Energy & Environmental Materials最新文献

The photovoltaic performance of metal halide perovskite solar cells often respond divergently to environmental conditions during storage. In particular, light exposure can either enhance or degrade device efficiency, yet the mechanisms underlying these antithetical behaviors are still under investigation. In this study, we explore the modulation of the open-circuit voltage (Voc) in triple-cation mixed-halide perovskite solar cells by systematically controlling storage environments. While light intensity exhibits minimal impact during storage, the spectral composition of illumination selectively enhances Voc comprising reversible and irreversible contributions. Structural characterization reveals that prolonged storage degrades the quality of perovskite crystals in the upper region of the perovskite layer, whereas light storage promotes the relaxation of microstrain at the buried interface with a p-type organic layer. This structural reorganization at the interface, accompanied by lattice expansion, accounts for suppressed nonradiative recombination and a corresponding increase in quasi-Fermi level splitting. Consequently, devices fabricated without chemical defect passivation achieve a power conversion efficiency of higher than 40% under indoor lighting conditions after preconditioned by continuous exposure to ambient light during storage. These findings highlight the critical role of controlled light exposure during storage not only in enhancing efficiency, but also in ensuring reproducibility of perovskite solar cell characterization.

Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance. However, the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals (HO˙), leading to excessive consumption of H₂O₂. Through interfacial engineering of Fe–Zr bimetallic catalysts (FeZrO_x), this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80% reduction in H₂O₂ dosage compared to traditional Fe₂O₃ systems. The chemical states of Fe and Zr at the (104)/(111) heterojunction interface in FeZrO_x exhibit marked modifications relative to their monometallic Fe₂O₃ and ZrO₂ counterparts. The elevated charge density at interfacial Fe sites in FeZrO_x promotes HO˙ generation, while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization. This Fe–Zr synergy at the (104)/(111) heterojunction concurrently suppresses HO˙ diffusion losses and directs phenolic pollutant (e.g., phenol and bisphenol A) polymerization within the reactive interface, thereby reducing H₂O₂ consumption compared to monometallic systems.

Hydrolysis of ammonia borane is deemed as a promising technique for robust hydrogen production, yet its deployment is still restricted due to the sluggish kinetics of the water dissociation step. An appropriate catalyst that can effectively reduce the H₂O dissociation barrier is quite desirable for sustainable ammonia borane-to-hydrogen conversion. Herein, an amino pre-coordination confinement strategy is profiled to achieve sub-2 nm ordered PtCo intermetallics uniformly on N-doped hollow mesoporous carbon spheres (O-PtCo/NHMS) for ammonia borane catalytic hydrolysis. Such a confined approach showcases the capacity of preventing nanoparticles from agglomeration and growth for accurate size control and can be extended to other ordered intermetallic systems (e.g. PtFe and PtCu). As for the ammonia borane hydrolysis, the ordered PtCo intermetallics have delivered a five times higher turnover frequency activity of 1264.1 min⁻¹ than that of the disordered PtCo catalyst, together with excellent catalytic durability. Mechanism studies indicate that the ordered PtCo structure promotes the balanced adsorption of H₂O and ammonia borane molecules at Co and Pt sites and reduces the energy barrier for the rate-determining H₂O dissociation step to boost the ammonia borane hydrolysis. This work provides valuable insights into the rational design of efficient ordered PtM intermetallic catalysts and expands their application in hydrogen production via ammonia borane hydrolysis.

As a core technology in flexible electronics systems, piezoresistive sensors exhibit significant application value in frontier fields such as medical health monitoring, intelligent human–machine collaboration, and bionic robot perception. A novel flexible piezoresistive sensing material was developed by combining biomass-derived carbon aerogel (CC) with polydimethylsiloxane (PDMS). The composites had excellent fatigue resistance, maintaining more than 90% shape recovery and less than 3.8% residual deformation after 100 000 cycles at 30% strain. Furthermore, combining biomass-derived carbon aerogel with polydimethylsiloxane composites exhibited excellent piezoresistive response characteristics at different temperatures. In the temperature range from −30 °C to 100 °C, its resistance decreased with increasing temperature, while showing a shortened response time. The composite achieved a stable resistance response through the reversible contact of the conductive network under the action of external forces and had a wide linear detection range, high sensitivity, and effective differentiation between static pressure and dynamic deformation signals. This work established the correlation between the microscopic deformation of the carbon skeleton and the macroscopic electrical behavior, and verified the stability and durability of combining biomass-derived carbon aerogel with polydimethylsiloxane composites under complex stress conditions. The collaborative design strategy provides an innovative platform for the development of sustainable, high-performance flexible sensors with important potential applications in health monitoring and intelligent human–machine interfaces.

This study investigates phase change materials (PCMs) for lithium battery thermal management. A PCM cooling model was developed and experimentally validated, showing ≤1.5 K temperature error and ≤5% PCM melting simulation deviation. A non-uniform battery arrangement was proposed to optimize temperature distribution. Key PCM parameters (melting point, conductivity, latent heat) were analyzed for thermal performance. A hybrid liquid-PCM cooling system was designed and optimized via an entropy-weighted TOPSIS-NSWOA strategy. At 4 C discharge, the optimized system achieved 311.41 K maximum temperature (5.89 K reduction) and 4.71 K temperature difference, meeting 18 650 battery safety standards. The findings guide PCM selection and integrated thermal management design, balancing heat dissipation and temperature uniformity

