Advanced Energy and Sustainability Research最新文献

Environmental and energy concerns surrounding the use of fossil fuels are driving an increasingly rapid transition to sustainable and eco-responsible processes. Electrochemical processes can provide the necessary sustainability and economic roadmap for storing intermittent and renewable electricity by synthesizing, in cogeneration electrolyzers, energy carriers and/or synthetic chemicals (hydrogen, ammonia, etc.) via flagship reduction reactions (hydrogen evolution reaction (HER), nitrogen reduction reaction (NRR), etc.). To balance the electrochemical process, these cathodic processes have long been coupled to the oxygen evolution reaction (OER), which ultimately consumes almost 90% of the energy input. Recent years have witnessed an overwhelming development of anode scenarios based on biomass substrates, because OER cannot be driven below a certain potential threshold, while organics are thermodynamically more favorable. Therefore, paired electrolysis, which refers to cases where electrochemical oxidation and reduction are desired, embraces the electrocatalysis community for the electrolytic production of hydrogen, ammonia, etc. (cathode side), in parallel with value-added chemicals (anode side), all with a modest electricity input. The trade-off is selectivity at relevant current densities. This review discusses, the progress, challenges, and potential of biomass-fueled paired electrosynthesis of valuable chemicals and fuels. Fundamental principles, main biomass solubilization methods, and different scenarios for paired electrosynthesis are presented.

High-entropy materials (HEMs) represent a revolutionary class of materials that have garnered significant attention in the field of materials science due to their extraordinary properties in diverse fields of applications such as catalysis and electrochemistry. The past decade has witnessed a substantial increase in the study of these materials, exploring new synthesis routes and compositions. What began as the synthesis of high-entropy alloys has expanded to encompass several classes of HEMs such as oxides, hydroxides, sulfides, nitrides, and carbides, among others. Several synthesis methods have been developed to produce these materials. This review therefore highlights the fundamental concepts of HEMs, including their core effects, with a major emphasis on their scalable synthesis routes. The advantages and drawbacks of these methods are also discussed. As HEMs transition from the lab to large-scale production, there is a growing need for cost-effective and scalable synthesis methods with high material yield suitable for a variety of applications like hydrogen storage, catalysis, batteries, supercapacitors, and fuel cells. Hence, this review serves as an introduction to scalable synthesis routes based on crystal structure, desired elements, synthesis times, and equipment costs.

Perovskite solar cells (PSCs) have gained tremendous research interest recently owing to several advantages, including low material cost, facile solution processability, bandgap tunability, and alluring device efficiency. The organic formamidinium (FA) cation-based perovskites are mainly considered as one of the potential candidates for charge carrier generation due to their excellent properties, such as bandgap and thermal stability than traditional perovskites. However, the inevitable unfavorable polymorphism (i.e., α to δ) at room temperature still forms the basis for numerous research works to allow the fabrication of a high-quality absorber and enhances the PSCs performance. The studies to resolve the polymorphism and several contemporary techniques (e.g., passivation strategy) with several recent novel fabrication methods presented in this review form the essence of the improvements in PSCs. The absorber morphology also influences the charge-transfer behavior and the device's lifetime. Therefore, understanding these properties is essential to improve the absorber quality and avoid many defects. This review focuses on the structure and properties of pure and mixed FA perovskites with various halides, mainly the FA cation's role in the absorber composition. And a comprehensive overview of recent FA cation-based double, triple, and quadrupole PSCs results with proper scientific explanations to understand the device physics.

The world is facing grand challenges in energy security, environmental pollution, and sustainable use (and re-use) of resources. Electrochemical processes, incorporating electrosynthesis, electrochemical catalysis, and electrochemical energy storage devices, provide pathways to address these challenges via green chemistry. However, the applicability of electrochemical processes for these systems is limited by the required energy input, the “electrons” in electrochemistry. Electrocatalysis as a subset of electrochemistry is set to underpin many of the United Nations Sustainable Development Goals, including “Affordable and Clean Energy” through the production of future fuels and abatement of carbon emissions; “Responsible Consumption and Production” through recycling and degradation of waste; and “Climate Action” through CO₂ (and other greenhouse gas) remediation. The rise of green photovoltaic power has lowered the carbon cost of these electrons, making electrocatalysis an even more viable, green(er), chemical conversion pathway. This perspective highlights the need for comprehensive understanding of catalyst structure via in situ and operando analysis to complement device design considerations. The challenges faced by the field of electrocatalysis in data reporting, elimination of electrochemical artifacts, catalyst stability, and scaling to industrial relevance, along with opportunities, emerging tools, are discussed with a view to achieve the maximum ‘potential’ of electrocatalysis.

Solar-driven evaporation using hydrogels and photothermal materials is a promising freshwater harvesting technology. However, due to the difficulty of removing volatile pollutants through evaporation and the fact that the evaporation efficiency has reached its limit, further improving efficiency becomes challenging. Therefore, a material simultaneously possessing low water evaporation enthalpy as well as the ability to inhibit volatile pollutants is desired. In this work, a dense inhibitory layer on the hydrogel framework of polyacrylamide introduced into polyvinyl alcohol is designed to enhance its suppression of volatile pollutants and regulate the water state. This not only reduces the energy demand for evaporation but also makes it more effective in treating wastewater containing volatile pollutant ammonia nitrogen. Finally, a high evaporation rate of 3.0 kg m⁻² h⁻¹ and an excellent ammonium rejection rate of 90% for high concentration ammonia wastewater are obtained under 1 kW m⁻² illumination. This work opens up new avenues of application for the use of photothermal materials in the use of clean solar energy for the separation of freshwater and volatile small molecules.

