High-capacity SiOx/graphite (SiO/G) anodes offer great potential for advancing lithium-ion battery technology; however, their practical application is limited by low initial coulombic efficiency (ICE) and rapid capacity decay. These challenges primarily arise from unstable phase transitions and the formation of the solid electrolyte interphase (SEI). Prelithiation strategies that aimed at compensating lithium loss have emerged as an effective solution, showing significant advancements in both anode and cathode research. Nevertheless, the interfacial evolution and mechanisms underlying performance enhancement remain unclear. In this work, we demonstrate roll-to-roll contact prelithiation of SiO/G anodes using an ultrathin lithium film, resulting in improved ICE, cycling stability, and rate capability. The contact prelithiation mechanism of silicon-based anodes was investigated via a combination of in situ and ex situ characterizations alongside electrochemical analyses. These studies reveal that the formation of SEI contains multiple lithium silicate phases during the first cycle of prelithiation. This SEI exhibits enhanced conductivity and stability, which contribute to improved cycling performance and rate capability of the prelithiated anode. The prelithiated silicon-carbon composite anode achieved an ICE of 96% in 5.4 Ah pouch cell tests and demonstrated excellent capacity retention of 74% after 500 cycles. This study not only elucidates the critical role of interfacial evolution in SiOx/graphite anodes but also proposes a rational strategy based on phase-phase interface synergistic design for developing durable, high-performance silicon-based anodes suitable for next-generation lithium-ion batteries. (sic)(sic)(sic)SiOx/(sic)(sic) ( SiO/G ) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)SiO/G(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic),(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)/(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) ( SEI ) (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)SiO/G(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)SEI.(sic)SEI(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)5.4 Ah(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)96%(sic)(sic)(sic)(sic)(sic)(sic) , (sic)500(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)74%(sic)(sic)(sic)(sic)(sic)(sic).(sic)(sic)(sic)(sic)(sic)(sic)SiOx/(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic) , (sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic)(sic).
Conventional powder-based oxygen evolution reaction (OER) catalysts typically require polymer binders, leading to poor mechanical stability, high interfacial resistance, and limited exposure of active sites, which hinder their performance in industrial applications. Herein, we report a flexible freestanding electrode with a novel triple-phase heterostructure composed of a Fe3C twinning core, an interfacial amorphous carbon layer, and an outer amorphous NiP shell, constructed via a facile electrospinning-electrodeposition method strategy. This integrated architecture enables intimate contact between the catalyst, conductive scaffold, and electrolyte, forming a well-defined interface that significantly accelerates electron transfer and gas evolution. Benefiting from the twin-interface-amorphous synergy, the electrode exhibits enthusiastic OER activity in alkaline media, achieving a low overpotential of 225 mV at 10 mA cm-2 and longterm stability under continuous operation at 100 mA cm-2, as well as impressive performance in anion exchange membrane electrolyzers. (c) 2025 Published by Elsevier Ltd on behalf of The editorial office of Journal of Materials Science & Technology.
Photothermal superhydrophobic coatings hold promise in engineering anti/de-icing but often lack sufficient functional robustness and tend to be performance-unstable under harsh environments. Here, a superhydrophobic polyurea coating (SHPC) without micro/nano fillers or complex processes like laser etching was developed via low-polarity polyurea modification and kinetically driven regulation of polyurea molecular chain conformational domains. Notably, SHPC's contact angle (CA) remained >150 degrees after 2000 400-mesh sandpaper abrasion cycles. Furthermore, by synergizing the presumed nanoconfinement enhancement effect, a superhydrophobic photothermal polyurea coating (SHPPC) was designed to overcome SHPC's robustness bottleneck. With the same thickness, SHPPC's surface robustness is significantly enhanced: CA remains >150 degrees after 16,000 cycles of 400-mesh sandpaper abrasion, 3810 cycles of 60-mesh sandpaper abrasion, 60 min of gravel impact, or 30 min of water jet impact, which, to our knowledge, is one of the more durable superhydrophobic coatings reported recently. Moreover, SHPPC shows outstanding photothermal robustness; after 2000 cycles of 60-mesh sandpaper abrasion, its light-irradiated area remains frost-free and it inhibits water droplet freezing for 90 min at -15 degrees C. Possessing exceptional functional robustness, anti/de-icing performance, and efficient natural light utilization, SHPPC holds substantial application potential in engineering anti/de-icing fields like unmanned aerial vehicle (UAV) propellers.
