Air-Stable High-Entropy Layered Oxide Cathode with Enhanced Cycling Stability for Sodium-Ion Batteries.

O3-type layered oxides have been extensively studied as cathode materials for sodium-ion batteries due to their high reversible capacity and high initial sodium content, but they suffer from complex phase transitions and an unstable structure during sodium intercalation/deintercalation. Herein, we synthesize a high-entropy O3-type layered transition metal oxide, NaNi0.3Cu0.05Fe0.1Mn0.3Mg0.05Ti0.2O2 (NCFMMT), by simultaneously doping Cu, Mg, and Ti into its transition metal layers, which greatly increase structural entropy, thereby reducing formation energy and enhancing structural stability. The high-entropy NCFMMT cathode exhibits significantly improved cycling stability (capacity retention of 81.4% at 1C after 250 cycles and 86.8% at 5C after 500 cycles) compared to pristine NaNi0.3Fe0.4Mn0.3O2 (71% after 100 cycles at 1C), as well as remarkable air stability. Finally, the NCFMMT//hard carbon full-cell batteries deliver a high initial capacity of 103 mAh g-1 at 1C, with 83.8 mAh g-1 maintained after 300 cycles (capacity retention of 81.4%).

In-Situ Polymerized High-Voltage Solid-State Lithium Metal Batteries with Dual-Reinforced Stable Interfaces.

Solid polymer electrolytes (SPEs) represent a pivotal advance toward high-energy solid-state lithium metal batteries. However, inadequate interfacial contact remains a significant bottleneck, impeding scalability and application. Inadequate interfacial contact remains a significant bottleneck, impeding scalability and application. Recent efforts have focused on transforming liquid/solid interfaces into solid/solid ones through in situ polymerization, which shows potential especially in reducing interface impedance. Here, we designed high-voltage SSLMBs with dual-reinforced stable interfaces by combining interface modification with an in situ polymerization technology inspired by targeted effects in medicine. Theoretical calculations and time-of-flight secondary ion mass spectrometry (TOF-SIMS) analysis demonstrate that tetramethylene sulfone (TMS) and bis(2,2,2-trifluoromethyl) carbonate (TFEC) exhibit selective adsorption at the interface of the LiNi0.8Co0.1Mn0.1O2 (NCM) cathode and Li anode, respectively. These compounds further decompose to form a stable cathode-electrolyte interface (CEI) film and a solid electrolyte interface (SEI) film, thereby simultaneously achieving a superior interface between the SPE and both the Li anode and NCM cathode. The developed Li||SPE||Li cell sustained cycling for more than 1000 h at 0.3 mA cm-2, and the NCM||SPE||Li cell also demonstrated an excellent capacity retention of 86.8% after 1000 cycles at 1 °C. This work will provide valuable insights for the rational design of high-voltage SSLMBs with stable interfaces, leveraging in situ polymerization as a cornerstone technology.

Phosphorous and Nitrogen Dual-Doped Carbon as a Highly Efficient Electrocatalyst for Sodium-Oxygen Batteries.

Sodium-oxygen batteries have been regarded as promising energy storage devices due to their low overpotential and high energy density. Its applications, however, still face formidable challenges due to the lack of understanding about the influence of electrocatalysts on the discharge products. Here, a phosphorous and nitrogen dual-doped carbon (PNDC) based cathode is synthesized to increase the electrocatalytic activity and to stabilize the NaO2 superoxide nanoparticle discharge products, leading to enhanced cycling stability when compared to the nitrogen-doped carbon (NDC). The PNDC air cathode exhibits a low overpotential (0.36 V) and long cycling stability (120 cycles). The reversible formation/decomposition and stabilization of the NaO2 discharge products are clearly proven by in-situ synchrotron X-ray diffraction and ex-situ X-ray diffraction. Based on the density functional theory calculation, the PNDC has much stronger adsorption energy (-2.85 eV) for NaO2 than that of NDC (-1.80 eV), which could efficiently stabilize the NaO2 discharge products.

A bio-based functional separator enables dendrite-free anodes in aqueous zinc-ion batteries.

