High Current Density Research Articles

Enhanced Adsorption Kinetics and Capacity of a Stable CeF3@Ni3N Heterostructure for Methanol Electro-Reforming Coupled with Hydrogen Production.

Alkaline methanol-water electrolysis system is regarded as an appealing strategy for electro-reforming methanol into formate and producing hydrogen with low energy-consumption compared with alkaline water electrolysis. However, stability and selectivity under high current densities for practical application remain challenging. Herein, a CeF3@Ni3N nanosheets array anchored on carbon cloth (CeF3@Ni3N/CC) was fabricated. The gradual extrusion of F species from Ni(OH)2 lattices can stabilize hierarchical structure and construct abundant heterostructure interfaces. Moreover, CeF3 can modulate electron distribution of Ni3N, thus simultaneously enhancing the surface adsorption kinetics and capability of methanol and OH-, which is conducive to enhanced methanol oxidation reaction (MOR) activity and selectivity. Therefore, bifunctional CeF3@Ni3N/CC exhibits low potential of 1.43 V at 500 mA cm-2, along with high stability over 72 h and high faradaic efficiency (FEs) in MOR, as well as an overpotential of 76 mV to achieve 50 mA cm-2 for hydrogen evolution reaction (HER). Furthermore, membrane-free CeF3@Ni3N/CC||CeF3@Ni3N/CC cell for MOR||HER delivers high electrocatalytic activity, long-term stability and FEs at high current density of 300 mA cm-2. This study highlights the importance of optimizing surface adsorption behavior of active species, as well as rational design of highly efficient heterostructure electrocatalysts for methanol upgrading coupled with hydrogen production.

Dendrite‐Free Zinc Anode for Zinc‐Based Batteries by Pre‐Deposition of a Cu–Zn Alloy Layer on Copper Surface via an In Situ Electrochemical Oxidation–Reduction Reaction

ABSTRACTThe prevention of uncontrollable growth of zinc dendrites on the zinc electrodes is one of the key challenges, hindering the widespread commercialization of zinc‐based energy storage technologies. Herein, we report a facile method to mitigate dendrite growth on a copper surface by an initial in situ coating of a Cu–Zn alloy layer, before zinc deposition. During further zinc deposition, the initially formed Cu–Zn alloy layer provides uniform nucleating sites and promotes homogeneous zinc deposition. A symmetrical cell, assembled using a Cu–Zn/Cu electrode could be stably cycled for over 1000 cycles in ZnSO4 solution, at a current density of 30 mA/cm2 and a coulombic efficiency of 99.9%. A zinc–air cell, assembled using Zn@Cu–Zn/Cu as the anode and rGO/Co3O4 composite as the cathode, exhibited a very stable performance at a high current density of 50 mA/cm2 and coulombic efficiency of ~93%, for over 400 cycles. After cycling experiments, the X‐ray photoelectron spectroscopy and the X‐ray diffraction analysis confirmed the formation of the Cu–Zn alloy layer. Hence, the present method provides an easy route for fabricating a dendrite‐free zinc electrode, for a wide range of zinc anode‐based batteries.

Proton Pool for the Mitigation of Salt Precipitate Enhancing CO2 Electroreduction in a Flow Cell

Flow cells featuring a gas diffusion electrode (GDE) have emerged as an attractive platform for electrochemical CO2 reduction, offering high current densities (~300 mA·cm−2) and low energy consumption. However, the formation of salt precipitates, particularly carbonate and bicarbonate, poses a significant deficiency by reducing the cell’s operational longevity. In this study, we present a novel approach to mitigate salt precipitates in real-time through acid–base interaction. Recovery efficiency and partial current density of the cell were used to evaluate the capability of removing salt precipitates and the maintenance of CO2 reduction reactions (CO2RRs). It was suggested that the direct treatment of intermittent acid rinse recovers the performance of CO2RRs to a large extent (>97%), and the modification of the proton exchange resin reduces the reduction rate of partial current densities to 1/15 than that of the unmodified. This improvement enhances the cell’s catalytic performance, enabling the stability test for catalysts within the GDE-based flow cell.

