Electrochemical Properties Research Articles

Influence of rare earth second phases on the salt spray corrosion and electrochemical corrosion properties of FeCrAl-Gd-Sc alloys

FeCrAl alloys have excellent oxidation and corrosion resistance and have been widely used in cladding materials and structural components. In this study, Fe-21Cr-4Al-xGd-xSc (x=0, 0.5, 1, 2 wt%) alloys were prepared by the vacuum hot press sintering method. The corrosion properties of the Fe-21Cr-4Al-xSc-xGd alloy have been investigated by salt spray and electrochemical corrosion methods. The results show that Sc and Gd doped FeCrAl alloys form nanoscale cubic phase ScAlO3, Gd monomer and intermetallic compounds between Gd and Fe as the second phase. The Sc and Gd doped FeCrAl alloy forms a corrosion film on the surface during the corrosion process. It can effectively hinder the erosion of corrosive ions on the alloy, thus improving the corrosion resistance of the FeCrAl alloy. The second phase (Gd monomer, Fe5Gd, Fe9Gd, ScAlO3) effectively prevents micro galvanic corrosion of inclusions when the addition of Sc and Gd is less than 1 wt%. When the content of Sc and Gd reaches 2 wt%, the role of the second phase tends to accelerate the corrosion of the alloy by acting as the cathode of micro galvanic corrosion. Therefore, FeCrAl-1wt%Sc-1wt%Gd alloy has a better corrosion resistance, and the corrosion rate is only 1.37 mm/year.

Comprehensive insight of charge storage and ion transport in bioinspired nanostructure electrode-patterned supercapacitors by multiscale investigation

Supercapacitors with bioinspired leaves-on-branchlet hybrid carbon nanostructure-patterned electrodes show high areal capacitance and outstanding rate capability. However, the fundamental mechanisms of charge storage and ion transport in such a bioinspired supercapacitor at multiple length scales remain little explored. Herein, we develop a multi-scale model to comprehensively explore the mechanism of charge storage and ion transport, in which the finite-element-based Nernst-Planck-Poisson calculations are used for the macro-scale understanding, and molecular dynamics simulations for the atomic-scale investigation. High-throughput simulations are conducted to quantify the effect of the bioinspired structure, thermal influence, and size effect on the electrochemical performance of supercapacitors. An in-depth analysis of the simulation and experimental results demo some design advice are concluded, (1) engineering the hierarchical ordered electrode structure with sharp edges to promote charge storage and transfer, (2) designing the channel architecture with a width of ∼4 nm for avoiding size effect and improving the ion transport and storage performance. This work explores the electrochemical performance and structure properties of the devices which probably provide the designing and optimizing bases for achieving high-performance supercapacitors.

Bifunctional heterostructure ZnWO4@ZnO nanocomposite for high-performance electrocatalysis and supercapacitor applications

Earth-abundant transition metal oxides (TMOs) represent a versatile class of electrode materials that excel in energy and environmental applications. Strategically incorporating additional metal oxides to form heterostructures significantly enhances electrical conductivity and cyclic stability, paving the way for better performance in energy storage and conversion technologies. In this study, we developed a ZnWO4@ZnO nanocomposite heterostructure using a straightforward solid-state synthesis method, positioning it as a bifunctional electroactive material for supercapacitor and catalytic applications. Importantly, the heterostructure’s increased surface area allows for more active sites for electrochemical reactions, which can boost current generation. The synergistic interaction between ZnO and ZnWO4 significantly enhances the electrochemical properties of the heterostructure, resulting in an impressive specific capacitance of 363 Fg−1 and exceptional cyclic stability over 10,000 charge–discharge cycles. These results underscore the potential of this material in energy storage and conversion technologies, making it a compelling candidate for high-performance supercapacitor and catalytic applications.

Nanocomposite solid polymer electrolytes: exploring the impact of GO-graft-P(MA-POSS) nanofiller on structural, dielectric, and electrochemical properties for enhanced lithium-ion conductivity in PEO-based system

Nanocomposite solid polymer electrolytes: exploring the impact of GO-graft-P(MA-POSS) nanofiller on structural, dielectric, and electrochemical properties for enhanced lithium-ion conductivity in PEO-based system

Effect of double hydrothermal synthesis technique on the electrochemical properties of Co3O4 microflowers for supercapacitor application

Effect of double hydrothermal synthesis technique on the electrochemical properties of Co3O4 microflowers for supercapacitor application