Aqueous zinc-ion batteries (AZIBs) have garnered considerable interest as potential solutions for large-scale energy storage systems, owing to their cost-effectiveness and high safety. Nonetheless, the development of AZIBs is hindered by significant challenges associated with dendrite growth and side reactions on Zn anodes. Here, a bio-based separator derived from cellulose was developed for the dendrite-free anode in AZIBs. In addition, the separator is notable for its ultra-low cost and biodegradability in contrast to the commonly used commercial glass fiber (GF) separators. The mechanical strength of the separator is enhanced by the cross-linking of hydrogen bonds, effectively inhibiting dendrite growth. The zinc-philic groups facilitate better binding to Zn2+, resulting in uniform nucleation and deposition. The hydrophilic groups aid in trapping water molecules, thereby preventing side reactions of the electrolyte. The Zn||Zn symmetric cell with this separator can sustain a long cycle life for over 800 h, indicating stable Zn2 + plating and stripping with suppressed dendrite growth. Concurrently, the assembled Zn||VO2 full batteries exhibited a capacity retention rate of 61.87% after 1,000 cycles at 1 A g-1 with an initial capacity of 140 mAh g-1. This work highlights a stable, economical, and eco-friendly approach to the design of bio-based separators in AZIBs for sustainable energy storage systems.

Regulation of Interface Ion Transport by Electron Ionic Conductor Construction toward High-Voltage and High-Rate LiNi0.5Co0.2Mn0.3O2 Cathodes in Lithium Ion Battery.

Simultaneously achieving high-energy-density and high-power-density is a crucial yet challenging objective in the pursuit of commercialized power batteries. In this study, atomic layer deposition (ALD) is employed combined with a coordinated thermal treatment strategy to construct a densely packed, electron-ion dual conductor (EIC) protective coating on the surface of commercial LiNi0.5Co0.2Mn0.3O2 (NCM523) cathode material, further enhanced by gradient Al doping (Al@EIC-NCM523). The ultra-thin EIC effectively suppresses side reactions, thereby enhancing the stability of the cathode-electrolyte interphase (CEI) at high-voltages. The EIC's dual conduction capability provides a potent driving force for Li+ transport at the interface, promoting the formation of rapid ion deintercalation pathways within the Al@EIC-NCM523 bulk phase. Moreover, the strategic gradient doping of Al serves to anchor the atomic spacing of Ni and O within the structure of Al@EIC-NCM523, curbing irreversible phase transitions at high-voltages and preserving the integrity of its layered structure. Remarkably, Al@EIC-NCM523 displays an unprecedented rate capability (114.7 mAh g-1 at 20 C), and a sustained cycling performance (capacity retention of 74.72% after 800 cycles at 10 C) at 4.6 V. These findings demonstrate that the proposed EIC and doping strategy holds a significant promise for developing high-energy-density and high-power-density lithium-ion batteries (LIBs).

Scalable Precise Nanofilm Coating and Gradient Al Doping Enable Stable Battery Cycling of LiCoO2 at 4.7†V.

The quest for smart electronics with higher energy densities has intensified the development of high-voltage LiCoO2 (LCO). Despite their potential, LCO materials operating at 4.7 V faces critical challenges, including interface degradation and structural collapse. Herein, we propose a collective surface architecture through precise nanofilm coating and doping that combines an ultra-thin LiAlO2 coating layer and gradient doping of Al. This architecture not only mitigates side reactions, but also improves the Li+ migration kinetics on the LCO surface. Meanwhile, gradient doping of Al inhibited the severe lattice distortion caused by the irreversible phase transition of O3-H1-3-O1, thereby enhanced the electrochemical stability of LCO during 4.7 V cycling. DFT calculations further revealed that our approach significantly boosts the electronic conductivity. As a result, the modified LCO exhibited an outstanding reversible capacity of 230 mAh g-1 at 4.7 V, which is approximately 28 % higher than the conventional capacity at 4.5 V. To demonstrate their practical application, our cathode structure shows improved stability in full pouch cell configuration under high operating voltage. LCO exhibited an excellent cycling stability, retaining 82.33 % after 1000 cycles at 4.5 V. This multifunctional surface modification strategy offers a viable pathway for the practical application of LCO materials, setting a new standard for the development of high-energy-density and long-lasting electrode materials.

Electric Double Layer Regulator Design through a Functional Group Assembly Strategy towards Long-Lasting Zinc Metal Batteries.

