One-step Electrodeposition Research Articles

Corrosion-resistant superhydrophobic films on galvanized steel by one-step electrodeposition

A simple one-step electrodeposition method is proposed to fabricate corrosion-resistant superhydrophobic films on hot-dip galvanized steel without using low surface-energy materials. The effects of electrodeposition time on surface morphology, surface composition, surface roughness, wettability, and corrosion resistance of the electrodeposited zinc films were investigated. The results revealed that the morphological structures and roughnesses of the deposited zinc films were varied by the electrodeposition times. The roughened zinc films naturally reduced their surface energy during storage for 10 days as the formation of functional groups, transforming them to superhydrophobic and/or nearly superhydrophobic. The electrodeposited superhydrophobic films significantly enhanced the corrosion resistance of the hot-dip galvanized steel. Among them, the 20 min electrodeposition time gave the appropriate morphology and roughness to achieve a superhydrophobic surface with the optimum corrosion inhibition property.

Ultra-sensitive label-free detection of haptoglobin using Au-rGO decorated electrochemical sensing platform: Towards endometriosis diagnostic application

In this research, for the first time, one-step electrodeposition of simultaneously gold nanoparticles (AuNPs) and reduced graphene oxide (rGO) on the surface of a glassy carbon electrode (GCE) was used as a sensing platform of highly sensitive and label-free immunosensing for the rapid voltammetric analysis for haptoglobin (HP) at ultra-trace levels. 11-mecaptoundecanoic acid (11-MUA) was self-assembled onto Au substrate, which was coupled to the antibody (ab-HP) via ethyl-N’-(3-dimethyl aminopropyl) carbodiimide hydrochloride–N-hydroxysuccinimide (EDC-NHS) coupling. The interaction between the antigen (HP) and antibody (ab-HP) is measured by square wave voltammetry in [Fe (CN)6]3−/4− solution. The proposed immunosensor exhibits a concentration that ranges from 10 fg mL−1 to 1000 ng mL−1, and 3.47 fg mL−1 of low detection limit (LOD). Moreover, an immunosensor has high sensitivity, selectivity, reproducibility, stability, and reusability. Ultimately, this system was successfully applied for the detection of HP in different positive and negative serum samples (positive: n = 40, negative: n = 10), whereas negligible change was observed in control samples and was compared with commercial ELISA kits. The specificity and sensitivity of the assay were 100% and 98%, respectively. The coincidence rate using the HP ELISA kit was 95.30% and 92.20%. The result demonstrated that the sensing platform could be used for clinical diagnosis of HP in clinical laboratories.

One-step electrodeposition of Co-Fe electrocatalysts with micro/nano-cauliflower like structure for highly efficient oxygen evolution reaction (OER)

In this study, Co-Fe coatings with different “Fe” contents were produced as catalysts for oxygen evolution reaction (OER) by a one-step electrodeposition method using 0–6 g/L FeSO4 in an electrolytic bath. The structure, electrochemical and electrical properties of the produced catalysts were carefully investigated. Scanning electron microscopy (SEM) results showed that the morphology of the prepared catalysts was varied with the “Fe” content. UV–vis diffuse reflectance spectroscopy (DRS) results along with Tauc plots indicated that the concentration of oxygen vacancy decreased by increasing the Fe content from 2 to 6 g/L, while the Co-Fe (2 g/L) catalyst with a band gap of 1.35 eV had the maximum concentrations of oxygen vacancies. Also, linear sweep voltammetry (LSV) results demonstrated that the Co-Fe (2 g/L) catalyst had the lowest overpotential (136 mV) at a current density of 10 mA.cm−2 and a small Tafel slope of 24.3 mV.dec− 1. The results confirmed the formation of the CoFe2O4 phase in the Co-Fe (2 g/L) catalysts. It was eventually concluded that the Co-Fe (2 g/L) catalyst with a nano-cauliflower like structure possesses the highest OER activity in 1 M KOH solution.

