N-doped Carbon Support Research Articles

Effect of N-Doped Carbon on the Morphology and Oxygen Reduction Reaction (ORR) Activity of a Xerogel-Derived Mn(II)O Electrocatalyst

This work synthesizes a xerogel from a sol–gel synthesis strategy and supports it on N-doped carbon support from spent coffee biomass (Mn(II)O/N-CC, hereafter MnO) as an efficient oxygen reduction reaction (ORR) catalyst in alkaline electrolytes. The effects of N-CC carbon content on MnO nanoparticle size, dispersion, distribution, morphology, and electrochemistry on ORR are discussed. The SEM and TEM measurements show that increasing the N-CC content during the MnO gelation reaction improved MnO dispersion and particle size during thermal treatment, increasing the ORR’s electrochemical active surface area. Several physiochemical and electrochemical characterizations show a clear relationship between N-CC catalysts and ORR activities. The best catalyst, MnO/N-CC-5, had an even distribution of 27 nm MnO nanoparticles on the N-CC support. The MnO/N-CC-5 catalyst had almost identical ORR kinetics and stability to those of the state-of-the-art Pt/C catalyst in 0.1 M KOH electrolytes, losing only 10 mV in half-wave potential after 5000 potential cycles and retaining 96% of current for over 10 h of continuous chronoamperometric stability. By measuring the electrochemical active surface areas of various catalysts by cyclic voltammetry at different scan rates and measuring the double layer capacitance (Cdl) and ECSA, MnO/N-CC-5 catalysts were shown to have enhanced ORR activity. The XPS analysis explains the ORR activity in terms of the Mn3+/Mn4+ ratio, and a mechanism was proposed. These findings suggest that the MnO/N-CC-5 catalyst could be a cathode catalyst in fuel cells, biofuel cells, metal–air batteries, and other energy conversion devices.

Efficient hydrodeoxygenation of lignin-derived phenolics to cyclohexanol with N-doped alumina- carbide‐based RuCo catalysts derived from MOF under mild conditions

In this work, a novel RuCo bimetallic supported on N-doped carbon support containing alumina was prepared by in-situ pyrolysis using MOF-303 as the support precursor (Ru3Co1@CN-Al2O3), and it was applied to the efficient hydrodeoxygenation (HDO) of guaiacol under mild conditions (0.01 MPa H2, 200 °C, 3h), the yield of cyclohexanol reaches an impressive 83.12 %. In the absence of external hydrogen (2 MPa N2, 220 °C, 2 h), complete conversion of guaiacol was achieved, along with a remarkable 97.81 % selectivity towards cyclohexanol. The HDO of guaiacol under different atmospheres was further studied, and the possible mechanism was proposed. Characterization results indicated that the supported metals (Ru and Co) not only interacted with the N in the MOF-303 to enhance catalyst stability but also that the synergistic effect between Ru and Co was key to promoting the high yield of cyclohexanol through catalytic transfer hydrodeoxygenation (CTHDO) in isopropanol. Additionally, Ru3Co1@CN-Al2O3 was also effective in achieving the HDO of macromolecular lignin. This study provides a feasible approach for the high value-added green transformation of lignin and its derivatives under mild conditions, highlighting the significant potential of MOFs for lignin valorization.

Structure-Stability Relation of Single-Atom Catalysts under Operating Conditions of CO2 Reduction.

Single-atom catalysts (SACs) have exhibited exceptional atomic efficiency and catalytic performance in various reactions but suffer poor stability. Understanding the structure-stability relation is the prerequisite for stability optimization but has been rarely explored due to complexity of the degradation process and reaction environments. Herein, we successfully established the structure-stability relation of N-doped carbon-supports SACs (MN4 SACs) under working conditions of CO2 reduction, by using advanced constant-potential density functional theory calculations. Systematic mechanism investigation that considered different factors identifies the key role of initial hydrogen adsorption on the coordination N atom in catalytic stability, where the feasibility of the adsorption eventually determines the leaching of the metal atom. On this basis, a simple descriptor consisting of electron number and electronegativity is constructed, realizing accurate and rapid prediction of the stability of SACs. Furthermore, strategies via modifying the local geometric structure to improve the stability without changing the active centers are proposed accordingly, which are supported by related experiments. These findings fill the current void in understanding SAC stability under practical working conditions, potentially advancing the widespread application of SACs in sustainable energy conversion systems.

