Carbon Neutralization最新文献

The Ni/CeO₂ catalyst stands out among various solid metal oxide catalysts for its exceptional catalytic proficiency, positioning it as a prime candidate for the industrialization of methanation processes. This review thoroughly examines the prevalent challenges associated with Ni/CeO₂ in methanation reactions, compiles current strategies to overcome these hurdles, and presents novel perspectives. The review elucidates the structural characteristics of Ni/CeO₂ and its applications in catalytic reactions, discusses various synthesis methods and their respective merits and demerits, explores catalytic reaction systems at both laboratory and industrial scales, and clarifies the underlying reaction mechanisms. Furthermore, it underscores the mainstream approaches to enhance the low-temperature activity of Ni/CeO₂ in methanation and to mitigate activity decrement due to Ni agglomeration. The review concludes by proposing future directions for improving low-temperature methanation activity and preventing catalyst deactivation, encompassing the development of innovative catalyst architectures, integrating in-situ characterization with theoretical calculations, and investigating photothermal methanation catalytic systems. Undoubtedly, scientific researchers will persistently strive to develop Ni/CeO₂ catalysts with high activity across a broad temperature range and robust stability, driving the industrialization of CO₂ methanation technology in the foreseeable future.

In military reserve power supplies, there is an urgent need for superior secondary batteries to replace conventional primary batteries, and lithium-ion batteries (LIBs) emerge as one of the best choices due to their exceptional performance. The life of LIBs includes cycle life and calendar life, with calendar life spanning from years to decades. Accurate prediction of calendar life is crucial for optimizing the deployment and maintenance of LIBs in military applications. Model-based prognostics are usually established to estimate calendar life using accelerated aging methods under various storage conditions. This review firstly outlines the general prognostic workflow for calendar life of LIBs, analyzes degradation mechanisms, and summarizes influencing factors; then, we introduce calendar life prognostic models, evolving from simplistic empirical models (EMs) to nonempirical mechanistic models (MMs) based on LIB calendar aging knowledge and then to traditional hybrid empirical-mechanistic models (trad-EMMs). Finally, the data-driven models (DDMs) based on machine learning (ML) are discussed due to the limitation of the traditional methods, evolving from pure data-driven to knowledge-integrated models and establishing a comprehensive framework for calendar life assessment. To the best of our knowledge, this paper presents the first comprehensive review in this field, summarizing calendar life prognostic models of LIBs and offering some insights into future model development directions. Model-based prognostics can facilitate researchers in calendar aging analysis and calendar life prolongation, thereby better serving the application of LIBs in national economic life.

Solid-state lithium batteries have attracted increasing attention due to their high ionic conductivity, potential high safety performance, and high energy density. However, their practical application is limited by a series of interface issues. In recent years, many efforts have been dedicated to solving these problems via interface engineering by providing feasible strategies for the optimization of lithiumion solid-state battery interfaces. This paper reviews the recent developments of interface engineering in addressing interfacial issues. The existing interface problems are first systematically summarized, including poor contact, electrochemical instability, lithium dendrites, space-charge layers, and element diffusion. Then, the corresponding interface characteristics and engineering strategies are thoroughly analyzed from the perspective of the cathode/electrolyte interface, the anode/electrolyte interface, and battery structure design. Finally, future research directions for the interface modification of solid-state lithium batteries are discussed.

Carbon-based nanomaterials play a significant role in the field of electrochemistry because of their outstanding electrical conductivity, chemical and thermal resistance, structural flexibility, and so on. In recent years, we have observed a rapid rise of research interest in the high-temperature shock (HTS) method, which is fast, stable, environmentally friendly, and versatile. The HTS method offers excellent controllability and repeatability while tackling challenges and limitations of traditional preparation methods, providing a new way to prepare and optimize carbon-based nanomaterials for electrochemical applications. During the HTS synthesis, the reaction is driven by the high temperature while further growth of obtained nanoparticles is inhibited by the rapid heating and cooling rates. The preparation of carbon-based nanomaterials by HTS has many advantages, including controlled carbon vacancy that may drive phase transformation, precise engineering of carbon, and other defects that may function as active centers, formation and preservation of metastable phase owing to the high energy and rapid cooling, fine-tuning of the interaction between loaded species and carbon support for optimized performance, and facile doping and compounding to induce synergy between different constituents. This article provides a comprehensive review of various carbon-based nanomaterials prepared by the HTS method and their applications in the field of electrochemistry during the past decade, emphasizing their synthesis and principles to optimize their performance. Studies showcasing the merits of HTS-derived carbon-based nanomaterials in advancing Lithium-ion batteries, Lithium-sulfur batteries, Lithium-air batteries, water-splitting reaction, oxygen reduction reaction, CO₂ reduction reaction, nitrate reduction reaction, other electrocatalytic reactions, and fuel cells are highlighted. Finally, the prospects of carbon-based nanomaterials prepared by HTS method for electrochemical applications are recommended.

