Defect-rich Surface Research Articles

Engineering p-d orbital hybridization in PdSb bimetallene for energy-saving H2 production parallel upgrade plastic waste

The electrochemical conversion of PET-derived ethylene glycol into high-quality chemicals parallel energy-saving H2 production is an optimal solution to the serious environmental pollution of plastics. In this paper, p-d orbital hybrid PdSb bimetallene with defect-rich crimped surface is synthesized by a one-step solvent approach. PdSb bimetallene exhibits excellent electrocatalytic performance in ethylene glycol and PET hydrolysate oxidation attributed to the unconventional p-d orbital hybridization feature and metallene structure. PdSb bimetallene shows better properties than Pd metallene and commercial Pd black catalysts under ethylene glycol conditions and PET hydrolysate. Besides PdSb bimetallene can oxidize ethylene glycol to produce the valuable product glycolic acid with high Faradaic efficiency and selectivity. Besides, PdSb bimetallene can oxidize PET-derived ethylene glycol into glycolic acid with high selectivity in EGOR||HER system. This study provides insights into the synthesis of metallene with p-d orbital hybridization properties, coupled with energy-saving H2 production parallel upgrade plastic waste.

Synergistic effect of oxygen vacancies and in-situ formed bismuth metal centers on BiVO4 as an enhanced bifunctional Li–O2 batteries electrocatalyst

Bismuth Vanadate (BiVO4) is a promising oxide-based photoanode for electrochemical applications, yet its practical use is constrained by poor charge transport properties, particularly under dark conditions. This study introduces a novel BiVO4 variant (Bi-BiVO4-10) that incorporates abundant oxygen vacancies and in-situ formed Bi metal, significantly enhancing its electrical conductivity and catalytic performance. Bi-BiVO4-10 demonstrates superior electrochemical performances compared to conventional BiVO4 (C-BiVO4), demonstrated by its most positive half-wave potential with the highest diffusion-limiting current in the oxygen reduction reaction (ORR) and earliest onset potential in the oxygen evolution reaction (OER). Notably, Bi-BiVO4-10 is explored for the first time as an electrocatalyst for lithium-oxygen (Li–O2) cells, showing reduced overcharge (610 mV) in the first cycle and extended cycle life (1050 h), outperforming carbon (320 h) and C-BiVO4 (450 h) references. The enhancement is attributed to the synergy of oxygen vacancies, Bi metal formation, increased surface area, and improved electrical conductivity, which collectively facilitate Li2O2 growth, enhance charge transport kinetics, and ensure stable cycling. Theoretical calculations reveal enhanced chemical interactions between intermediate molecules and the defect-rich surfaces of Bi-BiVO4-10, promoting efficient discharge and charge processes in Li–O2 batteries. This research highlights the potential of unconventional BiVO4-based materials as durable electrocatalysts and for broader electrochemical applications.

Near-infrared light-promoted engineering oxygen vacancy of Fe3Ov-Mo/P nanozyme for sensitive detection of glyphosate

The rapid and sensitive detection of glyphosate herbicide in agricultural products is urgent need. Herein, we develop a photosensitive Fe3Ov-Mo/P nanozyme with defect-rich rough surface by the co-precipitation method. In particular, the Fe3Ov-Mo/P nanozyme with high-percentage oxygen vacancy (OV) defects and rough surface exhibited superior peroxidase (POD)-like activity and kinetics. More intriguingly, Fe3Ov-Mo/P nanozyme with strong optical absorption in near-infrared (NIR) region showed excellent light-promoted POD-like activity. It was found that the defect-rich rough surface is conducive to the adsorption of glyphosate to inhibit the POD-like activity of Fe3Ov-Mo/P. Under near-infrared laser irradiation, the inhibitory effect of glyphosate on the oxidation of 3,3′,5,5′-tetramethylbenzidine (TMB) by Fe3Ov-Mo/P was increased by 2.64 times. A colorimetric platform was developed for the detection of glyphosate with a low detection limit of 0.032 mg L-1 and good selectivity. The method was used to determine the residual glyphosate in coffee, and the recovery efficiency was between 91.20–104.00 %. This work that combines the advantage of defect engineering and NIR provides a strategy for developing high-active nanozyme in pesticide assay.

