Strong Metal-support Interaction Research Articles

Embedding Reverse Electron Transfer Between Stably Bare Cu Nanoparticles and Cation-Vacancy CuWO4.

Cu nanoparticles (NPs) have attracted widespread attention in electronics, energy, and catalysis. However, conventionally synthesized Cu NPs face some challenges such as surface passivation and agglomeration in applications, which impairs their functionalities in the physicochemical properties. Here, the issues above by engineering an embedded interface of stably bare Cu NPs on the cation-vacancy CuWO4 support is addressed, which induces the strong metal-support interactions and reverse electron transfer. Various atomic-scale analyses directly demonstrate the unique electronic structure of the embedded Cu NPs with negative charge and anion oxygen protective layer, which mitigates the typical degradation pathways such as oxidation in ambient air, high-temperature agglomeration, and CO poisoning adsorption. Kinetics and in situ spectroscopic studies unveil that the embedded electron-enriched Cu NPs follow the typical Eley-Rideal mechanism in CO oxidation, contrasting the Langmuir-Hinshelwood mechanism on the traditional Cu NPs. This mechanistic shift is driven by the Coulombic repulsion in anion oxygen layer, enabling its direct reaction with gaseous CO to form the easily desorbed monodentate carbonate.

Crystalline-Amorphous IrOx Supported on Perovskite Nanotubes for pH-Universal OER.

Designing catalysts with desirable oxygen evolution reaction (OER) performance under pH-universal conditions is of great significance to promote the development of hydrogen production. Herein, we successfully synthesized a crystalline-amorphous IrOx supported on perovskite oxide nanotubes to obtain IrOx@La0.6Ca0.4Fe0.8Ni0.2O3 with superior OER performance in whole pH media. The overpotential of the IrOx@La0.6Ca0.4Fe0.8Ni0.2O3 catalyst in media of pH 14, 7.2, and 1 has been demonstrated to be 120, 400, and 143 mV, respectively, with no significant element dissolution as well as double-layer capacitance decay after the durability test. Through comparative experiments with IrOx@CNT and the physical mixture of IrOx and La0.6Ca0.4Fe0.8Ni0.2O3, it is found that the strong metal-support interaction (SMSI) in IrOx@La0.6Ca0.4Fe0.8Ni0.2O3 makes IrOx exist in an amorphous state rich in Ir3+, which is closely associated with the surface-active species Ir-OH. Through the regulation of Ir by a perovskite oxide support at the heterointerface, the reaction breaks through the limitation of the adsorbate evolution mechanism (AEM) and converts to a lattice-oxygen-mediated mechanism (LOM), which was fully demonstrated by the addition of the probe tetramethylammonium cation (TMA+), a LOM reaction intermediate, to the electrolyte. This work fills the research gap of perovskite oxide supported Ir-based catalysts with heterogeneous structures, providing an excellent strategy for the structural design of efficient pH-universal OER catalysts for hydrogen production systems.

Highly active ternary Ir/In2O3-ZrO2 catalyst for CO2 hydrogenation towards methanol: The role of zirconia

Indium oxide supported iridium catalyst has been verified to be highly active and selective for CO2 hydrogenation to methanol. In this work, zirconia is introduced into the Ir/In2O3 system as a novel Ir/In2O3-ZrO2 ternary catalyst. The solid solution generated between ZrO2 and In2O3 exhibits a strong electronic metal-support interaction with iridium, rendering the supported iridium species highly dispersed in a form of clusters. Thereout, an active interface between iridium and the solid-solution carrier is thus generated, on which electron transport is more feasible with a stronger CO2 adsorption than that of on the Ir−In2O3 interfacial site. Moreover, compared to Ir/In2O3, this ternary catalyst exhibits better catalytic activity as well as the stability. Density functional theory (DFT) simulations, combined with the in-situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) studies, further demonstrate the CO-hydrogenation pathway is the most favored for methanol synthesis, providing a rationale for the superior methanol selectivity of the Ir/In2O3-ZrO2 catalyst during CO2 hydrogenation.