The growing use of lithium iron phosphate (LFP) batteries has raised concerns about their environmental impact and recycling challenges, particularly the recovery of Li. Here, we propose a new strategy for the priority recovery of Li and precise separation of Fe and P from spent LFP cathode materials via H₂O-based deep eutectic solvents (DESs). Through adjusting the form of the metal complexes and precipitation mode, above 99.95% Li and Fe can be dissolved in choline chloride-anhydrous oxalic acid-water (ChCl-OA-H₂O) DES, and the high recovery efficiency of Li and Fe about 93.41% and 97.40% accordingly are obtained. The effects of the main parameters are comprehensively investigated during the leaching and recovery processes. The recovery mechanism of the pretreated LFP is clarified and the rate-controlling step of the heterogeneous dissolution reactions is also identified. Results show that soluble phases of Li₃Fe₂(PO₄)₃ and Fe₂O₃ are formed after roasting pretreatment, and Li(I) ions tend to form Li₂C₂O₄ precipitates with C₂O₄²⁻ during the leaching process so that Li can be recovered preferentially in purity of 99.82%. After UV-visible light irradiation, Fe(III) ions are converted into Fe(II) ions, which can react with C₂O₄²⁻ to form FeC₂O₄ precipitates by adjusting the H₂O content, and P is recovered as Na₃PO₄∙12H₂O (99.98% purity). Additionally, a plan for the recycling of used DES is proposed and the leaching and recovery performances still maintain stable after three recycling circles. The method offers an approach with a simple process, high efficiency, and waste-free recycling for priority recovery Li and precise separation of Fe and P from spent LFP batteries in DESs.

Front cover image: Zinc-ion batteries (ZIBs) demonstrate great potential for applications in extreme temperature environments. In the center of the cover image, a massive ZIB is depicted. On the left, a fiery volcano landscape with lava and a phoenix symbolizes the battery's adaptability to high temperatures. On the right, a snow-covered world with a majestic ice dragon represents the battery's durability in sub-zero cold conditions. Above the batteries, the ZIBs encircle the earth, demonstrating the wide range of applications for ZIB batteries around the world, from scorching deserts to frigid polar regions, showcasing their ability to provide reliable energy solutions in diverse environments.

Solid-state lithium metal batteries (SSLMBs), heralded as a promising next-generation energy storage technology, have garnered considerable attention owing to inherent high safety and potential for achieving high energy density. However, their practical deployment is hindered by the formidable interfacial challenges, primarily stemming from the poor wettability, (electro) chemical instability, and discontinuous charge/mass transport between solid-state electrolytes and Li metal. To overcome these obstacles, taking garnet-based electrolyte (Li_6.5La₃Zr_1.5Ta_0.5O₁₂, LLZTO) as a pathfinder, the ceramic metallization-assisted room-temperature ultrasound werlding (UW) has been developed to reinforce the Li/LLZTO interface. This ultrasound welding approach constructs a compact interface that facilitates rapid Li⁺/e⁻ transport, while the formation of Li−M (M = Au, Ag, and Sn) alloy homogenizes the distribution of Li⁺/e⁻ at the interface. By optimization, the atomic-level contact achieved by ultrasound welding, coupled with a nanosized Au modification layer, significantly reduces the Li/LLZTO interfacial resistance to 5.4 Ω cm², a marked decrease compared to the resistance achieved by static pressing methods (1727 Ω cm²). The symmetric cell exhibits a high critical current density of 1 mA cm⁻² and sustains long-term stability for over 1600 h at 0.3 mA cm⁻², with a Li plating/stripping overpotential of < 45 mV. By incorporating a robust anode-side interface into solid-state lithium metal batteries, the LiFePO₄-based full battery contributes 118.4 mAh g⁻¹ after 600 cycles at 1 C (capacity: ∼100%). This study offers a facile and effective approach to bolster the interfacial stability between Li and solid-state electrolytes, paving the way for the development of high-performance solid-state lithium metal batteries.

