Surface Engineering Strategy Research Articles

Regulating Zn Deposition Manner by Confining the Reactivity of Free Water in the Electric Double Layer.

Aqueous Zn ion batteries (AZIBs) are promising candidates of next-generation energy storage devices with high safety and theoretical capacity. However, the irreversibility of metallic Zn anode, attributed to dendrite growth and water decomposition, severely limits the cycling durability of AZIBs and restricts their further development. Herein, a facile surface engineering strategy is put forward to tackle the issue of poor reversibility of the Zn anode. Benzotriazole (BTA) is employed as a functional additive of ZnSO4 electrolyte to confine the reactivity of free water situated in the electric double layer (EDL). Experimental results and theoretical simulation reveal that BTA can preferiencially adsorb onto the Zn surface to uniform Zn2+ ion distribution and alleviate H2O-involved side reactions like hydrogen evolution, and surface passivation. Consequently, in BTA-modulated aqueous electrolyte, the lifespan of the Zn anode is extended from 170 h to 1092 h at 1 mA cm-2/1 mAh cm-2. The reversibility improvement of Zn anode also benefits the cycling durability of full devices including supercapacitors and batteries. Zn||I₂ batteries assembled in as-designed electrolyte witness only 11.3% capacity decay over 17000 cycles at 1 A g-1, far outstripping that observed in ZnSO4 counterpart (~ 4675 cycles).

Atomic scale etching of diamond: insights from molecular dynamics simulations

Abstract Diamond is a promising material for multiple applications in quantum information processing and sensing as well as applications in microelectronics. However, diamond devices can be limited by surface defects that compromise charge stability and spin coherence, among others. Improved strategies in plasma etching of diamond could play an important role in minimizing or eliminating these defects. In this work, we explore plasma-assisted atomic scale etching of diamond using argon ions (Ar+), hydrogen ions (H+) and hydrogen atoms (H). We employ classical molecular dynamics (MD) simulations and test several interatomic potentials based on the Reactive Empirical Bond Order (REBO) form with comparisons to a variety of published experimental results. We performed MD simulations of low-energy hydrogen ( ⩽ 50 eV) and argon ( ⩽ 200 eV) ion bombardment of diamond surfaces. Ar+ bombardment can be used to locally smooth initially rough diamond surfaces via the formation of an amorphous C layer, the thickness of which increases with argon ion energy. Subsequent exposure with hydrogen ions (or fast neutrals) will selectively etch this amorphous C layer, leaving the underlying diamond layer mostly intact if the H energy is maintained below about 10 eV. The simulations suggest that combining Ar+ smoothing with selective, near threshold energy H removal of amorphous C can be an effective strategy for diamond surface engineering, leading to more reliable and sensitive diamond color center devices.

Angiogenesis-osteogenesis coupling and anti-osteoclastogenesis zoledronate intermixed calcium silicate metal-organic/inorganic hybrid coating on biodegradable zinc-based intramedullary nails for osteoporotic fracture healing

Osteoporotic (OP) fractures remain a tough clinical challenge owing to their impaired healing outcome, which requires novel biomaterials with osteogenicity for effective healing. Metallic zinc (Zn) is attracting increasing attention for biodegradable intramedullary nails (IMNs) for OP fracture healing thanks to their comprehensive mechanical properties, biosafety, and bioactivity. However, the multiple biofunctions required for OP fracture healing have not been fully met by Zn. Herein, a zoledronate (ZA)-mediated calcium-zinc silicate (Ca(Zn)Si) metal-organic/inorganic hybrid coating was fabricated on Zn-based IMN by coordination chemistry driven via interactions between ZA and Ca2+/Zn2+ as well as in-situ directional growth of Ca(Zn)Si phase. The ZA&Ca(Zn)Si hybrid coating exhibited a homogeneous micro/nanostructure with a granular morphology, which prevented premature fracture failure of IMN in rat femur by ameliorating corrosion mode and decreasing degradation rate of the Zn matrix. More importantly, this hybrid coating enabled sustained release of Zn2+/Ca2+/Si4+ and ZA in the long term, achieving a remarkable effect on vascularized bone regeneration. The coated IMN enhanced angiogenesis–osteogenesis coupling through autocrine and paracrine effects between endothelial cells and bone marrow mesenchymal stem cells. Osteoclastogenesis was repressed by Zn2+ and ZA. This approach offers a new strategy for surface-engineering of biodegradable metals for bone fracture healing.

