficacy of EAOPs is the electrocatalytic electrode, whose performance dictates the overall efficiency, cost, and practicality of the technology. This review systematically summarizes recent advancements in the design strategies for three major electrode categories: boron-doped diamond (BDD), metal oxides, and sp2-hybridized carbon-based materials. We critically assess rational design approaches—including component regulation, structural design, and surface/interface engineering—to reveal intrinsic structure-performance relationships that enhance degradation efficiency and stability. Recognizing the gap between laboratory innovation and industrial application, this review further addresses critical engineering challenges impeding scale-up, including electrode deactivation mechanisms, reactor configuration optimization, mass transfer limitations, and techno-economic feasibility. Key scale-up parameters are discussed to establish a comprehensive framework for practical implementation. Finally, we outline future research directions, offering guidance for the rational design and application of next-generation electrocatalytic electrodes for organic wastewater treatment.

The growing demand for renewable energy has spurred the development of efficient electrochemical systems. Transition metal-based materials serve as key electrode materials due to their tunable structures and redox activity, with electrochemical reconstruction playing a critical role in modulation of their properties. A deep understanding of the evolution of active sites and local environments is essential for the rational design of energy materials. Focusing on aqueous energy storage and water splitting, this review discusses the behaviors, mechanisms, and thermodynamics of electrochemical reconstruction. It systematically summarizes recent advances in material design through electrochemical reconstruction across six aspects: doping, defects, active centers, high-valence sites, heterostructures, and electrode/electrolyte interfaces. A connection is established among the reconstruction techniques, the nature of active species, and the corresponding electrochemical behaviors. We also highlight milestone discoveries in reconstruction guided by external fields and the starting topology, alongside in situ/operando techniques for probing dynamic processes. Furthermore, we outline the growing role of artificial intelligence (AI)-driven methods in facilitating material discovery and process optimization, emphasizing the underlying principles of scientific synthesis and analysis. Besides, we discuss the remaining challenges and offer new insights, aiming to inspire future research in machine-learning-assisted design and fabrication of advanced materials for energy storage and conversion.

The electrocatalytic nitrite reduction reaction (eNO2-RR) presents an extraordinary surge in clean yet green ammonia (NH3) synthesis due to mild operation and its promising compatibility with renewable energy sources. Nevertheless, the sluggish NO2- reaction kinetics and the competing hydrogen evolution reaction (HER) remain challenging for efficient NO2--to-NH3 electrosynthesis. Herein, we reveal a strong dependence of H2O structure on KCl concentration in the electrolyte and decouple the KCl-induced water disordering mechanism for efficient NH3 electrosynthesis. This disrupts the hydrogen-bond network of H2O and increases the proportion of K+-H2O species, thereby transforming an ordered proton-hopping network into a disordered environment. This ordering-to-disordering transition increases the activation entropy and lowers the activation enthalpy, leading to a reduction in the apparent free energy and enabling a 2.9-fold enhancement in NH3 production compared to the conventional electrolyte. The KCl-water electrolyte exhibits an exceptional NH3 yield rate of 111.3 mg cm-2 h-1, a Faradaic efficiency of 99.6% at -0.5 V vs RHE, and stable operation for over 1000 h at 1 A cm-2. Multiscale theoretical simulations further confirm that the K+ ions suppress the HER by elevating the water dissociation barrier from 0.1 to 0.7 eV, while the Cl- ions lower the *NO-to-*NOH hydrogenation barrier, thereby promoting the eNO2-RR kinetics. Moreover, the proposed KCl-induced H2O disordering mechanism for efficient eNO2-RR is universal, delivering consistent performance gains across various catalysts.

