Nitrogen-doped Carbon Nanosheets Research Articles

Cobalt@Ruthenium Core@Shell nanoparticles embedded within nitrogen-doped carbon nanosheets as reversible oxygen electrocatalysts

Rational design and engineering of cost-effective, high-performance reversible oxygen electrocatalysts for both the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR) is imperative in advancing the progress of rechargeable metal-air batteries (r-MABs). Herein, nanocomposites based on Co@Ru core@shell nanoparticles embedded within N-doped carbon nanosheets (Co@Ru/CS) are prepared via facile galvanic exchange reactions of RuCl3 with Co/NC and used as an effective oxygen electrocatalyst for rechargeable zinc-air battery (r-ZAB). Electrochemical studies demonstrate a remarkable bifunctional catalytic performance of Co@Ru/CS towards both ORR and OER, featuring a low potential gap (ΔE) of only 0.69 V between the OER potential (E10,OER) at 10 mA cm−2 and half-wave potential (E1/2,ORR) of ORR, which is much lower than that of commercial Pt/C + RuO2 catalysts (0.76 V). Combined studies of experimental characterizations and density functional theory calculations show that the ORR activity arises primarily from the N-doped carbon and CoNx moieties in the composites, whereas RuO2/CoOOH produced at high electrode potentials is responsible for the OER activity. Co@Ru/CS based r-ZAB exhibits an open circuit voltage of 1.447 V, specific capacity of 781 mAh gZn−1, and maximum power density of 115 mW cm−2 at 0.83 V, a performance better than that with commercial Pt/C + RuO2 (1.412 V, 760.56 mAh gZn−1, and 91 mW cm−2). Results from this research underline the substantial impact of structural engineering on optimizing the electrocatalytic activity of nanocomposites for r-MABs.

Superhydrophobic Co/Fe sulfide nanoparticles and single-atoms doped carbon nanosheets composite air cathode for high-performance zinc-air batteries

Development of a high-performance bifunctional catalyst is essential for the actual implementation of zinc-air batteries in practical applications. Herein, a bifunctional cathode of Co3S4/FeS heterogeneous nanoparticles embedded in Co/Fe single-atom-loaded nitrogen-doped carbon nanosheets is designed. Cobalt-iron sulfides and single atomic sites with Co-N4/Fe-N4 configurations are confirmed to coexist on the carbon matrix by EXAFS spectroscopy. 3D self-supported super-hydrophobic multiphase composite cathode provides abundant active sites and facilitates gas-liquid-solid three-phase interface reactions, resulting in excellent electrocatalytic activity and batteries performance, i.e., an OER overpotential (η10) of 260 mV, a half-wave potential (E1/2) of 0.872 V for ORR, a ΔE of 0.618 V, and a discharge power density of 170 mW cm−2, a specific capacity of 816.3 mAh g−1. DFT analysis shows multiphase coupling of sulfide heterojunction through single-atomic metal doped carbon nanosheets reduce offset on center of electronic density of states before and after oxygen adsorption, and spin density of adsorbed oxygen with same spin orientation, leading to weakened charge/spin interactions between adsorbed oxygen and substrate, and a lowered oxygen adsorption energy to accelerate OER/ORR.

Ice/salt assisted synthesis of ultrathin two-dimensional nitrogen doped carbon nanosheets for fast lithium storage

Two-dimensional carbon nanosheets have garnered considerable interest as promising anode materials in energy storage devices due to their large specific surface area and excellent conductivity. The efficient synthesis of ultrathin nitrogen-doped carbon nanosheets is achieved with the aid of cysteine, employing a green ice/salt-assisted strategy. Ice influences the growth direction of salt crystals and determines the distribution of sodium lignosulfonate on the surfaces of both ice and salt crystals. The introduction of methionine incorporates heteroatoms, altering the electronic structure and chemical activity of the material, thereby effectively enhancing its lithium storage performance. The initial charge capacity of the optimized sample reached 766.4 mA h g−1 at a current density of 0.2 A g−1, maintaining a capacity of 571.1 mA h g−1 after 100 cycles. This study presents an innovative method for fabricating ultrathin carbon nanosheets using eco-friendly, cost-effective sodium lignosulfonate, showcasing a promising candidate for lithium-ion batteries and future energy storage technologies.

