Carbon Neutralization最新文献

The practical application of solid polymer electrolytes (SPE) is limited due to notorious high crystallinity and low ionic conductivity. Existing research concentrated on reducing crystallinity and increasing Li salt concentration have made certain process. However, the segmentation and isolation effects of large and numerous grains on amorphous region have always been overlooked and the effect of grain size remains largely unexplored. Herein, take polyethylene oxide (PEO) as an example, “grain size refinement” strategy is adopted to improve the related room-temperature ionic conductivity by simply placing PEO based SPE on Li sheets coated with ester monomers and conducting in-situ polymerization. During these processes, in addition to reducing the interaction force between polymer chains and decreasing the driving force for crystallization, ester monomers are conducive to form interface with polymer clusters, which serves as additional nucleation sites and promotes the formation of refined grains. Then instantaneous high-temperature provided by muffle furnace triggers rapid solidification of monomers, leading to the locking of refined grain structure and the formation of more interconnected amorphous regions. Time-of-flight secondary ion mass spectrometry and polarization microscope confirm these processes, while small-angle X-ray scattering results indicate that the grain size reduces to one-third of its original size. Then the room-temperature conductivity increased by at least two orders of magnitude for PEO-based SPE.

Wearable heaters with multifunctional capabilities and high performance are in high demand for future personal thermal management. However, the development of such devices remains challenging due to limitations in flexibility, complex fabrication, inadequate Joule heating efficiency, insufficient electromagnetic interference (EMI) shielding, and poor antibacterial performance. Here, Ag@PEDOT heterostructures were decorated on laser-induced graphene (LIG) through a simple spray-coating process followed by a facile chemical synthetic method to deposit silver nanoparticles (AgNPs) onto the PEDOT layers. The resulting composite retains the intrinsic flexibility and comfort of the original graphene matrices, while demonstrating exceptional Joule heating characteristics—achieving a broad temperature range (30°C–100°C) at low operating voltages (0.8–2.6 V) and a rapid photothermal response (reaching 89.6°C within 180 s at 1.5 sun irradiation). Moreover, the material exhibits superior electromagnetic shielding effectiveness (33 dB in the X-band) and outstanding antibacterial activity, with an inhibition rate exceeding 95% against Escherichia coli and Staphylococcus aureus. This study offers a promising strategy for designing multifunctional wearable heaters suited for personal healthcare and thermal management applications.

Iron-based Prussian blue analogs (PBAs) represent promising, facile-to-prepare, and low-cost positive electrode materials for sodium-ion batteries. However, their practical application is hindered by the markedly irreversible three-phase transitions and severe lattice distortion that occur during sodium ion storage, leading to capacity limitations and diminished cycling stability. Herein, a simple pyrrole-induced phase transition engineering strategy is proposed to successfully transform monoclinic PBAs into cubic polypyrrole-PBAs (PPy-PBAs). In situ X-ray diffraction (XRD) testing and density functional theory (DFT) calculations reveal that the phase transition mechanism transforms from an unfavorable three-phase process to a highly reversible two-phase transition. Compared to complex three-phase transition (PBAs), the efficient two-phase transition (PPy-PBAs) exhibits smaller lattice volume contraction/expansion and less Fe-C/Fe-N bond length stretching/shrinking, demonstrating remarkable structural stability. Moreover, this strategy effectively reduced the energy barrier for sodium-ion (Na⁺) migration, with the density of states crossing the Fermi level, significantly enhancing electronic conductivity, and thereby facilitating redox reactions and Na⁺ transport kinetics within the material. The reversible two-phase transition enables sustainable sodium-ion storage through phase-transition engineering. Compared with PBAs that undergo structural distortion and significant lattice strain, the optimized positive electrode material demonstrates a discharge capacity of 136 mAh/g and an ultralong stable cycling lifespan of 1700 cycles, establishing new possibilities for advanced sodium-ion batteries.