Sodium-ion batteries (SIBs) are spurring intensive research interest in energy storage community, while carbon anode as the crucial battery component suffer from the poor cycling stability due to the insufficient understanding and rational design of carbon microstructure. Herein, we report the design of ion-gate microstructure in coal-based carbon materials by carbon nanodomain curving. Ion-gate serves as the gate for the electrolyte-electrode (liquid-solid) interphase ion mass transfer. Microcrystal and pore structure characterizations observe locally curved configurations within carbon nanodomains and confirm the nanodomain assembly to form ion-gate. Systematic temperature-dependent spectroscopies uncover the chemistry evolution of polycyclic aromatic hydrocarbons (PAHs) in coal and its interaction with modified chitosan molecule. Molecular dynamic simulations present the aggregation state evolution of PAHs and identify the orientation force as the driving force for carbon nanodomain curving. The as-designed carbon anode realizes an initial Coulombic efficiency (ICE) of 93.23% and a capacity retention of 97.55% after 1000 cycles. This work initially presents a conceptual design of ion-gate microstructure and highlights the role of aggregation state regulation in developing highly-stable and high-efficiency carbon anodes of SIBs.

Two-dimensional transition metal borides (MBenes) are novel 2D materials synthesized by selectively etching Alayer elements from precursor MAB phases. Despite structural similarities between MBenes and MXenes, the former possess a distinct layered structure and characteristic properties: their surfaces offer abundant chemically active sites, metallic conductivity, and anisotropic mechanical properties. Although polymorphism and structural transformation tendencies present fundamental challenges to stabilizing MBenes, both theoretical calculations and experimental investigations have unequivocally confirmed their potential as high-performance lithium-ion battery anodes. Theoretically, monolayer V2B2 MBene exhibits a high specific capacity of 968 mAh g-1 and a low Li + diffusion barrier of 0.22 eV, surpassing both MXene and graphene in these metrics. Experimentally, molten-salt derived MoxBy MBene delivers a reversible capacity of 638 mAh g-1 at 0.1 A g-1 with no capacity decay over 100 cycles, significantly outperforming exfoliated pristine Ti3C2 MXene and graphene nanosheets. Benefiting from the polycrystalline arrangement and polymorphic characteristics of their precursors, MBenes can be tailored into diverse chemical configurations (e.g., MB, M2B2, MB2, M4/3B2) by controlling the etching process, thus significantly expanding their structural diversity. The distinctive chemical structure of MBenes necessitates tailored etching strategies, which in turn leads to divergent electrochemical behaviors in their corresponding battery systems. Although some preliminary progress has been made in the field of MBenes, the research on it is still in the early stage. It is necessary to further explore the relationship between its structure and performance, develop innovative etching technology, and expand its application scenarios in the field of energy storage. This review systematically summarizes the research progress on MBene materials from a multidimensional perspective, covering their evolutionary history, structural classifications, etching-based synthesis strategies (e.g., acid/ base etching and molten salt assisted methods), and electrochemical performance in various battery systems (lithium/sodium-ion batteries and lithium-sulfur batteries). By conducting an in-depth analysis of their fundamental mechanisms and energy storage performance, this work establishes a comprehensive reference framework for the field and offers forward-looking guidance for future research on MBene-based energy storage technologies.

The stability and efficiency of direct seawater electrolysis are constrained by competitive Cl- adsorption and corresponding chlorine oxidation reaction, which further restricts diffusion and accumulation of OH-, as well as transfer of electrons involved in counterpart oxygen evolution reaction (OER), leading to severe Cl--corrosion. Herein, intensified popular-OH- accumulation and electron transfer are achieved through Ag-mediated reactive chlorine-resistant AgCl layer integrated onto NiCo-oxyhydroxide (AgCl/NiCo-OOH). Specifically, under external electric field driving, Ag species on the NiCo-OOH surface undergo electrochemical transformation and free Cl--immobilization via in situ formation of robust AgCl layer, subsequently leveraging common-ion repulsion effect to sieve and control composition of ions in Stern layer, and thereby preventing Cl- corrosion. Simultaneously, the AgCl with high-curvature induces electric fields across scales, incorporating mesoscale proximal-tip and microscale built-in electric fields, which significantly accelerates OER kinetics by intensifying diffusion and accumulation of reactant OH- and transfer of electron. Resultantly, the AgCl/NiCo-OOH achieves an ultralow overpotential of 331 mV in alkaline simulated seawater and sustains stable operation for over 2200 h at Ampere-level current density in alkaline seawater without Cl--related corrosion. Further, the corresponding anion-exchange membrane electrolyzer demonstrates a low energy consumption (4.50 kWh m-3 H2) and long-term durability (over 1500 h) at 500 mA cm-2.