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.

High content pyridine nitrogen-doped carbon nanosheets derived from ZIF-L as anode materials of lithium-ion batteries with excellent capacity and rate performance

The precise control of nitrogen doping types in carbon materials is crucial for optimizing energy storage devices. In this study, we synthesize nitrogen-doped carbon nanosheets (NCS) using ZIF-L as a precursor. Comparatively, the two-dimensional crystal structure of ZIF-L provides several advantages over ZIF-8 as a precursor in terms of nitrogen doping efficiency, achieving a higher doping level (14.56 %) and an increased ratio of pyridinic nitrogen (53.60 %). Consequently, NCS display a greater capacity for pseudocapacitive lithium storage. Furthermore, by adjusting the carbonization temperature, we precisely tailor the graphite-nitrogen doping level of NCS within the range of 16.80–31.22 %. Remarkably, when employed as an anode material in lithium-ion batteries, NCS-800 demonstrates exceptional cycling stability, with a capacity retention of 1078 mAh g−1 after 500 cycles at a current density of 0.5 A g−1, as well as excellent rate capability (735 mAh g−1 at 5 A g−1). This study not only compares the impact of precursor crystal structure modifications on nitrogen doping and lithium storage performance but also introduces a novel synthesis methodology for highly nitrogen-doped carbon materials, offering new avenues for future research in this field.

Ultrafine Ni-MoOx Nanoparticles Anchored on Nitrogen-Doped Carbon Nanosheets: A Highly Efficient Noble-Metal-Free Catalyst for Ammonia Borane Hydrolysis.

The development of low-cost and high-efficiency catalysts for the hydrolytic dehydrogenation of ammonia borane (AB, NH3BH3) is still a challenging technology. Herein, ultrafine MoOx-doped Ni nanoparticles (~3.0 nm) were anchored on g-C3N4@glucose-derived nitrogen-doped carbon nanosheets via a phosphate-mediated method. The strong adsorption of phosphate-mediated nitrogen-doped carbon nanosheets (PNCS) for metal ions is a key factor for the preparation of ultrasmall Ni nanoparticles (NPs). Notably, the alkaline environment formed by the reduction of metal ions removes the phosphate from the PNCS surface to generate P-free (P)NCS so that the phosphate does not participate in the subsequent catalytic reaction. The synthesized Ni-MoOx/(P)NCS catalysts exhibited outstanding catalytic properties for the hydrolysis of AB, with a high turnover frequency (TOF) value of up to 85.7 min-1, comparable to the most efficient noble-metal-free catalysts and commercial Pt/C catalyst ever reported for catalytic hydrogen production from AB hydrolysis. The superior performance of Ni-MoOx/(P)NCS can be ascribed to its well-dispersed ultrafine metal NPs, abundant surface basic sites, and electron-rich nickel species induced by strong electronic interactions between Ni-MoOx and (P)NCS. The strategy of combining multiple modification measures adopted in this study provides new insights into the development of economical and high-efficiency noble-metal-free catalysts for energy catalysis applications.

Isolated Binary Fe-Ni Metal-Nitrogen Sites Anchored on Porous Carbon Nanosheets for Efficient Oxygen Electrocatalysis through High-Temperature Gas-Migration Strategy.