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.

Cell Surface Engineering by Phase‐Separated Coacervates for Antibody Display and Targeted Cancer Cell Therapy

AbstractCell therapies such as CAR−T have demonstrated significant clinical successes, driving the investigation of immune cell surface engineering using natural and synthetic materials to enhance their therapeutic performance. However, many of these materials do not fully replicate the dynamic nature of the extracellular matrix (ECM). This study presents a cell surface engineering strategy that utilizes phase‐separated peptide coacervates to decorate the surface of immune cells. We meticulously designed a tripeptide, Fmoc−Lys−Gly−Dopa−OH (KGdelta; Fmoc=fluorenylmethyloxycarbonyl; delta=Dopa, dihydroxyphenylalanine), that forms coacervates in aqueous solution via phase separation. These coacervates, mirroring the phase separation properties of ECM proteins, coat the natural killer (NK) cell surface with the assistance of Fe3+ ions and create an outer layer capable of encapsulating monoclonal antibodies (mAb), such as Trastuzumab. The antibody‐embedded coacervate layer equips the NK cells with the ability to recognize cancer cells and eliminate them through enhanced antibody‐dependent cellular cytotoxicity (ADCC). This work thus presents a unique strategy of cell surface functionalization and demonstrates its use in displaying cancer‐targeting mAb for cancer therapies, highlighting its potential application in the field of cancer therapy.

Cell Surface Engineering by Phase-Separated Coacervates for Antibody Display and Targeted Cancer Cell Therapy.

Cell therapies such as CAR-T have demonstrated significant clinical successes, driving the investigation of immune cell surface engineering using natural and synthetic materials to enhance their therapeutic performance. However, many of these materials do not fully replicate the dynamic nature of the extracellular matrix (ECM). This study presents a cell surface engineering strategy that utilizes phase-separated peptide coacervates to decorate the surface of immune cells. We meticulously designed a tripeptide, Fmoc-Lys-Gly-Dopa-OH (KGdelta; Fmoc=fluorenylmethyloxycarbonyl; delta=Dopa, dihydroxyphenylalanine), that forms coacervates in aqueous solution via phase separation. These coacervates, mirroring the phase separation properties of ECM proteins, coat the natural killer (NK) cell surface with the assistance of Fe3+ ions and create an outer layer capable of encapsulating monoclonal antibodies (mAb), such as Trastuzumab. The antibody-embedded coacervate layer equips the NK cells with the ability to recognize cancer cells and eliminate them through enhanced antibody-dependent cellular cytotoxicity (ADCC). This work thus presents a unique strategy of cell surface functionalization and demonstrates its use in displaying cancer-targeting mAb for cancer therapies, highlighting its potential application in the field of cancer therapy.

Fabrication of clickable bamboo-sourced cellulose nanofibrils for diverse surface modifications: Hydrophobicity and fluorescence functionalities

Surface functionalization of cellulose nanofibrils (CNF) is crucial for expanding their practical application. However, most functionalization processes are complicated and laborious. Herein, this work presents a facile surface engineering strategy to create a range of functionalized CNF via thiol-ene click reaction. Initially, clickable CNF was produced by grafting a compound with both carboxylate- and norbornene groups onto bamboo cellulose via norbornene-dicarboxylic anhydride esterification followed by homogenization. The introduction of negatively charged carboxylates facilitated nanofibrillation, resulting in CNF with a diameter of 3 nm and an aspect ratio of up to 600. The introduction of norbornenes enabled diverse functionalization of CNF through click reaction. Subsequently, hexadecanethiol successfully clicked with norbornene-grafting CNF, enhancing its hydrophobicity and dispersion in organic solvents. 7-mercapto-4-methyl coumarin was also able to click with norbornene-grafting CNF, yielding fluorescence-labeled CNF while maintaining excellent aqueous dispersibility. The fluorescence-labeled CNF was demonstrated to be utilized as an eco-friendly sensor for the detection of Fe3+ ions. Additionally, it could be converted into fluorescent films or intelligent inks suitable for anti-counterfeiting purposes. This study demonstrates that the proposed surface engineering strategy provides an effective approach for producing clickable CNF and fabricating cellulosic materials with diverse functionalities that meet the demands of various applications.