Regulating the electric double layer (EDL) structure of the zinc metal anode by using electrolyte additives is an efficient way to suppress interface side reactions and facilitate uniform zinc deposition. Nevertheless, there are no reports investigating the proactive design of EDL-regulating additives before the start of experiments. Herein, a functional group assembly strategy is proposed to design electrolyte additives for modulating the EDL, thereby realizing a long-lasting zinc metal anode. Specifically, by screening ten common functional groups, N, N-dimethyl-1H-imidazole-1-sulfonamide (IS) is designed by assembling an imidazole group, characterized by its high adsorption capability on the zinc anode, and a sulfone group, which exhibits strong binding with Zn2+ ions. Benefiting from the adsorption functionalization of the imidazole group, the IS molecules occupy the position of H2O in the inner Helmholtz layer of the EDL, forming a molecular protective layer to inhibit H2O-induced side reactions. Meanwhile, the sulfone group in IS, acting as a binding site to Zn2+, promotes the de-solvation of Zn2+ ions, facilitating compact zinc deposition. Consequently, the utilization of IS significantly extending the cycling stability of Zn||Zn and Zn||NaV3O8 ⋅ 1.5H2O full cell. This study offers an innovative approach to the design of EDL regulators for high-performance zinc metal batteries.

Development and validation of a clinical prediction model for ischemic stroke recurrence after successful stent implantation in symptomatic intracranial atherosclerotic stenosis.

OBJECTIVE: This study aimed to analyze the risk factors for recurrent ischemic stroke in patients with symptomatic intracranial atherosclerotic stenosis (ICAS) who underwent successful stent placement and to establish a nomogram prediction model. METHODS: We utilized data from a prospective collection of 430 consecutive patients at Jining NO.1 People's Hospital from November 2021 to November 2022, conducting further analysis on the subset of 400 patients who met the inclusion criteria. They were further divided into training (n=321) and validation (n=79) groups. In the training group, we used univariate and multivariate COX regression to find independent risk factors for recurrent stroke and then created a nomogram. The assessment of the nomogram's discrimination and calibration was performed through the examination of various measures including the Consistency index (C-index), the area under the receiver operating characteristic (ROC) curves (AUC), and the calibration plots. Decision curve analysis (DCA) was used to evaluate the clinical utility of the nomogram by quantifying the net benefit to the patient under different threshold probabilities. RESULTS: The nomogram for predicting recurrent ischemic stroke in symptomatic ICAS patients after stent placement utilizes six variables: coronary heart disease (CHD), smoking, multiple ICAS, systolic blood pressure (SBP), in-stent restenosis (ISR), and fasting plasma glucose. The C-index (0.884 for the training cohort and 0.87 for the validation cohort) and the time-dependent AUC (>0.7) indicated satisfactory discriminative ability of the nomogram. Furthermore, DCA indicated a clinical net benefit from the nomogram. CONCLUSIONS: The predictive model constructed includes six predictive factors: CHD, smoking, multiple ICAS, SBP, ISR and fasting blood glucose. The model demonstrates good predictive ability and can be utilized to predict ischemic stroke recurrence in patients with symptomatic ICAS after successful stent placement.

Understanding the charge transfer effects of single atoms for boosting the performance of Na-S batteries.

The effective flow of electrons through bulk electrodes is crucial for achieving high-performance batteries, although the poor conductivity of homocyclic sulfur molecules results in high barriers against the passage of electrons through electrode structures. This phenomenon causes incomplete reactions and the formation of metastable products. To enhance the performance of the electrode, it is important to place substitutable electrification units to accelerate the cleavage of sulfur molecules and increase the selectivity of stable products during charging and discharging. Herein, we develop a single-atom-charging strategy to address the electron transport issues in bulk sulfur electrodes. The establishment of the synergistic interaction between the adsorption model and electronic transfer helps us achieve a high level of selectivity towards the desirable short-chain sodium polysulfides during the practical battery test. These finding indicates that the atomic manganese sites have an enhanced ability to capture and donate electrons. Additionally, the charge transfer process facilitates the rearrangement of sodium ions, thereby accelerating the kinetics of the sodium ions through the electrostatic force. These combined effects improve pathway selectivity and conversion to stable products during the redox process, leading to superior electrochemical performance for room temperature sodium-sulfur batteries.

A Critical Review on Room-Temperature Sodium-Sulfur Batteries: From Research Advances to Practical Perspectives.