Bifunctional fluorine doped Ru/RuO2 clusters with dynamic electron modification and strong metal-support interaction boost proton exchange membrane water electrolyzer

The sluggish kinetics and inherent instability over the Ru/RuO2 clusters are still enormous challenges in proton exchange membrane (PEM) water electrolyzer. Herein, we innovatively report synergistic modulation of dynamic electron modification and strong metal-support interaction (SMSI) to activate and stabilize bifunctional fluorine doped Ru/RuO2 clusters anchored on carbon nanotube (CNT), thus achieving efficient and stable acidic overall water splitting. Theoretical and experimental studies found that surface metal-fluorine modification layer could dynamically regulate the interfacial electronic environment to stabilize and activate multiple active Ru species; and the SMSI between Ru/RuO2 cluster and CNT maintains stable electronic environment for dynamic electron modification and avoids migrating or shedding of active species in acidic environment. Therefore, the PEM electrolyzer assembled with optimal F5.5-Ru/RuO2@CNT can operate stably for 100 h at a high current density of 100 mA cm−2, which is the first time that bifunctional Ru-based nanocatalysts applied to PEM device at a high current density.

A strong metal-support interaction strategy for enhanced proton-coupled electron transfer and promoted photocatalytic H2O2 production in pure water

Proton-coupled electron transfer (PCET) is a key factor in determining the H2O2 production efficiency from oxygen reduction reaction (ORR) or direct H2/O2 reaction, which usually requires the aid of proton donors including alcohols. Here, we report a strong metal-support interaction (SMSI) strategy to facilitate the PCET process of a typical Pd/TiO2 photocatalyst for photocatalytic ORR into H2O2 production in pure water. Compared to conventional Pd/TiO2 photocatalysts, the Pd/TiO2 photocatalyst with SMSI between Pd and TiO2 (Pd/TiO2-850H) promotes photocatalytic H2O2 production in pure water by 4.21-fold, which can be ascribed to that the SMSI simultaneously promotes the H2O dissociation and the photogenerated charge transfer from TiO2 to Pd catalyst, enabling highly efficient proton transfer to be participated into converting •O2- to H2O2. Moreover, the formation of TiO2-x overlayer caused by SMSI suppresses the H2O2 decomposition and stabilizes Pd NPs, finally achieving an H2O2 production rate of 4.10 mmol g−1 h−1, which surpasses most metal/TiO2 photocatalytic system.

Ultrafine Fe-Mn bimetallic nanoparticles anchored in nitrogen-doped carbon nanofiber electro-Fenton membrane with strong metal-support interactions for sustainable water decontamination in wide pH ranges

Designing a membrane electrode with high activity and anti-scaling ability in a wide pH range is crucial to the development of flow-through electro-Fenton system. Herein, we reported a novel porous membrane composed of ultrafine FeMn bimetallic nanoparticles anchored in nitrogen-doped carbon nanofibers (FeMn/N-CNF) obtained through a facile electrospinning-carbonization process. The strong metal-support interaction (SMSI) phenomena including carbon encapsulation structure and electron transfer from metal to N-CNF, beneficial to the intrinsic activities, were successfully induced by the enhanced interfacial metal-nitrogen bonding in FeMn/N-CNF. Microstructural characterizations and leaching test revealed that the SMSI encapsulation structure could promote the formation of ultrafine FeMn nanoparticles in N-CNF during the high-temperature carbonization process and prevent leaching of active Fe/Mn metals into solution across a wide pH range. The constructed gravity-driven flow-through electro-Fenton system based on a FeMn/N-CNF cathode membrane exhibited superior performance to generate H2O2 (36.23 mmol L−1 h−1) and subsequent activate H2O2 decomposition to hydroxyl radicals (0.1024 min−1), achieving remarkable degradation efficiencies of 96.8%, 92.3%, and 90.3% within 60 min for Rhodamine B, Tetracycline, and Methyl Orange, respectively. Furthermore, the FeMn/N-CNF membrane filter demonstrated good pH adaptability, excellent cycle stability and anti-scaling ability during the degradation process. This work offers a viable avenue to enhance degradation performance and environmental robustness for practical water decontamination via achieving SMSI effect in carbon-supported electro-Fenton membranes.

Stability enhancement of molybdenum modified rutile – carbon composite supported platinum electrocatalysts by reductive pretreatment: Surface characteristics and advanced electrocatalytic properties

Development of strong metal-support interaction (SMSI) and its influence on the catalytic performance of the Pt/Ti0.8Mo0.2O2-C system, a representative of the mixed oxide-carbon composite supported Pt electrocatalyst family, were investigated. Structural, surface chemical and electrochemical properties of the as-prepared Pt/Ti0.8Mo0.2O2-C catalyst and its counterparts reduced in the 150–450 °C temperature range were compared. TEM elemental mapping confirmed the widespread formation of Pt-oxide-C triple junctions in all catalysts. XPS revealed electronic interaction between the Pt particles and the oxide both in the as-prepared and the reduced catalysts, moreover, demonstrated that transport of Mo to the surface of Pt is initiated by reduction in the 150–250 °C range. Electrochemical measurements pointed out the durability of these Pt-bound Mo species, which also enhance the oxygen reduction activity of the catalyst. Based on the results of 10,000-cycle stability tests, reductive pretreatment between 250–350 °C is recommended for enhancing the properties of Pt/Ti0.8Mo0.2O2-C catalysts by SMSI.

