Carbon Neutralization最新文献

The environmental issues caused by carbon dioxide (CO₂), a major greenhouse gas, have garnered increasing attention, driving the widespread application of electrocatalytic CO₂ reduction reactions (eCO₂RR) in pollutant treatment. Metal-CO₂ batteries (MCBs) have emerged as a promising alternative to conventional fuel cells, garnering significant interest due to their capacity to integrate energy storage with eCO₂RR. The electrolyte is of pivotal significance in MCBs, given its considerable impact on battery performance, service life, and safety. However, due to the inherent limitations of conventional electrolytes, such as flammability, thermal instability, poor low-temperature performance, side reactions, achieving simultaneous optimization of all required performance parameters remains a formidable scientific challenge. Electrolytes should simultaneously possess high ionic conductivity, substantial CO₂ solubility, broad electrochemical stability window, and thermodynamically robust interfaces with the electrode materials to ensure overall system performance and stability. It is fortunate that a range of methodologies have been established for the purpose of modifying electrolytes. In this review, we provide a concise overview of the structural characteristics of conventional MCBs, systematically classify MCBs electrolytes into liquid, solid-state, and semi-solid-state categories, and highlight the unique advantages and challenges. We further explore key optimization strategies like bulk composition tuning and additive engineering to enhance performance and put forward several suggestions for the future development of MCBs electrolytes according to persistent challenges. The findings of this study can provide valuable insights for the development of MCBs.

Chain diamines have gained attention in carbon capture recently for their high CO₂ absorption capacity and rate. However, how diamine structure regulates the activation barrier of CO₂ absorption remains unclear, and the large number of amine candidates hinders efficient screening of low-energy absorbents. To resolve these issues, this study first used DFT to investigate the regulation mechanism of diamines on CO₂ absorption and clarify key reaction pathways and structure-activity relationships. It was confirmed that diamines react with CO₂ via a zwitterion mechanism, while diamine/tertiary amine mixtures react with CO₂ through single-step proton transfer. Diamines with more primary amine sites have lower barriers; methyl/ethyl substitution, carbon chain extension (on either amine), or hydroxyl substitution (on diamines) increases the proton transfer barrier. To address low screening efficiency from excessive candidates, an efficient framework integrating DFT and active learning was constructed. Using DFT-calculated reaction barriers, a feature mapping with RDKit descriptors was built, and an active learning model was developed via 10 iterative rounds. The model achieved high prediction accuracy (R² = 0.821) for the rate-determining step's activation barrier. SHAP analysis identified the steric-related first-order molecular connectivity index (T_Chi1v) as the dominant feature. Finally, the optimal amine pair (AEEA + EDMA, activation barrier: 0.8 kcal·mol⁻¹) was identified. This work clarifies the core mechanism via DFT, enables efficient candidate screening via active learning, and explains the optimal combination's performance through mechanistic tracing—providing an interpretable route for developing low-energy, high-efficiency mixed amine absorbents and advancing carbon capture technology.

The porous carbon-coated Ni_0.5Zn_0.5Fe₂O₄ ferrite embedded within Ti₃C₂T_x MXene interlayers was successfully synthesized via solvothermal and electrostatic self-assembly, followed by carbonization. The resulting Ni_0.5Zn_0.5Fe₂O₄@C/Ti₃C₂T_x composites exhibit superior electromagnetic wave absorption properties, achieving a minimum reflection loss of −63.25 dB at 17.32 GHz with a coating thickness of only 1.53 mm. Notably, heat treatment at 800°C induces the formation of an open interlayer porous microstructure and abundant heterogeneous interfaces, which effectively suppress nanoparticle agglomeration, enhance interfacial polarization, and optimize impedance matching. This study demonstrates a novel strategy to integrate MOF-derived ferrite with MXene for constructing hierarchical porous structures, offering new insights into the rational design of lightweight, high-performance microwave absorbing materials.