Self-powered photodetectors (PDs) are particularly attractive in the construction of environmentally friendly and sustainable Internet of Things. Utilizing dual functions of PTFE of electrostatic field enhancement and dark current suppression, a high-performance self-powered ITO/PTFE/TiO₂/GaN UV PD is developed herein. The introduction of PTFE not only significantly reduces the dark current, but also facilitates the separation of photogenerated carriers by coupling the internal electrostatic field at the PTFE/TiO₂ interface with the built-in electric field of the TiO₂/GaN heterojunction. With 0 V bias, the light-to-dark current (I_light/I_dark) ratio of the PD with PTFE is improved by 2297 times and the response time is faster by 1.69/2.96 times compared to the ITO/TiO₂/GaN PD. In addition, a microstructured M-ITO/PTFE/TiO₂/GaN PD with micrometer-sized cylindrical TiO₂ arrays exhibits a high I_light/I_dark ratio of 3.65 × 10⁵, a responsivity of 280.1 mA W⁻¹, a high detectivity of 1.97 × 10¹³ Jones, and a response time of 4.3/3.0 ms under 360 nm illumination. Our strategy provides a promising way to develop high-performance self-powered PD.

Sodium-ion batteries (NIBs) as one of the next-generation energy storage devices are gradually used in energy field and entering lithium-ion batteries (LIBs) market. Graphite with low price exhibits excellent Li⁺ reversible intercalation properties, which has been widely applied in anodes of LIBs. But it has low capacity for sodium because of its weak chemical bonding with sodium. Here, a defect engineered graphite with low graphitization structure is reported. This graphite demonstrates a defect adsorption and solvated ion intercalation of sodium ions by introducing more active sites and ether electrolytes, effectively improving the storage capacity of sodium. Further experiments and characterization show defects increased after ball milling with surface area increased, and the favorable defects on the interface of graphite are significantly increased. The defect engineered graphite absorbs more sodium-ions and exhibits capacitive characteristics with fast sodiation/desodiation process, leading to an improved capacity storage than the defect-free graphite. Meanwhile, the defect engineered graphite can deliver a capacity of 175 mAh g⁻¹, and maintain a good capacity retention of 84% at 5 A g⁻¹ after 6000 cycles. This work discovers a general methodology to obtain defect engineered graphite, which will provide an experimental strategy to achieve large-scale industrialization for low-cost NIBs.

MnO₂@PCs (porous carbons) exhibiting high energy and power density are utilized as supercapacitor electrodes and prepared by impregnating porous carbons (PCs) derived from coal tar pitch (CTP) with KMnO₄ as the manganese source. This study systematically investigates the impact of MnO₂ loading on the microstructure and electrochemical performance in sample. It is found that the specific surface areas (SSA) of all MnO₂@PCs significantly reduced compared to that of the PCs 2789 m² g⁻¹. The suggested mechanism might be a combination of the energy storage mechanism of dual layer capacitors with pseudo-capacitance due to redox reactions of MnO₂. Notably, MnO₂@PCs-0.0075 exhibits a maximum SSA of 1454.62 m² g⁻¹. Its specific capacitance reached 561 F g⁻¹ at 0.5 A g⁻¹, while the capacitance of the PCs increased by 81.5% to 309 F g⁻¹. Remarkably, the Coulombic efficiency remained at 100%. The power density and energy density are determined in a two-electrode test system to be 0.5 kW kg⁻¹ and 58.01 Wh kg⁻¹, respectively, at 0.5 A g⁻¹. Concluding from these results and related literature, the MnO₂ content significantly influences the electrochemical performance, suggesting that [email protected] could be a promising supercapacitor (SC) electrode material, provided its capacitance retention is enhanced.

The enzymatic effectiveness in the reaction cascade that reduces CO₂ to methanol in water at room-temperature faces various constraints. One of the major challenges is the short life of costly enzymes: immobilization is used to make them more stable and recyclable. The comparative analysis of the several immobilization techniques reported in the literature is challenging due to the diverse reaction conditions (single enzyme test or pool of enzymes test) and experimental setups, as well as the high variability in the amount of enzymes and cofactor. In the present study, a comparison is presented among three different methods (co-encapsulation into Ca–alginate beads, co-absorption onto zirconium(IV) phosphate (ZrP) and covalent binding to dialdehydecellulose [DAC]) of co-immobilization of the three dehydrogenases F_atedehydrogenase (DH), F_aldDH, and alcohol dehydrogenase, used in equal amount and under the same experimental conditions, so to check at what extension the support and the immobilization method can influence the activity of the enzymatic pool. DAC is used for the first time to support the three DHs and results to be the best method of immobilization with respect to those used here, that also allows longer life on enzymes and repeated recycling of the supported enzymes, increasing the overall methanol production with respect to the free enzymes.

Wearable pressure sensors have attracted significant attention owing to their potential applications in health monitoring and connectivity to internet-based apps. Polymers such as poly(vinylidene fluoride) have been used in sensors. However, being petroleum-derived materials, they do not decompose and remain in the soil when disposed. Poly(l-lactic acid) (PLLA) is a promising material because of its biodegradable nature and its derivation from plant-based materials. In addition, the electrospun PLLA fiber mat contains real charges and exhibits electromechanical properties. However, the detailed charging properties of the PLLA fiber mats remain unclear. Herein, the charge distribution of these fiber mat is presented, and a charging model of the fiber mat and a numerical model of the output charges from the fiber mats with electrodes are proposed. Additionally, the retention properties of the stored charges are determined using surface potential measurements at different temperatures. In addition, a self-power-generating touch sensor and mask-type sensor are developed using biodegradable materials produced from biomass. These studies contribute to the improvement in the charge properties of PLLA fiber mats and the resulting wearable biodegradable sensors.