In situ reaction-induced strong metal-support interaction to enhance catalytic performance and stability of toluene oxidation

The construction of strong metal-support interaction (SMSI) represents an attractive strategy to enhance the catalytic performance of the catalysts. Herein, the SMSI state over the Pt/TiO2 catalyst that inductively formed with a toluene atmosphere at a temperature below 300 °C is reported. During this process, the Pt species is covered by TiOx overlayers, while the Pt species is endowed to an electron-sufficient state, and more defects on the surface are produced simultaneously. Owing to the existence of formed SMSI, the interface of Pt and TiO2 with an improved redox property is conducive for oxygen species activation to expedite toluene conversion. The experimental results demonstrate that the catalysts with SMSI state exhibit improved catalytic activity and stability (5 vol% water and 800 °C thermal treatment). This work posits that the SMSI state of noble metal-supported catalysts can be dynamically produced during toluene conversion, which paves a novel method for designing efficient catalysts for the practical elimination of VOCs.

Strong metal-support interaction between Ni and BaCO3 boosts CO2 hydrogenation

Strong metal-support interaction between Ni and BaCO3 boosts CO2 hydrogenation

Thermally Stable Oxide-Capsulated Metal Nanoparticles Structure for Strong Metal-Support Interaction via Ultrafast Laser Plasmonic Nanowelding.

Strong metal-support interaction (SMSI) has drawn much attention in heterogeneous catalysts due to its stable and excellent catalytic efficiency. However, construction of high-performance oxide-capsulated metal nanostructures meets great challenge in materials thermodynamic compatibility. In this work, dynamically controlled formation of oxide-capsulated metal nanoparticles (NPs) structures is demonstrated by ultrafast laser plasmonic nanowelding. Under the strong localized electromagnetic field interaction, metal (Au) NPs are dragged by an optical force toward oxide NPs (TiO2). Intense energy is simultaneously injected into this heterojunction area, where TiO2 is precisely ablated. With the embedding of metal into oxide, optical force on Au gradually turned from attractive to repulsive due to the varied metal-dielectric environment. Meanwhile, local ablated oxides are redeposited on Au NP. Upon the whole coverage of metal NP, the implantation behavior of metal NP is stopped, resulting in a controlled metal-oxide eccentric structure with capsulated oxide layer thickness ≈0.72-1.30nm. These oxide-capsulated metal NPs structures can preserve their configurations even after thermal annealing in air at 600°C for 10min. This ultrafast laser plasmonic nanowelding can also extend to oxide-capsulated metal nanostructure fabrication with broad materials combinations (e.g., Au/ZnO, Au/MgO, etc.), which shows great potential in designing/constructing nanoscale high-performance catalysts.

Deciphering promotion of MoP over MoC in Pt catalysts for methanol-assisted water splitting reaction

Molybdenum-based compounds show promising promotion effects on Pt catalysts for energy-relevant catalysis reactions. Herein, a more effective promotion effect of MoP than MoC was found in assisting Pt nanoparticles for methanol-assisted hydrogen generation in light of the strong metal-support interaction and synergistic effect between Pt and MoP/C nanospheres. Electrochemical analyses and theoretical calculations demonstrated that Pt-MoP/C facilitated the oxidation and removal of CO intermediates more effectively than Pt-MoC/C. This enhanced performance was attributed to the distinct 6-coordination environment of hexagonal MoP and the elevated electron density of Mo induced by phosphorus. These structural and electronic features significantly enhanced electron transfer to Pt, thereby creating strong metal-support interaction and synergistic effect to improve the overall catalytic efficiency. Especially, the unique activities of Moδ+ and Moδ- in the MoP modified the surface structure of Pt, lowered the Pt d-band center, and optimized the local chemical state of Pt atoms, which resulted in more optimized adsorption energy and charge transfer capabilities of intermediates. The Pt-MoP/C electrolyzer thus showed both lower cell voltage than that of Pt-MoC/C and Pt/C electrolyzers in water splitting and methanol-assisted water splitting for hydrogen generation. This study offers insightful information about the promotion effect of molybdenum-based compounds in Pt catalyst systems in energy-relevant catalysis reactions.