Fabrication of MnCo2O4@PANI nanocomposites as electrode material for high-energy density asymmetric supercapacitor

In this work, the co-precipitation method has been utilized to synthesize MnCo2O4 (MCO) and MnCo2O4@Polyaniline (PMCO) nanocomposites. The wt% of polyaniline (PANI) has been varied from 0 to 30 %, keeping the MnCo2O4 precursor quantity constant. The nanocomposite with 20 wt% PANI (P20MCO) exhibits better electrochemical properties compared to other synthesized nanocomposite samples. The P20MCO nanocomposite exhibits specific capacitances of 765 F g−1 at 0.5 A g−1 and 88.13 % capacitance retention over 10,000 consecutive cycles. An asymmetric supercapacitor (ASC) has been constructed using P20MCO as cathode and commercially activated carbon as anode. The fabricated ASC device exhibits outstanding cycling stability with 91.48 % capacitance retention for 45,000 cycles at 12 A g−1. The ASC has the highest power density of 14.3 kW kg−1 and specific energy density of 58 Wh kg−1. Moreover, a red LED is illuminated by a single device and putting two devices in series light the blue, green, and white LEDs. These ASCs glow a red LED for more than 13 min. Our results suggest that the P20MCO nanocomposite-based supercapacitor devices will be promising for energy storage applications because of their easy production approach and good electrochemical performance.

The preparation of porous carbon from bio-based phthalonitrile resins by a non-template method: Curing, carbonization and its basic properties

Resin-based porous carbon materials are considered to be an important direction for CO2 adsorption and supercapacitors due to their controllable chemical structure, large specific surface area, and stable physicochemical properties. But at present, the main source of resin-based porous carbon materials is petroleum-based polymer materials, which is incongruous with the tenets of green chemistry. Here, a bio-based phthalonitrile precursor containing s-triazine ring structure (TDPH) was synthesized from vanillin, then a nitrogen/oxygen co-doped hierarchical porous carbon with excellent properties, was prepared using TDPH via a two-step process, with urea/zinc chloride as hardener and potassium hydroxide as activator, respectively. The carbon material prepared under optimal conditions can achieve a maximum CO2 adsorption capacity of 6.81 mmol g−1 at 273 K due to its high specific surface area (1607 m2 g−1) and high N/O content (7.06 wt%/14.74 wt%). It is worth noting that the CO2 adsorption capacity at 298 K can still reach 96.3 % of the initial adsorption after 7 cycles. In addition, the electrochemical properties of the resultant porous carbon were tested under a 1 M H2SO4 three-electrode system, and the highest specific capacitance at a current density of 0.1 A g−1 was 473 F g−1 and the specific capacitance retention can still reach 87 % after 65,000 cycles. This work broadens the source of resin-based porous carbon materials and paves a new way for the functionalization of bio-based resins.

Electrifying energy storage by investigating the electrochemical behavior of CoCr2O4/graphene-oxide nanocomposite as supercapacitor high performance electrode material

This study reports novel three-step electrochemical fabrication of CoCr2O4/graphene-oxide nanocomposite on glassy carbon electrode including sequential synthesis of graphene-oxide using modified Hummer's method, CoCr2O4 nanoparticles using sol-gel method and the cost-effective co-precipitation technique for nanocomposite formation. The resulting nanocomposite was subjected to comprehensive analytical and morphological analysis. X-ray diffractometry (XRD) confirms nanocomposite formation with reduced average crystallite size value of 26.9 nm whereas SEM indicates spherical grains existence within nanocomposite. Energy-dispersive X-ray spectrometry (EDS) confirms no impurity peak existence whereas Raman spectroscopy clearly indicated D and G band existence at 1345 and 1587 cm−1 respectively. Photoluminescent spectra reveals decreasing trend in band gap value about 3.49 eV. The electrochemical properties of CoCr2O4/graphene-oxide nanocomposite electrode explored, showcasing remarkable capacitance with a surface area of merely 0.068 cm2, 574.8 F/g specific capacitance in alkaline 1M KOH and 488.6 F/g specific capacitance in acidic 0.1M H2SO4 electrolyte. Moreover, synthesized nanocomposite demonstrates remarkable electrochemical stability resulting capacitance retention about 95 % after 100 cycles in 1M KOH electrolyte. GCD analysis reveals impressive power and energy density values of 2489 W/kg and 14.88 Wh/kg respectively. These outstanding properties make the nanocomposite an attractive material for next-generation supercapacitors and energy storage solutions.