Tailoring of electrocatalytic oxygen evolution reaction performance of 2D conductive Co-catecholate metal-organic frameworks

Herein, we report the microwave hydrothermal synthesis of highly porous and conductive 2D Co-catecholate MOFs (Co-CATs) in the absence (Co-CAT-WO) and presence (Co-CAT-W) of N-methyl-2-pyrrolidone (NMP) polar solvent, and the study of these Co-CATs as electrocatalysts for oxygen evolution reaction (OER). The OER performance of Co-CAT-WO and Co-CAT-W is compared. The as-synthesized Co-CATs exhibit a 2D layered hexagonal structure. The electrical conductivity of Co-CAT-WO and Co-CAT-W is 6.9 and 5.8 S/m, respectively. The good conductivity and porous structure can initiate charge transport to achieve better OER performance under the 4e--transfer process. The as-prepared Co-CAT-WO and Co-CAT-W, respectively, show an overpotential of 455 and 424 mV at 10 mA/cm2 after performing the durability and chronoamperometry experiments for 13 h in 1 M KOH. From the electrochemical studies, it is apparent that the Co-CAT-W exhibits better OER performance with low overpotential, high current density, and excellent stability over extended cycling. Moreover, the lower HOMO-LUMO gap for Co-CAT-W than that of the Co-CAT-WO endorses its better electrocatalytic activity. The post-OER results show that the Co-CAT-W electrocatalyst acts as a "precatalyst" rather than the original catalyst, and it undergoes electrochemical transformation to metal hydroxide and metal oxyhydroxide after the OER studies, promoting the OER kinetics. The findings of this work offer valuable insights into the synthetic strategies for developing 2D conducting metal-catecholate MOF catalysts for efficient and sustainable OER processes, which is crucial in water splitting for sustainable energy production.

Fast Charging Sodium‐Ion Full Cell Operated From −50 °C to 90 °C

AbstractThe application of sodium‐ion batteries (SIBs) within grid‐scale energy storage systems (ESSs) critically hinges upon fast charging technology. However, challenges arise particularly with anodes such as hard carbon (HC), which exhibits a low working plateau (less than 0.1 V vs Na/Na+) and is susceptible to sodium dendrite issues under high current densities. In this study, a cost‐effective SIB system comprising Na2.4Fe1.8(SO4)3 (NFS) cathode, NaTi2(PO4)3 (NTP) anode, and ester‐based electrolyte is assembled to solve the fast‐charging obstacle. Benefiting from the fast sodium‐ion diffusion kinetics and relatively high voltage platform of NTP anode, this full cell can work for 10 000 cycles at 10 C rate with a notable capacity retention of 70.7%. Moreover, this investigation reveals that the full cell can operate safely between ‐50 to 90 °C even with an ester‐based electrolyte, thereby showcasing broad application prospects. This work provides a valuable guidance for designing fast charging and wide temperature SIBs.

Ru‐MnO Heterostructure Clusters Toward Efficient and CO‐Tolerant Alkaline Hydrogen Oxidation Reaction

AbstractDesigning efficient and CO‐tolerant catalysts for hydrogen oxidation reaction (HOR) in anode is one of the challenges for alkaline exchange membrane fuel cells in practical application. Herein, Ru‐MnO heterostructure with two adjacent clusters supported on commercial carbon (BP 2000) (denoted as Ru‐MnO/C) is designed to accelerate the sluggish kinetics of alkaline HOR. The cluster–cluster heterostructure interface modifies the electronic structure of Ru sites with electron transfer from Ru to MnO, then optimizes the adsorption of intermediates on Ru sites. Consequently, this catalyst exhibits high catalytic HOR activities in alkaline media with high exchange current density (3.71 mA cm−2) and mass activity (0.78 A mgRu−1). Meanwhile, the alkaline exchange membrane fuel cell delivers a specific peak power density (PPD) of 7.0 W mg−1Ru under H2/O2 condition, which is higher than that of most reported catalysts. More importantly, the catalyst also demonstrates the remarkable stability and CO‐tolerance. This work presents the superiority of cluster–cluster heterostructure interface toward efficient HOR, which is expected to further enlighten the design of advanced catalysts for electrocatalysis.

