Nanoneedle Arrays Research Articles

Bi2O3 nanosheet-coated NiCo2O4 nanoneedle arrays for high-performance supercapacitor electrodes

Supercapacitors are a promising option for next-generation clean energy storage devices, although their capacitance must still be improved through an appropriate choice of electrode material. Herein, NiCo2O4 nanoneedles coated with Bi2O3 nanosheets are successfully prepared using a two-step hydrothermal process to produce electrodes that may be used for supercapacitors. The proposed electrodes are analyzed using both a range of experimental measurement techniques and density functional theory simulations. The NiCo2O4 nanoneedles provide an ideal skeleton for improving specific surface area and present electrical active sites for the Faraday reaction, while Bi2O3 nanosheets have a great potential for use in supercapacitor applications. The proposed NiCo2O4@Bi2O3 electrode shows a high capacity of 766 F g−1 at 1 A g−1. In addition, an asymmetric supercapacitor based on a NiCo2O4@Bi2O3 positive electrode and activated carbon was produced, which provided a working voltage of 1.6 V, achieved a high energy density of 24 Wh kg−1 at 800 W kg−1, and demonstrated excellent cycling stability (capacitance retention of 82 % after 10,000 cycles at 10 A g−1). These results demonstrate that the proposed NiCo2O4@Bi2O3 heterostructure exhibits potential for application in high-performance supercapacitors.

Vertically Aligned Boron-Doped Diamond Hollow Nanoneedle Arrays for Enhanced Field Emission

Vertically Aligned Boron-Doped Diamond Hollow Nanoneedle Arrays for Enhanced Field Emission

Ordered Ag Nanoneedle Arrays with Enhanced Electrocatalytic CO2 Reduction via Structure-Induced Inhibition of Hydrogen Evolution.

Silver is an attractive catalyst for converting CO2 into CO. However, the high CO2 activation barrier and the hydrogen evolution side reaction seriously limit its practical application and industrial perspective. Here, an ordered Ag nanoneedle array (Ag-NNAs) was prepared by template-assisted vacuum thermal-evaporation for CO2 electroreduction into CO. The nanoneedle array structure induces a strong local electric field at the tips, which not only reduces the activation barrier for CO2 electroreduction but also increases the energy barrier for the hydrogen evolution reaction (HER). Moreover, the array structure endows a high surface hydrophobicity, which can regulate the adsorption of water molecules at the interface and thus dynamically inhibit the competitive HER. As a result, the optimal Ag-NNAs exhibits 91.4% Faradaic efficiency (FE) of CO for over 700 min at -1.0 V vs RHE. This work provides a new concept for the application of nanoneedle array structures in electrocatalytic CO2 reduction reactions.

Phosphorus-induced electronic structure reformation of hollow NiCo2Se4 nanoneedle arrays enabling highly efficient and durable hydrogen evolution in all-pH media

Phosphorus-induced electronic structure reformation of hollow NiCo2Se4 nanoneedle arrays enabling highly efficient and durable hydrogen evolution in all-pH media

Enhanced electrochemical performance of the cobalt chloride carbonate hydroxide hydrate via micromorphology and phase transformation

Micromorphology and conductivity are two vital factors for the practical capacitance of the electrode materials for supercapacitors. In this work, a novel two-step electrochemical activation method involving a cyclic voltammetry (CV) treatment within 0–0.7 V followed by a CV treatment within −1.2–0 V is explored to induce the micromorphology and phase transformation of the cobalt chloride carbonate hydroxide hydrate (CCCH) nanoneedle arrays. The first-step activation transforms the CCCH to Co(OH)2 and then the reversible transformation between Co(OH)2 and CoOOH generates plenty of pores in the sample, thereby increasing the specific capacitance from 0.54 to 1.74 F cm−2 at the current density of 10 mA cm−2. The second-step activation inducing the reversible transformation between Co(OH)2 and Co not only endows the final sample with a nanosheets-assembled fasciculate structure but also decreases the internal resistance via generating Co0 in the final sample (CCCH-P75N50). Consequently, the CCCH-P75N50 shows a high specific capacitance of 3.83 F cm−2 at the current density of 10 mA cm−2. Besides, the aqueous asymmetric supercapacitor assembled with CCCH-P75N50 and commercial conductive carbon cloth (CC) delivers a high energy density of 2.75 mWh cm−3 at a power density of 37.5 mW cm−3. This work provides a novel, facile and promising method to optimize the micromorphology and conductivity of Co-based electrodes.