ABSTRACT Direct seawater electrolysis offers a promising route for green hydrogen by utilizing marine resources and offshore renewables, but is hindered by chloride‐induced corrosion and poor catalyst durability. Herein, the Helmholtz plane microenvironment is reshaped by in situ MoO 4 2− release from a nickel‑molybdate precursor (Ni 0.36 Mo 0.64 ‐OH). The anions enrich within the Stern layer, forming a high‐concentration gradient of an anionic layer that electrostatically repels Cl − and prevents chloride‐corroded side reactions. Unlike the conventional strategy of bulk anion addition, this in situ self‐delivery approach bypasses long‐range diffusion and breaks mass‐transfer limitation, enabling rapid anion shielding via short‐range interfacial transport. Concurrently, the leaching of MoO 4 2− induces surface electronic redistribution that enhances Ni─O bond covalency, thereby triggering the lattice oxygen mechanism (LOM) for the oxygen evolution reaction (OER) while partially retaining the adsorbate evolution mechanism (AEM). The coexistence of two pathways ensures AEM‐induced structural stability and simultaneously enhances LOM‐dominated intrinsic activity. Consequently, the activated catalyst (A‐Ni 0.36 Mo 0.64 ‐OH) achieves low overpotentials (201 mV@10 mA cm −2 ; 560 mV@2 A cm −2 ) and long‑term stability (3500 h@250 mA cm −2 ) with negligible chlorine corrosion in alkaline seawater. This work presents an interfacial design that concurrently resists chloride corrosion and enhances OER activity by manipulating both ionic and electronic environments.

Activated carbon has aroused numerous research interest as electrode materials for supercapacitors because of its low cost, well-developed porosity, and large specific surface area. However, it usually suffers from low power output and inferior rate performance due to its inherently low electronic conductivity and sluggish ion dynamics in the micropores. Herein, three-dimensional N-doped hierarchical activated carbon materials (NHACs) are prepared from bituminous coal with well-defined porosity and optimized surface functional groups via KOHassisted one-step pyrolysis through tuning the KOH dosage. The NHAC3 sample obtained at a KOH/coal mass ratio of 3 achieves an exceptional specific surface area of 2292 m2 g- 1. The NHAC3-based symmetric supercapacitors display a high specific capacitance of 182 F g- 1 at 0.5 A g- 1 (based on the single electrode) and ultrafast charge-transfer kinetics with rate capability of 87.4% at 50 A g- 1 (159 F g- 1) in 1 mol L- 1 TEABF4/AN electrolyte, highly surpassing the commercial activated carbon (YP-50F, 118 F g- 1) and the coal-derived activated carbon reported previously. More impressively, it can deliver a high energy density of 39.4 Wh kg- 1 at 625 W kg- 1 and 34.4 Wh kg- 1 at 62.5 kW kg- 1. It also exhibits impressive cycling stability with 92.5% capacitance retention after 10,000 cycles, establishing a new benchmark for industrial-grade supercapacitors. This work provides a simple and cost-effective approach for the design and synthesis of high-performance coal-derived activated carbon for next generation supercapacitors.

For Li metal battery, Li metal anodes severely suffer from dendritic growth due to heterogeneous electrodeposition, which inhibits their development and application. While extensive studies for Li-dendrite suppression empirically utilize 3D hosts to homogenize the micro-scaled electric field within the host, the inherent correlation between host structure and electric field distribution and underlying principles remains elusive, and the corresponding design of hosts to enhance the electric effects remains challenging. Here, the host microstructure-electric field correlations are established via COMSOL simulations and demonstrate the enhanced redistribution of the electric field through structural redesign of hosts. Based on a structure model, an enhanced gradient electric field host (EGHx) with a supercontinuous gradient pore architecture is fabricated with the assistance of the porogen dissolution method, which achieves a self-leveling-like Li deposition through spatially programmed charge redistribution. Through further structural optimization, the EGH2 (with 2 wt% porogen) exhibits an similar to 98 % Coulombic efficiency (CE) over 350 cycles (1 mA cm-2, 1 mAh cm-2). Further multidimensional testing with argon protection reveals the role of the host in modulating solid-electrolyte interphase (SEI) composition. Accordingly, the EGH2 enables stable dendrite-free Li plating/stripping behaviors for 2100 h. The assembled full cell and pouch cell also display stable cycling performance with an LFP cathode. (c) 2025 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights are reserved, including those for text and data mining, AI training, and similar technologies.