Frustrated Lewis Pair Mediated f‐p‐d Orbital Coupling: Achieving Selective Seawater Oxidation and Breaking *OH and *OOH Scaling Relationship

AbstractThe development of oxygen evolution reaction (OER) electrocatalyst for seawater electrolysis plays a crucial role in producing renewable hydrogen energy. However, during the seawater electrolysis process, the anode inevitably undergoes chloride oxidation reaction (ClOR) due to Cl− adsorption, making the seawater electrolysis process difficult to sustain. Inspired by the selective permeability of cell membranes, we propose a biomimetic design of frustrated Lewis pairs (FLPs) layers for selective seawater oxidation. Combining experimental results and molecular dynamics simulations, it has been demonstrated that cerium dioxide layers with FLPs sites can decompose water molecules, capture hydroxyl anions, and repel chloride ions simultaneously. DFT theoretical analysis indicates that the FLP sites regulate the Ce 4 f−O 2p−Ni 3d gradient orbital coupling, providing additional oxygen non‐bonding (ONB) to stabilize the Ni−O bond and optimize the adsorption strength of intermediates, thereby breaking the *OH and *OOH scaling relationship. The assembled anion exchange membrane electrolyzers exhibit an efficiency of 95.7 % at a current density of 0.1 A cm−2 and can stably operate for 250 hours at a current density of 0.2 A cm−2.

3D-stacked electrospun iron-doped nickel cobalt oxide nanofibers as integrated electrodes for anion exchange membrane water electrolysis

The commercialization of anion-exchange membrane water electrolysis (AEMWE) requires the development of highly active, stable, and cheap anode catalysts for the oxygen evolution reaction (OER). In this study, we proposed electrospun iron-doped NiCo2O4 (NCO) nanofibers on nickel foam (NF) and evaluated the performances of the resulting samples (FeX-NCO/NF; X = iron loading in NCO (0, 5, 10, and 15 at %)) as unitized anodes for the OER. Among the fabricated electrodes, Fe10-NCO/NF exhibited the lowest overpotential of 352 mV at a current density of 50 mA cm−2 in a half-cell test owing to its improved intrinsic activity. In an AEMWE single-cell test, Fe10-NCO/NF as anode showed high current density (932 mA cm-2 at 1.8 V) and long-term stability for 150 h The improved AEMWE performance of Fe10-NCO/NF was attributed to efficient mass transport enabled by superhydrophilic three-dimensional porous structure featuring stacked nanofibers.

Frustrated Lewis Pair Mediated f-p-d Orbital Coupling: Achieving Selective Seawater Oxidation and Breaking *OH and *OOH Scaling Relationship.

The development of oxygen evolution reaction (OER) electrocatalyst for seawater electrolysis plays a crucial role in producing renewable hydrogen energy. However, during the seawater electrolysis process, the anode inevitably undergoes chloride oxidation reaction (ClOR) due to Cl- adsorption, making the seawater electrolysis process difficult to sustain. Inspired by the selective permeability of cell membranes, we propose a biomimetic design of frustrated Lewis pairs (FLPs) layers for selective seawater oxidation. Combining experimental results and molecular dynamics simulations, it has been demonstrated that cerium dioxide layers with FLPs sites can decompose water molecules, capture hydroxyl anions, and repel chloride ions simultaneously. DFT theoretical analysis indicates that the FLP sites regulate the Ce 4 f-O 2p-Ni 3d gradient orbital coupling, providing additional oxygen non-bonding (ONB) to stabilize the Ni-O bond and optimize the adsorption strength of intermediates, thereby breaking the *OH and *OOH scaling relationship. The assembled anion exchange membrane electrolyzers exhibit an efficiency of 95.7 % at a current density of 0.1 A cm-2 and can stably operate for 250 hours at a current density of 0.2 A cm-2.

A Segmented Along the Channel Test Cell for Locally Resolved Analysis at High Current Densities in PEM Water Electrolysis

Abstract For the scale-up of proton exchange membrane (PEM) water electrolysis, understanding the cell behavior on industrial scale is a prerequisite. A proper distribution of current and temperature in the cell can improve performance and decrease overall degradation effects. Due to water consumption as well as the concomitant gas evolution and accumulation, gradients and inhomogeneities along the reaction coordinate are expected. These effects increase along the water supply channels of a flow field and are expected to lead to spatial gradients in cell performance and temperature. At high current densities (> 5 A∙cm-2) these effects are anticipated to be critical due to the high amount of gas produced and the increased degradation rate resulting from the high overpotentials. 
In this study we present a new test cell that is segmented along the flow field channels and is designed for the operation at high current densities of up to 10 A∙cm-2. With this approach it is possible to analyze performance gradients and the spatial distribution of loss processes under industry-relevant conditions by measuring the current density and temperature distribution and by performing locally resolved electrochemical impedance spectroscopy (EIS).