Seed-assisted electrodeposition of multilayer Au nanoparticles-assembled films for sensitive surface-enhanced Raman scattering detection

Surface-enhanced Raman scattering (SERS) spectroscopy can be used to realize sensitive rapid detection of molecules. Three-dimensional (3D) SERS substrates can provide more hotspots within the excitation laser beam when compared with the corresponding two-dimensional (2D) SERS substrates. Most of the methods for fabrication of 3D SERS substrates involve complex processes. Therefore, it is significant to develop a simple and effective method for fabrication of 3D SERS substrates. Here, a seed-assisted electrodeposition approach is developed for fabrication of a 3D SERS substrate composed of multilayer Au nanoparticles. Interestingly, it is demonstrated that a uniform film composed of multilayer Au nanoparticles that can serve as a 3D SERS substrate can be achieved directly by one-step electrodeposition on a conductive surface coated with monolayer Au seeds. It is found that a diffusion-controlled growth during electrodeposition narrows the nanoparticle size distribution and results monosized Au nanoparticles. The as-prepared multilayer Au nanoparticles-assembled film shows high SERS sensitivity and good spectral uniformity. For SERS detection of rhodamine 6G, a limit of detection as low as 3.4×10−12 M has been achieved. Moreover, good spectral uniformity (relative standard deviation ∼7.8%) and high substrate-to-substrate reproducibility (relative standard deviation ∼8.6%) have also been demonstrated. The as-prepared multilayer Au nanoparticles-assembled film is used to detect organic pollutants such as dye molecule crystal violet (CV) and methylene blue (MB). Calibration curves with a linear correlation between the logarithmic SERS intensity and logarithmic concentration of CV and MB have been obtained. Limit of detections for CV and MB are 1.2×10−8 M and 9.8×10−10 M, respectively. Therefore, the fabricated 3D SERS substrate has good application prospects in sensitive detection of organic molecules.

Ultra-fast electrochemical preparation of Ni-Cu-Fe nano-micro dendrite as a highly active and stable electrocatalyst for overall water splitting

The development of highly active, durable, and low-cost electrocatalysts for both the hydrogen evolution reaction (HER) and the oxygen evolution reaction (OER) to advance the commercial applications of overall water electrolysis is regarded as a crucial matter. We describe an ultra-fast synthesis of multi-metal Ni-Cu-Fe micro-nano dendritic electrocatalysts were synthesized on nickel foam using a simple one-step constant current electrodeposition method. According to DFT simulations, Fe incorporation causes a downshift movement in the d-band center and the formation of additional catalytic active sites. Ni-Cu-Fe nano-micro dendrites have potential applications as bifunctional catalysts for electrochemical water splitting. Also, the increased electrical conductivity of the Ni-Cu-Fe electrode is due to the placement of more electronic states near the Fermi level and creating an optimal and porous dendritic structure that causes better electrolyte penetration in the pores. Experiments show that in the 1.0 M KOH electrolyte, Ni-Cu-Fe catalysts need an ultra-low overpotentials of 42 mV and 300 mV to supply a current density of −10 mA cm−2 for the HER and 50 mA cm−2 for the OER. Also, when Ni-Cu-Fe electrocatalyst is used as a bifunctional electrode in the overall water splitting system, it displays a low cell voltage of 1.54 V in a current density of 10 mA cm−2 can maintain this activity for more than 100 h.

Mo/P doped NiFeSe as bifunctional electrocatalysts for overall water splitting

Designing high-efficiency catalysts for overall water splitting is critical to reduce the cost of hydrogen fuel as a clean and renewable energy source in future society. In this work, a Mo-, P-codoped NiFeSe was successfully synthesized on nickel foam (NF) by one-step electrodeposition. Through the doping strategy, the conductivity can be well promoted, and the production of nanosheets on the catalyst surface and active phases during hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) provided much more active sites, which leaded to efficient HER/OER performances of as-synthesized Mo-, P-codoped NiFeSe catalysts, i.e., a low overpotential of 100 mV/200 mV at current density of 10 mA cm−2 in 1.0 M KOH with stability of 95 h/60 h, respectively. It only required 1.53 V to deliver a current density of 10 mA cm−2 in overall water splitting and maintained outstanding durability for 100 h. This work is beneficial to future design of high efficient and low-cost bifunctional catalysts for overall water splitting.