Effect of nickle on cerium oxide support to develop cyclic catalytic methane decomposition followed by CO2 gasification

Catalytic methane decomposition (CMD) offers an eco-friendly method to produce COx-free hydrogen and solid carbon. An innovative approach for catalyst regeneration involves utilizing CO2 as a reactant to produce CO via the Reverse Boudouard Reaction, which serves as a valuable feedstock for various chemicals and fuels. This study aims to investigate the role and interaction of Ni nanoparticles on cerium oxide support by comparing two catalysts: one synthesized via the conventional impregnation method (Imp) and the other through solution combustion synthesis (SCS). Both catalysts containing the same Ni loading of 5 wt% and were tested under identical conditions. Comprehensive characterization techniques, including XRD, H2 and O2 TPR, TEM, SEM, XPS, and Raman spectroscopy, were employed to elucidate the observed performances. The SCS catalyst resulted in smaller Ni nanoparticles with stronger metal-support interaction. Observations revealed both tip and base carbon growth for the SCS catalyst, whereas the Imp catalyst predominantly characterized by tip growth. For the SCS catalyst, carbon nanofibers and nanotubes were observed, and both appeared active in carbon CO2 gasification. For the Imp catalyst, more crystalline carbon is observed. The amount of carbon produced was much more and managed to cover the entire catalyst. For SCS carbon coverage was partial. Two rates of CO2 gasification were observed depending on the extent of carbon coverage. Across all tested temperatures and space velocities, the catalyst prepared by impregnation exhibited higher reaction rates. The Imp catalyst demonstrated 15 % higher CMD and 29 % more generated carbon than SCS. This work demonstrated the critical role of key factors influencing the catalytic performance of this cyclic process. This includes the Ni nanoparticle size and distribution, the metal-support interaction's strength, and the graphitic carbon's nature.

Strong metal-support interaction induced by oxygen vacancies to enhance the activity and durability of Pt/TiO2/ hollow carbon nanospheres ORR catalyst

For the commercial Pt-loaded carbon ORR catalysts used in proton exchange membrane fuel cells (PEMFC), carbon support corrosion, along with the migration and aggregation of Pt nanoparticles (NPs) due to the weak interaction between Pt NPs and carbon, leads to a drastic reduction in both electrocatalytic activity and stability. Hence, exploring active and steady supports is crucial to restrain the activity loss and stabilize Pt catalysts. In this work, a composite support consisting of hollow carbon nanospheres (HC) and TiO2 NPs with abundant oxygen vacancies (OV) loaded with Pt NPs (PTHC-H) was designed and synthesized. Experiment results show that PTHC-H exhibits superior activity and stability compared to PTHC-N (TiO2 with lower OV content) and commercial Pt/C catalyst. Specifically, PTHC-H delivers a half-wave potential of 0.883V versus reversible hydrogen electrode. And its mass activity and half-wave potential decrease by only 15.96% and 7mV, respectively, after 10,000 cycles of accelerated durability testing. The excellent activity and stability are ascribed to the enhanced metal-support interaction induced by OV, which can optimize the Pt d-band center and suppresses the migration and aggregation of Pt NPs. This work may be favorable for designing efficient and durable anti-corrosion nano catalysts.

Pd nanocubes supported on the porous V2CTx nanosheets with enhanced nanozyme activity and photothermal property for antibacterial application

Rational design and controllable construction of supported nanostructures with excellent antibacterial property remain a great challenge. Recently, transition metal carbides/nitrides/carbonitrides (MXenes) have attracted much interest in many fields due to their large specific surface areas and good photothermal property. Herein, a simple yet effective surface engineering strategy based on the tuning of MXene surface chemistry is presented, which allows in-situ controlled growth of the Pd nanocubes on the V2CTx nanosheets. Briefly, the exfoliated V2CTx nanosheets by HF are annealed, which changes the composition of surface terminations while creating the mesoporous structures. The annealing largely affects the exposure and oxidation states of the adjacent V atoms and allows the controllable growth of Pd nanocubes. Interestingly, the obtained Pd@V2CTx nanocomposites show enhanced peroxidase-/oxidase-like activities and intrinsic photothermal effect in the near infra-red (NIR) region due to the strong metal-support interaction. Furthermore, the combined nanocatalytic-photothermal treatment by their versatilities remarkably improves the antibacterial efficacy, giving a high killing rate (above 98 % for both Escherichia coli and Staphylococcus aureus). This work provides a new avenue to develop the supported metal nanostructures based on MXenes for antibacterial application.

