Catalysts For Rechargeable Zinc-air Batteries Research Articles

CoFe2O4 with the In-Situ Formed Oxygen Vacancies and Co Particles as an Efficient Bifunctional Catalyst for Rechargeable Zinc-Air Batteries.

Rechargeable zinc-air batteries (RZABs) are considered as one of the most promising clean energy device due to their abundant resources, low cost and environmental friendliness. However, their energy efficiency and cycle life are far from satisfactory due to the poor activity and stability of bi-functional electrocatalyst in air cathode. In this work, an efficient bi-functional catalyst (rGO-CoFe2O4/Co) was derived from its precursor (rGO-CoFe2O4) through a simple annealing process. Electrochemical measurements prove that rGO-CoFe2O4/Co with the in-situ formed Co nano particles and rich oxygen vacancies appears excellent oxygen reduction reaction and oxygen evolution reaction catalytic activity compared to its counterpart. Its half-wave potential is 0.81 V (vs RHE) and the OER overpotential is only 310 mV (vs RHE). In addition, rechargeable zinc-air batteries assembled with rGO-CoFe2O4/Co show the highest peak power density (128.9 mW cm-2) and cycling stability compared to rGO-CoFe2O4 and commercial Pt/C-RuO2 catalysts. This work provides a simple strategy for the design of advanced bifunctional catalysts.

Construction of atom-scale Co/Fe/Ni M-N-C active sites within nitrogen-doped carbon spheres for high-performance bifunctional oxygen catalysts in rechargeable zinc-air batteries

Developing carbon-based catalysts with metal‑nitrogen‑carbon (M-N-C) active sites as efficient and low-cost bifunctional catalysts to replace precious metal catalysts for rechargeable zinc-air batteries devices has garnered significant attention. Herein, nitrogen-doped submicron carbon-based spherical bifunctional electrocatalysts (CNPD-CoFeNi) with abundant atom-scale Co/Fe/Ni M-N-C active sites and defects were synthesized. The introduction of massive amounts of Zn species increases the spatial distance of Co/Fe/Ni metal sites to prevent aggregation during pyrolysis, and the evaporation of Zn at high temperatures creates defects synergizing with M-N-C. Consequently, CNPD-CoFeNi possesses a stable carbon-based spherical structure, high electrical conductivity, rich nitrogen content, abundant atom-scale Co/Fe/Ni M-N-C active sites, and defects, displaying outstanding durability, oxygen reduction reaction (ORR) activity with a half-wave potential of 0.87 V, and satisfactory OER performance, surpassing or comparable with the state-of-art Pt/C and RuO2, respectively. Notably, liquid Zn-air batteries with CNPD-CoFeNi catalyst exhibit an exceptional high peak power density of 146.5 mW cm−2 and stable charge-discharge cycling over 270 h, outperforming Pt/C-RuO2 based devices. Additionally, the all-solid-state Zn-air battery also displays satisfactory practicability and stability. The synthesis strategy and its remarkable results provide valuable guidance and inspiration for the future advancement of precious metal substitutes in ORR/OER and rechargeable zinc-air batteries.

Molten salt method for preparing Mn0.3Ru0.7O2 nanosheets as a superior bifunctional catalyst for rechargeable zinc-air batteries

Integrating components for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) while optimizing their electronic structure is an effective strategy for developing excellent bifunctional catalysts for rechargeable zinc-air batteries (ZABs). In this study, we successfully fabricated Mn0.3Ru0.7O2 nanosheets based on a solid solution oxide using a simple molten salt method. The Mn0.3Ru0.7O2 nanosheets exhibits abundant Ru and Mn sites through the Ru-O-Mn structure, which serve as excellent OER and ORR active centers. Experimental and theoretical studies validate the coccurrence of charge transefer between the Ru-O-Mn bond, modulating the valence state and d-band center of the Mn and Ru, thereby subsequently improving their ORR/OER intrinsic activity. Remarkably, the Mn0.3Ru0.7O2 nanosheets displays superior electropcatalytic performance with a charge/discharge voltage gap (ΔE) of only 0.59 V, which is the best among all reported counterpart catalysts. A rechargeable ZAB utilizing Mn0.3Ru0.7O2 nanosheets achieved a power density of 154 mW cm−2 and a specific capacity of 821 mA h g−1, surpassing that of the commercial Pt/C + RuO2 mixing catalyst. This study offers a new strategy for preparing highly active and durable bifunctional catalysts for rechargeable ZABs.