Conventional SnO2 anodes exhibit immense potential for the electrocatalytic oxidation of organic wastewater. However, doping with toxic metals (e.g., Sb and Pb) is prone to causing secondary water pollution. To address this issue, a highly efficient and eco-friendly Sb-free Fe-SnO2/Ti anode was fabricated via a high-pressure spray-impregnation method for the electrocatalytic degradation of 2-(methylamino)benzoic acid (2-MBMA) in simulated wastewater. Structural characterizations confirmed the successful substitution of Sn4+ by Fe3+ in the crystal lattice, which increased the surface oxygen vacancy concentration from 13.2% to 24.1% and reduced the crystallite size. These structural optimizations effectively expanded the electrochemically active surface area (ECSA) and enhanced the charge transfer kinetics. Electrocatalytic performance evaluations demonstrated that at a current density of 10 mA cm-2, the Fe-SnO2/Ti anode achieved a 2-MBMA degradation efficiency of >90% and a chemical oxygen demand (COD) removal of 44.1% within 180 min. Notably, the electrocatalytic activity of the Fe-SnO2/Ti anode was highly comparable to that of the conventional Sb-SnO2/Ti electrode, while exhibiting superior anti-passivation durability under a high applied voltage of 5.0 V. Radical quenching experiments revealed that the degradation of pollutants in this system was predominantly governed by direct electron transfer and intense near-interface oxidation at the electrode surface, rather than by bulk free radical oxidation. Furthermore, the electrode maintained excellent electrocatalytic efficiency and crystal phase integrity after 20 consecutive degradation cycles. This study provides a highly competitive and viable strategy for the design of durable and non-toxic anodes for organic wastewater treatment.

Localized "water-in-salt" (LWIS) electrolytes featuring low viscosity offer a promise for high-voltage supercapacitors with rapid charge/discharge capability. However, the electrochemical performances of LWIS electrolytes rely heavily on the selection of the diluent. By screening 20 organic solvents, 1,3-dioxolane (1,3-DX) that featuring low viscosity and weak interactions with H2O, is identified as an optimal spacer/diluent, which refines the electrolyte coordination structure through the formation of interconnected yet dynamic networks to dissipate dense crosslinked cation-anion-water clusters into loose isolated ones, triggering a spacial redistribution that alleviates ionic crowding while preserving the essential Na+-ClO4 --H2O coordination structure. This molecule-scale design endows the resulting 8 mol kg-1 LWIS electrolyte with a high output voltage of 2.8 V in an asymmetric supercapacitor, low viscosity (7.33 mPa s), and a remarkable 1,622-fold enhancement in ion diffusion coefficient at 25 degrees C compared to the conventional 17 m WIS electrolyte. Accordingly, the electrolyte endows symmetric supercapacitors with exceptional charge-discharge kinetics, reliable operation at -30 degrees C, and robust cycling stability over 150 000 cycles. Our work presents a foundational guideline for diluent selection in advanced LWIS electrolytes, paving the way for aqueous supercapacitors that deliver concurrently high energy and power density.