Metallic bilayer Kagome borophene as a promising anode material for Li and post-Li ion batteries

For future breakthroughs in alkali metal ion batteries, it is essential to explore new anode materials with high storage capacity. Recently, a novel two-dimensional material, bilayer Kagome borophene (BK-borophene), consisting of lightweight elemental boron and having excellent metal conductivity, has been proposed. Thus, the structure, stability, electronic and electrochemical properties of BK-borophene are investigated using first-principles calculations to examine its feasibility as an anode material. Our results show that a single Li/Na/K can stably adsorb on the BK-borophene surface with adsorption energy values of −0.46/-0.25/-0.69 eV. Besides, the low diffusion barrier values (0.55/0.30/0.15 eV) ensure that Li/Na/K can migrate rapidly on its surface, and the low open circuit voltage values are favorable for increasing the operating voltage of the assembled battery. Most importantly, BK-borophene shows high theoretical storage capacities of 826 mA h g−1 for Li, 1377 mA h g−1 for Na, and 275 mA h g−1 for K, which is much more favorable than other reported anode materials. Not only that, BK-borophene also exhibits good cycling stability. The above-mentioned findings suggest that BK-borophene can be a promising and convincing anode material for alkali metal ion batteries.

Fuel-Dependent combustion synthesis of CeCrO3 nanomaterials: Morphological control and its impact on electrochemical properties and device applications

Perovskites exhibiting pseudocapacitance are among the leading energy storage materials as supercapacitors. The cations in perovskites significantly affect storage due to their involvement in redox reactions. CeCrO3 (CCO), a challenging-to-synthesis perovskite, has not yet been investigated for its electrochemical performance. The electrochemical properties of a material heavily depend on each step of the synthesis method. The combustion synthesis of CCO is carried out with different fuels, such as glycine (G), citric acid (C), and sucrose (S), resulting in samples CCO–G, CCO–C, and CCO–S, respectively. This makes combustion with different fuels yield products with peculiar properties and variations in morphology. Consequently, all CCO samples using different fuels exhibit noticeable differences in their electrochemical properties. A systematic investigation is conducted to understand the suitability of CCO for supercapacitor applications. Cyclic voltammetry (CV) and galvanostatic charge-discharge (GCD) techniques are performed in a 2 M KOH electrolyte. CCO–G exhibits the highest specific capacity among the samples, achieving the specific capacity of 461 C g-1 at 1 A g-1 current density. It maintains good cyclic stability of 72.98 % even after 10,000 cycles at the current density of 10 A g-1. To explore its practical applicability, a hybrid supercapacitor device is fabricated with activated carbon (AC) AC@Ni-foam as the negative electrode and CCO–G@Ni-foam as the positive electrode in a 2 M KOH electrolyte. This device demonstrates a specific capacity of 204.80 C g-1 at 1 A g-1 current density. The maximum specific energy, the device achieved is 36.92 Wh kg-1 at 1 A g-1 current density, and the maximal specific power is 7.91 kW kg-1 at current density of 20 A g-1. These significant values emphasize the applicability of this novel material in the field of supercapacitors, paving the way for advanced energy solutions.

Selective Electrocatalytic Oxidation of Ammonia by Ru-dpp Complexes Containing Aromatic Nitrogen Donor as Axial Ligand.

Inspired by the rapid growth of Ru-based complexes as molecular ammonia oxidation catalysts, we propose novel Ru-dpp complexes bearing a nitrogen donor as the axial ligand into the ammonia oxidation catalysts family. Herein, a series of Ru-dpp complexes [Ru(K3-N,N',N″-dpp)(bpy)(L)]·PF6 (where Hdpp = 2-[5-(pyridin-2-yl)-1H-pyrrol-2-yl]pyridine; bpy = 2,2'-bipyridine; L = pyridine (Ru-py); 4-methylpyridine (Ru-pic); pyrimidine (Ru-pmd); isoquinoline (Ru-isoq)) containing aromatic nitrogen donor axial ligand are synthesized and fully characterized by NMR, IR, and ESI-MS. The structural analysis displays that dpp- as a pincer ligand coordinates to ruthenium, and nitrogen donor L binds to ruthenium at an axial ligand. The reaction of Ru-L with ammonia generates ammonia-ligated Ru-L-NH3 complexes, which are monitored by NMR and UV-vis spectra. The electrochemical properties are studied by cyclic voltammetry and density functional theory calculation. These titled complexes have good electrocatalytic performances for selective oxidation of ammonia into hydrazine at 0.6 V versus Cp2Fe+/0 onset potential. The turnover frequency of N2H4 formation is 326.4-393.4 h-1, and the faraday efficiency of generating hydrazine exceeds 97%. The N-N formation mechanism via bimolecular coupling of ruthenium amide/imide is proposed. The aminyl character of ruthenium amide intermediate is confirmed by EPR spectra.