TiO2 nanotubes modified with cobalt oxyphosphide spheres for efficient electrocatalytic hydrogen evolution reaction in alkaline medium

Electronic and surface modulation through coupling between oxygen and phosphorous in cobalt oxyphosphide (CoOP) is identified as an effective approach to enhancing the electrocatalytic hydrogen evolution reaction (HER) in an alkaline medium. This work demonstrates a one-step and safe electrodeposition method to modify the surface of ordered titania nanotubes (TNTs) with CoOP spheres. The effect of electrodeposition charge density, pH of the electrodeposition bath, and presence of citric acid on the electrocatalytic HER performance of CoOP-modified TNTs was investigated. The Ti/TNTs/CoOP electrode requires only 130 mV overpotential to deliver 10 mA cm−2 in a 1.0 M KOH electrolyte. The Tafel slope is estimated to be 72.5 mV dec−1. Both the HER performance and Tafel value of Ti/TNTs/CoOP are superior to CoOP deposited on bare Ti foil (165 mV and 78.4 mV dec−1), FTO (185 mV; 88.1 mV dec−1), and glassy carbon (214 mV; 93 mV dec−1). The electrochemically active surface area (ECSA) and impedance spectroscopy findings revealed that the synergistic coupling between the CoOP and TNTs enhances the surface area and density of accessible active sites while reducing the charge transfer resistance at the electrode/electrolyte interface. Such a synergistic effect is ascribed to the effective electronic interaction between CoOP and TNTs, and the faster electron transfer kinetics because of the unidirectionality of the 1-D TNTs.

One-Step High-Temperature Electrodeposition of Fe-Based Films as Efficient Water Oxidation Catalysts

Electrolysis of water to produce hydrogen requires an efficient catalyst preferably made of cheap and abundant metal ions for the improved water oxidation reaction. An Fe-based film has been deposited in a single step by electrochemical deposition at temperatures higher than the room temperature. Until now, the electrodeposition of iron oxide has been carried out at 298 K or at lower temperatures under a controlled atmosphere to prohibit atmospheric oxidation of Fe2+ of the iron precursor. A metal inorganic complex, ferrocene, and non-aqueous electrolyte medium propylene carbonate have been used to achieve electrodeposition of iron oxide without the need of any inert or controlled atmosphere. At 298 K, the amorphous film was formed, whereas at 313 K and at higher temperatures, the hematite film was grown, as confirmed by X-ray diffraction. The transformation of iron of the ferrocene into a higher oxidation state under the experimental conditions used was further confirmed by X-ray photoelectron spectroscopy, ultraviolet-visible, and electron paramagnetic resonance spectroscopic methods. The films deposited at 313 K showed the best performance for water oxidation with remarkable long-term electrocatalytic stability and an impressive turnover frequency of 0.028 s-1 which was 4.5 times higher than that of films deposited at 298 K (0.006 s-1). The observed overpotential to achieve a current density of 10 mA cm-2 was found to be 100 mV less for the film deposited at 313 K compared to room-temperature-derived films under similar experimental conditions. Furthermore, electrochemical impedance data revealed that films obtained at 313 K have the least charge transfer resistance (114 Ω) among all, supporting the most efficient electron transport in the film. To the best of our knowledge, this is the first-ever report where the crystalline iron-based film has been shown to be electrodeposited without any post-deposition additional treatment for alkaline oxygen evolution reaction application.

Green fabrication of nanostructured Ni(OH)2/Ni/Carbon felt electrodes with water-containing deep eutectic solvent for enhanced water electrolysis performance

To produce green hydrogen, the development of high-performance, environmentally friendly, and cost-effective electrocatalysts for efficient hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) is imperative. This study explores the potential application of water-containing deep eutectic solvents (DESs) in the synthesis of nanostructured electrocatalysts for water electrolysis. Ni(OH)2/Ni/carbon felt (CF) composite electrodes are developed via one-step electrodeposition in a water-containing choline chloride/urea DES as a green reaction medium. Heterostructured Ni(OH)2/Ni nanosheets are formed and uniformly deposited on the CF substrate with the addition of 10 wt% water to DES (CU10W), which increases active sites for HER and OER. The initial confinement of water molecules by the DES is found to be crucial in forming the hierarchical structure of the electrocatalysts. Notably, the CU10W electrode exhibits excellent bifunctional activity toward HER and OER, with reduced overpotentials of 192 and 564 mV, respectively, at 100 mA cm−2. This renders the CU10W electrode-based electrolysis system stable with a reduced cell voltage of 1.69 V and a high Faradaic efficiency of over 99% for the HER. The augmented electrochemical active surface area and reduced charge transfer resistance of the CU10W electrode account for the improved HER/OER performance associated with the special hierarchical Ni(OH)2/Ni nanostructure.