Room-temperature sodium-sulfur (RT-Na/S) batteries are promising alternatives for next-generation energy storage systems with high energy density and high power density. However, some notorious issues are hampering the practical application of RT-Na/S batteries. Besides, the working mechanism of RT-Na/S batteries under practical conditions such as high sulfur loading, lean electrolyte, and low capacity ratio between the negative and positive electrode (N/P ratio), is of essential importance for practical applications, yet the significance of these parameters has long been disregarded. Herein, it is comprehensively reviewed recent advances on Na metal anode, S cathode, electrolyte, and separator engineering for RT-Na/S batteries. The discrepancies between laboratory research and practical conditions are elaborately discussed, endeavors toward practical applications are highlighted, and suggestions for the practical values of the crucial parameters are rationally proposed. Furthermore, an empirical equation to estimate the actual energy density of RT-Na/S pouch cells under practical conditions is rationally proposed for the first time, making it possible to evaluate the gravimetric energy density of the cells under practical conditions. This review aims to reemphasize the vital importance of the crucial parameters for RT-Na/S batteries to bridge the gaps between laboratory research and practical applications.

Routes to high-performance layered oxide cathodes for sodium-ion batteries.

Sodium-ion batteries (SIBs) are experiencing a large-scale renaissance to supplement or replace expensive lithium-ion batteries (LIBs) and low energy density lead-acid batteries in electrical energy storage systems and other applications. In this case, layered oxide materials have become one of the most popular cathode candidates for SIBs because of their low cost and comparatively facile synthesis method. However, the intrinsic shortcomings of layered oxide cathodes, which severely limit their commercialization process, urgently need to be addressed. In this review, inherent challenges associated with layered oxide cathodes for SIBs, such as their irreversible multiphase transition, poor air stability, and low energy density, are systematically summarized and discussed, together with strategies to overcome these dilemmas through bulk phase modulation, surface/interface modification, functional structure manipulation, and cationic and anionic redox optimization. Emphasis is placed on investigating variations in the chemical composition and structural configuration of layered oxide cathodes and how they affect the electrochemical behavior of the cathodes to illustrate how these issues can be addressed. The summary of failure mechanisms and corresponding modification strategies of layered oxide cathodes presented herein provides a valuable reference for scientific and practical issues related to the development of SIBs.

Advancements in aqueous zinc-iodine batteries: a review.

Aqueous zinc-iodine batteries stand out as highly promising energy storage systems owing to the abundance of resources and non-combustible nature of water coupled with their high theoretical capacity. Nevertheless, the development of aqueous zinc-iodine batteries has been impeded by persistent challenges associated with iodine cathodes and Zn anodes. Key obstacles include the shuttle effect of polyiodine and the sluggish kinetics of cathodes, dendrite formation, the hydrogen evolution reaction (HER), and the corrosion and passivation of anodes. Numerous strategies aimed at addressing these issues have been developed, including compositing with carbon materials, using additives, and surface modification. This review provides a recent update on various strategies and perspectives for the development of aqueous zinc-iodine batteries, with a particular emphasis on the regulation of I2 cathodes and Zn anodes, electrolyte formulation, and separator modification. Expanding upon current achievements, future initiatives for the development of aqueous zinc-iodine batteries are proposed, with the aim of advancing their commercial viability.

Linearly Interlinked Fe-Nx-Fe Single Atoms Catalyze High-Rate Sodium-Sulfur Batteries.

Linearly interlinked single atoms offer unprecedented physiochemical properties, but their synthesis for practical applications still poses significant challenges. Herein, linearly interlinked iron single-atom catalysts that are loaded onto interconnected carbon channels as cathodic sulfur hosts for room-temperature sodium-sulfur batteries are presented. The interlinked iron single-atom exhibits unique metallic iron bonds that facilitate the transfer of electrons to the sulfur cathode, thereby accelerating the reaction kinetics. Additionally, the columnated and interlinked carbon channels ensure rapid Na+ diffusion kinetics to support high-rate battery reactions. By combining the iron atomic chains and the topological carbon channels, the resulting sulfur cathodes demonstrate effective high-rate conversion performance while maintaining excellent stability. Remarkably, even after 5000 cycles at a current density of 10 A g-1, the Na-S battery retains a capacity of 325 mAh g-1. This work can open a new avenue in the design of catalysts and carbon ionic channels, paving the way to achieve sustainable and high-performance energy devices.

Lithium-Ion Charged Polymer Channels Flattening Lithium Metal Anode.