As nature's most abundant renewable carbon source, biomass enables a closed–loop carbon-neutral paradigm for producing industrial oxygenates. Biomass electrocatalytic oxidation reaction (BOR) replaces the energy-intensive oxygen evolution reaction (OER), simultaneously achieving green synthesis of value-added oxygenates and enhancing electrolytic energy efficiency, thereby displacing fossil–based production routes. This review systematically elucidates the electrocatalytic conversion of biomass derivatives (e.g., alcohols, furanal, and sugars, etc.) into value-added products coupled with hydrogen production from the perspectives of catalyst design principles and reaction mechanisms. Further focus on integrated anode–cathode systems that synergistically couple biomass oxidation with cathodic carbon dioxide reduction (for fuel synthesis) or nitrate reduction (for ammonia production and pollutant remediation), overcoming limitations of standalone hydrogen generation while enabling coproduction of chemicals and carbon/nitrogen resource cycling. Advanced multi-field coupling strategies are analyzed for their efficacy in enhancing reaction selectivity and efficiency, including photo-electrocatalysis to excite charge carriers, thermo-electrocatalysis to optimize kinetics, and high-pressure electrocatalysis to regulate mass transfer. Future efforts should prioritize non-precious metal active site engineering and scalable reactor design to advance biomass refining from conceptual frameworks toward industrial implementation.

The practical application of lithium−sulfur (Li−S) batteries is hindered by the shuttle effect of soluble lithium polysulfides and sluggish sulfur redox kinetics, resulting in rapid capacity fading and limited cycle life. Here, we present a rationally engineered yolk–shell nanoreactor architecture that integrates dual confinement and catalytic functionality to address these challenges. The nanoreactor comprises a polar, catalytically active core encapsulated within a conductive nitrogen-doped carbon shell, offering synergistic physical restriction of polysulfides and accelerated multistep sulfur conversion. Density functional theory calculations reveal uniformly low-energy barriers along the Li₂S₈-to-Li₂S pathway, with no evident rate-limiting step. Benefiting from this cooperative design, the sulfur host achieves a ultralow capacity decay (0.028% per cycle over 1000 cycles at 2 C) and enables a high areal capacity (493 mAh g⁻¹ at 4.3 mg cm⁻² sulfur loading) with 76.3% retention after 100 cycles at 0.3 C. This work offers a versatile strategy for constructing catalysis-integrated sulfur hosts and highlights the potential of yolk–shell nanoreactors in advancing practical Li−S energy storage systems.

Understanding and chemically tailoring the interfacial properties is essential for improving both efficiency and stability of perovskite solar cells (PSCs). All-inorganic cesium-based perovskites have emerged as promising candidates for thermally stable PSCs, however, their poor phase stability and high density of surface defects continue to impede device performance. Herein, we introduce functionalized halogenated phenethylammonium iodide (X-PEAI, X = H, F, Cl, Br) as modifiers, and a synergistic optimization of the perovskite bulk and interface is achieved through an integrated regulation strategy. It is found that Cl-PEAI with a strong dipole moment, achieves the optimal regulatory effect. It not only improves the film morphology but also effectively passivates the defect states through strong Lewis acid-base interactions. In addition, it also introduces an additional dipole layer at the interface, which enhances the carrier transport effect. Consequently, Cl-PEAI-treated devices deliver a champion power conversion efficiency (PCE) of 19.53% and retain 92.9% of their initial efficiency after 720 h of ambient storage, thereby underscoring the potential of rational ligand design within this specific ammonium salt category for advancing stable, high-performance all-inorganic PSCs.

High-performance and temperature-resistant lithium metal batteries (LMBs) can operate at extremely high temperatures (i.e., > 150°C), and there is a high demand for them in high-temperature scenarios or in special fields such as military application. However, due to the unstable organic solvents, traditional liquid electrolytes usually undergo severe degradation and pose serious safety risks at elevated temperatures (i.e., > 60°C). Herein, functional Li₇La₃Zr₂Ta_0.5O₁₂@methoxy polyethylene glycol (LLZT@mPEG) is synthesized via a novel and effective method known as in situ coupled macromolecular bridge, and corresponding all-solid-state composite polymer electrolyte (LLZT@mPEG-CPE) is further prepared. Rigid LLZT cores and flexible ionic conductive polymer side-chains are closely combined by electrostatic interaction, thus resolving the challenge of interface compatibility between different phases. The introduction of mPEG-COOH can further improve the dispersibility of LLZT@mPEG, enhance the stability of electrolyte/electrode interface, effectively inhibit the continuous decomposition of the polymer, enabling LMBs with high thermal tolerance and fast-cycling ability. As a consequence, our LLZT@mPEG-CPE shows great thermal stability and outstanding electrochemical performance. Remarkably, Li|LLZT@mPEG-CPE|LFP cell delivers superior temperature-resistance with a capacity retention of 94% after 500 cycles at high rate of 5 C and extreme temperature as high as 160°C. This study provides an innovative design principle for advanced all-solid-state CPEs of LMBs capable of extremely high temperature operation.