Carbon-Free, Binder-Free MnO2@Mn Catalyst for Oxygen Reduction Reaction

Reasonable design and feasible preparation of low-cost and stable oxygen reduction reaction (ORR) catalysts with excellent performance play a key role in the development of fuel cells and metal-air batteries. A 3D porous superimposed nanosheet catalyst composed of metal manganese covered with MnO2 nanofilms (P-NS-MnO2@Mn) was designed and synthesized by rotating disk electrodes (RDEs) through one-step electrodeposition. The catalyst contains no carbon material. Therefore, the oxidation and corrosion of the carbon material during use can be avoided, resulting in excellent stability. The structural and composition characterizations indicate that the nanosheets with sharp edges exist on the surface of the wall surrounding the macropore (diameter ∼ 5.07 μm) and they connect tightly. Both the nanosheets and the wall of the macropore are composed of metal manganese covered completely with MnO2 film with a thickness of less than 5 nm. The half-wave potential of the synthesized P-NS-MnO2@Mn catalyst is 0.86 V. Besides, the catalyst exhibits good stability with almost no decay after a 30 h chronoamperometric test. Finite element analysis (FEA) simulation reveals the high local electric field intensity surrounding the sharp edges of the nanosheets. Density functional theory (DFT) calculations reveal that the novel nanosheet structure composed of MnO2 nanofilms covered on the surface of the Mn matrix accelerates the electronic transfer of the MnO2 nanofilms during the ORR process. The high local electric field intensity near the sharp edge of the nanosheets effectively promotes the orbital hybridization and strengthens the adsorbing Mn-O bond between the active site Mn in the nanosheets and the intermediate OOH* during the ORR process. This study provides a new strategy for preparing transition metal oxide catalysts and a novel idea about the key factors affecting the catalytic activity of transition metal oxides for the ORR.

Controlled tuning the morphology of CoNiP catalysts with ultra-high activity for water splitting at large current densities in alkaline medium

Developing efficient, robust and low-cost bifunctional electrocatalyst with high activity and strong stability for overall water splitting has received extensive attention. Herein, a 3D porous nanoflower spherical catalyst Co6Ni4P/NF was synthesized by one-step pulse electrodeposition, and regulating morphology of nanostructure through tuning the ratio of Co2+ and Ni2+ in the planting bath. This morphology combined the superiorities of the 3D spherical and the 2D film structures, which not only retain a large specific surface area, but also ensure the high-density of active sites. The as-prepared Co6Ni4P/NF only needs overpotentials of 336 mV and 373 mV to reach the large current density 1000 mA cm−2 for HER and OER and shows long-term stability under alkaline condition. Meanwhile, to drive overall water splitting requires only the cell voltages of 1.56 V, 1.61 V and 2.19 V to reach 50, 100 and 1000 mA cm−2. In this work, the influence of catalyst morphology is discussed specifically, and we find the nanoflower spherical Co6Ni4P/NF presents the best performance compared with nanospheres and nanosheets in overall water splitting process, which is appealing to practical application at large current condition.

High-entropy (Oxy)hydroxide Prepared by Electrodeposition for Highly Efficient OER in Alkaline Medium

With the development of the economy and society, energy shortage and environmental pollution are increasingly in the spotlight. Electrolytic water to hydrogen technology is considered to be the best way to produce green hydrogen. However, the slow thermodynamic/kinetic limitations make it difficult to scale application due to an anodic oxygen evolution reaction (OER) involving four electrons. Recently, transition metal-based materials become popular research subjects because properties of abundant reserve and low cost. Fortunately, the performances for water splitting are surprising compared to some noble metal-based materials which means these materials have huge potential for practical application in reality. The transition metal (oxy)hydroxides are confirmed to be a category of promising electrocatalysts for OER. To improve the activity of catalysts, many effective strategies (including defects engineering, vacancy engineering, interface engineering, high-entropy effect, etc.) are adopted to modulate the electronic structure and enrich active site density. In this work, we have successfully synthesized high-entropy transition metal (oxy)hydroxides by one-step electrodeposition for water oxidation. The results obtained confirmed the high-entropy effect results in high intrinsic activity and high stability for electrochemical water oxidation.