Co/Ce-MOF-Derived Oxygen Electrode Bifunctional Catalyst for Rechargeable Zinc-Air Batteries.

Improving the practicality of rechargeable zinc-air batteries relies heavily on the development of oxygen electrode catalysts that are low-cost, durable, and highly efficient in performing dual functions. In the present study, a catalyst with atomic Ce and Co distribution on a nitrogen-doped carbon substrate was prepared by doping the rare earth elements Ce and Co into a metal-organic framework precursor. Rare earth element Ce, known for its unique structure and excellent oxygen affinity, was utilized to regulate the catalytic activity. The catalyst prepared in this study demonstrated an exceptional electrocatalytic performance. At a current density of 10 mA cm-2, the catalyst exhibited an overpotential of 340 mV for the oxygen evolution reaction (OER), which was lower than that of commercial IrO2 (370 mV), while achieving a half-wave potential of 0.79 V for the process of oxygen reduction reaction (ORR), exhibiting a similar level of effectiveness as commercially accessible Pt/C catalysts (0.8 V). The catalyst's porous structure, interconnected three-dimensional carbon network, and large specific surface area are the factors contributing to the significant improvement in catalytic performance. Furthermore, in comparison to commercial Pt/C+IrO2, the catalyst exhibited good cycling stability and high efficiency in rechargeable zinc-air batteries.

Metal–organic framework–derived trimetallic particles encapsulated by ultrathin nitrogen-doped carbon nanosheets on a network of nitrogen-doped carbon nanotubes as bifunctional catalysts for rechargeable zinc–air batteries

Economical oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) bifunctional catalysts with high activity aimed at replacing precious metal catalysts for rechargeable zinc-air batteries (ZABs) must be developed. In this study, a multiple hierarchical-structural material is developed using a facile dielectric barrier discharge (DBD) plasma surface treatment, solvothermal reaction, and high-temperature carbonization strategy. This strategy allows for the construction of nanosheets using nitrogen-doped carbon (NC) material-encapsulated ternary CoNiFe alloy nanoparticles (NPs) on a network of NC nanotubes (NCNTs), denoted as CoNiFe–NC@p–NCNTs. Precisely, the presence of abundant CoNiFe alloy NPs and the formation of M–N–C active sites created by transition metals (cobalt, nickel, and iron) coupled with NC can provide superior OER/ORR bifunctional properties. Moreover, the prepared NC layers with a multilevel pore structure contribute to a larger specific surface area, exposing numerous active sites and enhancing the uniformity of electron and mass movement. The CoNiFe0.08–NC@p–NCNTs show remarkable dual functionality for electrochemical oxygen reactions (ORR half-wave potential of 0.811 V, limiting current density of 5.73 mA cm−2 measured with a rotating disk electrode at a rotation speed of 1600 rpm, and OER overpotential of 351 mV at 10 mA cm−2), which demonstrates similar ORR performance to 20 wt% Pt/C and better OER performance than the commercial RuO2. A liquid ZAB prepared using the proposed material has excellent bifunctionality with an open-circuit voltage of 1.450 V and long-term cycling stability of 230 h@10 mA cm−2.

CoTe2/NiTe2 heterojunction embedded in N-doped hollow carbon nanoboxes as high-efficient ORR/OER catalyst for rechargeable zinc-air battery

Interface engineering has been recognized as one of the most promising strategies for tuning the catalytic properties of catalysts. However, building well-defined nanointerfaces for efficient oxygen reduction/evolution reactions (ORR/OER) remains a challenge. Herein, a hollow heterostructure composed of highly-dispersed CoTe2 inside the mesoporous walls of nitrogen-doped carbon nanoboxes and uniformly-dispersed NiTe2 outside the mesoporous walls (H-CoTe2/NiTe2@NCBs) is designed via a ZIF67-involved etching-anchoring-tellurization strategy. Promising half-wave potential of 0.86 V and overpotential of 320 mV at 10 mA cm−2 are obtained by H-CoTe2/NiTe2@NCBs. The excellent ORR/OER activity of H-CoTe2/NiTe2@NCBs is ascribed to the synergistic coupling based on nanointerfaces between CoTe2 and NiTe2. Density functional theory calculations confirm that the nanointerface-based electronic coupling between CoTe2 and NiTe2 facilitates the charge transfer between two components and generates abundant catalytically active sites at the heterointerface, thereby significantly promoting the ORR/OER activities. This work provides the design principles for transitional bimetallic tellurides as bifunctional electrocatalysts.