Single step grown porous polycrystalline nickel microstructures with ultra-thin defect rich surface oxide for alkaline water oxidation

Investigation on the intrinsic catalytic activity of structurally diverse polycrystalline nickel microstructures such as porous nickel sheets (PNS), porous folded/curled nickel structures (PFNS) and porous nickel balls (PNB) revealed the surface bounded electrocatalytic activities within an alkaline reaction environment for water oxidation. Nickel microstructures were grown via template/surfactant-free, single step solution combustion technique in air atmosphere. The distinct morphologies (porous nickel sheets, porous folded/curled nickel structures and porous nickel balls) were achieved through changing the quantity of HNO3 in the reaction mixture. The physicochemical characterisations were done with XRD, FESEM, EDS and XPS. Microscopic studies revealed the growth of nickel grains with numerous macro pores forming microstructures in distinct morphologies. The O ls spectra of XPS studies revealed the presence of O−/O2− sites and Ni 2p spectra were distinguished between the formation of Ni0/Ni2+/Ni3+ states, implied the existence of surface oxide with plenty of defects. The synergistic effect results from the formation of microscopic porous architectures with defect rich surface oxide on the electrochemical behaviour and OER activity of PNS, PFNS and PNB were discussed with electrochemical techniques such as CV, LSV, EIS and CP. The OER kinetics in terms of relatively low value of overpotential at 10 mA cm−2 and Tafel slope along with high specific activity of PNS/GCE with respect to PFNS/GCE and PNB/GCE were attributed to the combined effect of increase in electrochemical surface area, high roughness factor and fast charge transfer kinetics. The better electrochemical performance and OER activities of porous nickel sheets in comparison with folded/curled nickel structures and nickel balls is contributed to the unique 2D porous architecture with plenty of oxygen vacancies. This structure not only expose more surface for the formation of passive oxide layer in an alkaline reaction environment but also exhibit facile charge transport properties, causes the generation of numerous surface-active sites for electrocatalytic water oxidation. The outcome of our work gives new insights on the surface electrochemistry of polycrystalline nickel, enables micro-structuring as a prospective strategy towards the optimization of electrocatalysts as anode material for alkaline water oxidation.

Structure and defect engineering synergistically boost Mo6+/Mo4+ circulation of Sv-MoS2 based photo-Fenton-like system for efficient levofloxacin degradation

The kinetics of redox couples based exclusively on peroxymonosulfate (PMS) are notably slow and inefficient. In this study, urchin-like Sv-MoS2 were in situ deposited onto defect-rich NBC-C3N5 surfaces using a hydrothermal method. The inherent defects in NBC-C3N5@Sv-MoS2 (NCM) along with sulfur vacancies (Sv) directionally inject electrons into Mo sites through a “stabilize-then-accelerate” strategy, culminating in the self-regeneration of Mo sites. Both experimental data and Density Functional Theory (DFT) calculations confirm that NCM effectively activates PMS, generating hydroxyl radicals (•OH) and sulfate radicals (SO4•-) for the degradation of Levofloxacin (LFX) under visible light. The presence of Sv-MoS2 notably extends the peroxy bond (O-O) length in PMS, enhancing electron flux and thereby facilitating superior radical generation compared to singlet oxygen (1O2). Furthermore, experimental assessments of reactors and stirring devices within the NCM system underscore its potential applications in water environmental remediation.

Highly dispersed Cu loaded on HNO3-treated activated carbon for enhanced NH3 adsorption performance

Activated carbon (AC) is highly desirable as an adsorbent for NH3 due to its low cost. Metal chlorides, such as CuCl2, are also known as efficient components for NH3 adsorption. However, once loaded onto AC, CuCl2 tends to aggregate easily, thereby reducing its utilization efficiency. In this work, a facile approach involving HNO3 treatment followed by Cu loading was employed to prepare a high-performance AC adsorbent for NH3 adsorption at room temperature. The AC with a defect-rich surface and a well-developed pore structure was obtained by 30% HNO3 treatment. The subsequently loaded 5 wt% Cu exhibited a highly dispersed state. Consequently, compared to AC directly loaded with Cu without HNO3 treatment, the NH3 adsorption capacity was increased more than 5-fold. Meanwhile, the acidic functional groups introduced by HNO3 treatment also played a significant role in this enhancement. Furthermore, the structure-performance relationship of the prepared adsorbent and the mechanism of NH3 adsorption were elucidated according to characterization results. This work provides a facile strategy for enhancing metal dispersion on activated carbon and its adsorption performance.

Multifunctional Nanomaterials for Advancing Neural Interfaces: Recording, Stimulation, and Beyond.