ABSTRACT Nowadays, fast‐charging capability in battery materials is intensively pursued in both academia and industry, yet the crystallographic factors that fundamentally determine rapid Li + transport remain unclear. Here, we identify the theoretical structural capacity for collective Li + transport, defined by the availability of crystallographically accessible Li diffusion sites, as a decisive but previously underappreciated structural origin governing interfacial Li + transport, and introduce Li‐site density (ρ Li‐site ) as a quantitative descriptor to guide surface architecture design for accelerated Li + migration. Guided by this principle, we construct a coherent and fluorinated 1T‐Li 1 + x CoO 2 − y F y surface structure on LiCoO 2 , which simultaneously preserves crystallographic compatibility with the O3 matrix and provides an exceptionally high ρ Li‐site (∼48 sites·nm −3 ), substantially exceeding those of commonly employed frameworks (≤ 31 sites·nm −3 ). The modified cathode delivers unprecedented rate capability, achieving 183 and 175 mAh g −1 at 10C and 20C, respectively. In‐situ synchrotron x‐ray and neutron diffraction results further reveal that the 1T phase effectively suppressed O3 to H1‐3 phase transitions and stabilized oxygen frameworks, enabling outstanding cycling stability with 87% capacity retention after 500 cycles. This work establishes Li site density‐guided surface engineering as a general structural principle for simultaneously improving interfacial reaction kinetics and structural durability in high‐voltage layered oxide cathodes.
Sustainable development for our life is important task, which is driven by key materials and technologies. In this roadmap, we discuss three main aspects in addressing environmental questions, green chemical processes and energy challenges. They are included, such as gas treatment and separation, wastewater treatment, waste gas treatment, solid waste treatment, lithium extraction, hydrogen production, water splitting, CO2 reduction, photocatalytic clean technologies, plastic degradation, fuel cells, lithium batteries, sodium batteries, aqueous batteries, solid state batteries, metal air batteries and supercapacitors. Their status, challenges, progress and future perspectives are also discussed. We hope that this paper can give clear views on sustainable development in materials and technologies.
The widespread industrial application of copper is significantly hindered by its susceptibility to oxidation. Chromate passivation, a conventional protection method, is however notoriously associated with substantial environmental concerns. This study presents an ultrafast chromium-free passivation strategy capable of forming a protective film on copper foil within 2-6 s. The resulting film demonstrates exceptional oxidation resistance, rivaling commercial chromate standards. It exhibits superior high-temperature stability, with a minimal weight gain of only 1.21 wt% up to 400 degrees C, significantly outperforming its chromate counterpart (3.81 wt%). XPS analysis reveals that the performance originates from an organic-inorganic composite structure: a compact copper-organic acid coordination layer ensures robust adhesion, while MoO3 and aluminum hydroxyl oxides/ hydroxides intertwine as reinforcing phases within the network, collectively forming a stable barrier. This work provides an efficient and environmentally benign anti-oxidation strategy for copper foil, highlighting its significant potential for broad industrial adoption.
With the rapid development of large-scale energy storage and electric vehicles, sodium-ion batteries (SIBs) are regarded as a promising alternative to lithium-ion batteries (LIBs) due to higher earth-abundance. Among cathode materials, NASICON-type Na3V2(PO4)3/C (NVP) shows extensive potential which suffers from poor intrinsic electronic conductivity. This work reports an NVP composite (DJH-NVP) synthesized via a direct Joule heating (DJH) method. This method involves the in-situ introduction of conductive carbon during synthesis, constructing a unique integrated conductive network that eliminates the necessity for additional conductive additives. DJH-NVP exhibits anisotropic lattice contraction induced by a "thermal-mechanical" coupled field, resulting in a denser, more integrated composite structure with a thicker carbon coating and higher tap density. Benefiting from these structural merits, DJH-NVP demonstrates superior electrochemical performance in ester-based electrolyte half-cells, including minimal polarization, outstanding rate capability (93.6 mAh/g at 50 C), and excellent long-term cycling stability (93.5 % capacity retention after 1000 cycles at 1 C; 97.1 % after 2000 cycles at 50 C). The enhanced performance benefits from DJH strategy, including improved electronic conductivity, a robust composite architecture, and a stable cathode-electrolyte interphase after cycling. This work provides a novel and efficient strategy for fabricating high performance cathode materials for SIBs.