Enhanced oxygen reduction reaction with rare-earth metal-based Ce-N-C catalyst

An atomically dispersed single atom catalyst based on rare-earth metal, Cerium embedded into the porous N-doped carbon (Ce-N-C), has been synthesized by using metal-organic framework method. The Ce-N-C catalyst have been physiochemically and electrochemically characterized in detail. Transmission electron microscope studies revealed atomically dispersed Ce atoms on the N-doped carbon support. The electrochemical oxygen reduction reaction (ORR) kinetics of Ce-N-C-3 catalyst revealed an admirable activity with a half-wave potential of 0.89 V, nearly equal to state-of-the-art Pt/C catalyst. The K-L plots and RRDE measurements revealed a nearly direct 4 electron reduction of O2 to H2O by Ce-N-C-3 catalyst. In addition, the chronoamperometry studies with a simulated H2O2 environments clearly revealed the significance of Ce3+/Ce4+ redox couple in deactivating hydrogen peroxide and/or hydroperoxide radicals. The commendable ORR activity, stability and peroxide resistance of Ce-N-C-3 catalysts is credited to the high surface area, atomically dispersed Ce atoms, formation of Ce-N4-C active sites in the catalysts, evidenced from the XPS analysis, in addition to the significance of Ce3+/Ce4+ redox couple in the catalyst. Most importantly, chronoamperometric studies revealed clear evidence of Ce3+/Ce4+ couple significance, helping in effectively mitigating the peroxide related detrimental effects to the ORR catalyst.

Development of Iron-Based Single Atom Materials for General and Efficient Synthesis of Amines.

Earth abundant metal-based heterogeneous catalysts with highly active and at the same time stable isolated metal sites constitute a key factor for the advancement of sustainable and cost-effective chemical synthesis. In particular, the development of more practical, and durable iron-based materials is of central interest for organic synthesis, especially for the preparation of chemical products related to life science applications. Here, we report the preparation of Fe-single atom catalysts (Fe-SACs) entrapped in N-doped mesoporous carbon support with unprecedented potential in the preparation of different kinds of amines, which represent privileged class of organic compounds and find increasing application in daily life. The optimal Fe-SACs allow for the reductive amination of a broad range of aldehydes and ketones with ammonia and amines to produce diverse primary, secondary, and tertiary amines including N-methylated products as well as drugs, agrochemicals, and other biomolecules (amino acid esters and amides) utilizing green hydrogen.

Lignin-tailored fabrication of Ni single atom catalyst with Ni-N3 active site for efficient and selective catalytic transfer hydrogenation of lignin-derived aldehydes

Developing sustainable catalytic processes for catalytic transfer hydrogenation (CTHDO) of lignin-derived aldehydes to renewable fuels and chemicals is essential for scale valorization of vast underused lignin. Herein, the work contributes to the efficient and selective vanillin (VAN) CTHDO process using formic acid (FA) as the H-donor over a novel lignin-coordinated N-anchoring Ni single-atom catalyst (Ni SAs-N@LC). Ni SAs-N@LC was fabricated through facile pyrolysis of lignin-Ni/Zn complex mixed with melamine, in which lignin localized the Ni atoms through its negatively charged groups (e.g. phenolic OH) and the dispersed Ni atoms were further anchored by the N-doped carbon support to form Ni-N3 active structure. DFT calculations revealed that the Ni-N3 structure preferentially adsorbed the –CHO end of VAN and endowed the catalyst with superior hydrogen evolution capacity. Therefore, Ni SAs-N@LC exhibited outstanding catalytic performance (98.93% of VAN conversion and 97.3% of 2-methoxy-4-methylphenol selectivity) which was significantly higher than two reference catalysts Ni NPs@LC (without N-anchoring) and Ni@C (without lignin coordination and N-anchoring) as well as the previously reported Ni-based catalysts. Moreover, Ni SAs-N@LC presented excellent feasibility to the CTHDO of a wide range of lignin-derived aldehydes and exhibited superior cycling durability in FA system owing to its acid resistance property. Consequently, this work provides a facile preparation method for atomically dispersed biomass-based catalysts and further demonstrates its favorable applicability in the CTHDO of lignin-derived aldehydes.