The concentration difference in the near-surface region of lithium metal is the main cause of lithium dendrite growth. Resolving this issue will be key to achieving high-performance lithium metal batteries (LMBs). Herein, we construct a lithium nitrate (LiNO3)-implanted electroactive ß phase polyvinylidene fluoride-co-hexafluoropropylene (PVDF-HFP) crystalline polymorph layer (PHL). The electronegatively charged polymer chains attain lithium ions on the surface to form lithium-ion charged channels. These channels act as reservoirs to sustainably release Li ions to recompense the ionic flux of electrolytes, decreasing the growth of lithium dendrites. The stretched molecular channels can also accelerate the transport of Li ions. The combined effects enable a high Coulombic efficiency of 97.0% for 250 cycles in lithium (Li)||copper (Cu) cell and a stable symmetric plating/stripping behavior over 2000 h at 3 mA cm-2 with ultrahigh Li utilization of 50%. Furthermore, the full cell coupled with PHL-Cu@Li anode and LiFePO4 cathode exhibits long-term cycle stability with high-capacity retention of 95.9% after 900 cycles. Impressively, the full cell paired with LiNi0.87Co0.1Mn0.03O2 maintains a discharge capacity of 170.0 mAh g-1 with a capacity retention of 84.3% after 100 cycles even under harsh condition of ultralow N/P ratio of 0.83. This facile strategy will widen the potential application of LiNO3 in ester-based electrolyte for practical high-voltage LMBs.

Multifunctional Separator Enables High-Performance Sodium Metal Batteries in Carbonate-Based Electrolytes.

Sodium metal has become one of the most promising anodes for next-generation cheap and high-energy-density metal batteries; however, challenges caused by the uncontrollable sodium dendrite growth and fragile solid electrolyte interphase (SEI) restrict their large-scale practical applications in low-cost and wide-voltage-window carbonate electrolytes. Herein, a novel multifunctional separator with lightweight and high thinness is proposed, assembled by the cobalt-based metal-organic framework nanowires (Co-NWS), to replace the widely applied thick and heavy glass fiber separator. Benefitting from its abundant sodiophilic functional groups and densely stacked nanowires, Co-NWS not only exhibits outstanding electrolyte wettability and effectively induces uniform Na+ ion flux as a strong ion redistributor but also favors constructing the robust N,F-rich SEI layer. Satisfactorily, with 10 µL carbonate electrolyte, a Na|Co-NWS|Cu half-cell delivers stable cycling (over 260 cycles) with a high average Coulombic efficiency of 98%, and the symmetric cell shows a long cycle life of more than 500 h. Remarkably, the full cell shows a long-term life span (over 1500 cycles with 92% capacity retention) at high current density in the carbonate electrolyte. This work opens up a strategy for developing dendrite-free, low-cost, and long-life-span sodium metal batteries in carbonate-based electrolytes.

Unobtrusive Refractive Power Monitoring: Using EOG to Detect Blurred Vision.

The rise in population and aging has led to a significant increase in the number of individuals affected by common causes of vision loss. Early diagnosis and treatment are crucial to avoid the consequences of visual impairment. However, in early stages, many visual problems are making it difficult to detect. Visual adaptation can compensate for several visual deficits with adaptive eye movements. These adaptive eye movements may serve as indicators of vision loss. In this work, we investigate the association between eye movement and blurred vision. By using Electrooculography (EOG) to record eye movements, we propose a new tracking model to identify the deterioration of refractive power. We verify the technical feasibility of this method by designing a blurred vision simulation experiment. Six sets of prescription lenses and a pair of flat lenses were used to create different levels of blurring effects. We analyzed binocular movements through EOG signals and performed a seven-class classification using the ResNet18 architecture. The results revealed an average classification accuracy of 94.7% in the subject-dependent model. However, the subject-independent model presented poor performance, with the highest accuracy reaching only 34.5%. Therefore, the potential of an EOG-based visual quality monitoring system is proven. Furthermore, our experimental design provides a novel approach to assessing blurred vision.

Soft-Rigid Heterostructures with Functional Cation Vacancies for Fast-Charging and High-Capacity Sodium Storage.