Electrochemical CO₂ reduction (CO₂RR) holds promise for sustainable fuel and chemical production but faces fundamental challenges rooted in limited CO₂ availability and high activation reaction barriers. These issues manifest as slow kinetics, low selectivity, and poor stability under industrial operational conditions. While the catalyst/electrolyte interface engineering plays a decisive role in modulating the local microenvironment, which directly influences the kinetics and thermodynamics of CO₂RR, current understanding remains fragmented due to the complex interplay of interfacial factors. Herein, in this review, we address this gap by moving beyond conventional categorization by materials or products. We present a unified mechanism-oriented framework that directly links interfacial design strategies for tackling the core challenges of CO₂ availability, site accessibility, and reaction affordability. We systematically decouple the interface interactions and survey interfacial engineering strategies for CO₂ reduction, including mass-transport control, electrostatic microenvironment tuning, molecular functionalization, and device–interface engineering. By elucidating the mechanistic principles behind these strategies and their interconnections, this review provides actionable guidelines for engineering robust interfaces that break inherent trade-offs among activity, selectivity, and stability. We aim for this perspective to not only advance understanding of microenvironment modulation but also accelerate the development of scalable, carbon-neutral energy conversion technologies.

This study explored thermal and electrodeposition impacts of distinct chaotic current waveforms to enhance current efficiency and reduce heat loss through the regulation of electrode interfacial reaction dynamics, advancing current efficiency, energy conservation, and carbon neutrality. Two universal control methodology was developed to achieve independent amplitude and offset boosting of arbitrary chaotic signals, implemented through a specially designed chaotic circuit. Three distinct waveforms (w-, F-, and G-signals) were systematically investigated for their thermal and electrochemical effects. Experimental and COMSOL simulation results demonstrated that Joule heating was governed by both fluctuation amplitude and frequency characteristics, following the sequence w < F < G. When the current density was about 1500 A/m², the corresponding optimal voltage fluctuations were identified as 2.8 V (w), 0.51 V (F), and 0.23 V (G), yielding current efficiency improvements of 2.2%, 0.7%, and 5.1%, respectively, based on the electrodeposition experiments. Combining experiments on electrolytes at different temperatures with corresponding SEM characterization revealed that chaotic current suppresses manganese nodules not only through Joule heating-induced temperature rise, but also via effective regulation of the interfacial electrochemical environment, thus allowing effective inhibition even at lower temperatures. These findings provide both theoretical insights and practical methodologies for implementing chaotic currents in industrial electrodeposition processes.

V-based materials, with the high specific capacity and multi-electron redox reactions, are considered as preferred cathodes for low-cost and high-safety aqueous zinc-ion batteries. Nevertheless, poor electronic conductivity, sluggish kinetics, vanadium dissolution, and unstable structure pose severe challenges for the further practical applications. To address these issues, in this study, transition metal ions Mo⁶⁺ and polyaniline were incorporated into V₂O₅ derived from vanadium acetylacetonate via a one-step hydrothermal method (MPVO). The results reveal that MPVO exhibits a unique three-dimensional (3D) sea urchin-like morphology with a satisfactory specific surface area and high concentration of oxygen vacancies. These characteristics offer more reaction sites for Zn²⁺ and adjust the electronic conductivity. Moreover, kinetic analysis and density-functional-theory calculations indicate that MPVO performs metallic behavior, with the lowest Zn²⁺ diffusion barrier and outstanding pseudocapacitive storage capacity. Hence, the MPVO cathode delivers a reversible capacity of approximately 457.5 mAh g⁻¹ at 0.1 A g⁻¹. Moreover, it demonstrates remarkable high-rate capacity and robust long-cycle performance. This study realizes a triple-strategy approach of enlarging the interlayer spacing, evolving from a zero-dimensional (0D) to 3D sea urchin-like morphology, and introducing abundant defects. These synergistic strategies significantly enhance the rapid kinetics and high stability of the MPVO cathode and provide new insights for designing V-based cathodes.