High-performance electrocatalyst for PEMFC cathode: Combination of ultra-small platinum nanoparticles and N-doped carbon support

To accelerate the implementation of zero-emission power installations based on proton-exchange membrane fuel cells, it is necessary to maximize the power characteristics of these devices. For this purpose, we have obtained and tested a new N-doped carbon support and a synthesized Pt/C catalyst based on it with a platinum loading of about 37.3 %. A comparison of the degradation resistance of the initial support and the N-doped one has shown greater stability of the latter. At the same time, Raman spectroscopy has confirmed the presence of the C–N bond, which indicates the successful doping of carbon with nitrogen. The resulting Pt/C catalyst based on an N-doped support is characterized by a substantially narrow size dispersion and an ultra-small nanoparticle size of about 2.6 nm. The high-angle annular dark-field scanning transmission electron microscopy images of the synthesized catalyst have confirmed the presence of individual platinum atoms/clusters uniformly distributed over the surface of the support, and their presence is due to nitrogen embedded into the carbon structure. This material is characterized by a 50 m2 gPt-1 larger electrochemically active surface area and a 227 A gPt-1 greater mass activity compared to the commercial JM40 analog (40 % platinum loading). Meanwhile, the electrochemical parameters remaining after the accelerated stress testing are almost 2 times higher than those of JM40. And the power characteristics in the membrane electrode assembly for the catalyst synthesized by the facile one-pot synthesis method are 13 % (575 mW cm-2) higher than those of the commercial analog (500 mW cm-2). The Pt/C catalyst obtained during the research is deemed promising for commercial use in proton-exchange membrane fuel cells.

Deciphering nanostructural evolution of PtCu/C–N electrocatalyst via identical location transmission electron microscopy imaging: Gram-scale synthesis and superior activity in oxygen reduction reaction

Electrocatalysts play a pivotal role in advancing proton-exchange membrane fuel cell (PEMFC) for hydrogen energy applications. In this study, we investigate a novel PtCu/CN electrocatalyst synthesized via a gram-scale synthesis approach, which demonstrates remarkable activity and stability in the oxygen reduction reaction (ORR). The catalyst's effectiveness stems from its unique structure, combining bimetallic nanoparticles (NPs) and an N-doped carbon support. Employing identical location transmission electron microscopy (IL-TEM) imaging, we observe significant NP structure reorganization upon activation influenced by the upper limiting potential. Notably, the PtCu/CN catalyst activated to 1.0 V surpasses the United States Department of Energy (DOE) target for ORR activity by 3.3-fold. These findings underscore the potential of this catalyst in enhancing the performance of PEMFCs, marking a significant advancement in hydrogen energy technology.

Insightful Understanding of Synergistic Oxygen Reduction on PtCo3(111) Toward Zinc-Air Batteries.

Theory-guided materials design is an effective strategy for designing catalysts with high intrinsic activity whilst minimizing the usage of expensive metals like platinum. As proof-of-concept, herein it demonstrates that using density functional theory (DFT) calculations and experimental validation that intermetallic PtCo3 alloy nanoparticles offer enhanced electrocatatalytic performance for the oxygen reduction reaction (ORR) compared to Pt nanoparticles. DFT calculations established that PtCo3(111) surfaces possess better intrinsic ORR activity compared to Pt(111) surfaces, owing to the synergistic action of adjacent Pt and Co active sites which optimizes the binding strength of ORR intermediates to boost overall ORR kinetics. With this understanding, a PtCo3/NC catalyst, comprising PtCo3 nanoparticles exposing predominantly (111) facets dispersed on an N-doped carbon support, is successfully fabricated. PtCo3/NC demonstrates a high specific activity (3.4mAcm-2mgPt -1), mass activity (0.67AmgPt -1), and cycling stability for the ORR in 0.1M KOH, significantly outperforming a commercial 20wt.% Pt/C catalyst. Moreover, a zinc-air battery (ZAB) assembled with PtCo3/NC as the air-electrode catalyst delivered an open-circuit voltage of 1.47V, a specific capacity of 775.1mAhgZn -1 and excellent operation durability after 200 discharge/charge cycles, vastly superior performance to a ZAB built using commercial Pt/C+IrO2 as the air-electrode catalyst.

Features of behavior and morphological stability of the N-doped PtCu/C catalyst

A high-performance electrocatalyst based on bimetallic platinum-containing nanoparticles for PEMFCs has been presented. The combination of bimetallic nanoparticles and an N-doped carbon support ensures high ORR activity and stability of the catalyst. The single-reactor method to obtain the material and its higher functional characteristics allow considering the resulting PtCu/C-N electrocatalyst as a promising commercial product. An extended study of morphological characteristics has been conducted to understand the processes of evolution for this material. The in-situ IL-TEM research has allowed studying in detail the degradation process for the material during high-temperature treatment by analyzing changes in the type of histograms of the nanoparticles size distribution and testing the method for calculating the number of their intersections to assess the dynamics of the material degradation.