Optimizing charge transfer and alleviating volume expansion in electrode materials are critical to maximize electrochemical performance for energy-storage systems. Herein, an atomically thin soft-rigid Co9 S8 @MoS2 core-shell heterostructure with dual cation vacancies at the atomic interface is constructed as a promising anode for high-performance sodium-ion batteries. The dual cation vacancies involving VCo and VMo in the heterostructure and the soft MoS2 shell afford ionic pathways for rapid charge transfer, as well as the rigid Co9 S8 core acting as the dominant active component and resisting structural deformation during charge-discharge. Electrochemical testing and theoretical calculations demonstrate both excellent Na+ -transfer kinetics and pseudocapacitive behavior. Consequently, the soft-rigid heterostructure delivers extraordinary sodium-storage performance (389.7 mA h g-1 after 500 cycles at 5.0 A g-1 ), superior to those of the single-phase counterparts: the assembled Na3 V2 (PO4 )3 ||d-Co9 S8 @MoS2 /S-Gr full cell achieves an energy density of 235.5 Wh kg-1 at 0.5 C. This finding opens up a unique strategy of soft-rigid heterostructure and broadens the horizons of material design in energy storage and conversion.

Recent Advances in Structural Optimization and Surface Modification on Current Collectors for High-Performance Zinc Anode: Principles, Strategies, and Challenges.

The last several years have witnessed the prosperous development of zinc-ion batteries (ZIBs), which are considered as a promising competitor of energy storage systems thanks to their low cost and high safety. However, the reversibility and availability of this system are blighted by problems such as uncontrollable dendritic growth, hydrogen evolution, and corrosion passivation on anode side. A functionally and structurally well-designed anode current collectors (CCs) is believed as a viable solution for those problems, with a lack of summarization according to its working mechanisms. Herein, this review focuses on the challenges of zinc anode and the mechanisms of modified anode CCs, which can be divided into zincophilic modification, structural design, and steering the preferred crystal facet orientation. The possible prospects and directions on zinc anode research and design are proposed at the end to hopefully promote the practical application of ZIBs.

Reactive boride as a multifunctional interface stabilizer for garnet-type solid electrolyte in all-solid-state lithium batteries.

All-solid-state batteries are one of the most important game changers in electrochemical energy storage since they are free from the risk of leakage of hazardous flammable liquid solvents. Among the various types of solid-state electrolytes, Li7-xLa3Zr2-xTaxO12 garnets possess many desirable advantages to be considered a suitable candidate for lithium-ion batteries. However, their practical application has been hindered by premature short-circuits due to lithium dendrite growth, nonnegligible electronic conductivity and interfacial air sensitivity issues. Herein, we propose a multifunctional layer strategy to simultaneously address both the interface and electronic conductivity issues. With the help of a facile chemical process based on reactive cobalt boride, electron leakage was effectively blocked and the electrochemical performance/stability could be well maintained over extended cycles. The cobalt boride-coating layer also possessed an impressive Li metal wetting ability while sustaining a low interfacial resistance. A full cell paired with a commercialized cathode showed satisfactory performance with low overpotentials and a high specific capacity over 150 mA h g-1. Moreover, first-principle calculations further revealed the status of the rearrangement of the electron cloud behind the charge-density difference, and the nature of the low diffusion energy barrier of the reactive cobalt boride protective layer. Our strategy highlights the necessity of designing proper multifunctional layers in the garnet-type solid-state lithium-ion battery system.

Key Roles of Interfacial OH- ion Distribution on Proton Coupled Electron Transfer Kinetics Toward Urea Oxidation Reaction.

Enhancing alkaline urea oxidation reaction (UOR) activity is essential to upgrade renewable electrolysis systems. As a core step of UOR, proton-coupled electron transfer (PCET) determines the overall performance, and accelerating its kinetic remains a challenge. In this work, a newly raised electrocatalyst of NiCoMoCuOx Hy with derived multi-metal co-doping (oxy)hydroxide species during electrochemical oxidation states is reported, which ensures considerable alkaline UOR activity (10/500 mA cm-2 at 1.32/1.52 V vs RHE, respectively). Impressively, comprehensive studies elucidate the correlation between the electrode-electrolyte interfacial microenvironment and the electrocatalytic urea oxidation behavior. Specifically, NiCoMoCuOx Hy featured with dendritic nanostructure creates a strengthened electric field distribution. This structural factor prompts the local OH- enrichment in electrical double layer (EDL), so that the dehydrogenative oxidation of the catalyst is directly reinforced to facilitate the subsequent PCET kinetics of nucleophilic urea, resulting in high UOR performance. In practical utilization, NiCoMoCuOx Hy -driven UOR coupled cathodic hydrogen evolution reaction (HER) and carbon dioxide reduction reaction (CO2 RR), and harvested high value-added products of H2 and C2 H4 , respectively. This work clarifies a novel mechanism to improve electrocatalytic UOR performance through structure-induced interfacial microenvironment modulation.