Three-dimensional Setaria viridis-like NiCoSe2 nanoneedles array: As an efficient electrochemical hydrazine sensor

Transition metal selenides are widely used in electrocatalysis on account of high electrical conductivity, good stability and low cost. In this study, using nickel-cobalt layered double hydroxide (NiCo-LDH) as precursor, a simple two-step method was used to prepare three-dimensional (3D) Setaria viridis-like NiCoSe2 nanoneedles arrays on nickel foam (NiCoSe2 NNA/NF). Benefiting from the abundant catalytic active sites provided by the 3D nanoneedles array structure, the covalent reciprocity between Ni, Co and Se can effectively facilitate the free movement of ions and electrons on the electrode surface. As a hydrazine sensor, the electrochemical performance of the NiCoSe2 NNA/NF was studied by cyclic voltammetry (CV) and other electrochemical techniques, which exhibits outstanding electrocatalytic performance. When the signal-to-noise ratio is 3 (S/N = 3), the sensitivity is 16170 μA mM−1 cm−2, the lower detection limit is 0.5 μM. It also shows well anti-interference and long-term stability. In addition, the successful applications in water environments samples also demonstrated the feasibility of the sensor. This method provides a new idea for the development of selenide-based electrochemical sensors.

Electroplating CuO nanoneedle arrays on Ni foam as superior 3D scaffold for dendrite-free and stable Li metal anode

Undesirable dendrite growth and infinite volume expansion are the major barriers to the potential application for next-generation safe Li metal batteries. To solve these problems, we herein report electroplating CuO nanoneedle arrays on Ni foam (NCNF) as 3D porous framework for Li metal batteries. The influence of different morphologies of CuO on guiding Li plating/stripping behavior has been investigated. The homogenous deposition of Li can be attributed to the interspace between the CuO nanoneedles, which is remarkably superior over granular CuO on Ni foam (GCNF) at high areal capacity. The hierarchical skeleton can not only decrease local current inhomogeneity but also alleviate the volume change of Li. The NCNF electrode delivers a higher Coulombic efficiency of Li deposition comparing with the bare Ni foam and GCNF. Furthermore, enhanced cycling stability with small overpotential can be achieved in symmetric cells. In a Li/LiFePO4 full cell, the excellent cycling performance also proves the superiority of NCNF@Li composite electrode.

Abstract 3919: MosaicNeedles: A tool for large-scale proteomics combining antibodies and aptamers

Abstract Proteomics have the potential to transform biomarker discovery, diagnostics, and personalized medicine as it provides functional and actionable information linked to disease phenotypes. However, mass spectrometry (MS) – based proteomics has not been possible at large scale due to limited dynamic range, complex workflow and high experimental cost per sample. Antibody-based methods, although widely used in targeted proteomics for their better sensitivity, have been limited to the profiling of a few hundred selected proteins, partly due to the limited availability of antibody pairs. NanoMosaic has demonstrated antibody-aptamer sandwich assays on the MosaicNeedle࣪ platform. This expands the content size from a few hundred to a few thousand, achievable in one reaction with high sensitivity and specificity and low cross-reactivity. MosaicNeedles࣪ are densely integrated nanoneedle sensors fabricated on a planar substrate. 94,000 sensors with more than 2 billion total nanoneedles can be integrated on to a standard SBS plate, which can also be grouped into 96, 384 or 1536 formats. Each sensor contains an array of nanoneedles, dedicated to detecting one analyte of interest. All nanoneedles comprising the same sensor are functionalized with the same capture antibodies or aptamers. At low analyte concentration, the binding of proteins to the nanoneedles follows a Poisson distribution. Therefore, statistically, no more than one molecule is bound per nanoneedle. A further addition of aptamers or antibodies will form a sandwich complex with the target analyte. Since each of the nanoneedles has an intrinsic optical resonance spectrum and will red-shift as the sandwich complex forms on its surface, the number of analytes can be quantitated by simply counting the number of nanoneedles that display a color change. At high analyte concentration, each nanoneedle has more than one analyte, so the number of analytes can be calculated by averaging the spectrum shifts of all nanoneedles. This combined single molecule counting (digital) and spectrum shift (analog) analysis allows the platform to detect both high abundance and low abundance protein analytes in one reaction. We have demonstrated that the aptamer-antibody assay on the MosaicNeedle࣪ platform achieves better sensitivity than the well-developed antibody-pair assay. It also achieves larger dynamic range and alleviates the antibody cross-reactivity by refining aptamers during the SELEX process. The scalability in manufacturing nanoneedles combined with the low sample requirement and no fluorescent labeling all help to drive down the cost-per-protein to enable large-scale, unbiased proteomics. We envision researchers will use MosaicNeedle࣪ platform for both the upstream target discovery phase and then transfer seamlessly to the downstream validation phase by building customized and targeted panels for proteins of high interest that emerge from the discovery phase. Citation Format: Qimin Quan, Alaina Kaiser, Joshua Ritchey, Joe Wilkinson, John Geanacopoulos, John Boyce. MosaicNeedles: A tool for large-scale proteomics combining antibodies and aptamers [abstract]. In: Proceedings of the American Association for Cancer Research Annual Meeting 2022; 2022 Apr 8-13. Philadelphia (PA): AACR; Cancer Res 2022;82(12_Suppl):Abstract nr 3919.