Hard Carbon as Anodes for Potassium-Ion Batteries: Developments and Prospects

Potassium-ion batteries (PIBs) are regarded as a potential substitute for LIBs owing to the benefits of potassium’s abundance, low cost, and high safety. Nonetheless, the practical implementation of potassium-ion batteries still encounters numerous challenges, with the selection and design of anode materials standing out as a key factor impeding their progress. Hard carbon, characterized by its amorphous structure, high specific surface area, and well-developed pore structure, facilitates the insertion/extraction of potassium ions, demonstrating excellent rate performance and cycling stability. This review synthesizes the recent advancements in hard carbon materials utilized in PIB anodes, with a particular focus on the potassium storage mechanism, electrochemical properties, and modification strategies of hard carbon. Ultimately, we present a summary of the current challenges and future development directions of hard carbon materials, with the objective of providing a reference for the design and optimization of hard carbon materials for PIBs.

Unraveling the Nature of Interfacial Behavior in the LiTFSI-LiCl Aqueous Biphasic System.

Aqueous biphasic systems (ABSs) with water-in-salt electrolytes are gaining significant attention for their role in aqueous biphasic interphase studies, particularly in energy storage devices. Aqueous salt-salt biphasic electrolytes are considered a promising alternative to replace traditional liquid electrolytes commonly used in battery technologies, for example, membrane-less redox flow batteries, owing to their low cost and high ionic conductivity. However, the stability of the interphase over time must be considered, as it can impact the long-term electrochemical performance in various applications. This study reports the unstable interfacial behavior of lithium bis(trifluoro-methanesulfonyl)imide and lithium chloride (LiTFSI-LiCl) system using an optical microscope and electrochemical properties. These observations reveal the liquid-liquid instability phenomenon at the interphase over time. Moreover, this research discovers and analyzes the unwanted solid phase formation at the LiTFSI-LiCl interphase. This study not only contributes to fundamental knowledge in interfacial science but also holds significant implications for developing novel applications reliant on ABSs stability.

Electrochemical Properties of Powdery LiNi1/3Mn1/3Co1/3O2 Electrodes with Styrene-Acrylic-Rubber-Based Latex Binders at High Voltage.

Efforts to improve the energy density and cycling stability of lithium-ion batteries have focused on replacing LiCoO2 in cathodes with LiNixMnyCo1-x-yO2. However, reliance on polyvinylidene fluoride (PVdF) as the binder limits the application of the LiNixMnyCo1-x-yO2 composite electrode for lithium-ion batteries. Here, we evaluate the electrochemical properties of a LiNi1/3Mn1/3Co1/3O2 (NMC111) powder electrode formed using a waterborne-styrene-acrylic-rubber (SAR) latex binder combined with sodium carboxymethylcellulose. The composite electrodes prepared with the SAR-based binder copolymerized with the butyl acrylate monomer and styrene exhibited high adhesive strength and excellent cyclability and rate capability. The results of surface analysis via X-ray photoelectron spectroscopy suggested that the electrode with the SAR-based binder is more resistant to electrolyte decomposition during charge and discharge cycling compared with the NMC111 electrode comprising the conventional PVdF binder. The SAR-derived passivation resulted in enhanced capacity retention during long-term cycling tests of both half- and full-cells (NMC111//graphite). An electrode with a higher Ni content, LiNi0.6Mn0.2Co0.2O2 (NMC622), fabricated using the SAR-based binder, retained 87.1% of its capacity after 50 cycles at 4.6 V and exhibited excellent cycling stability.

A Genetically Encoded Redox-Active Nicotinamide Amino Acid.

Nicotinamide-containing cofactors play an essential role in many enzymes that catalyze two-electron redox reactions. However, it is difficult to engineer nicotinamide binding sites into proteins due to the extended nature of the cofactor-protein interface and the precise orientation of the nicotinamide moiety required for efficient electron transfer to or from the substrate. To address these challenges, we genetically encoded a noncanonical amino acid (ncAA) bearing a nicotinamide side chain in bacteria. This redox-active amino acid, termed Nic1, exhibits similar electrochemical properties to the natural cofactor nicotinamide adenine dinucleotide (NAD+). Nic1 can be reversibly reduced and oxidized using chemical reagents both free in solution and when incorporated into a model protein. This genetically encodable cofactor can be introduced into proteins in a site-specific fashion and may serve as a tool to study electron-transfer mechanisms in enzymes and to engineer redox-active proteins.