A High-Performance Polyimide Composite Membrane with Flexible Polyphosphazene Derivatives for Vanadium Redox Flow Battery.

A sulfonated polyimide, S-F-abSPI, with alkyl sulfonic acid side chains, and a polyphosphonitrile derivative, poly[4-methoxyphenoxy (4-fluorophenoxy) phosphazene] (PFMPP), were designed and synthesized. Composite modification of the S-F-abSPI membrane was carried out using PFMPP, resulting in the preparation of composite membranes with different composite ratios, which were then subjected to performance testing and characterization. Experimental results revealed a significant enhancement in the proton conductivity of the S-F-abSPI membrane, reaching 0.116 S cm-1, slightly higher than that of the N212 membrane. The S-F-abSPI/1% PFMPP composite membrane exhibited the optimal comprehensive performance, with a surface resistance as low as 0.54 Ω cm2, comparable to that of the N212 membrane. At a high current density of 200 mA cm-2 during charge-discharge, the composite membrane achieved a voltage efficiency (VE) of 83.12% and an energy efficiency (EE) of 81.95%. Cycling tests over 200 cycles demonstrated the composite membrane's excellent long-term cycling stability. The alkyl sulfonic acid side chains enhanced the proton conductivity of the membrane, while electrostatic potential distribution calculations indicated strong interactions between PFMPP and the base membrane, enhancing the membrane's mechanical strength, reducing vanadium ion permeability, and improving chemical stability and vanadium ion selectivity. This composite membrane holds promise for high-performance VRFB applications.

Nickel coated paper electrode constructed by interfacial electrodeposition for biomass upgrading at industrial current density

Substituting the kinetically slow oxygen evolution reaction (OER) with biomass electrooxidation significantly decreases the energy demand of water electrolysis. However, exploring and optimizing efficient electrocatalysts remains a challenge for large−scale production of valuable chemicals and hydrogen. Herein, we have constructed a nickel coated paper electrode (NiCo@Ni/CP) composed of crystalline Ni metal and amorphous NiCo hydroxide nanosheets layers via interfacial electrodeposition on carbon paper (CP) for monosaccharide oxidation reactions (MOR), which achieved a formate yield of 82.4 %. Remarkably, the flow electrolyzer maintained an industrial−grade current density of 1 A cm−2 at 1.70 V with exceptional stability over 100 h, also displaying significant co−generation Faradaic efficiencies of approximately 80.0 % and 97.3 % for formate and hydrogen production, respectively. The superior performance is attributed to the redistribution of electrons at the Ni and amorphous NiCo hydroxide interface, which enhances charge transfer and reactant adsorption by adjusting the d−band center, hence reducing deprotonation and C−C bond cleavage energies of xylose during MOR. This work provides a promising strategy for the design of efficient catalysts for biomass upgrading and the production of hydrogen at high current densities.

Triplet supercurrents in lateral Josephson junctions with a half-metallic ferromagnet

In the area of superconducting spintronics, spin-triplet supercurrents in half-metallic ferromagnets (HMFs) could yield dissipationless spin transport over large distances and high current density. Promising among the HMFs is the perovskite oxide La0.7Sr0.3MnO3 (LSMO), and recent studies in combination with the high-Tc superconductor YBa2Cu3O7, or the conventional superconductor NbTi, showed long-range effects. Here we focus on two issues that as yet have received less attention: the value of the critical current in the HMF in the limit of a very small electrode distance (20 nm) and the nature of the spin-triplet generator. We use lateral junctions shaped as a bar, square, and disk, and find high supercurrent densities of the order of 1011 A/m2, pointing to an efficient triplet generation mechanism. This is surprising in the sense that no magnetic inhomogeneity is purposely built in, as is done in conventional metal triplet junctions. Furthermore, from the magnetic field dependence of the critical current interference patterns, we find a uniform supercurrent distribution in bar-shaped devices, but one more constricted to the rim in disk devices, which is an expected consequence of the geometry. We also analyze the temperature dependence of the critical current and find the quadratic dependence that was predicted in the limit of small junction lengths. From studying the NbTi/LSMO interface with scanning electron transmission microscopy, we conclude that the magnetic inhomogeneity required for triplet generation resides in the LSMO layer adjacent to the interface. Published by the American Physical Society 2024