Proteogenomic detection of circulating biomarkers for clinical oncology.

e15010 Background: Circulating biomarkers have the potential to detect cancer in its earliest stages and monitor patients in remission. The integration of proteogenomics in circulating biomarkers may transform the molecular diagnostics of cancer and accelerate basic and clinical oncology research. Proteomics bridges the gaps of functional information lost due to post-transcriptional and post-translational modifications in a genomic approach. A recent study showed that adding just 8 protein biomarkers to a panel of circulating DNA biomarkers increased the diagnostic accuracy up to 98% sensitivity and 99% specificity. However, the proteogenomic approach normally requires the use of multiple different assay technologies and laboratory workflows, including mass spectrometry. Methods: MosaicNeedles are densely integrated nanoneedle sensors fabricated on a planar substrate that integrates proteogenomic analysis in one platform. 94,000 sensors with more than 2 billion total nanoneedles can be integrated on to a standard SBS plate, which can be configured into 96, 384 or 1536 well format. Each sensor contains an array of nanoneedles, dedicated to detecting one analyte of interest. All nanoneedles comprising the same sensor are functionalized with the same capture probes. The capture probe can be either an antibody for protein detection or an oligonucleotide with a specific target sequence to a DNA fragment, mRNA, or miRNA of interest. Results: At low analyte concentration, the binding of proteins to the nanoneedles follows a Poisson distribution. Therefore, statistically, no more than one molecule is bound per nanoneedle. A further addition of aptamers or antibodies will form a sandwich complex with the target analyte. Since each of the nanoneedles has an intrinsic optical resonance spectrum and will red-shift as the sandwich complex forms on its surface, the number of analytes can be quantitated by simply counting the number of nanoneedles that display a color change. At high analyte concentration, each nanoneedle has more than one analyte, so the number of analytes can be calculated by averaging the spectrum shifts of all nanoneedles. This combined single molecule counting (digital) and spectrum shift (analog) analysis allows the platform to detect both high abundance and low abundance protein analytes in one reaction. A 10,000-plex study can be achieved with a total of 2.5 billion nanoneedles on a 50mm by 50mm consumable. In this consumable, a 2,000-plex proteome and 8,000 cell-free DNA fragments can be detected. Conclusions: A full proteogenomic quantification can be performed on the NanoMosaic platform in one reaction with high sensitivity and large dynamic range. It simplifies the workflow and allows users to integrate proteomic and genomic information to discover new circulating biomarkers.

Dense high aspect ratio nanostructures for cell chip applications - Fabrication, replication, and cell interactions

Culturing human cells on the surface of a microchip brings living cells in direct contact with artificial microstructured surfaces. This work focuses on the effect of high aspect ratio nanostructures – dense nanoneedle arrays – on the mechanical response and proliferation of fibroblasts. We present a fabrication process for micropatterned chips that feature areas with hierarchical high aspect ratio nanostructures directly adjacent to flat chip areas. The chip was pre-patterned by conventional lithography. We have fabricated “black silicon” arrays of densely packed, sharp, vertical nano-needles for high aspect ratio structures by cryogenic reactive ion etching in an SF 6 /O 2 plasma. An essential requirement for many real-life applications is to make such complex high aspect ratio 3D nanostructures available in larger areas. We have successfully demonstrated the 3D replication of black silicon by a UV- nanoimprint lithography process. This study provides insight into the extent to which such nanoneedle arrays influence the growth of human fibroblasts. We have investigated microstructured samples featuring a combination of (i) smooth surfaces and (ii) nanoneedle surfaces for the mechanical behavior and proliferation of fibroblasts. Our results show that the bonding viability and proliferation of the fibroblast on the high aspect ratio nano-needle surfaces differ significantly from flat surfaces. The nanoneedles only provide a minimum area for cell attachment compared to the neighboring flat, unstructured chip areas. • Development of a fabrication process for a dense nano-needle array. • Reproduction of black silicon using nanoimprint lithography. • Black silicon structures were investigated with regard to NIL replication and cell proliferation.