In the pursuit of advanced energy storage technologies that promote sustainable energy solutions, zinc-ion batteries (ZIBs) have emerged as a promising alternative to lithium-ion batteries due to their abundance, safety, and environmental advantages. However, the failure mechanisms of ZIBs under extreme temperatures are still not fully understood, presenting significant challenges to their development and commercialization. Therefore, innovative strategies are essential to enhance their adaptability to temperature extremes. In this review, we first explore the thermodynamic and kinetic aspects of performance degradation under extreme temperatures, focusing on key factors such as ion diffusion and redox processes at electrode interfaces. We then comprehensively summarize and discuss the existing approaches for various electrolyte types, including aqueous, nonaqueous, and solid state. Finally, we highlight the key challenges and future prospects for ZIBs operating under extreme temperature conditions. The insights presented in this review are expected to accelerate the advancement of ZIBs and facilitate their practical implementation in large-scale energy storage systems.

Lithium metal battery (LMB) is regarded as one of the most promising high-energy energy storage systems. However, the high reactivity of lithium metal and the formation of lithium dendrites during battery operation have caused safety concerns. Herein, we present the design and synthesis of fire-extinguishing microcapsules to enhance LMB safety. The encapsulation strategy addressed perfluoro(2-methyl-3-pentanone)'s volatility and storage challenges, yielding microcapsules with stable and uniform size distributions. The rapid release and effective fire-extinguishing performance of the microcapsules upon exposure to high temperatures has been demonstrated. Integration of these microcapsules into LMBs showed no significant impact on electrochemical performance, maintaining high lithium-ion conductivity, and stable cycling capacity. Notably, practical safety tests on pouch cells indicated that the presence of microcapsules effectively prevented ignition and improved thermal stability under mechanical damage and flame intrusion, underscoring their potential for significantly improved battery safety. These findings provide a robust strategy for mitigating fire hazards of high-energy-density battery systems without compromising their electrochemical performances.

The solvent-rich solvent sheath in low-concentration electrolytes (LCEs) not only results in high desolvation energy of Li⁺, but also forms organic-rich solid electrolyte interface film (SEI) with poor Li⁺ conductivity, which hinders Li⁺ transport at the electrode-electrolyte interface and greatly limits the application of LCEs. Here, the electrochemical performance of the LCEs is enhanced by dual interfacial modification with LiNO₃ and vinylene carbonate (VC) additives. Results show that LiNO₃ is preferentially reduced at about 1.65 V to form an inorganic-rich but incomplete SEI inner layer. The formation of Li₃N and LiN_xO_y inorganic components helps to achieve rapid Li⁺ transport in the SEI film, and the bare electrode surface caused by the incomplete SEI inner layer provides a place for the subsequent decomposition of VC. Then, at a lower potential of about 0.73 V, VC is reduced to generate the poly(VC)-rich SEI outer layer, which provides lithium-philic sites and greatly weakens the interaction between Li⁺ and ethylene carbonate (EC). The interaction modulates the Li⁺ solvation structure at the interface and reduces the desolvation energy of Li⁺. This ingenious design of the bilayer SEI film greatly enhances Li⁺ transport and inhibits the decomposition of traditional carbonate solvents and the swelling of graphite. As a result, the electrochemical performance of the battery using 0.5 M LiPF₆ EC/diethyl carbonate (DEC) + 0.012 M LiNO₃ + 0.5 vt% VC is improved to a higher level than the one using 1.0 M LiPF₆ EC/DEC electrolyte. This research expands the design strategy and promising applications of LCEs by constructing a favorable SEI to enhance Li⁺ transport at the electrode-electrolyte interface.