Renewable lignin-derived heteroatom-doped porous carbon nanosheets as an efficient oxygen reduction catalyst for rechargeable zinc-air batteries

Lignin upgrading to various functional products is promising to realize high-value utilization of low-cost and renewable biomass waste, but is still in its infancy. Herein, using industry waste lignosulfonate as the biomass-based carbon source and urea as the dopant, we constructed a heteroatom-doped porous carbon nanosheet structure by a simple NaCl template-assisted pyrolytic strategy. Through the synergistic effect of the NaCl template and urea, the optimized lignin-derived porous carbon catalyst with high content of active nitrogen species and large specific surface area can be obtained. As a result, the fabricated catalysts exhibited excellent electrocatalytic oxygen reduction activity, as well as good methanol tolerance and stability, comparable to that of commercial Pt/C. Moreover, rechargeable Zn-air batteries assembled with this electrocatalyst have a peak power density of up to 150 mW cm-2 and prominent long-term cycling stability. This study offers an inexpensive and efficient way for the massive production of highly active metal-free catalysts from the plentiful, inexpensive and environmentally friendly lignin, offering a good direction for biomass waste recycling and utilization.

NiFe layered double hydroxide (LDH) anchored, Fe single atom and nanoparticle embedded on nitrogen-doped carbon-CNT (carbon nanotube) framework as a bifunctional catalyst for rechargeable zinc-air batteries

Zinc-air batteries (ZAB) have significant potential for practical energy storage, but their rechargeability has been limited by the lack of a suitable bifunctional catalyst. Here, we developed NiFe LDH-A-Fe/NC-CNT, a remarkable bifunctional catalyst that is built on a hierarchically porous nitrogen-doped carbon and carbon nanotube (NC-CNT) framework enriched with iron single atoms and nanoparticles, with nickel‑iron layered double hydroxides (NiFe LDH) anchored onto it. The NiFe LDH-A-Fe/NC-CNT exhibited remarkable performance in the ORR, with Eonset of 0.94 V, a half-wave potential of 0.84 V, and a limited current of 6.89 mA cm−2. A remarkable Eonset of 1.47 V and a potential of 1.59 V at 10 mA cm−2 (Ej = 10) in the OER were also observed. Significantly, the difference in potential (ΔE) between the ORR and OER was only 0.74 V. The stability tests, tolerance assessments, and poisoning experiments consistently demonstrated the superior performance of this cutting-edge catalyst in comparison to the commercial Pt/C and RuO2. In ZAB tests, it achieves a discharge capacity of 818 mAhg−1 and an impressive power density of 293 mWcm−2, enduring nearly 1000 cycles (320h). Flexible ZABs with this catalyst maintain a 629 mAhg−1 capacity, a power density of 195 mWcm−2, and a lifespan of 95 h (280 cycles), outperforming benchmark catalysts. In conclusion, a remarkable bifunctional catalyst was synthesized, demonstrating its immense capacity for utilization in zinc-air batteries.

Pre-implanting metal oxides to endow the N-doped carbon with boosted bifunctional catalytic activities towards oxygen reduction and oxygen evolution reactions

Nitrogen-doped carbon-based materials exhibit promising prospect as the catalysts to oxygen reduction reaction (ORR). Incorporating transition metal oxides with the catalysts can endow them with oxygen evolution reaction (OER) activity to construct bifunctional catalysts for rechargeable zinc-air batteries. In this work, a catalyst (named as 300NiFe-Mi-C) was prepared by a metal oxide-implanting strategy. The mixed metal salts of Ni and Fe were first heated to produce metal oxides, and then blended with 2-methylimidazole and carbon black, and subsequently pyrolyzed at a high temperature. In the pyrolysis, a part of metal oxides was reduced to metallic state to facilitate the doping of nitrogen atoms into carbon to form the ORR active sites while a part of metal oxides was retained to afford OER activity. Benefiting from the pre-implanting strategy of metal oxides, the resultant 300NiFe-Mi-C presents enhanced OER performance with 1.56 V of OER potential at 10 mA cm−2, outperforming the 1.68 V of the controlled sample NiFe-Mi-C (without pre-implanting) and 1.70 V of RuO2. The 0.83 V of ORR half-wave potential of 300NiFe-Mi-C is also comparable to the 0.82 V of NiFe-Mi-C and 0.86 V of Pt/C, revealing satisfactory bifunctional catalytic activities. The rechargeable zinc-air battery equipped with 300NiFe-Mi-C can stably operate at ∼1.25 V with 10 mA cm−2, being higher than ∼1.21 V of Pt/C+RuO2. The battery also presents outstanding durability and rechargeability, demonstrating the bifunctional activities of 300NiFe-Mi-C can be realized in practical applications.