Cell Membrane-Camouflaged Biomimetic Magnetic Fluorescent Nanoparticles with Enhanced Stability for High-Performance Lead Drug Discovery.

Biomimetic nanoengineering empowers nanoparticles with enhanced biointerfacial capabilities by directly utilizing cell membranes (CMs) of natural origin. This top-down technique provides a powerful tool for the screening of potentially active compounds in complex matrices. Herein, cartilaginous end plate (CEP) cell membrane biomimetic Nile red (NR)-loaded zeolitic imidazolate frameworks-8 (ZIF-8) modified magnetic graphene oxide (CEP/MGO-ZIF-8-NR) nanocomposites with enhanced stability were accurately prepared by chemical bonding and used as a drug discovery platform for the specific identification and effective extraction of drug leads with anti-intervertebral disc degeneration (IDD) in Yaobitong capsules (YBTCs). The constructed CEP/MGO-ZIF-8-NR exhibited excellent magnetic properties, fluorescence properties, and stability. In addition, drug binding experiments showed that the CEP/MGO-ZIF-8-NR nanocomposites possessed higher adsorption capacity, faster adsorption rate, and superior selectivity compared with uncoated MGO-ZIF-8-NR. Ultimately, four potential bioactive molecules, including ginsenoside Ro, ginsenoside Rg1, astringin, and chikusetsusaponin V methyl ester, were successfully screened and identified in vitro from YBTC. The results of the CCK-8 assay and BrdU ELISA kit showed that the screened compounds promoted CEP cell proliferation in a concentration-dependent manner. Cellular distribution experiments revealed that CEP/MGO-ZIF-8-NR could rapidly escape from lysosomes and into the cytoplasm. And the pharmacological activity of these compounds was further confirmed by real-time cytomorphological imaging of CEP cells by confocal laser scanning microscopy (CLSM). Overall, this surface engineering strategy endows bioaffinity sample pretreatment materials with tremendous versatility, improves drug screening efficiency, and broadens the horizons and methodologies for drug lead discovery.

A systematic study on wear behavior of TiCrNbTaWx refractory high-entropy alloy: Inducing amorphization to achieve anti-wear

Refractory high-entropy alloys (RHEAs) possess exceptional properties at elevated temperatures. However, their limited wear resistance at room temperature (RT) hinders their widespread application. In this work, based on compositional modulation and surface engineering strategies, two TiCrNbTaWx (x = 0, 0.5) RHEAs were prepared using spark plasma sintering. The results show that the addition of W can effectively improve the hardness (10.3 GPa) and deformation resistance of the BCC matrix, alleviating the severe adhesion and the fracture behavior. In addition, the friction-induced oxidized amorphous layer with high hardness (12.3 GPa) can further improve the anti-wear properties. Because of these, the TiCrNbTaW0.5 alloy has a low wear rate of 9 × 10−5 mm−3·N−1·m−1, which is 67 % lower than the pristine TiCrNbTa alloy. In conclusion, our design strategy provides a new idea for designing RT wear-resistant RHEAs.

Improving Triethylamine-Sensing Performance of WO3 Nanoplates through In Situ Heterojunction Construction.

Surface engineering techniques can be used to develop high-performance gas sensing materials and advance the development of sensors. In this study, we improved the gas sensing performance of two-dimensional (2D) WO3 nanoplates by combining surface Zn modification and the in situ formation of ZnWO4/WO3 heterojunctions. Introducing Zn atoms by surface modification can reconstruct the atomic surface of 2D WO3 nanoplates, creating additional active sites. This allowed for the preparation of various types of ZnWO4/WO3 heterojunctions on the surface of the WO3 nanoplates, which improved the selectivity and sensitivity to the target gas triethylamine. The sensor exhibited good gas sensing performance for triethylamine even at low operating temperatures and strongly resisted humidity changes. The ZnWO4/WO3 material we prepared demonstrated a nearly threefold improvement in the triethylamine (TEA) response, with a gas sensing responsivity of 40.75 for 10 ppm of TEA at 250 °C. The sensor based on ZnWO4/WO3 has a limit of detection (LOD) for TEA of 200 ppb in practical measurements (its theoretical LOD is even as low as 31 ppb). The method of growing ZnWO4 on the surface of WO3 nanoplates using surface modification techniques to form surface heterojunctions differs from ordinary composites. The results suggest that the in situ construction of surface heterojunctions using surface engineering strategies, such as in situ modifying, is a practical approach to enhance the gas sensing properties and resistance to the humidity changes of metal oxide materials.