ConspectusNeurotechnology has seen dramatic improvements in the last three decades. The major focus in the field has been to design electrical communication platforms with high spatial resolution, stability, and translatability for understanding and affecting neural pathways. The deployment of nanomaterials in bioelectronics has enhanced the capabilities of conventional approaches employing microelectrode arrays (MEAs) for electrical interfaces, allowing the construction of miniaturized, high-performance neuroelectronics (Garg, R.; et al. ACS Appl. Nano Mater. 2023, 6, 8495). While these advancements in the electrical neuronal interface have revolutionized neurotechnology both in scale and breadth, an in-depth understanding of neurons' interactions is challenging due to the complexity of the environments where the cells and tissues are laid. The activity of large, three-dimensional neuronal systems has proven difficult to accurately monitor and modulate, and chemical cell-cell communication is often completely neglected. Recent breakthroughs in nanotechnology have provided opportunities to use new nonelectric modes of communication with neurons and to significantly enhance electrical signal interface capabilities. The enhanced electrochemical activity and optical activity of nanomaterials owing to their nonbulk electronic properties and surface nanostructuring have seen extensive utilization. Nanomaterials' enhanced optical activity enables remote neural state modulation, whereas the defect-rich surfaces provide an enormous number of available electrocatalytic sites for neurochemical detection and electrochemical modulation of cell microenvironments through Faradaic processes. Such unique properties can allow multimodal neural interrogation toward generating closed-loop interfaces with access to more complete neural state descriptors. In this Account, we will review recent advances and our efforts spearheaded toward utilizing nanostructured electrodes for enhanced bidirectional interfaces with neurons, the application of unique hybrid nanomaterials for remote nongenetic optical stimulation of neurons, tunable nanomaterials for highly sensitive and selective neurotransmitter detection, and the utilization of nanomaterials as electrocatalysts toward electrochemically modulating cellular activity. We highlight applications of these technologies across cell types through nanomaterial engineering with a focus on multifunctional graphene nanostructures applied though several modes of neural modulation but also an exploration of broad material classes for maximizing the potency of closed-loop bioelectronics.

Role of passivation ligand in exciton diffusion and emission mechanism of metal halide perovskite nanocrystal solid

Shorter-ligand passivated metal halide perovskite nanocrystal (PNC) solids possess smaller inter-NC edge distance which can potentially activate shorter-range nonradiative routes of energy transfer. However, these PNCs are prone to develop surface defects due to ligand detachment and the photogenerated excitons also have high probability to undergo dissociation. It remains unclear how these factors influence the exciton diffusion and emission mechanism of PNC solids. Herein, we prepare two PNC solids passivated with alkylamine and alkylacid ligands of different chain lengths and investigate the exciton diffusion and emission properties by combining time-resolved photoluminescence (PL) and low temperature PL spectroscopy. Our results show that due to the easy ligand detachment and rich surface defects, no prominent exciton transfer occurs in PNC solid passivated with short ligands, despite of the shorter distance between adjacent PNCs. In comparison, the PNC solid passivated with long ligands shows significant occurrence of exciton diffusion from high energy sites towards low energy sites. Accordingly, the PL spectra of thick PNC solid passivated with different ligands show a strikingly different evolution trend with decreasing temperature: in short ligand passivated PNC solid, an intrinsic emission is observed along with a defect-related emission arising from carrier trapping and subsequent radiative recombination, and both emissions are enhanced at lower temperature; in long ligand passivated PNC solid, high energy emission quenches while low energy emission is strengthened at lower temperature due to enhanced exciton transfer. This work reveals that the exciton diffusion and emission properties of PNC solid is strongly mediated by the passivation ligands, providing important insights for their applications in optoelectronic devices.

Nano-roughness effect on the interfacial thermal oxidation and surface catalytical recombination characteristics for silicon carbide based materials under non-equilibrium flow

With the rapid development of high-speed aircraft, the demanding for light, strong, reliable and high temperature resistive thermal protection material (TPM) is becoming urgent. High temperature material interface, such as silicon carbide (SiC) ceramic matrix composite, has received strong interest recently due to its high mechanical and thermochemical stability. For reactive interface development with nano-roughness under extremely hyperthermal non-equilibrium flow conditions for TPM applications, however, has not been reported yet. This work performs a systematic reactive molecular dynamics (RMD) study of the SiC surface morphology effect withstanding hyperthermal atomic oxygen (AO) impact via a gas–solid interface reaction model. The results show that a self-healing trend of the defect-rich silicon carbide surface with original nano-roughness is revealed towards a flatter interface accompanying with the oxidation process. The surface catalytic recombination coefficient is more sensitivity to the surface defects when wall temperature Tw > 500 K. Nano-roughness structure can also vary the main thermochemical reaction path at the thermochemical reactive interface: For the nano-groove surface model, the thermal oxidation reaction becomes dominant, while more pronounced surface catalytic recombination characteristics are revealed for the flat surface model. The mechanisms of roughness effect, surface temperature and gas impacting angle on the surface catalytic recombination, surface oxidation, and interface evolution are revealed, which advance our microscopic understanding of SiC interfacial performance with nano-roughness under non-equilibrium flow conditions.