Regulating the frontier orbital of iron phthalocyanine with nitrogen doped carbon nanosheets for improving oxygen reduction activity.

Iron phthalocyanine (FePc) has attracted widespread attention for its tunable electronic structure. However, the Fe-N sites suffer from undesirable oxygen reduction activity due to the symmetric geometries. A suitable substrate was thus needed to induce electron redistribution around Fe-N to improve the activity. Herein, ultrathin nitrogen-doped carbon nanosheets (N-CNSs) were prepared by a simple high temperature pyrolysis. Then iron phthalocyanine was loaded on the ultrathin nitrogen-doped carbon nanosheets (FePc@N-CNSs) by a low-cost and simple solution method. This composite catalyst shows an excellent ORR activity with a half potential of 0.88 V, an onset potential of 0.99 V and durability superior to commercial Pt/C. When used as an air cathode catalyst for rechargeable zinc-air batteries, FePc@N-CNS modified batteries outperform Pt/C + RuO2 modified batteries with higher power density and superior constant current charge-discharge cycling stability of 37 hours. The regulated electronic structure of FePc by the N-CNS substrate was revealed further by DFT calculations, which explained the enhanced adsorption of the active center to the intermediates and the increased ORR performance.

Bifunctional Single Atom Catalysts for Rechargeable Zinc-Air Batteries: From Dynamic Mechanism to Rational Design.

Ever-growing demands for rechargeable zinc-air batteries (ZABs) call for efficient bifunctional electrocatalysts. Among various electrocatalysts, single atom catalysts (SACs) have received increasing attention due to the merits of high atom utilization, structural tunability, and remarkable activity. Rational design of bifunctional SACs relies heavily on an in-depth understanding of reaction mechanisms, especially dynamic evolution under electrochemical conditions. This requires a systematic study in dynamic mechanisms to replace current trial and error modes. Herein, fundamental understanding of dynamic oxygen reduction reaction and oxygen evolution reaction mechanisms for SACs is first presented combining in situ and/or operando characterizations and theoretical calculations. By highlighting structure-performance relationships, rational regulation strategies are particularly proposed to facilitate the design of efficient bifunctional SACs. Furthermore, future perspectives and challenges are discussed. This review provides a thorough understanding of dynamic mechanisms and regulation strategies for bifunctional SACs, which are expected to pave the avenue for exploring optimum single atom bifunctional oxygen catalysts and effective ZABs.

FeNiCrCoMn High-Entropy Alloy Nanoparticles Loaded on Carbon Nanotubes as Bifunctional Oxygen Catalysts for Rechargeable Zinc-Air Batteries.

An efficient and stable bifunctional oxygen catalyst is necessary to complete the application of the rechargeable zinc-air battery. Herein, an economical and convenient process was adopted to successfully coat high-entropy alloy Fe12Ni23Cr10Co55-xMnx nanoparticles on carbon nanotubes (CNTs). In 0.1 M KOH solution, with a bifunctional oxygen overpotential (ΔE) of only 0.7 V, the catalyst Fe12Ni23Cr10Co30Mn25/CNT exhibits excellent bifunctional oxygen catalytic performance, exceeding most catalysts reported so far. In addition, the air electrode assembled with this catalyst exhibits high specific capacity (760 mA h g-1) and energy density (865.5 W h kg-1) in a liquid zinc-air battery, with a long-term cycle stability over 256 h. The density functional theory calculation points out that changing the atomic ratio of Co/Mn can change the adsorption energy of the oxygen intermediate (*OOH), which allows the ORR catalytic process to be accelerated in the alkaline environment, thereby increasing the ORR catalytic activity. This article has important implications for the progress of commercially available bifunctional oxygen catalysts and their applications in zinc-air batteries.