Engineering hierarchical quaternary superstructure of an integrated MOF-derived electrode for boosting urea electrooxidation assisted water electrolysis

Controllable design of the catalytic electrodes with hierarchical superstructures is expected to improve their electrochemical performance. Herein, a self-supported integrated electrode (NiCo-ZLDH/NF) with a unique hierarchical quaternary superstructure was fabricated through a self-sacrificing template strategy from the metal–organic framework (Co-ZIF-67) nanoplate arrays, which features an intriguing well-defined hierarchy when taking the unit cells of the NiCo-based layered double hydroxide (NiCo-LDH) as the primary structure, the ultrathin LDH nanoneedles as the secondary structure, the mesoscale hollow plates of the LDH nanoneedle arrays as the tertiary structure, and the macroscale three-dimensional frames of the plate arrays as the quaternary structure. Notably, the distinctive structure of NiCo-ZLDH/NF can not only accelerate both mass and charge transfer, but also expose plentiful accessible active sites with high intrinsic activity, endowing it with an excellent electrochemical performance for urea oxidation reaction (UOR). Specially, it only required the low potentials of 1.335, 1.368 and 1.388 V to deliver the current densities of 10, 100 and 200 mA cm−2, respectively, much superior to those for typical NiCo-LDH. Employing NiCo-ZLDH/NF as the bifunctional electrode for both anodic UOR and cathodic HER, an energy-saving electrolysis system was further explored which can greatly reduce the needed voltage of 213 mV to deliver the current density of 100 mA cm−2, as compared to the conventional water electrolysis system composed of OER. This work manifests that it is prospective to explore the hierarchically nanostructured electrodes and the innovative electrolytic technologies for high-efficiency electrocatalysis.

Exploration on the influence mechanism of nitrogen doped CoO on oxygen reduction and evolution reaction in Li–O2 battery

Admitting that the validity of heteroatom doped transition metal oxides in improving electrochemical performances in Li–O2 battery, the reasons for the improvement remains ambiguous. In this study, nitrogen as a heteroatom is introduced to the CoO nanoneedle arrays grown on the carbon cloth (NCoO NAs/CC), and the effects of nitrogen on the electrochemical behavior of Li–O2 batteries are comprehensively studied by experimental and theoretical calculations. With the incorporation of nitrogen, the catalytic activity of the prepared cathode is heavily enhanced through a combined set of factors, including enhanced electronic conductivity, optimized reactant/intermediates affinity, as well as improved reaction kinetics. In addition, further investigation on the morphology of the discharge products demonstrates that the introduction of nitrogen can also promote the solvation discharge path of the battery, which is conducive to the release of the battery capacity. Moreover, the introduction of nitrogen makes the discharge products on the cathode show nano-sheet structure, which is easier to be decomposed during charging. The electrochemical performances of the NCoO NAs/CC cathode including battery cycle efficiency, capacity and cycle stability are heavily enhanced due to the above advantages. The combination of doping engineering and electrochemical performances provides an ingenious way to develop a new type of economic and efficient cathode for Li–O2 batteries.

Constructing CoO Nanoneedle Hierarchical Structure Based on Cassie States for Highly Efficient Fog Harvesting

Collecting water from the fog becomes a promising strategy to address the water shortage. In this work, the CoO nanoneedle hierarchical structure was designed and prepared on the surface of the copper mesh by hydrothermal synthesis. The number of nanoclusters on the CoO nanoneedle array was changed by adjusting the mass concentration of the precursor solution. CoO nanoneedle array and nanoclusters form a hierarchical structure, which is conducive to the binding of air and the aggregation of water droplets. The results show that the surface of CoO nanoneedle hierarchical structure with good orientation and moderate sparsity has weak adhesion and stronger air binding capacity. Compared with other CoO nanoneedle structures, the hierarchical structure can effectively maintain the Cassie state wetting model for a long time, which improves the fog harvesting efficiency. This research offers a new strategy to design nanostructures for efficient fog collection, which has important implications on water harvesting from the air.