Furan derivatives, including 2,5-diformylfuran (DFF) and 2,5-furandicarboxylic acid (FDCA), are platform molecules for renewable plastics and fine chemicals. However, due to mismatched reaction kinetics and thermodynamics, a sustainable process for the co-synthesis of DFF and FDCA from 5-hydroxymethylfurfural (HMF) is highly desirable and urgently required, being challengeable. Here we firstly proposed a bifunctional aqueous/non-aqueous system for the efficient co-synthesis of DFF and FDCA, and further identified the biphasic bifunctionality as well as interfacial catalysis mechanism at multiple scales. Simultaneously, an integrated multi-unit process was presented and developed, where the hydrogen bond network and molecular spatial orientations at the 7.5 Å-thick aqueous/non-aqueous interface facilitate products formation and transport, overcoming kinetic and thermodynamic limitations to achieve high mole fractions of DFF (98.0%) in the non-aqueous phase and FDCA (94.0%) in the aqueous phase. Additionally, this system enables efficient recycling of non-aqueous solvent and catalysts, with recovery rates of 85.0% and 95.0%, and increases the total yields of DFF and FDCA by 2.2 and 3.3 times compared to traditional non-aqueous and aqueous systems, respectively. Moreover, this double-duty system shows broad universality and performs well at industrial substrate concentrations (800mmol L−1). The bifunctional aqueous/non-aqueous system will be of potential in value-added chemical synthesis, especially for special reaction process with mismatched kinetics and thermodynamics.

Herein, a hierarchical heterostructure of Mo3N2-MoO2@Mo2C MXene (MNO@MX) with strongly coupled interfaces was innovatively constructed using Mo2C MXene as a precursor via an in-situ ammoniation method, nitrogen-rich Mo3N2 and oxygen-rich MoO2 phases were simultaneously generated on the MXene surface, forming a heterointerface. Lithium-sulfur (Li-S) batteries based on S/MNO@MX electrode demonstrate a stabilized capacity of 1019 mAh g-1 after 1000 cycles at 1C with an average capacity decay rates of 0.022 %, demonstrating excellent cyclic stability. Besides, the S/MNO@MX electrode shows a stable capacity of 623 mAh g-1 under 0.5C after 100 cycles at 60 degrees C and delivers a stabilized capacity of 490 mAh g-1 under 0.5C after 100 cycles at-20 degrees C, exhibiting improved low-temperature tolerance and superior reversible capacities in a wide temperature ranges. Density functional theory (DFT) calculations indicated that the strong electronic coupling between MoO2 and Mo3N2 substantially increases the density of states and intensifies the built-in electric field (BIEF) strength. MNO@MX heterostructure leverages a "Heterointerface-BIEF-Confinement space" trinity synergistic mechanism. The strong polar adsorption of MoO2 and fast catalytic conversion ability of Mo3N2 for polysulfides collaboratively suppress the polysulfide shuttle effect, while the work function difference between the two phases induces interfacial charge rearrangement to establish a BIEF, significantly enhancing the catalytic activity. Concurrently, the MXene framework provides continuous channels for electron/ion transport. This work offers an innovative strategy of interfacial engineering and multi-mechanism synergy for developing highperformance lithium-sulfur batteries.

The growing demand for high-energy-density power sources driven by smart devices has positioned Li metal anodes as a focal point of research. However, the practical application was hindered by uncontrolled Li dendrite growth and interfacial instability. Achieving simultaneous morphological control of Li metal and robust electrode-electrolyte interphase stability remained a critical challenge to be addressed. Here, a carbon host with long-range ordered groove microchannels was fabricated by a flow field-driven technique, and the surface was functionalized with a nanoscale LiF and LiBO2 coating. The long-range groove channels concentrated the electric field within their confines, thereby promoting uniform Li deposition. Simultaneously, the engineered interface promoted the formation of an inorganic-rich solid electrolyte interphase (SEI) dominated by LiF and LiBO2. The synergy between ‘structure-guided deposition’ and ‘interfacial encapsulation’ function enabled stable Li metal anodes, which achieved over 2150 h of cycling in Li@CH-BF0.05||Li symmetric cells and maintained a coulombic efficiency of ∼ 98 % over 200 cycles in half-cells at 1 mA/cm2 and 1 mAh/cm2. This study demonstrated that coupling structural engineering with designed interface chemistry is an effective strategy for achieving stable long-cycle-life Li metal batteries.