One-step electrodeposition of polypyrrole/Ti3C2Tx MXene composite coating for 304SS bipolar plates in PEMFC

Polypyrrole (PPY) coating is promising for the anticorrosion of stainless steel (SS) bipolar plates (BPs) in virtue of its good conductivity and corrosion resistance. However, the poor adhesion and pore defects of pure PPY coating limit its application. In this work, a PPY/Ti3C2Tx MXene composite coating was synthesized on 304SS BPs by one-step electrodeposition, which is a facile method to realize the polymerization of PPY and the doping of MXene at the same time. The PPY/MXene coating exhibits better long-term immersion stability in simulated proton exchange membrane fuel cell (PEMFC) environment than pure PPY. The enhanced corrosion resistance is mainly benefited from the enhanced barrier effect, anodic protection effect and adhesion by the introduction of MXene. Meanwhile, the introduction of MXene significantly improves the conductivity of the coating and decreases the interfacial contact resistance at 1.4 MPa from 108.16 mΩ·cm2 to 55.24 mΩ·cm2.

Constructing robust NiFe LDHs–NiFe alloy gradient hybrid bifunctional catalyst for overall water splitting: one-step electrodeposition and surface reconstruction

Constructing robust NiFe LDHs–NiFe alloy gradient hybrid bifunctional catalyst for overall water splitting: one-step electrodeposition and surface reconstruction

Phase Segregation in Cu0.5 Ni0.5 Alloy Boosting Urea-Assisted Hydrogen Production in Alkaline Media.

Coupling urea oxidation reaction (UOR) and hydrogen evolution reaction (HER) is promising for energy-efficient hydrogen production. However, developing cheap and highly active bifunctional electrocatalysts for overall urea electrolysis remains challenging. In this work, a metastable Cu0.5 Ni0.5 alloy is synthesized by a one-step electrodeposition method. It only requires the potentials of 1.33 and -28mV to obtain the current density of ±10mA cm-2 for UOR and HER, respectively. The metastable alloy is considered to be the main reason causing the above excellent performances. In the alkaline medium, the as-prepared Cu0.5 Ni0.5 alloy exhibits good stability for HER; and conversely, NiOOH species can be rapidly formed during the UOR due to the phase segregation of Cu0.5 Ni0.5 alloy. In particular, for the energy-saving hydrogen generation system coupled with HER and UOR, only 1.38V of voltage is needed at 10mA cm-2 ; and at 100mA cm-2 , the voltage decreases by ≈305mV compared with that of the routine water electrolysis system (HER || OER). Compared with some catalysts reported recently, the Cu0.5 Ni0.5 catalyst owns superior electrocatalytic activity and durability. Furthermore, this work provides a simple, mild, and rapid method for designing highly active bifunctional electrocatalysts toward urea-supporting overall water splitting.

Tailoring Ni-Fe-Se film on Ni foam via electrodeposition optimization for efficient oxygen evolution reaction

The development of efficient non-precious metal electrocatalysts is essential for oxygen evolution reaction (OER) for water splitting. Among them, amorphous bimetallic NiFe-based compounds are recognized as one of the excellent candidates for efficient OER. Herein, the Ni-Fe-Se film is rationally designed via facile one-step electrodeposition with tailored active sites and thicknesses. Accordingly, the optimized sample, with an increased Fe-incorporation level and a thickness of ∼50 nm, shows a low overpotential of ∼290 mV at a current density of 40 mA cm−2 and long-term durability in 1 M KOH solution, representing its overall excellent OER performance. Furthermore, operando Raman and ex-situ XPS are used to identify the active sites for OER. This work provides some new insights into exploring earth-abundant free-standing catalysts for OER toward overall water-splitting applications.

Electrochemical Fabrication and Characterization of Cu2ZnSnS4 (CZTS) Thin Film Deposits on Gold Substrate for Hydrogen Production

In this paper, room temperature one-step electrodeposition of chalcogenide CZTS followed by annealing at different temperatures was studied. The scanning electron microscopy images of the deposits confirmed the presence of agglomerated particles in the deposits. The deposits annealed at [Formula: see text]C did not show the presence of voids whereas deposits annealed at [Formula: see text]C showed severe sulfur loss and were off-stoichiometric. Annealing at [Formula: see text]C resulted in the deposits of compositions closer to the required ratio. Good absorbance over the entire visible range makes both the annealed deposits suitable absorber materials for thin-film photovoltaic cells. Current–voltage characteristics resulted in Ohmic trend and the slope of the plot increased with annealing temperature. The deposits showed good photosensitive behavior where resistance decreased upon shining the light source. The Mott–Schottky plot showed that the deposits were made of positively charged particles. CZTS thin film annealed at [Formula: see text]C provided higher H2 production rate (68.68 [Formula: see text]mol ⋅ [Formula: see text] ⋅ [Formula: see text], which was 32 times higher than that of CZTS annealed at [Formula: see text]C (2.08 [Formula: see text]mol ⋅ [Formula: see text] ⋅ [Formula: see text]. What’s more, photocatalytic activity of CZTS thin film remained 94% after 48 h which confirmed the good stability and reusability of CZTS thin film. CZTS thin film is a potential and durable candidate for photocatalysis.