Comparison of three different industrial lignin-based porous carbon electrodes for electrochemical applications

Abstract In order to fully utilize industrial lignin, a comparative study was conducted on the properties of porous carbon electrodes prepared by activating different industrial lignin as precursors. The results revealed that carbon electrodes prepared with sodium lignosulfonate (CM-S) exhibited superior specific surface area (SSA) (1,593.5 m2 g−1) and pore volume (PV) (1.03 cm3 g−1) due to the largest relative molecular mass (Mn = 4,539, Mw = 7,290), which is greater than that prepared with alkali lignin (CM-A) and kraft lignin (CM-K), and displayed a well-developed micro-mesoporous macropore hierarchy which was feasible for the efficiency of electron mobility. The electrochemical properties of materials were evaluated, and CM-S showed a mass-specific capacitance of 201 F g−1 at 0.2 A g−1 current density, along with an impressive capacitance retention rate of 54.7 % at 10 A g−1 current density, which is more potential than CM-A and CM-K (specific capacitances: 100 F g−1 and 75 F g−1 respectively). Additionally, maximum energy and power density of CM-S were measured to be 6.98 W h kg−1 and 2306 W kg−1 with excellent retention rate of 95.5 % after 10,000 charge–discharge cycles at a current density of 5 A g−1. Comparatively, sodium lignosulfonate, compared with alkali lignin and kraft lignin, emerges as a more ideal precursor material for porous carbon electrode.

Skeletal Nitrogen Functionalization of Isostructural 2D Conjugated MOFs for Enhancement of the Dual-Ion Storage Capacity.

Two-dimensional conjugated metal-organic frameworks (2D c-MOFs) are emerging as promising electrode materials for electrochemical energy storage. However, a viable path to realize superior dual-ion storage in 2D c-MOFs has remained elusive. Here, we report the synthesis of Cu2(Nx-OHPTP) 2D c-MOFs (x=0,1,2; OHPTP=octahydroxyphenanthrotriphenylene) with precise aromatic carbon-nitrogen arrangements, based on the π-conjugated OHPTP ligand incorporated with one or two nitrogen atoms. The skeletal nitrogen modification in Cu2(Nx-OHPTP) allows the synergistic introduction of additional redox sites, and thus substantially favors the unique dual-ion adsorption capacity. Consequently, the Cu2(N2-OHPTP) cathode exhibits a largely enhanced electrochemical performance for dual-ion storage (i.e., Li+ and Cl-) with a high specific capacity of 53.8 mAh g-1, which is twice that of Cu2(N0-OHPTP) and 1.3 times that of Cu2(N1-OHPTP). Furthermore, the Cu2(N2-OHPTP) electrode displays a favorable rate performance of 52% and good cycling stability of 96% after 1000 cycles. We identify N-centered redox sites as additional Li+ adsorption sites. In addition, calculations underline the synergistic enhancement of the Cl- adsorption energy by about 1.0 eV at the more electron-poor CuO4 linkages after N-incorporation. This work paves the way for the precise design of 2D c-MOFs with superior electrochemical properties, advancing their application in dual-ion storage applications.

Facile and ecofriendly green synthesis of Co3O4/MgO-SiO2 composites towards efficient asymmetric supercapacitor and oxygen evolution reaction applications.