Surface engineering and concentration-dependent emission activated flexible tunable fluorescence from lignin-based N-doped carbon dots

Achieving the flexible and tunable fluorescence of lignin-based N-doped carbon dots (LCDs) remains a win–win yet challenging strategy. In this study, combining the surface engineering and concentration regulation strategy enabled the flexible adjustment of LCDs fluorescence emission from blue to yellow regions (345 to 560 nm). The surface electron-donor –OH groups not only enhanced the photoluminescence quantum yield (PLQY) to 14.75 % but activated the spectral shift of reduced LCDs (RLCDs). These arose from the reinforced π-electron conjugation and generated new –OH-related extrinsic defects with elevating concentration. Conversely, the electron-withdrawing CO groups participated in the blue-to-green fluorescence modulation. Still, they drastically reduced the PLQY of oxidized LCDs (OLCDs) to 2.13 %, due to the larger particle size and more non-radiative transfer induced by CO groups. Based on these, CDs/PVA films and printed fluorescent patterns with multicolor fluorescence were realized for anti-counterfeiting, and the RLCDs@Al2O3 hybrid facilitated the precise fluorescence fingerprint tracking and recognition. This study provided a facile strategy for enriching and developing novel LCDs with flexible fluorescence for their advanced applications.

Surface engineering of nickel-rich single-crystal layered oxide cathode enables high-capacity and long cycle-life sulfide all-solid-state batteries

Sulfide all-solid-state lithium batteries (SASSLBs) with a single-crystal nickel-rich layered oxide cathode (LiNixCoyMn1-x-yO2, x ​≥ ​0.8) are highly desirable for advanced power batteries owing to their excellent energy density and safety. Nevertheless, the cathode material's cracking issue and its severe interfacial problem with sulfide solid electrolytes have hindered the further development. This study proposes to employ surface modification engineering to produce B-NCM cathode materials coated with boride nanostructure stabilizer in situ by utilizing NCM encapsulated with residual lithium. This approach enhances the electrochemical performance of SASSLBs by effectively inhibiting electrochemical-mechanical degradation of the NCM cathode material on cycling and reducing deleterious side reactions with the solid sulfide electrolyte. The B-NCM/LPSCl/Gr SASSLBs demonstrate impressive cycling stability, retaining 84.19 ​% of its capacity after 500 cycles at 0.2 ​C, which represents a 30.13 ​% increase vs. NCM/LPSCl/Gr. It also exhibits a specific capacity of 170.4 mAh/g during its first discharge at 0.1 ​C. This work demonstrates an effective surface engineering strategy for enhancing capacity and cycle life, providing valuable insights into solving interfacial problems in SASSLBs.

Surface Engineering Enables Efficient AgBiS2 Quantum Dot Solar Cells.

Surface ligand chemistry is vital to control the synthesis, diminish surface defects, and improve the electronic coupling of quantum dots (QDs) toward emerging applications in optoelectronic devices. Here, we successfully develop highly homogeneous and dispersed AgBiS2 QDs, focus on the control of interdot spacing, and substitute the long-chain ligands with ammonium iodide in solution. This results in improved electronic coupling of AgBiS2 QDs with excellent surface passivation, which greatly facilitates carrier transport within the QD films. Based on the stable AgBiS2 QD dispersion with the optimal ligand state, a homogeneous and densely packed QD film is prepared by a facile one-step coating process, delivering a champion power conversion efficiency of approximately 8% in the QD solar cells with outstanding shelf life stability. The proposed surface engineering strategy holds the potential to become a universal preprocessing step in the realm of high-performance QD optoelectronic devices.