Atomically dispersed dual-site catalysts can regulate multiple reaction processes and provide synergistic functions based on diverse molecules and their interfaces. However, how to synthesize and stabilize dual-site single-atom catalysts (DACs) is confronted with challenges. Herein, we report a facile high-temperature gas-migration strategy to synthesize Fe-Ni DACs on nitrogen-doped carbon nanosheets (FeNiSAs/NC). FeNiSAs/NC exhibits a high half-wave potential (0.88 V) for the oxygen reduction reaction (ORR) and a low overpotential of 410 mV at 10 mA cm-2 for the oxygen evolution reaction (OER). As an air electrode for Zn-air batteries (ZABs), it shows better performances in aqueous ZABs and excellent stability and flexibility in solid-state ZABs. The high specific surface area (1687.32 m2/g) of FeNiSAs/NC is conducive to electron transport. Density functional theory (DFT) reveals that the Fe sites are the active center, and Ni sites can significantly optimize the free energy of the oxygen-containing intermediate state on Fe sites, contributing to the improvement of ORR and the corresponding OER activities. This work can provide guidance for the rational design of DACs and understand the structure-activity relationship of SACs with multiple active sites for electrocatalytic energy conversion.

In-situ approach to porous nitrogen-doped carbon nanosheets functionalized by Brønsted acidic ionic liquids for microwave-assisted upgrading fructose to 5-hydroxymethylfurfural

In the search for robust and recoverable supported Brønsted acidic ionic liquids (BAILs) catalysts for efficient upgrading bio-sugars to value-added chemicals, an in-situ strategy of supramolecular preorganization-thermal polycondensation is designed to fabricate porous ultrathin nitrogen-doped carbon nanosheets (NCNSs), and then BAILs-functionalized NCNSs catalysts are prepared via successive quaternary ammonization by sultones and anion exchange with Brønsted acids. By adjusting the molar composition of the starting monomers, the textural properties of NCNSs supports are tuned; and by functionalization with different sultones (1,3-propanesultone and 1,4-butanesultone) and organic (trifluoromethanesulfonic acid and p-toluenesulfonic acid) or inorganic (H2SO4 and H3PO4) acids, the surface hydrophobicity and Brønsted acid strength of the catalysts are regulated. The catalysts are applied in microwave-assisted upgrading fructose to 5-hydroxymethylfurfural, and influences of Brønsted acid nature, surface hydrophobicity and textural properties on the catalytic performance are explored. For the most active [C4SO3HN][OTf]-NCNSs-MA-3 catalyst with the advantages of superstrong Brønsted acidity, higher surface hydrophobicity and perfect porous ultrathin sheet-like nanostructure, the conversion of fructose and the yield of 5-hydroxymethylfurfural of 100% and 87.7% are achieved after microwave irradiation for 15 min, outperforming Amberlyst-15 resin and HY zeolite. The catalysts also demonstrate the robust catalytic reusability, and after five consecutive catalytic runs, the obvious activity loss hardly occurs, along with little acid sites leaching.

Silicon Nanoparticles Wrapped in a Double-Layer Coating of Chitin-Derived Nitrogen-Doped Carbon Nanosheet and Pitch-Based Carbon Enabling Efficient Lithium Storage

Silicon Nanoparticles Wrapped in a Double-Layer Coating of Chitin-Derived Nitrogen-Doped Carbon Nanosheet and Pitch-Based Carbon Enabling Efficient Lithium Storage

NiCo-LDH coupled with 2D ZIF-derived Co nitrogen doped carbon nanosheet arrays as a self-supporting electrocatalyst for detection of formaldehyde.

Formaldehyde is susceptible to illegal addition to foodstuffs to extend their shelf life due to its antimicrobial, preservative and bleaching properties. In this study, a self-supporting "nanosheet on nanosheet" arrays electrocatalyst with core-shell heterostructure was prepared in situ by coupling NiCo layer double hydroxide with 2D ZIF derived Co-nitrogen-doped porous carbon on carbon cloth (Co-N/C@NiCo-LDH NSAs/CC). Co-N/C nanosheet arrays act as a scaffold core with good electrical conductivity, providing more NiCo-LDH nucleation sites to avoid NiCo-LDH agglomeration, thus having fast mass/charge transfer performance. While the NiCo-LDH nanosheet arrays shell with high specific surface area provide more active sites for electrochemical reactions. As an electrocatalytic sensing electrode, Co-N/C@NiCo-LDH NSAs/CC has a wide linear range of 1 μM to 13 mM for formaldehyde detection, and the detection limit is 82 nM. Besides, the sensor has been applied to the detection of formaldehyde in food samples with satisfactory results.