High-sensitivity and point-of-care detection of SARS-CoV-2 from nasal and throat swabs by magnetic SERS biosensor

The outbreak of COVID-19 caused by SARS-CoV-2 urges the development of rapidly and accurately diagnostic methods. Here, one high-sensitivity and point-of-care detection method based on magnetic SERS biosensor composed of Fe3O4-Au nanocomposite and Au nanoneedles array was developed to detect SARS-CoV-2 directly. Among, the magnetic Fe3O4-Au nanocomposite is applied to capture and separate virus from nasal and throat swabs and enhance the Raman signals of SARS-CoV-2. The magnetic SERS biosensor possessed high sensitivity by optimizing the Fe3O4-Au nanocomposite. More significantly, the on-site detection of inactivated SARS-CoV-2 virus was achieved based on the magnetic SERS biosensor with ultra-low limit of detection of 100 copies/mL during 15 mins. Furthermore, the contaminated nasal and throat swabs samples were identified by support vector machine, and the diagnostic accuracy of 100% was obtained. The magnetic SERS biosensor combined with support vector machine provides giant potential as the point-of-care detection tool for SARS-CoV-2.

Boosting Electrocatalytic Oxygen Evolution over Ce-Co9 S8 Core-Shell Nanoneedle Arrays by Electronic and Architectural Dual Engineering.

An dual electronic and architectural engineering strategy is a good way to rationally design earth-abundant and highly efficient electrocatalysts of the oxygen evolution reaction (OER) for sustainable hydrogen-based energy devices. Here, a Ce-doped Co9 S8 core-shell nanoneedle array (Ce-Co9 S8 @CC) supported on a carbon cloth has been designed and developed to accelerate the sluggish kinetics of the OER. Profiting from valance alternative Ce doping, a fine core-shell structure and vertically aligned nanoneedle arrayed architecture, Ce-Co9 S8 @CC integrates modulated electronic structure, highly exposed active sites, and multidimensional mass diffusion channels; together, these afford a favorable catalyzed OER. Ce-Co9 S8 @CC exhibits remarkable performance in the OER in an alkaline medium, where the overpotential requires only 242 mV to deliver a current density of 10 mA cm-2 for the OER; this is 70 mV superior to that of Ce-free Co9 S8 catalyst and other counterparts. Good stability and impressive selectivity (nearly 100 % Faradic efficiency) are also demonstrated. When integrated into a two-electrode OER//HER electrolyzer, the as-prepared Ce-Co9 S8 @CC displays a low operation potential of 1.54 V at 10 mA cm-2 and long-term stability, thus demonstrating great potential for economical water electrolysis.

Hollow CoNiS polyhedrons/MnCoNi layered double hydroxide nanorod arrays on nickel foam as integral electrodes for improved oxygen evolution reaction in alkaline media

AbstractThe oxygen evolution reaction (OER) with sluggish kinetics in electron transportation has been the key process to develop water splitting technology for the hydrogen production. Here, we successfully prepared hollow CoNiS polyhedrons/MnCoNi layered double hydroxide (MCN LDH) nanorod arrays on Ni foam (labeled as CNS/MCN LDH/NF) through a two‐step wet chemical route, employing NF‐supported MCN LDH nanoneedle arrays as the substrate. ZIF‐67 polyhedrons first loaded on MCN LDH to form ZIF‐67/MCN LDH/NF, and then ZIF‐67/MCN LDH/NF was sulfurized to obtain the final product. The investigations revealed that MCN LDH could not be sulfurized under the current sulfurization conditions and simultaneously nickel element entered the sulfurized product to form hollow CoNiS polyhedrons. Electrochemical tests showed that the as‐obtained CNS/MCN LDH/NF electrode merely required 259 mV of overpotential in 1.0 M KOH solution to deliver the current density of 50 mA cm−2, which was lower than 372 mV of the hollow Co9S8polyhedrons/NF electrode. Furthermore, the as‐constructed CNS/MCN LDH/NF electrode could continuously and stably work at the current density of 100 mA cm−2for 110 h, indicating its superb long‐term stability.