Enhancing the sodium storage performance of hard carbon by constructing thin carbon coatings via esterification reactions

Hard carbons derived from pitch are considered a competitive low-cost anode for sodium-ion batteries. However, the preparation of pitch-based hard carbon (PHC) requires the aid of a pre-oxidation strategy, which introduces unnecessary defects and oxygen elements, which leads to low initial Coulombic efficiency (ICE) and poor cycling stability. Herein, we demonstrate a new surface engineering strategy by grafting chemically active glucose molecules on the PHC surface via esterification reactions, which can achieve low-cost nano-scaled carbon coating. Thin glucose coating can be carbonized at a lower temperature, which results in a more closed pore structure and fewer functional groups. The as prepared PHC exhibits a high reversible capacity of 328.5 mAh/g with a high ICE of 92.08 % at 0.02 A/g. It is noteworthy that the PHC can be adapted to a variety of cathode materials for full-cell assembling without pre-sodiation, which maintains the characteristics of high capacity and excellent cycling stability. The performance of resin-based hard carbon coated with a similar method was also improved, demonstrating the universality of the technique.

Surface engineering of metal-organic framework nanoparticles-based miRNA carrier: Boosting RNA stability, intracellular delivery and synergistic therapy

MicroRNAs (miRNAs) are small noncoding RNAs that are critical for the regulation of multiple physiological and pathological processes, thus holding great clinical potential. However, the therapeutic applications of miRNAs are severely limited by their biological instability and poor intracellular delivery. Herein, we describe a dual-layers surface engineering strategy to design an efficient miRNA delivery nanosystem based on metal–organic frameworks (MOFs) incorporating lipid coating. The resulting nanoparticle system was demonstrated to protect miRNA from ribonuclease degradation, enhance cellular uptake and facilitate lysosomal escape. These ensured effective miRNA mediated gene therapy, which synergized with MOF-specific photodynamic therapy and pre-encapsulated doxorubicin (Dox) chemotherapy to provide a multifunctional with therapeutic effectiveness against cencer cells The mechanisms of miRNA binding and Dox loading were revealed, demonstrating the potential of the present MOFs surface-engineered strategy to overcome their inherent pore-size restriction for macromolecular miRNA carrying, enableefficient co-delivery. In vitro studies revealed the potential of our multifunctional system for miRNA delivery and the demonstrated the therapeutic effectiveness against cancer cells, thereby providing a versatile all-in-one MOFs strategy for delivery of nucleic acids and diverse therapeutic molecules in synergistic therapy.

Decoupling hydrophilicity and superaerophobicity on amorphous molybdenum sulfide for high-rate water splitting

The development of water splitting electrocatalysts with earth-abundant materials capable of delivering high current density is crucial for sustainable H2 production. However, the mass transfer including reactants and bubbles usually suffered from the shielding effect of gas adhesion under such circumstance. Here, we report a surface engineering strategy over amorphous molybdenum sulfide (a-MoSx) to synergistically boost its generation and departure of gas bubbles. To begin with, a hydrophilic surface featuring hydroxy groups was constructed via palladium−doping induced sulfur vacancies on a-MoSx, which could enhance the local access of aqueous reactant. Furthermore, the departure of gas bubbles could be accelerated by regulating the roughness of the synthesized Pd-MoSx(OH)y nanoarrays. For demonstration purpose of practical applications, the bifunctional Pd-MoSx(OH)y nanoarrays could deliver a high current density of 1000 mA cm−2 at 1.99 V for overall water splitting over 100 h.

Dual Modulation of Bulk Electronic Structure and Surficial Active Sites in Sea Urchin‐Like MoO2 Nanoreactors Promoting Electrocatalytic Hydrogen Evolution

AbstractElectrocatalytic hydrogen evolution reaction (HER) is a promising strategy for realizing carbon neutralization as well as for the production of green hydrogen. Molybdenum dioxide (MoO2), possesses acid corrosion resistance and near‐metal‐level conductivity, endowing its widespread application in acidic HER. However, due to spatial barriers at the edge of sites and weak H* adsorption, the HER activity of MoO2 is greatly limited. Herein, a sea urchin‐like Pt@N‐MoO2 nanoreactor is designed, in which the bulk electronic structure and surface‐active sites are modulated by N doping and Pt single atoms anchoring, respectively. DFT calculations indicate that Mo─N coupling changes the charge density of Mo atoms, enhances the adsorption of H*, and thus optimizes the Gibbs free energy. The appearance of Pt‐O/N sites compensates for the lack of active sites exposed by MoO2, while promoting the desorption of H2 from the catalyst surface and accelerating the HER process. This work provides an effective strategy for activating inert electrocatalysts to promote energy conversion via a dual modulation strategy of bulk and surface engineering.