The development of low-cost, eco-friendly, and earth-friendly electrode materials for energy storage and conversion applications is a highly desirable but challenging task for strengthening the existing renewable energy systems. As part of this study, orange peel extract was utilized to synthesize a magnesium oxide-silicon dioxide hybrid substrate system (MgO-SiO2) for coating cobalt oxide nanostructures (Co3O4) via hydrothermal methods. A variety of MgO-SiO2 compositions were used to produce Co3O4 nanostructures. The purpose of using MgO-SiO2 substrates was to increase the porosity of the final hybrid material and enhance its compatibility with the electrode material. This study investigated the morphology, chemical composition, optical properties, and functional group properties. In hybrid materials, the shape structure is inherited from nanoparticles with uniform size distributions that are well compacted. A relative decrease in the optical band was observed for Co3O4 when deposited onto an MgO-SiO2 substrate. An improvement in the electrochemical properties of Co3O4/MgO-SiO2 composites was observed during the measurements of supercapacitors and oxygen evolution reaction (OER) in alkaline solutions. The Co3O4/MgO-SiO2 composite prepared on 0.4 g of the MgO-SiO2 substrate (sample 2) demonstrated excellent specific capacitance, high energy density, and recycling stability for 40 000 galvanic charge-discharge cycles. The assembled asymmetric supercapacitor (ASC) device demonstrated a specific capacitance of 243.94 F g-1 at a current density of 2 A g-1. Co3O4/MgO-SiO2 composites were found to be highly active towards the OER in 1 M KOH aqueous solution with an overpotential of 340 mV at 10 mA cm-2 and a Tafel slope of 88 mV dc-1. It was found that the stability and durability were highly satisfactory. Based on the use of orange peel extract, a roadmap was developed for the synthesis of porous hybrid substrates for the development of efficient electrode materials for energy storage and conversion.

High-entropy Li-rich layered oxide cathode for Li-ion batteries

High-entropy oxides (HEOs) are emerging as promising cathode materials for Li-ion batteries (LIBs) due to their stable solid-state phase and compositional flexibility. Herein, we investigate the structural and electrochemical properties of a novel non-equimolar high-entropy cathode material, termed high-entropy Li-rich layered oxide (HE-LLO, Li1.15Na0.05Ni0.19Mn0.56Fe0.02Mg0.02Al0.02O1.97F0.03), in comparison to a pristine Li-rich layered oxide (PR-LLO, Li1.2Ni0.2Mn0.6O2). The incorporation of multiple cations (Na+, Al3+, Mg2+, Fe3+) and anion (F−) into HE-LLO introduces compositional diversity, enhancing structural stability through the entropy stabilization effect. Theoretical calculations confirm a significantly higher configurational entropy in HE-LLO compared to PR-LLO, supporting its high-entropy nature. Electrochemical evaluations demonstrate that HE-LLO exhibits considerable capacity retention, preserving 76.8 % of its discharge capacity at 0.5C after 200 cycles, compared to only 36.2 % for PR-LLO. Even under high-temperature conditions, HE-LLO outperformed PR-LLO, maintaining 76.1 % of its discharge capacity after 100 cycles at 5C, while PR-LLO retained only 12.4 %. These enhancements are attributed to the improved phase reversibility and higher Li+ ion diffusion coefficients of HE-LLO, validated by ex-situ characterizations using a synchrotron X-ray technique, along with density functional theory (DFT) calculations. These findings highlight the promise of non-equimolar HEOs as a novel design strategy for high-performance cathode materials.

Skeletal Nitrogen Functionalization of Isostructural 2D Conjugated MOFs for Enhancement of the Dual‐Ion Storage Capacity

Two‐dimensional conjugated metal‐organic frameworks (2D c‐MOFs) are emerging as promising electrode materials for electrochemical energy storage. However, a viable path to realize superior dual‐ion storage in 2D c‐MOFs has remained elusive. Here, we report the synthesis of Cu2(Nx‐OHPTP) 2D c‐MOFs (x=0,1,2; OHPTP=octahydroxyphenanthrotriphenylene) with precise aromatic carbon‐nitrogen arrangements, based on the π‐conjugated OHPTP ligand incorporated with one or two nitrogen atoms. The skeletal nitrogen modification in Cu2(Nx‐OHPTP) allows the synergistic introduction of additional redox sites, and thus substantially favors the unique dual‐ion adsorption capacity. Consequently, the Cu2(N2‐OHPTP) cathode exhibits a largely enhanced electrochemical performance for dual‐ion storage (i.e., Li+ and Cl‐) with a high specific capacity of 53.8 mAh g−1, which is twice that of Cu2(N0‐OHPTP) and 1.3 times that of Cu2(N1‐OHPTP). Furthermore, the Cu2(N2‐OHPTP) electrode displays a favorable rate performance of 52% and good cycling stability of 96% after 1000 cycles. We identify N‐centered redox sites as additional Li+ adsorption sites. In addition, calculations underline the synergistic enhancement of the Cl− adsorption energy by about 1.0 eV at the more electron‐poor CuO4 linkages after N‐incorporation. This work paves the way for the precise design of 2D c‐MOFs with superior electrochemical properties, advancing their application in dual‐ion storage applications.