Enhanced electrocatalytic conversion of tellurium with MnO hollow nanospheres modified hierarchical n-doped carbon nanosheets in high-performance aqueous Zn-Te battery

Rechargeable aqueous zinc batteries (AZBs) are increasingly recognized as an alternative to conventional energy storage systems due to their environmentally safe nature, abundant zinc resources, and high theoretical capacity. However, the intercalation or surface redox mechanisms limit the development of AZBs cathode materials due to low specific capacity and energy density. The tellurium-based (Te) materials with conversion mechanisms are promising cathode materials for AZBs. Nevertheless, the slow kinetics are detrimental to the increase in specific capacity and energy density for Zn-Te battery. Therefore, a hierarchical structure of manganese oxide (MnO) hollow nanospheres loaded on nitrogen-doped carbon nanosheets (MnO@NC) was rationally designed and used as Te hosts (Te/MnO@NC) for Zn-Te battery. This hierarchical structure facilitates the loading of more Te species. Meanwhile, the MnO hollow nanospheres can expose more active sites, which can promote the kinetics of Te redox reactions thereby lowering the reaction energy barrier. The Te/MnO@NC cathode exhibits high specific capacity and high energy density (429 mAh g−1 and 407 Wh Kg−1 at 0.1 A g−1). Additionally, the conversion mechanism was investigated by systematic characterization and density functional theory (DFT) calculations. This study presents a new design platform for developing AZBs with high specific capacity and energy density.

Nitrogen-Doped Carbon Nanosheets Supported Co for Efficient and Stable Electrocatalytic Oxygen Reduction

Nitrogen-Doped Carbon Nanosheets Supported Co for Efficient and Stable Electrocatalytic Oxygen Reduction

Construction of oxygen-vacancy-rich 2D nitrogen-doped carbon nanosheets with CoFe@CoFe2O4 heterogeneous interfacial structure for rechargeable Zn–air batteries

Integration of cations doping by using unpaired high-spin electrons through the valence state substitution is deemed as a prospective strategy for construction of oxygen vacancies, regulation of inner electronic structures and enhancement of surface properties. Herein, an effective strategy is proposed to construct massive oxygen vacancies into 2D nitrogen-doped carbon nanosheets by the design of heterogeneous interfaces between CoFe alloy and CoFe2O4 nanoparticles. The valence state transition for Fe and Co endows electronic transfer capability and charge density around the oxygen atoms. The prepared CoFe-CoFe2O4@NCs-4 catalyst exhibits maximum content of oxygen vacancies (Density of Ovac 50.1 %). It shows excellent ORR activity with a half-wave potential of 0.83 V and OER overpotential of 320 mV. Reversible Zn-air batteries assembled by the CoFe-CoFe2O4@NCs-4 catalysts exhibit a power density of 106.32 mW cm−2 and durable stability (500 h at the current density of 10 mA cm−2), which also are superior to those of the commercial 20 wt% Pt/C + RuO2 catalyst. The excellent bifunctional catalytic performance can be attributed to synergistic effects between massive oxygen vacancies, ultrahigh specific surface area (545.9 m2 g−1) and heterogeneous interfacial structure. This work provides valuable insight into designing efficient bifunctional oxygen electrocatalysts for rechargeable Zn-air batteries.