Wide-bandgap (WBG) perovskite solar cells (PSCs) are critical for tandem architectures but suffer from light-induced halide segregation and non-radiative recombination. Although conventional rare-earth doping passivates defects, it concurrently introduces vacancies and lattice strain that exacerbate halogen migration. Herein, we report a thermally induced doping strategy where Pr³⁺/Sm³⁺ ions pre-embedded in MeO-4PACz diffuse into the perovskite during annealing. Through combined tolerance factor analysis, structural characterization, and DFT calculations, we identify a dual doping mechanism: predominant interstitial incorporation with minor B-site substitution. This approach reduces defect density, increases iodine migration energy barriers (from 0.85 to 0.94 and 1.12 eV), and minimizes lattice distortion. Consequently, the experimental results show that the open-circuit voltage increases from 1.198 V to 1.230 V (Pr³⁺) and 1.233 V (Sm³⁺), and the fill factor increases from 83% to 86%. Finally, the PCE reached 23.04% (Pr³⁺) and 23.39% (Sm³⁺) (20.12% for control) with > 90% stability retention after 1500 h. In addition, the optimized semitransparent WBG device PCE was 19.48% (Pr³⁺) and 19.85% (Sm³⁺), and the PCE of 4-T perovskite was 27.05% (Pr³⁺) and 27.56% (Sm³⁺). This method will be beneficial for the development and application of WBG PSCs and TSCs.

SnSe₂ is a promising thermoelectric (TE) material with intrinsic n-type characteristics and a high theoretical ZT value of 2.95 along the a-axis. However, its densely packed crystal lattice in the plane perpendicular to the c-axis leads to weak phonon scattering, limiting improvements through conventional defect or nanostructure-based strategies. In this study, the rare-earth element Yb is introduced into tin-rich SnSe₂, predominantly segregating at grain boundaries and enhancing phonon scattering, while a small fraction incorporates into the lattice and modifies the electronic structure, simultaneously tuning both electrical and thermal transport behaviors. Yb incorporation enhances multiple phonon scattering mechanisms, significantly reducing lattice thermal conductivity, reaching a minimum of ~0.48 W·m⁻¹·K⁻¹. Meanwhile, it modulates the electronic structure by introducing impurity states, altering band alignment, and enhancing band degeneracy, collectively increasing the density-of-states (DOS) effective mass and Seebeck coefficient, contributing to a maximum power factor of 436.47 μW·m⁻¹·K⁻² at 773 K. As a result, the Yb-doped SnSe₂ sample with 1.0 wt% achieves a peak ZT_max of ~0.53 at 773 K along the direction parallel to the pressing direction, representing an ~95.3% enhancement over the undoped sample. This study presents a synergistic and effective strategy for optimizing SnSe₂-based TE materials via rare-earth doping, paving the way for next-generation high-performance TE devices.

For decades, the industry has believed that spherical graphite (SG) yield correlates strongly with graphite flake size. To clarify natural graphite (NG) spheroidization mechanisms, a comprehensive evaluation was conducted by extracting intermediate products from an industrial production line and utilizing separated jet mills to simulate continuous processing in the study. Focused ion beam-scanning electron microscope (FIB-SEM) cross-sectional analysis and nanocomputed tomography (Nano-CT) imaging revealed that flakes of different thicknesses underwent distinct morphological changes (folding, bending, or fragmentation) under mechanical force, with only flakes above a critical thickness (∼2 μm) forming SG cores. Statistical correlation between thickness (measured via statistical method under SEM) and yield demonstrated that thickness—not only size—is the dominant factor, redefining “effective SG flakes” to include small but thick flakes. Therefore, prioritizing thickness protection over size preservation in grinding-flotation and spheroidization processes increased SG yield by 7% in industrial validation. The work provides new insights for high-efficiency SG production.

Aqueous zinc-ion batteries (AZIBs) have gained great attention due to their nontoxicity, low-cost, and high theoretical capacity. However, the scarcity of suitable cathode materials with excellent performance limits the practical application of AZIBs. Herein, we develop a conducting polymer (polyaniline) and divalent ions (Ca²⁺) co-intercalated method to synergistically regulate the property of V₂O₅ to enhance Zn²⁺ storage performance. The synergistic effect of co-insertion Ca²⁺ and polyaniline (PANI) not only enlarges the interlayer spacing but also regulates multiple oxidation states of vanadium, which dramatically improves the conductivity, diffusion kinetics, and structural stability of host V₂O₅. Consequently, the resultant Ca/PANI/V₂O₅•nH₂O (CPVO) as AZIBs cathodes exhibits extraordinary specific capacity of 512 mAh g^–1 (0.5 A g^–1) and cycling stability with an outstanding coulombic efficiency of around 100% after 2000 cycles (25 A g^–1). Moreover, the Zn²⁺ storage mechanism is elaborated by combining comprehensive characterizations and DFT calculations.