Recycled industrial waste silicon steel as high-performance electrode for oxygen evolution reaction using electroless plating surface modification

Exploring the large-area, cost-effective, and high-performance electrocatalyticoxygen evolution reaction (OER) electrode for water splitting is of great significance. Inspiring from the ‘waste to resource’ toward the circular economy, herein, the waste silicon steels (SS) were transformed into high-performance CoxFe3-xP/SS OER electrode through a facile electroless plating method. The plating layer of CoxFe3-xP not only endows the CoxFe3-xP/SS with outstanding electrocatalytic OER activity but also improves the corrosion resistance and stability of CoxFe3-xP/SS. The obtained Co2Fe1P/SS electrode exhibits the lowest overpotential of 244 mV at a current density of 10 mA/cm2 in 1 M KOH with a low Tafel slope of 48.7 mV/dec. Even at high current densities and in 6 M KOH and alkaline seawater (seawater + 1 M KOH), the Co2Fe1P/SS electrode also shows relatively low overpotentials, as well as high long-term durability. Specially, a large-area Co2Fe1P/SS OER electrode(40 × 40 cm2)was successfully prepared via the electroless plating approach. Toward the CoxFe3-xP/SS, the bimetallic Co-Fe synergies and phosphating effect promote the exposure of active sites and charge transfer. In addition, generated M(OH)x/MOOH (M = Co or Fe) species during OER activation could synergize with CoxFe3-xP and contribute excellent catalytic activity and stability.

Extrinsic tungsten doping to improve the intrinsic electrocatalytic activity of NiBP spheres for overall water splitting under high current density operation

Extrinsic heteroatom doping is an effective approach to enhance the electrochemical performance of electrocatalysts by the creation of new active sites, improved conductivity and optimization of adsorption/desorption energies. In this study, a W-doped NiBP electrocatalyst is designed by using hydrothermal synthesis and soaking doping approach for overall water splitting application. The W-doped NiBP spheres exhibit the overpotentials of 260 and 380 mV at 500 mA/cm2 in 1 M KOH for hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) respectively. The bifunctional W-doped NiBP electrode demonstrates superior 2-E water splitting efficiency, requiring a low cell voltage of only 2.66 V at the high current density (HCD) of 2000 mA/cm2, significantly surpassing the benchmark Pt/C||RuO2 system. Additionally, it exhibits good stability with the continuous 120 h of water splitting operation without noticeable degradation. A hybrid Pt/C||W-doped NiBP demonstrates a further reduced voltage of 2.54 V at 2000 mA/cm2.The substantial performance enhancement can be attributed to the increased active sites, enhanced conductivity and optimized adsorption/desorption energies of intermediates through tungsten heteroatom doping.

Improved breakdown voltage and dynamic Ron characteristics in normally-off GaN-based HEMTs featuring fully-recessed and bilayer-dielectric gate structure

Abstract The degradation of dynamic on-resistance (Ron) is a major challenge in GaN-based high electron mobility transistors (HEMTs), which seriously affects their performance and reliability. The degradation area of dynamic Ron mainly comes from two aspects. One is the region below the gate that also affects the threshold voltage (Vth) of the devices. And the other one is the interface region of the gate to drain access. The optimal device exhibits a Vth of 0.97 V, a small Vth hysteresis of only 20 mV, a high current density of 723 mA/mm, and a breakdown voltage (BV) of 760 V which could be further boosted when additional field plate design is employed. It is found that when high voltage drain stress is applied, a positive Vth shift is induced, leading to the decrease of the effective gate driving voltage, and thus the dynamic Ron of the devices is increased. Of particular concern is the effects of dielectric layer and/or interface of the access region on the dynamic Ron degradation, which can be alleviated by removing the dielectric layer of the access region.