Exploring the Role of Carbon Nanosheets for Detoxification of Cr(VI) from Aqueous Solution

Toxic pollutants in wastewater must be reduced in order to protect the aquatic ecosystem's stability and the public's health. Finding affordable and effective technologies for treating municipal, horticultural, aquacultural and industrial wastewater is urgently needed. Nitrogen-doped carbon nanosheets (N-CNS), which are produced by hydrothermal reaction from glycerol, sulfuric acid and melamine, have strong adsorptive behaviour against hazardous aqueous pollutants such as heavy metals and organic compounds. The overall elemental composition of CNS is altered by nitrogen incorporation, favouring CNS interaction with pollutants. The objective of the current investigation was to investigate the possibility for Chromium(VI) [Cr(VI)] adsorption on the CNS from a liquid solution. The ideal pH for Cr (VI) adsorption was noted to be 2.0. The Cr(VI) adsorption was enhanced when the starting metal concentration is more up to 700 mg L-1. A maximum removal of 256.41 mg g-1was seen when pH was 2.0 at 700 mg L-1 initial Cr(VI) concentration. We employed both the Freundlich and the Langmuir adsorption isotherms to determine the adsorption equilibrium constants. Using fitting curves and correlation coefficients (R2), it has been found that the model of the Langmuir isotherm is a best fit and it indicates homogeneous surface of CNS.

In-situ construction of nitrogen-doped porous carbon nanosheets supported well-dispersed Fe3O4 nanoparticles for efficient purification of antibiotic wastewater via peroxydisulfate activation

Heterogeneous catalysts composed of transition metal oxides and carbon-based materials have displayed significant potential in persulfates activation for the elimination of diverse refractory organic pollutants. Herein, the nitrogen-doped porous carbon (N-pC) nanosheets supported well-dispersed Fe3O4 nanoparticles (Fe3O4/N-pC) were meticulously designed and fabricated. This fabrication process involved the creation of Fe3+/(CN@PDA) precursor through loading polydopamine-Fe3+ complex on graphitic carbon nitride (g-C3N4) and the following calcination process, resulting in in-situ formation of Fe3O4 nanoparticles on the N-pC nanosheets that were derived from polydopamine coated g-C3N4. The large specific surface area, coupled with accessible Fe2+/Fe3+ species, facilitated the synergy of adsorption and catalysis, enabling the rapid elimination of antibiotics via peroxydisulfate (PDS) activation. The optimal Fe3O4/N-pC catalyst demonstrated a remarkable efficacy in the degradation of tetracycline-hydrochloride (TC), reaching a quasi-first-order kinetic constant of 0.1479 min−1, which was 1.95 times that of the degradation reaction using g-C3N4 (0.0758 min−1). Mechanistic investigations revealed that both radicals (·O2-,·OH and SO4·-) and non-radical (1O2 and electron transfer) oxidation pathways were involved in TC degradation. The toxicities of degradation intermediates were assessed through a bean-sprout planting experiment and the quantitative structure-activity relationship (QSAR) analysis. This work offers some guidance on the preparation and application of heterogeneous catalysts for effectively removing organic contaminants from water.

A nitrogen-doped carbon nanosheet composited platinum-cobalt single atom alloy catalyst for effective hydrogen evolution reaction.

An electrocatalyst with ultra-small PtCo single atom alloy species evenly dispersed on nitrogen-doped ultra-thin carbon nanosheets (PtCo SAA/NC) was designed. The introduction of single-atom Pt not only maximizes the atomic utilization efficiency of Pt species, but also synergistically enhances the charge transfer characteristics of Co cluster surfaces, thereby increasing the migration and evolution rate of hydrogen ions. The PtCo SAA/NC catalyst exhibits a Tafel slope of 42 mV dec-1 and a low overpotential of 45 mV at 10 mA cm-2 in 0.5 M H2SO4 solution.

A novel electrochemical sensor based on a Cu-coordinated molecularly imprinted polymer and MoS2 modified chitin-derived carbon for selective detection of dextromethorphan.