Hollow Raspberry-like CoSx/C Sub-Microspheres as a Highly Active Air Cathode Catalyst for Rechargeable Zinc-Air Batteries

Hollow Raspberry-like CoS_<i>x</i>/C Sub-Microspheres as a Highly Active Air Cathode Catalyst for Rechargeable Zinc-Air Batteries

Construction of Co/FeCo@Fe(Co)3O4 heterojunction rich in oxygen vacancies derived from metal–organic frameworks using O2 plasma as a high-performance bifunctional catalyst for rechargeable zinc-air batteries

Developing high-efficient, good-durability, and low-cost bifunctional non-precious metal catalysts for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is urgent and significant for promoting the practical rechargeable zinc-air batteries (RZABs). Herein, N-doped carbon coated Co/FeCo@Fe(Co)3O4 heterojunction rich in oxygen vacancies derived from metal–organic frameworks (MOFs) is successfully constructed by O2 plasma treatment. The phase transition of Co/FeCo to FeCo oxide (Fe3O4/Co3O4) mainly occurs on the surface of nanoparticles (NPs) during the O2 plasma treatment, which can form rich oxygen vacancies simultaneously. The fabricated catalyst P-Co3Fe1/NC-700-10 with optimal O2 plasma treatment time of 10 min can reduce the potential gap between the OER and ORR to 760 mV, which is much lower than commercial 20% Pt/C + RuO2 (910 mV). Density functional theory (DFT) calculation indicates that the synergistic coupling between Co/FeCo alloy NPs and FeCo oxide layer can promote the ORR/OER performance. Both liquid electrolyte RZAB and flexible all-solid-state RZAB using P-Co3Fe1/NC-700-10 as the air–cathode catalyst display high power density, specific capacity and excellent stability. This work provides an effective idea for the development of high performance bifunctional electrocatalyst and the application of RZABs.

Morphology Engineering toward High-Surface-Area Mno2 Bifunctional Catalysts for Rechargeable Zinc-Air Batteries

Morphology Engineering toward High-Surface-Area Mno2 Bifunctional Catalysts for Rechargeable Zinc-Air Batteries

Pomegranate-Like FeNC with Optimized FeN4 Configuration as Bi-Functional Catalysts for Rechargeable Zinc-Air Batteries.

Catalysts with FeNC moieties have demonstrated remarkable activity toward oxygen reduction reaction (ORR), but precise synthesis and configuration regulation of FeNC to achieve bi-functional catalytic sites for ORR and oxygen evolution reaction (OER) remain a great challenge. Herein, a pomegranate-like catalyst with optimized FeN4 configuration is designed. The unique framework affords a large surface area for sufficient active site exposure and abundant macroporous channels for mass transport. By twisting chemical bonds, the electronic structure of FeN4 is regulated, and the adsorption/desorption of oxygen species is facilitated. Compared to noble metal-based catalysts (Pt/C+IrO2 ), the optimized FeNC exhibits impressive onset potential (0.96V versus reversible hydrogen electrode), larger limiting current density (5.85mA cm-2 ), and better long-term life for ORR, as well as, lower OER overpotential. When integrated into Zn-air batteries, it demonstrates a respectable peak power density (71.6mW cm-2 ) and ideal cycling stability (30h), exceeding that of commercial Pt/C+IrO2 . The exploration offers a guideline for designing advanced bi-functional electrocatalysts.

Outstanding platinum group metal-free bifunctional catalysts for rechargeable zinc-air batteries

Developing highly active and durable catalysts for zinc-air batteries (ZAB) is critical for energy conversion and storage. Herein, we prepared Fe-N-C catalysts at a kilogram scale by the commercial VariPore™ method and the effect of synthesis conditions on the catalyst performance at ZAB air electrode was investigated. The results show the PA-450-HT exhibits excellent electrocatalytic activity toward oxygen reduction reaction (ORR) and it is the most suitable catalyst for primary ZAB with the galvanostatic polarization discharge peak power density of 149 mW cm−2, outperforming commercial Pt-Ru/C catalysts. Additionally, the NCB-600-HT catalyst displays the half-wave potential of 0.87 V vs. RHE for ORR and ∆E value of 0.81 V (indicating outstanding ORR and OER reversibility) and exhibits excellent charge-discharge cycling durability similar to NCB-550-LT around 160 h for the secondary ZAB. This work reports outstanding bifunctional Fe-N-C catalysts for rechargeable ZAB at mass production for the first time.