Liquid metal embrittlement (LME) induced by gallium severely degrades the mechanical properties of aluminum alloys. This study combines experimental characterization (XRD, SEM-EDS, EBSD) with density functional theory (DFT) and ab initio molecular dynamics (AIMD) simulations to elucidate the atomic-scale mechanisms of Ga-induced embrittlement in 7050 Al alloy. Experimental results show that Ga preferentially diffuses along grain boundaries and subsequently penetrates into grain interiors, with cracks initiating and propagating exclusively along grain boundaries. DFT calculations reveal that the Σ5(210) grain boundary exhibits a significantly higher grain-boundary energy and stronger Ga adsorption than the Σ3(111) coherent twin boundary. The Nudged elastic band (NEB) calculations further indicate that migration barriers along the Σ5(210) grain boundary are lower than those along the Σ3(111) grain boundary. AIMD simulations combined with mean squared displacement (MSD) analysis yield temperature-dependent diffusion coefficients that follow Arrhenius behavior, with activation energies of 68.13 kJ/mol for the Σ3(111) grain boundary and 43.09 kJ/mol for the Σ5(210) grain boundary. This work establishes a direct atomic-scale mechanistic link between grain boundary structure, Ga diffusivity, and susceptibility to liquid metal embrittlement.
The safe transportation of hydrogen via natural gas pipelines is threatened by hydrogen embrittlement of high-strength steels, which is further affected by corrosion product films (CPFs) on the pipe inner wall. This work explored the effects of FeCO3, Fe2O3 and FeS films on hydrogen permeation and embrittlement of X80 pipeline steel using experiments and first-principles calculations. All three films were n-type semiconductors and act as hydrogen barriers with different efficiencies. The hydrogen-blocking effect followed the order FeCO3< Fe2O3 < FeS. The hydrogen embrittlement index droped from 45.0% (bare steel) to 12.5% (FeS-covered steel). As the effective hydrogen concentration in the steel decreases, the fracture mode changed from HEDE-dominated brittle fracture to a mixed HEDE/HELP mechanism. First-principles calculations revealed that hydrogen adsorption energies and diffusion barriers increased sequentially in the three films, explaining their enhanced hydrogen resistance. This study clarified the effects of corrosion product films on hydrogen behavior in X80 pipeline steel and provided a basis for the safety evaluation of hydrogen-blended pipelines.
Developing high efficient and stable non-noble metal catalyst for water electrolysis is particularly crucial. Herein, we reported B-doped FeCoNi (Oxy) Hydroxides (FeCoNiB) on the surface of Ni foam substrate (NF) synthesized through a facile and mild two-step strategy of electrodeposition followed by impregnation. This synthesis strategy can efficiently introduce surface defects by B doping to FeCoNi (Oxy) Hydroxides while maintaining its original morphology. The obtained FeCoNiB/NF catalyst displayed an unique three-dimensional (3D) flower-like cluster architecture composed of thin nanosheets. The FeCoNiB/NF exhibited outstanding OER electrocatalytic activity, requiring the low overpotential of only 308 mV to achieve the current density of 100 mA cm-2 with the low Tafel slope of 59.0 mV dec-1. The enhanced catalytic activity of FeCoNiB/NF is mainly attributed to the synergistic enhancement effect of high-valence Fe and Co, surface defect, and amorphous-crystalline interfaces. When FeCoNiB/NF was employed as the anode catalyst for overall water electrolysis, it requires only 1.62V to achieve 20 mA cm-2, and operates stably for over 50 h, verifying its great potential applicability. This work provides an effective strategy for the design of high-performance non-noble metal electrocatalyst for water electrolysis.