Strong electronic metal-support interaction of Ni4Mo/N-SrMoO4 promotes alkaline hydrogen electrocatalysis

Ni4Mo electrocatalyst stands out as the promising candidate for hydrogen evolution/oxidation reaction (HER/HOR), yet the intensive hydrogen adsorption leads to sluggish kinetics, decreasing hydrogen catalysis efficiency. Herein, the structure of Ni4Mo nanoparticles anchored on wafer-biscuit-like N-SrMoO4 nanorods (Ni4Mo/N-SrMoO4) is developed to accelerate reaction kinetics by modulating electronic structure. The designed N-SrMoO4 support enables strong electronic metal-support interaction with Ni4Mo, resulting in a downward shift of d-band center and achieving thermally neutral hydrogen adsorption. Ni4Mo/N-SrMoO4 exhibits HER performance with an ultralow overpotential of 15 mV at 10 mA cm−2, superior to Pt/C (η10=18 mV). The outstanding exchange current density of 10.2 mA cm−2 for HOR is three times higher than that of Pt/C (3.5 mA cm−2). Ni4Mo/N-SrMoO4 is further assembled in anion exchange membrane water electrolyzer (AEMWE), resulting in a current density of 100 mA cm−2 at voltage of 1.71 V and the excellent stability of 300 hours. Theoretical calculations and in-situ spectroscopy indicate that the introduction of Sr in N-SrMoO4 effectively enhances electronic metal-support interaction, facilitates the enrichment of adsorbed hydroxyl (OHads) on active sites and weakens hydrogen adsorption on Ni4Mo, thereby accelerating reaction kinetics of hydrogen electrocatalysis.

CO2 hydrogenation to methanol over Cu-CeO2-ZrO2 catalysts: The significant effect of metal-support interaction

CO2 hydrogenation to methanol is an important pathway to achieving carbon neutrality, with metal-support interaction (MSI) being crucial in the design and optimization of catalysts for this process. In this study, Cu-CeO2-ZrO2 catalysts (CuCe + Zr, CuZr + Ce, CeZr + Cu, and CuCeZr) with different interactions between metal Cu and supports were successfully prepared. We mainly address the problem that how the MSI affects the catalytic performance. The CuCeZr prepared by one step solid-phase method shows the optimal catalytic activity and stability for CO2 hydrogenation, even better than the benchmark commercial Cu-ZnO-Al2O3 catalyst for syngas to methanol. Based on the investigation of the structure-performance relationship of catalysts, we propose that the excellent catalytic activity of CuCeZr is mainly determined by its largest surface area of metallic Cu (SCu) and the most amount of Cu species at Cu-support interface, both resulting from the strongest MSI between metallic Cu and CeO2-ZrO2 support. Furthermore, in situ DRIFTS showed that the strong SMI in CuCeZr promotes the formation of formate and its rapid transfer to methoxy, thereby efficiently producing methanol. This work reveals the intrinsic active sites of Cu-CeO2-ZrO2 catalysts from a MSI perspective, providing useful insights for researchers to design highly efficient Cu-based catalysts.

Robust palladium oxide nano-cluster catalysts using atomic ions and strong interactions for high-performance methane oxidation

Optimizing metal catalyst structures to achieve desired states is vital for efficient surface reactions, yet remains challenging due to the lack of well-defined precursor materials and weak metal-support interaction. Palladium-based catalysts, when not properly tailored for complete methane oxidation exhibit insufficient performance. Herein, we fabricate Pd oxide nano-clusters supported on SSZ-13 using atomic ions with strong metal-support interaction (SMSI). Steam treatment of Pd/SSZ-13 transforms Pd particles into ions and induces SMSI. Subsequently, CO reduction and O2 oxidation yield mildly sintered Pd oxide nano-clusters firmly anchored on extra-framework Alpenta sites of SSZ-13, facilitating superior activity. The robustness from SMSI prevents irreversible deactivation, and water-resistance by complete dehydration suppresses reversible degradation in wet conditions. This catalyst exhibits high performance in bench-scale reactions using monolith catalysts, ensuring applicability for industrial methane abatement. The results demonstrate that sequential treatment to Pd/SSZ-13 offers a promising approach for tailoring metal structures to enable high-performance methane oxidation.