Ultrafast Exciton Dynamics of CH3NH3PbBr3 Perovskite Nanoclusters.

Exciton dynamics of perovskite nanoclusters has been investigated for the first time using femtosecond transient absorption (TA) and time-resolved photoluminescence (TRPL) spectroscopy. The TA results show two photoinduced absorption signals at 420 and 461 nm and a photoinduced bleach (PB) signal at 448 nm. The analysis of the PB recovery kinetic decay and kinetic model uncovered multiple processes contributing to electron-hole recombination. The fast component (∼8 ps) is attributed to vibrational relaxation within the initial excited state, and the medium component (∼60 ps) is attributed to shallow carrier trapping. The slow component is attributed to deep carrier trapping from the initial conduction band edge (∼666 ps) and the shallow trap state (∼40 ps). The TRPL reveals longer time dynamics, with modeled lifetimes of 6.6 and 93 ns attributed to recombination through the deep trap state and direct band edge recombination, respectively. The significant role of exciton trapping processes in the dynamics indicates that these highly confined nanoclusters have defect-rich surfaces.

Facile fabrication of carbon supported Bi2O3-BiOCl-Bi heterostructure to boost ammonia under visible light

In this paper, carbon supported Bi2O3-BiOCl-Bi heterostructures were successfully synthesized via a facile and simple hydrothermal method. A series of structure and morphology testing clearly showed that carbon and metallic Bi were deposited on the surface margin of Bi2O3-BiOCl, which benefited the rapid transfer of internal photogenerated electrons. Photophysical experiments including electron paramagnetic resonance (EPR) and X-ray photoelectron spectroscopy (XPS) indicated that the amount of surface oxygen vacancies (OVs) was significantly increased, which act as reactive active sites and therefore effectively enhance the photocatalytic performance. The photocatalytic N2 reduction yield of C@Bi2O3-BiOCl-Bi was remarkably improved to 400 μg·L−1, which was 3.63 times higher than that of BiOCl. This research demonstrated a feasible strategy to construct advanced photocatalyst by incorporating defect-rich structures and surface engineering.

One-step synthesis of δ-MnO2 with rich defects for efficient ozone decomposition under humid conditions

The catalytic performance of manganese oxides (MnOx) for ozone (O3) decomposition is affected by moisture and stability, for which MnOx with abundant defects offers a promising solution. In this study, a simple and mild one-step synthesis route was developed for highly defective δ-MnO2 preparation. The optimal catalyst was operated at 35 % relative humidity (RH) for 12 h, and the O3 conversion maintained over 99 %. Characterizations revealed that the K+ insertion into the interlayers preserved a highly defective layered structure. Rich surface defects and grain boundaries facilitated the generation of oxygen vacancies and the migration of oxygen species, stabilizing the elimination of O3. In addition, a combination of characterization and experiments determined that physisorbed water is critical for inhibiting activity, and thus, weak physisorption of water on the catalyst represents excellent water resistance. This work aims to provide guidance and new insights into the design of stable and water-resistant MnOx catalysts.

Variations in proton transfer pathways and energetics on pristine and defect-rich quartz surfaces in water: Insights into the bimodal acidities of quartz

HypothesisUnderstanding the mechanisms of proton transfer on quartz surfaces in water is critical for a range of processes in geochemical, environmental, and materials sciences. The wide range of surface acidities (>9 pKa units) found on the ubiquitous mineral quartz is caused by the structural variations of surface silanol groups. Molecular scale simulations provide essential tools for elucidating the origin of site-specific surface acidities. SimulationsWe used density-functional tight-binding-based molecular dynamics combined with rare-event metadynamics simulations to probe the mechanisms of deprotonation reactions from ten representative surface silanol groups found on both pristine and defect-rich quartz (101) surfaces with Si vacancies. FindingsThe results show that deprotonation is a highly dynamic process where both the surface hydroxyls and bridging oxygen atoms serve as the proton acceptors, in addition to water. Deprotonation of embedded silanols through intrasurface proton transfer exhibited lower pKa values with less H-bond participation and higher energy barriers, suggesting a new mechanism to explain the bimodal acidity observed on quartz surface. Defect sites, recently shown to comprise a significant portion of the quartz (101) surface, diversify the coordination and local H-bonding environments of the surface silanols, changing both the deprotonation pathways and energetics, leading to a wider range of pKa values (2.4 to 11.5) than that observed on pristine quartz surface (10.4 and 12.1).