The utilization of coal resources is critically important in the modern era, and advancements in coal chemical technology are key to maximizing their value. Integrating modern coal chemical technology with the promotion of low-carbon products is essential for achieving efficient coal resource utilization while supporting sustainable economic development. However, several challenges remain, including low conversion rates, high pollutant emissions, and insufficient residue reuse. Although researchers have made significant progress in addressing these issues, further in-depth studies are needed to improve conversion efficiency, enhance gas recovery, and optimize secondary utilization of residues to ensure more sustainable development. The study systematically reviews advancements in traditional coal chemical technology and elaborates on the progress and advantages of modern coal chemical processes. Additionally, it highlights the pivotal role of carbon capture, utilization, and storage (CCUS) technologies in reshaping the energy structure. Furthermore, the reuse of coal chemical residues represents a crucial step forward in refining coal chemical technology. By addressing these aspects, this work serves as a reference for promoting cleaner and more efficient coal resource utilization.

Organic semiconductor photocatalysts hold promise for solar-driven hydrogen evolution, yet their efficiency is often constrained by weak intermolecular interactions, limited light-harvesting ability, and inefficient charge transport. Addressing these challenges requires precise structural modulation of donor–acceptor assemblies to establish robust electronic coupling and broaden absorption profiles. In this study, a molecular engineering strategy is introduced that simultaneously tailors the donor side chains and tunes the size of the fullerene acceptor cage, thereby promoting electron transport and enhancing light absorption, which ultimately leads to improve photocatalytic activity. Three fullerene-indacenodithiophene (IDT) derivatives—SA-C₆₀-DTIDTT (SA-C1), SA-C₆₀-IDTT (SA-C2), and SA-C₇₀-IDTT (SA-C3)—are synthesized and assembled into supramolecular architectures through a liquid–liquid interfacial deposition method. Replacing the thiophene ring in the donor side chain with a benzene ring strengthens π–π stacking interactions, resulting in more efficient charge transport pathways. Incorporation of C₇₀, with its extended π-system, further facilitates electron delocalization and broadens visible-light absorption. As a result, the SA-C₇₀-IDTT photocatalyst achieves a hydrogen evolution rate of 17.16 mmol g⁻¹ h⁻¹. This study highlights the effectiveness of donor–acceptor structural modulation for constructing high-performance, solar-driven hydrogen evolution photocatalysts.

ZnIn₂S₄ (ZIS) has garnered significant interest in photocatalytic energy conversion and environmental remediation due to its tunable band gap, strong visible-light response, and facile synthesis. However, its practical application is severely hindered by inherent limitations, including low charge carrier separation efficiency and sluggish surface reaction kinetics. Constructing heterojunctions has emerged as an effective strategy to enhance ZIS performance by leveraging precise band alignment and interface engineering to optimize charge separation. While excellent reviews on ZIS-based photocatalysis have been published, comprehensive reviews focusing specifically on the design and evaluation of ZIS-based heterojunctions remain scarce. This review systematically summarizes recent advances in ZIS-based heterojunctions, providing a detailed discussion of heterojunction types and key synthesis strategies. Multi-scale modification strategies for synergistically enhancing photocatalytic activity are also examined. Furthermore, the charge separation mechanisms and surface reaction pathways are elucidated through advanced in situ characterization techniques and density functional theory (DFT) calculations. ZIS-based heterojunctions demonstrate great potential across various photocatalytic applications, including H₂ evolution, CO₂ reduction, H₂O₂ production, N₂ fixation, pollutant degradation, and emerging fields such as plastic reforming and tumor therapy. Finally, future research directions are outlined, encompassing crystal phase regulation, adaptive heterojunction design, and AI-driven screening, thereby providing theoretical guidance for the development of highly efficient ZIS-based photocatalysts.