Architecturing ultra-stable multi-dimensional MXene/MAX self-supporting electrode anchored with Low-Pt for efficient hydrogen evolution reaction in harsh environments

The design of self-supporting structure is particularly important to improve the stability and electrochemical performance of hydrogen evolution reaction electrode. Here, a facile strategy for building novel ultra-stable 0D-2D-3D integrated self-supporting electrode with high conductivity, sufficient diffusion channels and large reactive surface area was proposed. In the heterostructure, 2D Ti3C2Tx flakes in-situ synthesized on 3D network porous Ti3AlC2 surface which provides the multiple reactive surface areas and aggregation resistance to facilitating 0D ultrafine Pt nanoparticles uniform anchorage. Combined with structural characterization and first-principles calculations revealed that, the highly dispersed ultrafine Pt synergistically coupling strong metal-support interactions creates a unique multifunctional catalytic interface with high stability and atomic utilization efficiency of Pt to promote the HER in acidic and seawater. The resultant self-supporting electrode (support 0.48 wt% Pt) exhibits much superior activity to 10 % commercial Pt/C (loaded on foam nickel) in 0.5 M H2SO4 (55 mV@10 mA cm−2) and simulate seawater (196 mV@10 mA cm−2) while reducing the Pt usage by 15 times. Meanwhile, the electrode also illustrates outstanding stability under high current densities (100 h@100 mA cm−2). This study provides a new design idea for developing integrated self-supporting catalytic electrodes to meet the durability of hydrogen evolution reaction applications in harsh environments.

Ultra-Fast Synthesis of Highly Dispersed Pt Nanoclusters Anchored on Sulfur-Doped Porous Carbon Carriers by Nanosecond Pulsed Laser for Hydrogen Evolution Reaction.

Nanosecond pulsed laser irradiation is employed for synthesis of highly active and stable Pt-based electrocatalysts by anchoring Pt nanoclusters on porous sulfur-doped carbon supports (L-Pt/SC). Strong metal-support interaction (SMSI) between Pt and S induces a local charge rearrangement and modulates the electronic structure of Pt surroundings, thus boosting the reaction kinetics and enhancing stability in long-term hydrogen evolution reaction (HER). The L-Pt/SC catalyst exhibits high activity toward HER, with an overpotential of 23 mV at current densities reaching 10 mA cm-2 and a Tafel slope of 24mV dec-1. The unit mass activity of L-Pt/SC is calculated to be -10.8 A cm-2 mgPt -1 at an applied voltage of -0.3V versus RHE. In situ Raman spectra reveals that L-Pt/SC catalyst exhibits fast hydrogen production efficiency and its electrocatalytic HER process is determined by the Tafel step. Density functional theory calculations suggest the strong bonding energy between SC and Pt induces the formation of smaller nanoclusters of L-Pt/SC during fast pulsed laser preparation, which increases the effective contact area during the HER process thereby increasing the activity per unit mass.

In-situ observation of defects evolution of graphene nanoflakes in Pt/C catalyst for boosting ORR performance

The structural stability of supported metal nanoparticles determines the activity and longevity of heterogeneous catalysts. Unfortunately, the chemical/thermal working environment inevitably accelerates metal sintering to larger crystallites that leads to the degradation of catalytic performance. Here, we demonstrate that the distribution of defects in carbon support as an inherent parameter plays a crucial role in catalyst sintering. Based on in-situ transmission electron microscopy studies, the strong metal-support interaction between platinum (Pt) nanoparticles and defect-rich graphene nanoflakes largely suppresses metal sintering up to 700 °C. Particularly, the optimal carbon support can be achieved in the annealing process, in which the mass transfer and charge transport can be enhanced by accurately manipulating the distribution of defects in carbon matrix and graphitization degree. It is worth noting that the screened Pt/GNs-300 exhibits impressive oxygen reduction reaction performance with high half-wave potential (0.91 V), mass activity (108.1 A g–1Pt) and excellent stability. By its ascendancy in ORR, the Pt/GNs-300 exhibits a high open-circuit voltage of 1.41 V and a maximum power density of 198.6 mW cm−2 in Zn-air battery, implying its brilliant practicability. This work paves a pathway for achieving sinter-resistant metal-loaded catalysts in energy electrocatalysis.