Dextromethorphan (DXM) is a widely utilized central antitussive agent, which is frequently abused by individuals seeking its recreational effect. But DXM overdose can cause some adverse effects, including brain damage, loss of consciousness, and cardiac arrhythmias, and hence its detection is significant. Herein, an electrochemical sensor based on a Cu-coordinated molecularly imprinted polymer (Cu-MIP) was fabricated for its detection. For constructing the sensor, nitrogen-doped carbon nanosheets (CCNs) were prepared through calcining chitin under an argon atmosphere, and molybdenum disulfide (MoS2) was allowed to grow on their surface. Subsequently, the obtained MoS2/CCNs composite was employed to modify a glassy carbon electrode (GCE), and the Cu-MIP was electrodeposited on the electrode in a Cu-1,10-phenanthroline (Cu-Phen) solution containing DXM, where Cu2+ played a role in facilitating electron transfer and binding DXM. Due to the large specific surface area, good electrocatalytic properties and recognition of the resulting composite, the resulting Cu-MIP/MoS2/CCNs/GCE showed high selectivity and sensitivity. Under optimized experimental conditions, the peak current of DXM and its concentration exhibited a good linear relationship over the concentration range of 0.1-100 μM, and the limit of detection (S/N = 3) was 0.02 μM. Furthermore, the electrochemical sensor presented good stability, and it was successfully used for the determination of DXM in pharmaceutical, human serum and urine samples.

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.

High density iridium synergistic sites boosting CO-tolerate performance for PEMFC anode

The usage of cheap crude H2 in proton-exchange membrane fuel cells (PEMFCs) is still unrealistic to date, due to the suffering of the current Pt based nano-catalysts from impurities such as CO in anode. Recently, synergistic active sites between single atom (SA) and nanoparticle (NP) have been found to be promising for overcoming the poisoning problem. However, lengthening the nanoparticle-single atom (SA-NP) interface, i.e., constructing high density synergistic active sites, remains highly challenging. Herein, we present a new strategy based on molecular fusion strategy to create abundant SA-NP interfaces, with high density SA-NP interfaces created on a 2D nitrogen doped carbon nanosheets (Ir-SACs&NPs/NC). Owing to the abundance of SA-NP interface sites, the catalyst was empowered with a high tolerance towards up to 1000 ppm CO in H2 feed. These findings provide guidelines for the design and construction of active and anti-poisoning catalysts for PEMFC anode.

Three-dimensional N-doped carbon nanosheets loaded with heterostructured Ni/Ni3ZnC0.7 nanoparticles for selective and efficient CO2 reduction.

Electrocatalytic CO2 reduction (CO2RR) has emerged as a promising approach for converting CO2 into valuable chemicals and fuels to achieve a sustainable carbon cycle. However, the development of efficient electrocatalysts with high current densities and superior product selectivity remains a significant challenge. In this study, we present the synthesis of a porous nitrogen-doped carbon nanosheet loaded with heterostructured Ni/Ni3ZnC0.7 nanoparticles through a facile hydrothermal-calcination method (Ni/Ni3ZnC0.7-NC). Remarkably, the Ni/Ni3ZnC0.7-NC catalyst exhibits outstanding performance towards CO2RR in an H-cell, demonstrating a high CO faradaic efficiency of 92.47% and a current density (jCO) of 15.77 mA cm-2 at 0.87 V vs. RHE. To further explore its potential industrial applications, we constructed a flow cell and a rechargeable Zn-CO2 flow cell utilizing the Ni/Ni3ZnC0.7-NC catalyst as the cathode. Impressively, not only does the Ni/Ni3ZnC0.7-NC catalyst achieve an industrial high current density of 254 mA cm-2 at a voltage of -1.19 V vs. RHE in the flow cell, but it also exhibits a maximum power density of 4.2 mW cm-2 at 22 mA cm-2 in the Zn-CO2 flow cell, while maintaining excellent rechargeability. Density functional theory (DFT) calculations indicate that Ni/Ni3ZnC0.7-NC possesses more spontaneous reaction pathways for CO2 reduction to CO, owing to its heterogeneous structure in contrast to Ni3ZnC0.7-NC and Ni-NC. Consequently, Ni/Ni3ZnC0.7-NC demonstrates accelerated CO2RR reaction kinetics, resulting in improved catalytic activity and selectivity for CO2RR.