The herbicide 2-methyl-4-chlorophenoxyacetic acid (MCPA) poses a significant threat to aquatic organisms and human health due to its resistant biodegradability. It is urgent to develop efficient removal methods for MCPA, especially advanced oxidation technologies based on metal organic frameworks (MOFs) catalysts. This study aims to remove MCPA by catalyzing peroxymonosulfate (PMS) with Co@MOF-808(C) and optimizing the catalytic degradation conditions with the Central Composite Design (CCD) of Response Surface Methodology (RSM). In addition, the reusability of Co@MOF-808(C) and the mineralization effect of MCPA, along with the potential degradation pathway of MCPA and the ecotoxicity of the degradation intermediates, were investigated. Results revealed that temperature, catalyst concentration, and PMS had significant impacts on MCPA degradation, and the optimal conditions were Co@MOF-808(C) 625mg·L⁻¹, PMS 5.85mM, pH 4.0, 45 ℃ and rotate speed 236rpm. The total organic carbon removal efficiency of 85.9% and MCPA degradation rate of 98.1% were oobtained under the optimal conditions, and the degradation rate remained as high as 94.4% when the catalyst was reused five times. The contribution rate of reactive oxygen species (ROS) for MCPA degradation was SO4·− (77.8%) > ·OH (18.5%) > O2·− (3.7%), and the degradation pathways included decarboxylation, hydroxylation and ring opening. Moreover, the ecotoxicity of MCPA was significantly reduced after the degradation by Co@MOF-808(C)/PMS system. In consequence, the Co@MOF-808(C)/PMS process may be an efficient alternative for treating MCPA wastewater.
Cl--induced rebar corrosion is one of the primary factors compromising the durability of reinforced concrete. Corrosion inhibitors are regarded as an effective corrosion preventive technique, and impressed current cathodic protection (ICCP) is extensively applied in concrete durability protection. Integrating these two approaches to promote the enrichment of corrosion inhibitors on the rebar surface is expected to address the reduction in corrosion inhibition performance resulting from the low inhibitor concentration at the rebar surface during longterm immersion. Meanwhile, compared with bidirectional electromigration technology, the low polarization potential of cathodic protection helps to reduce hydrogen evolution reactions (HER). In this study, tris (hydroxymethyl)aminomethane (THAM) was employed as the corrosion inhibitor. The synergistic effect of ICCP and THAM on the corrosion resistance and mechanical performance of HRB400 reinforced concrete was comprehensively evaluated through analyses of surface composition, electrochemical behavior, hydrogen permeation characteristics, and bond strength between rebar and concrete. The results revealed that under ICCP, protonation of the N atom rendered THAM positively charged, facilitating its enrichment on the rebar surface. XPS and DFT results demonstrated that THAM adsorbed on the rebar surface and formed a stable protective layer by forming N-Fe bonds. This adsorption behavior mitigated the Cl--induced degradation of the passivation film. Furthermore, THAM reduced Ca(OH)2 deposition on the rebar surface, inhibiting the conversion of Fe(II) to Fe (III) within the passivation film. Meanwhile, the THAM adsorption layer suppressed the hydrogen permeation rate of the rebar. Under a cathodic potential of -1.15 V, the addition of THAM reduced the steady-state current density from 4 mu A/cm2 to 1.8 mu A/cm2. In addition, the presence of THAM improved the bond strength between rebar and concrete. In the 3.5 wt% NaCl environment, the average and maximum bond strengths remained 4.5 MPa and 12 MPa, respectively.
ZnO/CeO2 and CeO2/ZnO composite films were prepared by combining electrodeposition with hydrothermal methods. The study focused on how the heterojunction interface affects the resistance behavior and corrosion resistance of the films. The surface morphology, composition, structure, semiconductor type, and oxygen vacancy concentration of the films were observed and analyzed. Furthermore, the surface adsorption energy, oxygen vacancy formation energy, heterojunction binding energy, and diffusion barrier energy were calculated using density functional theory (DFT). The corrosion resistance and resistance switching properties of the films were examined through electrochemical methods tests. The results show that the oxygen vacancy concentration in the CeO2/ZnO film is lower than in the single-layer thin film (ZnO, CeO2), and its corrosion resistance is higher than that of the single-layer film. Conversely, ZnO/CeO2 film exhibits the opposite trend. After applying a polarization voltage, the formation energy and diffusion barrier of oxygen vacancies in the CeO2/ZnO system decrease, and the applied voltage promotes the generation and migration of oxygen vacancies. The polarization treatment enables cyclic switching between high and low resistance states, which significantly extends the film's service life and is expected to expand the application of resistance switching technology in the field of corrosion protection.