Three-dimensional Co3O4/CoS hierarchical nanoneedle arrays electrode grown on nickel foam for high-performance asymmetric capacitors

Asymmetric capacitors have attracted attention owing to their advantage of high power density, safety and low cost, while the limited energy density and cyclic stability impact the applications in high-energy storage field. In this work, the nano-Co3O4/CoS core-shell structures are successfully designed on nickel foam via a facile hydrothermal method for Co3O4 nanoneedle arrays and electrodeposition for ultrathin CoS nanosheets. The energy density of the asymmetric capacitor using a nano-Co3O4/CoS electrode can reach 22 Wh kg−1 at 1 A g−1, which is several times larger than the single Co3O4 electrode. The results show that the hierarchical porous structure can accelerate electron and ion transport, reduce the charge transfer resistance, and thus improve the capacitive performance of hybrid electrodes. Moreover, the modified asymmetric capacitor shows good cycling stability with 90.1% energy density retention over 5000 cycles at 5 A g−1.

Vertical Cu Nanoneedle Arrays Enhance the Local Electric Field Promoting C2 Hydrocarbons in the CO2 Electroreduction.

Electrocatalytic reduction of CO2 to multicarbon products is a potential strategy to solve the energy crisis while achieving carbon neutrality. To improve the efficiency of multicarbon products in Cu-based catalysts, optimizing the *CO adsorption and reducing the energy barrier for carbon-carbon (C-C) coupling are essential features. In this work, a strong local electric field is obtained by regulating the arrangement of Cu nanoneedle arrays (CuNNAs). CO2 reduction performance tests indicate that an ordered nanoneedle array reaches a 59% Faraday efficiency for multicarbon products (FEC2) at -1.2 V (vs RHE), compared to a FEC2 of 20% for a disordered nanoneedle array (CuNNs). As such, the very high and local electric fields achieved by an ordered Cu nanoneedle array leads to the accumulation of K+ ions, which benefit both *CO adsorption and C-C coupling. Our results contribute to the design of highly efficient catalysts for multicarbon products.

Polycrystalline CoO−Co9S8 Heterostructure Nanoneedle Arrays as Bifunctional Catalysts for Efficient Overall Water Splitting

AbstractIt is a great challenge to synthesize efficient electrocatalysts for overall water splitting, especially non‐noble metal catalysts. Herein, one‐dimensional polycrystalline nanoneedles composed of CoO−Co9S8 nano heterostructures, in situ grown on carbon fiber paper are prepared for efficient overall water electrolysis. Due to strong electronic coupling, charge densities of Co2+/Co3+ in Co9S8 and Co2+ in CoO are favorably modified at the interface of CoO and Co9S8, resulting in optimized reaction intermediates absorption and greatly enhanced bifunctional HER/OER activities. CoO−Co9S8/CFP delivers a current density of 10 mA cm−2 in alkaline electrolyte at overpotentials of 184 mV and 270 mV for HER and OER, respectively. When used as electrocatalyst for overall water splitting, it needs a low cell potential of 1.66 V to realize water electrolysis at 10 mA cm−2. This work provides a new strategy to tune the electronic structures of transitional metal active sites via constructing nano heterostructures for efficient water electrolysis.

Three-dimensional self-supporting superstructured double-sided nanoneedles arrays of iron carbide nanoclusters embedded in manganese, nitrogen co-doped carbon for highly efficient oxygen reduction reaction

Nitrogen- and transition metal-dual doped carbon materials with low cost and high catalytic performances are considered as one of promising alternatives for noble metal catalysts in acceleration of oxygen reduction reaction (ORR). In this work, three-dimensional (3D) self-supporting superstructures of iron carbide (Fe3C) nanoclusters entrapped in manganese (Mn)- and nitrogen (N)-dual doped carbon nanosheets covered with double-sided nanoneedles carbon arrays (Fe3C/Mn,N-NCAs) are simply synthesized by a coordination pyrolysis method, in which dicyandiamide mainly behaves as nitrogen source and 1-(2-pyridylazo)-2-naphthol (PAN) as carbon source. Integration of the unique 3D self-supporting superstructures and synergistic effects of the multi-compositions, the as-obtained catalyst displays appealing ORR performance such as the much positive onset potential (Eonset = 0.98 V vs. RHE) and half-wave potential (E1/2 = 0.88 V vs. RHE), as well as a just 10 mV negative shift in E1/2 after 2000 cycles, surpassing commercial Pt/C. This work provides some valuable perspectives for preparation of high-efficiency and low-cost non-noble metal ORR electrocatalysts in energy transformation and storage correlated systems.