Porous carbon materials (PCMs) have emerged as key players in energy storage and environmental remediation thanks to their highly tunable pore structure parameters. However, traditional empirical approaches for optimizing these parameters are time-consuming and resource-intensive. Herein, a workflow is introduced that integrates machine learning-assisted pore parameters prediction with experimental validation for PCMs, thereby facilitating the identification of candidate PCMs for different application requirements. Coal-based activated carbon (CAC) is first employed to validate the effectiveness of this workflow, given its high tunability and extensive application potential. During the validation process, machine learning models are developed to establish a predictive map linking precursor and preparation parameters to the resulting specific surface area and total pore volume. The proposed strategy for CAC is applied to the design of a high-performance supercapacitor electrode (specific capacitance of 491.2 F g-1 at 0.1 A g-1) and a methylene blue adsorbent (adsorption capacity of 2196.8 mg g-1 at room temperature), demonstrating its effectiveness. Furthermore, the workflow is extended to coal tar pitch-based carbon materials, a more complex system, and demonstrates encouraging outcomes. This work extends the strategies for controlling pore structure parameters of CAC and provides a transferable workflow for exploring other PCMs.

2D Ti3C2Tx MXenes are of great potential in catalysis, energy storage, and conversion, yet the controlled tuning of their structure, intrinsic activity, and stability remains a challenge. Herein, we address this challenge through a dual-modification strategy, synthesizing a Cl-terminated MXene/MAX (Ti3C2Clx/Ti3ZnC2) heterostructure by a dynamic etching approach for efficient electrocatalytic nitrogen reduction reaction (NRR). This catalyst achieves an NH3 yield of 20.1 µg h-1 mg-1 and a Faradaic efficiency of 38.1% at -0.2 V vs. RHE in 0.1 m KOH electrolyte, with high stability for over 70 h, positioning it among the top-performing MXene-based NRR electrocatalysts. Experimental and theoretical analyses demonstrate that the Ti3C2Clx/Ti3ZnC2 heterostructure modulates the electronic structure of Ti sites, thus optimizing the intermediate adsorption and reducing the energy barrier of *NH2 → NH3 conversion in the distal pathway to 0.7 eV. The Zn-N2 battery assembled with Ti3C2Clx/Ti3ZnC2 can reach a peak power density of 36.5 µW cm-2, with an NH3 yield of 13.1 µg h-1 mg-1. This study has demonstrated that the dual modification strategy involving surface terminations regulation and heterostructure construction is effective to improve both NRR activity and stability of MXene-based electrocatalysts, which is crucial for efficient NH3 production and energy generation. This improvement paves the way for efficient ammonia and energy co-generation, providing a viable materials design strategy and deeper mechanistic insights.

ABSTRACT Efficient ion desolvation and rapid mass transport are crucial yet often competing requirements for stabilizing Zn anodes in aqueous Zn‐ion batteries. This dilemma arises because ion desolvation introduces additional energy barriers that increase ion diffusion resistance. To reconcile this inherent trade‐off, a hydrogen‐bonded organic framework (HOF) based on C 3 ‑symmetric trigonal carboxyl ligands is engineered as an ion‐sieving interface. This design integrates precise pore size control with tailored chemical environment to regulate Zn 2+ desolvation behavior. As expected, the flexible HOF incorporating an electron‐deficient triazine core (HOF‐TAT) dynamically strips solvated water molecules while maintaining continuous ion flux. This process fosters a gradient solid electrolyte interphase that synergizes with the self‐adaptive porous framework to guide dense (101)‐oriented Zn deposition. The HOF‐TAT@Zn symmetric cells stably cycle exceeding 3400 h at 5 mA cm −2 . Furthermore, the iodophilic porous framework immobilizes shuttling polyiodides through strong physicochemical interactions. When integrated with an ultrathin Zn anode (10 µm), the Zn‐iodine batteries deliver a high‐rate capacity (142.2 mAh g −1 at 5 A g −1 ) and long‐term lifetime (50 000 cycles). This work offers an intelligent strategy to concurrently overcome the high energy barriers of ion desolvation and the kinetic limitations of ion transport for building advanced electrochemical devices.