Defect-rich Pt-Ru metallic aerogels for highly efficient ethanol oxidation reaction

Direct ethanol fuel cells (DEFCs) are a new type of green and efficient energy conversion devices, but the slow anodic reaction kinetics limit their application. Herein, a series of Pt-Ru metallic aerogels (MAs) with controllable composition, rich surface defects, and large specific surface area were prepared for ethanol oxidation reaction (EOR) by freeze–thaw method. Pt6Ru MAs exhibit the highest mass activity (1.264 A mgPt−1) toward EOR among all the catalysts we have prepared, which is 2.0, 1.8, and 3.7 times higher than those of Pt MAs (0.632 A mgPt−1), the commercial Pt/C (0.696 A mgPt−1), Pt6Ru NPs (0.339 A mgPt−1). 1H nuclear magnetic resonance spectroscopy confirms that only acetic acid was the liquid product of Pt6Ru MAs during EOR catalysis. Furthermore, Pt6Ru MAs show little attenuation and satisfactory reactivation abilities in stability assessment, demonstrating their good stability. This proves that the introduction of Ru makes feasible adjustments to the electronic structure of Pt in MAs, improving the electrocatalysis activity of Pt6Ru MAs in EOR. Mechanistic investigations reveal that the optimal electronic structure is the intrinsic reason for the excellent EOR performance of Pt6Ru MAs. The findings open a new way to develop high-performance Pt-based materials electrocatalysts.

The controlled engineering of surface oxygen defects on Bi2Zr2O7 compounds for catalytic soot combustion by adjusting the preparation methods.

The quantity of surface oxygen vacancies/defects is critical to promote the reactivity of metal oxide catalysts. Therefore, for the controlled engineering of Bi2Zr2O7 with rich surface defects for soot combustion, four different methods have been adopted. Bi2Zr2O7 compounds with a defective fluorite phase but with varied surface vacancy concentrations have been successfully synthesized by various methods. The best catalyst (Bi2Zr2O7-CP) was fabricated by a facile co-precipitation method. Both O2- and O22- were the active surface sites whose number positively correlated to the number of surface oxygen vacancies and determined the activity. Moreover, a sample with more surface vacancies usually had weaker Zr-O bonds, which could be the intrinsic factor to enhance the activity. In addition, a novel and simple method has been developed to accurately titrate the absolute amount of soot reactive oxygen sites and calculate the TOF values. In conclusion, by optimizing the preparation methods, Bi2Zr2O7 catalysts with rich surface defects can be tuned, which may help in designing more applicable soot oxidation catalysts.

Bimetallic Pt–M (M = Fe, Co, Ni) nanobunches composed of ultrathin nanowires with strong synergy and rich surface defects for enhanced methanol oxidation electrocatalysis

High performance and cost-effective electrocatalysts have been intensively pursued to push forward the commercialization of direct methanol fuel cells (DMFCs).

The 5d-5p-3d orbital hybridization induced by light incorporation of Cu into surface-uneven Pt3Sn intermetallic nanocubes customizes dual-intermediates adsorptions for CO-resilient methanol oxidation

Catalysts with excellent performances for methanol oxidation reaction (MOR) are supposed to equip with a weaker *CO adsorption but a stronger *OH adsorption. Herein, light incorporation of Cu is implemented into surface-uneven Pt3Sn intermetallic nanocubes to manipulate crucial CO*/OH* intermediates adsorptions for boosting MOR electrocatalysis. The generated ternary Cu0.2Pt3Sn/CNTs intermetallic preserves the uneven cubic shape of non-doped Pt3Sn/CNTs, providing a defect-rich surface structure for affording abundant available active sites. More importantly, the incorporated Cu induces a strong Pt 5d-Sn 5p-Cu 3d orbital hybridization, which upgrades the electron density of Pt but reversely downgrades that of Sn. Such delicately tailored local coordination environments of Pt and Sn result in an intrinsically attenuated CO* adsorption on Pt sites but a promoted OH* adsorption on Sn sites, remarkably diminishing the energy barrier of CO* oxidation. The elaborately customized dual-intermediates adsorptions combined with the defect-rich cubic architecture superiorities consequently contribute to highly elevated MOR performance.