Controlled dispersion of Ni catalyst on N-doped carbon support for stable and selective hydrogen production from formic acid

Formic acid is a liquid organic hydrogen carrier from which hydrogen can be released together with CO2 by catalytic decomposition. The development of supported Ni catalysts for H2 production is important. Here, the effects of Ni state/dispersion are considered. For this purpose, three samples were prepared with about 3 wt% Ni deposited on porous N-doped carbon. The first sample contained predominantly Ni nanoparticles (∼2 nm), the second contained Ni clusters (<1 nm), and the third – single-atom Ni sites. The catalysts showed close activity in the gas-phase reaction. However, a minimum apparent activation energy of 105 kJ/mol and a maximum selectivity towards H2 production of 99% were achieved for the single-atom Ni catalyst. The nature of its single-atom sites was established to correspond to Ni-N4 and Ni-O4, which showed greater stability under the conditions of the catalytic reaction.

Sulfur-Induced Electronic Optimization of N-Doped Carbon with CoP/Co2P Heterostructure by Precursor Design for Rechargeable Zinc-Air Batteries.

Heteroatom doping and heterostructure construction are the key methods to improve the performance of electrocatalysts. However, developing such catalysts remains a challenging task. Herein, we designed two comparable polymers, phytic acid/thiourea polymer (PATP) and phytic acid/urea polymer (PAUP), as precursors, which contain C, N, S/O, and P by microwave heating. To pinpoint how the introduction of sulfur would affect the electronic structure and catalytic activity, these two polymers were physically blended with CoCo-Prussian blue analogue (CoCo-PBA) and further calcination, respectively. The highly dispersed CoP/Co2P-rich interfacial catalysts anchored on the N,S-codoped or N-doped carbon support were successfully prepared (CoP/Co2P@CNS and CoP/Co2P@CN). The prepared CoP/Co2P@CNS catalyst showed good ORR properties (E1/2 = 0.856 V vs RHE) and OER properties (Ej10 = 1.54 V vs RHE), which were superior to the commercial Pt/C and RuO2 catalysts. The reversible oxygen electrode index (ΔE = Ej10 - E1/2) can reach ∼0.684 V. Meanwhile, the rechargeable zinc-air battery assembled with a CoP/Co2P@CNS catalyst as the air cathode also showed excellent performance, with a charge-discharge cycle stability of up to 900 h. DFT calculations further confirm that the introduction of S atoms can affect the electronic structure and enhance the catalytic activity of C and N atoms on carbon support.

Highly coordinated Ni-N5 sites for efficient electrocatalytic CO2 reduction toward CO with faradaic efficiency exceeding 99%

Electrochemical production of high value-added CO from CO2 on transition metal-nitrogen-carbon (M−N−C) catalysts is a promising approach to achieve carbon neutral economy, yet the quest for robust catalysts is driven by achieving > 96 % CO faradaic efficiency (FE) under low overpotential and wide potential range. Herein, we report a novel synthetic approach involving post-metallization of the pre-synthesized N-doped carbon (NC-T) support for the fabrication of robust and efficient Ni@NC-T quasi-molecular catalysts toward CO2 electroreduction reaction (CO2RR). The optimum Ni@NC-1100 catalyst exhibited an extremely high FECO > 99 % at −0.72 V vs. reversible hydrogen electrode (RHE). Of interest is the FECO maintained above 96 % over a wide potential window from −0.52 V to −1.12 V. Density functional theory (DFT) calculation validated that the presence of axial pyrrolic-N significantly enhances the Ni-N5 active site for CO2 activation, resulting in the lowest activation energy for the *COOH intermediate generation compared to other axial ligands.