ABSTRACT Prelithiation is a key strategy for developing high‑performance lithium‑ion batteries (LIBs) with high energy density and long cycle life. It compensates for the lithium loss caused by solid electrolyte interphase (SEI) formation and improves the initial Coulombic efficiency (ICE). Anode prelithiation, which offers high reversible capacity and industrial applicability, is particularly promising compared with cathode or electrolyte prelithiation. However, a systematic comparison and practical guidance for selecting anode prelithiation routes in manufacturing are still lacking. This review focuses on industrially scalable anode prelithiation technologies, systematically categorizing their reaction mechanisms, implementation processes, and technical advantages. Special attention is paid to contact prelithiation routes using stabilized lithium metal powder (SLMP), microporous ultrathin lithium foil, and other routes, with comparisons in terms of precision, uniformity, and mass‑production compatibility. Additionally, this review analyzes the interfacial regulation mechanisms of different prelithiation strategies on graphite and silicon‑based anodes and discusses how prelithiation amount and lithium source structure influence electrode morphology, SEI composition, rate capability, and long‑term cycling stability. Based on these discussions, future directions for industrial‑grade anode prelithiation are proposed to guide the selection of optimal routes. It provides a rational foundation for guiding practical anode prelithiation techniques and accelerating the commercialization of next‑generation high performance LIBs.
Green hydrogen production exacerbates water scarcity and further contributes to climate change when using fossil-based electrical energy. In this work, a device with long-term durability combining solar energy was proposed and designed for the sustainable production of water and green hydrogen over 24 h. The water production device was based on a high-heat-resistant and salt-resistant bio-based moisture sorption gel, whose water sorption capacity is 2.03 times that of pure lithium chloride in a simulated desert environment (18 degrees C, 15% relative humidity [RH]). Notably, the prepared aerogel exhibited cumulative water sorption of 2.045 gwater & sdot;gsample-1 and performance fluctuation < 2% after 2,000 h of cyclic testing. Therefore, we used this material in our device to achieve 24 h of continuous water and electrolytic hydrogen production by atmospheric water harvesting. This study introduces a potential solution aimed at providing a new 24-h continuous production method for both water and green hydrogen in arid regions.
Aqueous rechargeable zinc-nickel battery based on spherical beta-nickel hydroxide has suffered the unsatisfactory cathode stability for a long time though continuous achievements have been made in Zn anode performance. This study introduces the facile and ambient sulfur anion exchange to prepare a conformal surface-sulfured nickel hydroxide (S-SNH), employing commercial low-cobalt spherical nickel hydroxide (C-SNH) as the precursor and the benchmark, aiming to amplify the effect of sulfuration on pouch cell performance and clarify the regulating roles of nickel sulfides on cathode. The discharge capacity of S-SNH exhibits more than 1.3 times of the C-SNH at about 4 C rate (normalized by activated capacity), beyond the traditionally-tested low active mass loading (> 120 mg cm(-2)). Extended cycling tests further reveal the superior CE and energy efficiency of S-SNH, significantly surpassing C-SNH. Characterizations and electrochemical measurements verify an inhibition of the inherent lattice expansion in S-SNH. Partial replacement of high-cobalt SNH (Co-SNH) with S-SNH enhances cycling stability while lowering costs. This work demonstrates a cost-effective strategy to improve the performance of pouch Zn-Ni battery via sulfur-modified cathodes, offering insights into sustainable energy storage solutions.
Highly efficient catalysts require precisely engineered intricate structures, yet conventional thermodynamically controlled syntheses often involve cumbersome procedures and limited structural precision. We report a nonequilibrium transient assembly strategy for the ultrafast synthesis of intricately structured nanocatalysts, including core-shell platinum (Pt)-skinned intermetallic nanocrystals exemplified by Pt@PtFe-i. By using a periodic thermal-pulse protocol to drive the continuous evolution of high-energy transient PtFe configurations, we achieved the synchronous assembly of a high-order PtFe intermetallic core and an atomic-layer-precise Pt skin. The Pt@PtFe-i catalyst exhibits coordination-dependent compressive strain within the Pt skin, creating a high density of highly active sites for the oxygen reduction reaction. The H2-air fuel cell with Pt@PtFe-i delivers a peak power of 1.25 watts per square centimeter at a cathode Pt loading of 0.1 milligrams per square centimeter, with a small peak power loss of 3.2% after 30,000 accelerated durability testing cycles.