Direct observation on single-crystal-to-single-crystal transformation via lattice-matched nucleation and growth

Single-crystal-to-single-crystal (SCSC) phase transformation has been showing its great significances for controllable synthesis of advanced materials. From this point of view, the atomic-scale understanding of structural dynamics during SCSC transformation is of fundamental criticality for its utilizations in many disciplines, which, however, remains a grand challenge due to the lack of direct and effective experimental probes. Here, we report a complete observation regarding atomic-scale mechanisms for nucleation and growth of a hexagonal phase in a monoclinic matrix during a heating-induced structural transformation using in situ transmission electron microscopy. The overall process consists of several distinct steps; namely, defect generation, phase nucleation, phase growth and propagation. In particular, the new hexagonal phase is found to nucleate at defect-rich high-energy surface regions of the matrix, and subsequently grow in a lattice-matched manner between the old monoclinic and new hexagonal phases, thus maintaining the single-crystalline nature of the product phase during the whole transformation, even in the case of discrete nucleation at multiple sites. Such findings provide crucial insights for the understanding of microscopic mechanisms and kinetics of solid-state phase transitions.

Enhanced Sequestration of Chromium by Mechanochemically Silicified Microscale Zerovalent Iron: Role of the Silicate-Modified Surface

Remediation of chromium-contaminated groundwater remains a significant environmental challenge around the world. Herein, we synthesized silicified microscale zerovalent iron (Si-mZVIbm) using a mechanochemical method and demonstrated that the silicate modification could significantly improve the Cr(VI) removal efficiency (up to 37.5-fold) compared with its un-silicified counterpart. Results of atomic force microscopy, scanning transmission electron microscopy, and positron annihilation measurements revealed that silicate acted as a milling lubricant to boost strain within zerovalent iron particles, inducing more plastic deformation and surface defects. The defect-rich silicified surface accelerates the electron transfer and subsequent in situ generation of Fe(II). More importantly, the surface-modified silicate can act as a ligand to coordinate leached Fe(II) ions, thus strengthening the reduction of Cr(VI) via surface-bound Fe(II) and favoring subsequent co-precipitation of Cr(III) and Fe(III) species on Si-mZVIbm surfaces. During column experiments using real Cr-contaminated groundwater, Si-mZVIbm (4 wt % in sand) was able to reduce the Cr(VI) concentration from 2 to 0.05 mg L–1, the World Health Organization drinking water standard for up to 1720 bed volumes with an empty-bed contact time of 5.1 min. These results demonstrate the potential field applicability of Si-mZVIbm in real contaminated groundwater remediation.

Defect-enriched red phosphorus nanosheets as efficient and stable photothermal absorber material for interfacial solar desalination

The development of efficient photothermal materials has gained increasing attention for solar thermal-energy conversion. A good photothermal material has a strong light-absorption property, low thermal conductivity, high wettability, and high solar-to-thermal conversion efficiency. In this study, we prepared uniform, sub-micron, and defect-rich red phosphorus (RP) nanosheets via a simple ball-milling method to demonstrate their efficient and durable solar steam generation properties. Three RPs of different sizes were prepared by controlling the milling time (0 h: RP0, 30 h: RP30, and 60 h: RP60). Notably, RP60 exhibited the smallest particle (lateral) size, nanosheet morphology, and defect-rich surface. Furthermore, RP60 exhibited the distinctive properties of a small band gap (1.44 eV), low thermal conductivity (0.07 W/m·K), and low heat capacity (0.66 J/g·K) with exceptional wettability. With simulated sunlight illumination (100 mW/cm2, 1 sun), the RP60 photothermal absorber demonstrated a high water evaporation rate of 1.34 kg/m2·h with a stable solar steam generation efficiency of 74.1 % for over 10 h. A one-dimensional water path and porous polyurethane support facilitated the water supply, large contact area, heat localization, and steam escape. By employing plasmonic resonance-heating silver nanoparticles on the RP60, we achieved a significantly improved solar steam generation efficiency of over 96.0 % and a water evaporation rate of 1.75 kg/m2·h. This study highlights the critical role of morphology, particle size, and defects control in improving the photothermal properties for efficient and durable interfacial seawater desalination.