Controllable Multilayer of High‐performance Si/C Anode Materials Synthesized at Low Temperature from Industrial Ca‐Si Alloy and CCl4 for Lithium‐ion Batteries

AbstractA simple and energy‐saving synthesis process for the high‐performance Si/C anode material of lithium‐ion batteries is advantageous for application. In this paper, the layered Si/C composite was synthesized by a low temperature one‐pot synthesis from industrial Ca−Si alloy and CCl4. The effect of synthesis temperature on the structure and performance of the products was investigated. We found that low temperature favors to the multilayer structure of Si/C. Taking the advantage of the layered structure, the Si/C‐300 anode material prepared at the temperature of 300 °C has good electrochemical performance of a reversible capacity of more than 1000 mAh g−1 at a current density of 2 A g−1 for 300 cycles, with a capacity retention ratio of 82.8 %, and an ICE of 77.0 %. At a high current density of 6 A g−1, the specific discharge capacity of 721.6 mAh g−1 can be achieved. The synthesis method provides a promising route to high performance silicon‐carbon anode materials.

Highly Effective Polyacrylonitrile-Rich Artificial Solid-Electrolyte-Interphase for Dendrite-Free Li-Metal/Solid-State Battery.

Lithium metal anode batteries have attracted significant attention as a promising energy storage technology, offering a high theoretical specific capacity and a low electrochemical potential. Utilizing lithium metal as the anode material can substantially increase energy density compared with conventional lithium-ion batteries. However, the practical application of lithium metal anodes has encountered notable challenges, primarily due to the formation of dendritic structures during cycling. These dendrites pose safety risks and degrade battery performance. Addressing these challenges necessitates the development of a reliable and effective protection layer for lithium metal. This study presents a cost-effective and convenient method to spontaneously produce lithium metal protective layers by creating polymeric layers by using acrylonitrile (AN). This method remarkably extends 6× of the lifetime of lithium metal anodes under high current density (1 mA/cm2) cycling conditions. While the cycle life of bare lithium metal is approximately 150 h under high current cycling conditions, AN-treated lithium metal anodes exhibit an impressive longevity of over 900 h. The AN-treated lithium metal anodes are further integrated and tested with sulfide-based Li10GeP2S12 (LGPS) solid-state electrolytes to evaluate its interfacial stability at a solid-solid interface. The formation of the polyacrylonitrile (PAN)-rich ASEI, due to AN-treatment, effectively reduces and stabilizes the cell overpotential to only one-tenth of that with the interface without treatment. This strategy paves a route to enable a highly efficient and highly stable Li/LGPS solid-state battery interface.

Pyrolysis‐Free Synthesis of Synergistic Single‐Atom/Nanocluster Electrocatalysts for Hydrogen Evolution

Constructing catalysts that simultaneously containing single atom/metal nanocluster active sites is a promising strategy to enhance the original catalytic behavior and accelerate the catalysis involving multi‐electron reactions or multi‐intermediates. Herein, the pyrolysis‐free synthetic method is developed to integrate single atoms and nanoclusters towards highly satisfactory catalytic performances for both acidic and alkaline hydrogen electrocatalysis. The controllable pyrolysis‐free strategy allows the precise modulation of the active centers, realizing the optimization of the adsorption energy and the regulation of the synergistic active components. Specially, the as‐prepared catalysts with hybrid single‐atom/nanocluster sites exhibited superior catalytic activities for hydrogen evolution in both acidic and alkaline media with low over‐potentials at ‐10 mA cm‐2 of 25 mV and 8.6 mV, respectively, combining with outstanding durability towards high current density and methanol poisoning. This work developed a universal synthetic strategy for the single atom/nanocluster synergy systems and further demonstrated the superiority of heterogeneous components.

Pyrolysis-Free Synthesis of Synergistic Single-Atom/Nanocluster Electrocatalysts for Hydrogen Evolution.

Constructing catalysts that simultaneously containing single atom/metal nanocluster active sites is a promising strategy to enhance the original catalytic behavior and accelerate the catalysis involving multi-electron reactions or multi-intermediates. Herein, the pyrolysis-free synthetic method is developed to integrate single atoms and nanoclusters towards highly satisfactory catalytic performances for both acidic and alkaline hydrogen electrocatalysis. The controllable pyrolysis-free strategy allows the precise modulation of the active centers, realizing the optimization of the adsorption energy and the regulation of the synergistic active components. Specially, the as-prepared catalysts with hybrid single-atom/nanocluster sites exhibited superior catalytic activities for hydrogen evolution in both acidic and alkaline media with low over-potentials at -10 mA cm-2 of 25 mV and 8.6 mV, respectively, combining with outstanding durability towards high current density and methanol poisoning. This work developed a universal synthetic strategy for the single atom/nanocluster synergy systems and further demonstrated the superiority of heterogeneous components.