Electrochemical reconstruction of electrocatalysts is critical to their practical performances. However, the relevant influencing factors for the evolution process are still rare, restricting the design of high-performance electrocatalysts. Herein, using acidic CO2 electroreduction reaction (CRR) over Cu2O as a model system, we systemically studied how organic additives regulate the reconstruction of high-valent Cu species and the CRR mechanism. Theoretical calculations reveal the relationship between additive physicochemical properties and Cu2O. Notably, in situ characterization reveals that DMSO strongly interacts with the catalyst, partially reducing Cu2O to form a Co-lattice OD-Cu/Cu2O heterostructure with interfacial Cu atoms belong to both Cu2O and Cu lattices and exhibits an intermediate valence state. Based on the Co-lattice OD-Cu/Cu2O, the Faradaic efficiency (FE) of C2H4 was up to 67.5% at -1.5 V vs. RHE in H2SO4 & Li2SO4 electrolyte with a low FEH2 of 16.8%. Moreover, the combination achieves a stability of over 100 h in membrane electrode assembly (MEA) electrolyzes. Simulations uncover that the DMSO-modified Co-lattice OD-Cu/Cu2O optimizes *CO adsorption, lowers C-C coupling barriers and promote the generation of C2H4. Meanwhile, DMSO spontaneously adsorbs on the catalyst surface and effectively inhibits HER. This work deepens the understanding of electrocatalyst reconstruction behavior and contributes to the development of efficient electrocatalytic systems.
High-spin cobalt-based catalysts represent promising candidates for the oxygen evolution reaction (OER) under alkaline conditions. However, during the OER process, the irreversible transformation of the high-spin Co3+(HS-Co3+) species to a low-spin state due to insufficient sustainable electron compensation is a key factor leading to catalyst deactivation. We report a Co2VO4/VN heterojunction exhibiting a three-dimensional layered porous micronanostructure resembling puffed-rice-sphere. The interfacial structure anchored by strong V-N covalent bonds reduce crystal field splitting energy, promotes eg orbitals occupation, and stabilizes HS-Co3+. Concurrently, dynamic charge compensation from the V4+/V5+ redox pair serves as an electron reservoir for Co sites, thereby suppressing the transition to low-spin states. Results demonstrate that the Co2VO4/VN catalyst achieves an ultralow OER overpotential of 253.2 mV at 10 mA·cm-2 in alkaline media, maintaining a stable current density of 1 A cm-2 at 1.866 V for 500 h in 1.0 M KOH. Through a life cycle assessment (LCA) of its preparation and application, the carbon footprint of the catalyst synthesis process is only 48.47 kg CO2-eq This work demonstrates that heterostructure engineering can overcome spin relaxation induced deactivation in high-spin cobalt catalysts, offering a general strategy for designing spin state-tuned electrocatalysts that combine high activity with extended lifetime.
Purpose The purpose of this paper is to develop high-performance anticorrosive epoxy coatings by regulating the orientation of two-dimensional (2D) nanosheets. This is achieved by synthesizing superparamagnetic boron nitride nanosheets (m-BNNSs) and applying a parallel external magnetic field to induce highly ordered in-plane alignment. Design/methodology/approach Few-layer BNNSs prepared via liquid-phase exfoliation were functionalized with Fe3O4 nanoparticles through in situ co-precipitation to obtain Fe3O4/BNNSs (denoted as m-BNNSs). These fillers were incorporated into an epoxy matrix with a parallel magnetic field applied during curing. Composite structures and magnetic behavior were verified by scanning electron microscopy, transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and vibrating sample magnetometer. Electrochemical measurements and pull-off adhesion tests were conducted to evaluate the anticorrosion performance and coating-substrate bonding strength, respectively. Findings Application of a 200 mT magnetic field successfully reduced the average tilt angle of m-BNNSs from 46.1° ± 27.0° to 12.5° ± 12.0°, achieving highly ordered parallel orientation. The coating with 1.0 wt % m-BNNSs under a 200 mT field exhibited the best performance, maintaining a low-frequency impedance modulus of 1.52 × 109 Ω·cm2 after 30 days of immersion. Pull-off tests confirmed that the filler incorporation and magnetic alignment did not significantly alter the coating adhesion. However, excessive filler loading or higher field strengths (300 mT) caused possible local re-stacking and structural defects, leading to the deterioration of protective performance. Originality/value This work provides an effective strategy for regulating the orientation of inert 2D nanosheets in polymer coatings. The enhanced long-term protection is attributed to the synergistic effects of Fe3O4 spacers in suppressing restacking and the field-induced alignment in maximizing the tortuous diffusion path for corrosive species.