Corrosion protection of superhydrophobic/amphiphobic cobalt coating with anti-icing and self-cleaning properties fabricated by a one-step electrodeposition method

Fabrication of superhydrophobic cobalt-based coatings is a useful way to provide metals, including copper, with corrosion protection, anti-icing, and self-cleaning properties to enhance their industrial applications. A one-step electrodeposition process was applied to synthesize a cobalt coating on a copper substrate. Superhydrophobicity, amphiphobicity, anti-freezing, self-cleaning, corrosion protection, and long-term stability of the coating were investigated. The coating surface was studied using SEM and the water contact angles (CAs) were measured by an optical tensiometer. The coating showed a water CA of 155.6 ± 0.6° with a sliding angle of 4.8 ± 0.3°, denoting its superhydrophobicity. Also, it was amphiphobic with CAs over 120° for glycerol and ethylene glycol. The coating was highly corrosion resistant with a high charge transfer resistance of 756.3 kΩ.cm2. This was compatible with the stability of coating during 16 days of immersion in 3.5 wt% NaCl solutions (pH 1 and 14), when it remained hydrophobic with CA over 90°. The 23 min longer freezing time of water droplets on the coating at − 15° compared to the copper substrate was a proof of its excellent anti-icing. Only three rolling water drops were required to remove the alumina powder from 1.13 cm2 of the coating area, denoting excellent self-cleaning with a rare superiority over other similar research.

Facile electrodeposition synthesis and super performance of nano-porous Ni-Fe-Cu-Co-W high entropy alloy electrocatalyst

Establishing efficient nano-porous electrocatalysts for facilitating electron transfer is a one of the useful ways for enhance water splitting. Herein, Ni-Fe-Cu-Co-W high entropy alloy (NFCCW-HEA) electrocatalysts on the iron sheet substrate have been successfully prepared by a simple and efficient one-step electrodeposition method. High entropy alloys have a variety of active sites and unique atomic scale synergies, which makes the catalyst have good catalytic performance and stability. Meanwhile, the HEA coating like cauliflower by electrodeposition can provide more attachment sites, and significantly upgrade the OER catalytic activity. NFCCW-HEA catalysts exhibit an excellent overpotential of 247.3 mV under the current density of 10 mA·cm−2, and a low Tafel slope of 62.9 mV dec−1. The electrocatalyst shows long term stability of electrolysis for over 24 h in 1 mol·L−1 KOH alkaline solution, which shows good stability. We expect to provide a new idea for the preparation of nano porous high entropy alloy electrocatalysts by one-step electrodeposition technology.

One-step nickel-cobalt alloy electrodeposition from spent lithium-ion battery via synergistic pH adjustment and Mn2+ supplementation

Alloy productization of nickel (Ni) and cobalt (Co) in spent lithium-ion batteries (LIBs) is an effective way for their high-value conversion. Herein, we dynamically supplemented divalent manganese (Mn2+) ions into the LIBs leachate while synergistically adjusting the pH for rapid electrodeposition of Ni-Co alloys on the cathode. Benefiting from the suitable redox potential, Mn2+ ions can be easily oxidized to MnO2 at the anode thus providing electrons push the cathodic reaction, and without being reduced by the cathode. The electrons provided by the oxidation of Mn2+ ions occupied 51% of the required for the cathodic electrodeposition. However, the oxidation of Mn2+ gave rise to a decrease in pH (from 3 to 2 within 30 min), which caused protonation on the cathode surface, resulting in electrostatic repulsion of Ni2+ and Co2+ by the cathode. By dynamically adjusting the pH to 3 every half hour using ammonia, the protonation of the cathode can be effectively suppressed, thereby converting electrostatic repulsion into attraction. The methods of dynamic supplementation of Mn2+ ions and pH adjustment have complementary effects. Compared with the control group, the deposition rates of Ni and Co are increased by 6.59 and 11.09 times, and the obtained Ni-Co alloys with the purity of 99.80%. Concurrently, the MnO2 by-product of 99.52% purity is obtained on the anode. This strategy does not cause additional contamination of the LIBs leachate because the LIBs leachate contains Mn2+.