This study investigated the efficient conversion of greenhouse gases (GHGs), CO₂ and CH₄ mixtures, into few-walled carbon nanotubes (FWCNTs) through an optimized single-step and dual-step chemical vapor deposition (CVD) process. In the single-step process for directly synthesizing FWCNTs from greenhouse gases, CO₂ concentration, gas flowrates, and H₂ addition were identified as factors influencing the growth of FWCNTs. It was demonstrated that minimizing the amounts of CO₂ and H₂ was essential for achieving complete CO₂ conversion because CO₂ acts as an oxidizing agent that hinders CNT growth, while an excess of H₂ disrupts the chemical equilibrium of the CO₂ conversion reaction, leading to side reactions that suppress FWCNTs formation. To overcome these limitations, a dual-step approach incorporating sequential catalytic reactions was developed. In the first step, the Ni/SiO₂ catalyst was utilized to facilitate CO₂ methanation, reducing CO₂ amounts while generating CH₄-rich gas. In the second step, CH₄ pyrolysis was performed over the FeMo/MgO catalyst, enabling the growth of high-quality FWCNTs. This sequential configuration successfully synthesized FWCNTs under conditions previously unattainable in the single-step process, validating the effectiveness of the dual-step design. The strategic optimization of process parameters and sequential catalytic reactions established a viable route for converting GHGs into valuable FWCNTs.

Redox mediators (RMs) represent the most promising strategy to address the sluggish kinetics of lithium–oxygen (Li–O₂) batteries. To achieve high-energy and cost-effective Li–O₂ batteries, carbon materials are typically regarded as ideal cathodes in these systems. However, the impact of their surface properties—which often regulate specific discharge pathways—on the RM-mediated oxygen reduction reaction (ORR) remains unclear. In this study, CNTs electrodes with different surface properties are fabricated. Results suggest that CNTs with more surface defects not only promote the unmediated discharge pathway even in RMs-involved battery systems but also exacerbate the corrosion of carbon cathodes. This, in turn, leads to the undesired accumulation of Li₂O₂ and Li₂CO₃ on the cathode surface, which hinders effective and continuous electron transfer between the cathode and RMs, ultimately decreasing the catalytic activity of RMs. As a result, the discharge capacity of the battery is seriously diminished, especially at large current densities. These findings underscore the significance of surface engineering in advancing the performance of RMs-assisted Li–O₂ batteries.

Amorphous metal-based catalysts are highly promising for water splitting due to their abundance of unsaturated active sites. Herein, we report a one-step, surfactant-free synthesis of amorphous nickel nanoparticles (NPs) encapsulated in nitrogen-doped carbon shells (A-Ni@NC) via pulsed laser ablation in liquid (PLAL). The synergistic integration of the amorphous Ni core and a defect-rich N-doped carbon shell markedly enhanced the catalytic activities for both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), with low overpotentials of 182 mV for HER and 288 mV for OER at 10 mA cm⁻² in 1.0 m KOH. Furthermore, the bifunctional catalyst achieved a current density of 10 mA cm⁻² at 1.63 V and retained 98.9% of its initial performance after 100 h of operation. The nitrogen-rich carbon shell not only offered abundant active sites and structural protection but also promoted charge transport. Density functional theory (DFT) calculations revealed that N-doping optimized intermediate adsorption energies, while the amorphous Ni core facilitated efficient electron transfer. This green and scalable synthesis strategy provides a promising platform for developing a wide range of transition metal@N-doped carbon hybrid catalysts for sustainable energy conversion applications.

Efficient photocatalytic reduction of CO₂ is crucial to decrease the atmospheric concentration of CO₂. Pairing this process with H₂O₂ production is of considerable importance for simultaneously producing value-added chemicals. However, the photocatalysts reported for such a process suffer from a high recombination rate of the surface/bulk charges, as well as inefficient enrichment and activation toward CO₂ and O₂, resulting in low conversion efficiency even in the presence of organic sacrificial agents and expensive metal co-catalysts. Herein, two 1,3,5-triphenylbenzene-based organic polymers with high ionic density and porosity are prepared through a facile Sonogashira polymerization. The ionic imidazolium sites embedded in the polymeric skeleton provide the two polymers (iCMP-1 and iCMP-2) with adsorptive selectivity for CO₂/N₂ up to 98–102 at 273 K, facilitating the enrichment of CO₂ and O₂ molecules around the catalytic centers, thus boosting their catalytic conversion directly from air under solar light (100 mW cm⁻²). Benefiting from the improved charge separation and broad light absorption, along with high CO₂ and O₂ uptake, iCMP-2 can deliver excellent CO and H₂O₂ yields (611.8 and 810.6 μmol h⁻¹ g⁻¹, respectively) under an atmosphere composed of water vapor and air without any co-catalysts.

Global water scarcity and pollution present critical challenges for human society. Solar-driven wastewater treatments, such as photocatalytic degradation of organic pollutants and photothermal conversion water evaporation, offer promising solutions. TiO₂ has garnered extensive attention in these fields, but its large bandgap limits light absorption, affecting its performance and broader applications in energy and environmental fields. Consequently, modifying TiO₂ to improve its photocatalytic and photothermal conversion performance has become a research hotspot. Among various modification strategies, self-doping with Ti³⁺ and oxygen vacancies can reduce the bandgap of TiO₂, improve sunlight utilization, and increase the separation efficiency of photogenerated electron–hole pairs, thereby significantly enhancing the photocatalytic and photothermal conversion performance. This review focuses on the inorganic chemical reduction methods for preparing Ti³⁺/oxygen vacancies self-doped TiO₂ and their current applications in solar-driven photothermal conversion water evaporation. It highlights the challenges faced during synthesis and application while offering insights into future development prospects. This review is expected to provide a valuable reference for further research on the preparation and application of Ti³⁺/oxygen vacancies self-doped TiO₂.