Surface Molecular Engineering for Fully Textured Perovskite/Silicon Tandem Solar Cells.

Developing large-scale monolithic perovskite/silicon tandem devices based on industrial Czochralski silicon wafers will likely have to adopt double-side textured architecture, given their optical benefits and low manufacturing costs. However, the surface engineering strategies that are widely used in solution-processed perovskites to regulate the interface properties are not directly applicable to micrometric textures. Here, we devise a surface passivation strategy by dynamic spray coating (DSC) fluorinated thiophenethylammonium ligands, combining the advantages of providing conformal coverage and suppressing phase conversion on textured surfaces. From the viewpoint of molecular engineering, theoretical calculation and experimental results demonstrate that introducing trifluoromethyl group provide more effective surface passivation through strong interaction and energy alignment by forming a dipole layer. Consequently, the DSC treatment of this bifunctional molecule enables the tandem cells based on industrial silicon wafers to achieve a certified stabilized power conversion efficiency of 30.89 %. In addition, encapsulated devices display excellent operational stability by retaining over 97 % of their initial performance after 600 h continuous illumination.

Engineering Single‐Atom Catalysts on Conjugated Porphyrin Polymer Photocatalysts via E‐Waste for Sustainable Photocatalysis

AbstractThis study presents a surface engineering strategy utilizing electronic waste (e‐waste) to incorporate single‐atom catalysts on conjugated polymers. Employing a conjugated porphyrin polymeric photocatalyst, gold single‐atom‐site catalysts are successfully introduced using the acidic metal leachates from e‐waste, where metal speciation and composition are regulated during the metal loading processes. The resulting photocatalyst with gold single atoms demonstrates a remarkable hydrogen peroxide (H2O2) selectivity of up to 97.56%, yielding a pure H2O2 solution at 73.3 µm h−1 under white LED illumination. The produced H2O2 is activated to •OH radicals on the same polymer with mixed gold and iron atoms, enabling a photo‐Fenton reaction and the complete degradation of toxic microcystin‐LR within 10 min under visible light. This study highlights the universal applicability of the metal mining strategy in various photoreactions. It is believed that this discovery pioneers sustainable photocatalysis, allowing the tuning of reactivity and selectivity on photocatalytic surfaces using metal waste.

Modulating the synergy of Pt single atoms and quantum dots on NiFe LDH for efficient and robust hydrogen evolution

Hydrogen evolution reaction (HER) from water electrolysis is an ideal alternative solution to address the energy crisis and develop clean energy. However, the construction of an efficient electrocatalyst with multiple active sites that can ensure high metal utilization and promote reaction kinetics simultaneously still leaves a major challenge. Herein, we present a facile strategy to synthesize a HER catalyst comprising Pt single atoms (PtSA) anchored in Fe vacancies and Pt quantum dots (PtQD) on the surface of NiFe LDH. Benefitting from the hierarchical and ultrathin nanosheet arrays and strong electronic interaction between PtSA/PtQD and NiFe LDH matrix, the optimized sample (PtSA/QD-NiFeV9 LDH) exhibits outstanding HER performance in 1 M KOH with ultra-low overpotentials of 20 and 67 mV at 10 and 100 mA cm−2, respectively, outperforming the benchmark Pt/C electrocatalyst. In addition, the electrolyzer using PtSA/QD-NiFeV9 LDH as a cathode requires voltages of only 1.48 and 1.73 V to yield current densities of 10 and 1000 mA cm−2, respectively. The combination of in situ tests and density functional theory (DFT) calculations reveal that the synergy of PtSA and PtQD can optimize the kinetics of water dissociation and hydrogen desorption, thus the Volmer-Tafel pathway prevailing the HER process. This work provides a promising surface engineering strategy to develop catalysts for efficient and robust hydrogen evolution.