Fe-N4/Co-N4 active sites engineered porous carbon with encapsulated FeCo alloy as an efficient bifunctional catalyst for rechargeable zinc-air battery

Design and synthesis of earth-abundant elements-based electrocatalysts with sufficient activity and stability remain challenging for oxygen-involved electrochemical energy conversion and storage devices. In this work, catalyst with simultaneously engineered Fe-N4 and Co-N4 active sites and graphitic carbon multilayer-encapsulated FeCo alloy is developed by pyrolysis of metal salts doped G-g-C3N4. The obtained composite material exhibits promising catalytic activity and good stability for both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) in alkaline electrolyte, as evidenced by the positive shift of half-wave potential by 44 mV compared to 20% Pt/C for ORR and the potential of 1.596 V at current density of 10 mAcm−2 for OER. In addition, the thus-assembled rechargeable zinc-air battery using the synthesized material as cathode delivers a maximum power density of 311.2 mWcm−2 with an open circuit potential of 1.51 V and a long-term cycling stability. DFT calculation results indicate that catalyst with composite active sites displays smaller energy barrier than that with single active site.

Ag Decorated Co3O4-Nitrogen Doped Porous Carbon as the Bifunctional Cathodic Catalysts for Rechargeable Zinc-Air Batteries

The use of transition metals as bifunctional catalysts for rechargeable zinc-air batteries has recently attracted much attention. Due to their multiple chemical valence states, the cobalt oxides are considered to be promising catalysts for oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). In this work, bifunctional Ag-decorated Co3O4-nitrogen doped porous carbon composite (Co3O4-NC&amp;Ag) catalysts were synthesized by annealing ZIF-67 in N2 and O2, respectively, followed by Ag deposition using chemical bath deposition. Due to the decoration of Ag nanoparticles and high specific surface area (46.9 m2 g−1), the electrochemical activity of Co3O4 increased significantly. The optimized Co3O4-NC&amp;Ag catalysts possessed superior ORR performance with a half-wave potential of 0.84 V (vs. RHE) and OER activity with an overpotential of 349 mV at 10 mA cm−2. The open circuit voltage of the Co3O4-NC&amp;Ag-based zinc-air battery was 1.423 V. Meanwhile, the power density reached 198 mW cm−2 with a specific discharge capacity of 770 mAh g−1 at 10 mA cm−2, which was higher than that of Pt/C-based zinc-air battery (160 mW cm−2 and 705 mAh g−1). At a current density of 10 mA cm−2, the charge-discharge performance was stable for 120 h (360 cycles), exhibiting better long-term stability than the Pt/C&amp;RuO2 counterpart.

Nickel hydroxide anchored CNT-Co3O4-N-carbon bifunctional catalyst for rechargeable zinc-air batteries

BackgroundA rechargeable zinc-air battery (RZAB) is a hopeful alternative battery solution to meet the world's ever-increasing energy storage need. Developing a high-performance electrocatalyst is one of the most critical challenges that need to be addressed for the RZAB to fulfill that role. MethodsA Ni(OH)2-CNT-Co3O4/NC catalyst consisting of carbon nanotube (CNT), cobalt oxide, and nitrogen-doped functionalities embedded in a porous carbon framework with two-dimensional Ni(OH)2 nanosheets is reported. Significant findingsThe prepared catalytic material, Ni(OH)2-CNT-Co3O4/NC, showed a high limit current density of -6.409 mA cm−2 during the oxygen reduction reaction (ORR), surpassing that of the commercial Pt/C (-5.625 mA cm−2). The oxygen evolution reaction (OER) potential for this electrocatalyst also reached 1.653 V at a current density of 10 mA cm−2, which is close to that of the commercial RuO2 and thus showed excellent catalytic activity for the OER. As a bifunctional catalyst in the RZAB, the Ni(OH)2-CNT-Co3O4/NC electrocatalyst exhibited a high power density of 244.5 mW cm−2, and cycled 4500 times at a current density of 10 mA cm−2 while displaying good charge and discharge stability. Based upon these performances, we believe that the Ni(OH)2-CNT-Co3O4/NC catalyst can serve as an excellent bifunctional catalyst in the next-generation RZAB.