Manipulating electrochemical CO2 reduction pathway by engineering energy level of Cu/Zn dual-metal single atom catalysts

Dual-metal single atom catalysts (DSACs) demonstrate outstanding catalytic performance in the CO2 reduction reaction. However, the complexity of catalyst structures and interface environments has led to an unclear understanding of the synergistic catalysis mechanism involved. Here, we developed a series of catalysts with atomically dispersed Cu–N4 and Zn–N4 sites on N-doped carbon supports (Cu1-xZnx-NC), which can efficiently reduce CO2 to C2 products by optimizing the Zn loading. Specifically, a remarkable faradaic efficiency of 65 % at −1.1 VRHE for the C2 products on the Cu0.75Zn0.25-NC catalyst has been obtained. Structural characterizations and density functional theory calculations demonstrate that Cu/Zn DSACs synergistically lower the energy barrier of the rate-determining step and facilitate proton transfer kinetics. Among them, Zn atoms activate CO2, while Cu atoms aid in the adsorption and dissociation of intermediates. The electron energy redistribution induced by adjacent Cu–N4 and Zn–N4 site optimizes the 3d orbitals of Cu centers, thereby accelerating and promoting C–C coupling. The energy level optimization of Cu/Zn DSACs results in Cu0.75Zn0.25-NC with a high C2 selectivity and activity, improved kinetics. In summary, these findings provide new insights into the development of highly efficient DSACs and its synergistic catalysis mechanism in CO2 reduction.

Ni─Co─O─S Derived Catalysts on Hierarchical N-doped Carbon Supports with Strong Interfacial Interactions for Improved Hybrid Water Splitting Performance.

Simultaneously improving electrochemical activity and stability is a long-term goal for water splitting. Herein, hierarchical N-doped carbon nanotubes on carbon nanowires derived from PPy are grown on carbon cloth, serving as a support for NiCo oxides/sulfides. The hierarchical electrodes annealed in N2 or H2/N2 display improved intrinsic activity and stability for hydrogen evolution reaction (HER) and glucose oxidation reaction. Compared with Pt/C||Ir/C in alkaline media, the glucose electrolysis assembled with electrodes exhibits a cell voltage of 1.38V at 10mAcm-2, durability for >12h at 50mAcm-2, and resistance to glucose/gluconic acid poisoning. In addition, electrocatalysts can also be applied in ethanol oxidation reactions. Systematic characterizations reveal the strong interactions between NiCo and N-doped carbon support-induced partial charge transfer at the interface and regulate the local electronic structure of active sites. Density functional theory calculations demonstrate that the synergistic effect between N-doped carbon supports, metallic NiCo, and NiCo oxides/sulfides optimize the adsorption energy of H2O and the H* free energy for HER. The energy barrier of the dehydrogenation of glucose effectively decreased. This work will attract attention to the role of metal-support interactions in enhancing the intrinsic activity and stability of electrocatalysts.

Ir nanoclusters on ZIF-8-derived nitrogen-doped carbon frameworks to give a highly efficient hydrogen evolution reaction

The precise change of the electronic structure of active metals using low-active supports is an effective way of developing high-performance electrocatalysts. The electronic interaction of the metal and support provides a flexible way of optimizing the catalytic performance. We have fabricated an efficient hydrogen evolution reaction (HER) electrocatalyst, in which Ir nanoclusters are uniformly loaded on a nitrogen-doped carbon framework (Ir@NC). The synthesis process entails immersing an annealed zeolitic imidazolate framework-8 (ZIF-8), prepared at 900 °C as a carbon source, into an IrCl3 solution, followed by a calcination-reduction treatment at 400 °C under a H2/Ar atmosphere. The three-dimensional porous structure of the nitrogen-doped carbon framework exposes more active metal sites, and the combined effect of the Ir clusters and the N-doped carbon support efficiently changes the electronic structure of Ir, optimizing the HER process. In acidic media, Ir@NC has a remarkable HER electrocatalytic activity, with an overpotential of only 23 mV at 10 mA cm−2, an ultra-low Tafel slope (25.8 mV dec−1) and good stability for over 24 h at 10 mA cm−2. The high activity of the electrocatalyst with a simple and scalable synthesis method makes it a highly promising candidate for the industrial production of hydrogen by splitting acidic water.

Dehydrative decarbonylation of fatty acids into long-chain olefins over CoNx/NC catalysts

The development of highly efficient, low-cost supported catalysts is crucial for directly deoxygenating biomass fatty acids to long-chain olefins. However, additive-free olefin production, by dehydrative decarbonylation from fatty acids, is scarcely conducted owing to competing decarboxylation reactions. Herein, a green and cost-effective strategy is presented to improve the Co-catalyzed dehydrative decarbonylation of stearic acid, which produces a mixture of heptadecenes with yields of up to 41.3 % and a paraffin yield of 14.7 %. Experimental data, along with a detailed catalyst characterization, revealed that the surface CoNx species acted as the dominant active sites. Furthermore, the specific catalytic performance can be attributed to the dense defect sites, abundant vacancies, and mesoporous structures of the N-doped Carbon (NC) support. The as-prepared CoNx/NC catalysts were recovered and reused up to three times without significant deactivation. Additionally, we propose a possible reaction mechanism for fatty acid deoxygenation. This research makes a significant contribution toward advancing the performance of noble-metal-free deoxygenation catalysts for the production of unsaturated compounds in biomass conversions.

Hierarchically porous architecture of metal–organic framework-derived and S induced electron localization of Fe single atom sites for boosted ORR

Metal-organic frameworks (MOFs), with their high specific surface area, excellent stability and high electron transfer ability, are ideal supports for accommodating single metal atoms. However, the low utilisation of single-atom active sites limits the improvement of oxygen reduction reaction (ORR) performance.In this work, NH2-MIL-53(Al), a MOF possessing a mesoporous cage architecture, is used as the precursor to prepare N-doped carbon supports (denoted herein as N-HPC) with a well-defined mesoporous structure through pyrolysis. Thiourea was further employed for S doping and impregnated with a FePc, and heated again to yield Fe@S/N-HPC catalysts rich in accessible FeNx single atom sites. The porous structure is more accessible to Fe center atoms by exposing the active sites, provide easy electron conductivity and facilitate mass transport of ORR-intermediates. The prepared hierarchically porous architecture of NH2-MIL-53(Al)-derived and S induced electron localization of Fe SAs sites exhibit excellent ORR performance in alkaline (E1/2 = 0.88 V) medium.

Activity of Platinum-Based Cathode Electrocatalysts in Oxygen Redaction for Proton-Exchange Membrane Fuel Cells: Influence of the Ionomer Content

Studying the ORR activity of platinum-based electrocatalysts is an urgent task in the development of materials for proton-exchange membrane fuel cells. The catalytic ink composition and the formation technique of a thin layer at the RDE play a significant role in studying ORR activity. The use of a polymer ionomer in the catalytic ink provides viscosity as well as proton conductivity. Nafion is widely used as an ionomer for research both at the RDE and in the MEA. The search for ionomers is a priority task in the development of the MEA components to replace Nafion. The study also considers the possibility of using the LF4-SK polymer as an alternative ionomer. The comparative results on the composition and techniques of applying the catalytic layer using LF4-SK and Nafion ionomers are presented, and the influence of the catalytic ink composition on the electrochemical characteristics of commercial platinum–carbon catalysts and a highly efficient platinum catalyst based on an N-doped carbon support is assessed.

Enhancing oxygen reduction activity of dinuclear copper complexes loaded on an N-doped carbon support via a low-temperature pyrolysis strategy.

Bioinspired by the active sites of multicopper oxidases (MCOs), bi/multinuclear copper complexes have attracted great attention in promoting catalytic activity for the oxygen reduction reaction (ORR). Herein, we report the preparation of a Cu-N-C electrocatalyst Cu-BPOZ@CNB-400 for efficient ORR, which was obtained by low temperature pyrolysis of a dinuclear 2,5-bis(2-pyridyl)-1,3,4-oxadiazole (BPOZ) copper complex loaded on a N-doped carbon support at 400 °C. Cu-BPOZ@CNB-400 exhibited a half-wave potential (E1/2) of 0.86 V vs. RHE for the ORR in 0.1 M KOH solution, which was significantly higher than that of the Cu-BPOZ@CNB-800 (E1/2 = 0.83 V) catalyst treated under high temperature (at 800 °C) and the control catalyst Cu-Phen@CNB-400 (E1/2 = 0.82 V) derived from low-temperature-treatment (at 400 °C) of a mononuclear phenanthroline-coordinated-Cu complex loaded on a N-doped carbon support. When Cu-BPOZ@CNB-400 was applied as the cathode catalyst in zinc-air batteries a maximum power density (Pmax) of 127 mW cm-2 could be achieved, demonstrating comparable catalyst performance to the commercial 20 wt% Pt/C (Pmax = 122 mW cm-2) and the control Cu-Phen@CNB-400 catalyst (Pmax = 105 mW cm-2) under similar experimental conditions. Low-temperature pyrolysis of dinuclear copper complexes on a carbon support improved the charge transfer efficiency, inhibited metal aggregation, and could produce highly dispersed Cu-N-C catalysts with dinuclear copper sites for promoting the 4e--reduction selectivity of the ORR. It thus provides a cost-effective approach for the controllable fabrication of efficient ORR catalysts to be applied for energy conversion devices.