Selective hydrodeoxygenation of waste oil into high-value bio-aviation fuel precursor via catalytic pyrolysis was a crucial pathway for producing renewable green fuels and enhancing biomass resource high-valuable utilization. However, achieving a balance between catalytic activity and selectivity remains challenging, often leading to poor selectivity for hydrocarbon-rich product. Herein, a series of efficient and stable Ni–Sn bimetallic catalysts supported on a hybrid carbon shell and MgO were fabricated and applied to catalytic deoxygenation of oleic acid for bio-aviation fuel production. Detailed experiments and characterization revealed that Sn loading promoted the well-dispersion of Ni nanoparticles, suppressing their aggregation and increasing the number of accessible active sites, thereby enhancing hydrodeoxygenation and selective C–C bond cleavage. More importantly, Sn introduction promoted Sn0 species formation, which acted as Lewis acidic centers and/interfacial sites, thereby enhancing catalyst’s aromatization capability. Consequently, the optimized 1Ni-2Sn/MgO-C catalyst exhibited outstanding catalytic deoxygenation performance with 90.83 % total hydrocarbon yield, 87.25 % aviation fuel selectivity and nearly complete oleic acid conversion due to the synergistic interaction between Ni and Sn species that facilitated to C–C bond cracking and lower energy barrier. Furthermore, Sn species incorporation significantly improved catalyst stability by geometric isolation and electron donating properties. This work provided a novel and practical strategy for designing non-noble metal catalysts to selectively upgrade low-grade vegetable oils into high-value aviation fuel.
Bamboo-derived biochar had emerged as a promising electrode material for supercapacitors owing to its cost-effectiveness, renewability and exceptional electrochemical performance. However, limited energy density and challenges in pore structure regulation hindered its practical application. Herein, N-heteroatom doped biochar with superior electrochemical activity was successfully fabricated via pre-carbonization, N-heteroatom (N/O, N/S, N/P, N/B, N/F) co-doping, and K2C2O4-enhanced KOH activation process. Combined experimental and DFT analyses revealed that N-heteroatom co-doping regulated pore structure, shorten ion transport distance and provided abundant active adsorption site to enhance K+ affinity. NO co-doped exhibited remarkable Vmicro/Vtotal ratio (89.33), higher N-heteroatom content (N+S+O, 30.02%), nitrogen content (2.44%) and N/O functional groups, therefore achieving ultra-high specific capacitance of 382F/g at 0.5A/g and 98.33% capacitance retention after 10000 cycles in tri-electrodes systems. Additionally, DFT calculation demonstrated that N-heteroatom introduction facilitated to K+ adsorption and diffusion on graphene surface and enhanced conductivity. Meanwhile, to evaluate the practical performance, AC-BPC-NO was used as electrodes material in an assembled symmetric supercapacitor exhibited outstanding energy density of 29.44Wh/kg and power density of 1000W/kg, validating its practical viability. Furthermore, even over 10,000 cycles, the optimized AC-BPC-NO electrodes also retention 95.33% of initial capacity in double electrodes systems, demonstrated excellent cycling stability. This work not only provided a novel insight and theoretical support for designing high-energy-density energy storage materials and but also enhanced the potential value-added utilization of waste biomass.
Selective conversion of vegetable oils into high-value gasoline/aviation fuel precursors via catalytic hydrodeoxygenation presents a promising strategy to address global energy challenges while advancing agricultural/ forestry sustainability. However, practical implementation has been constrained by low product selectivity, high costs, and catalyst deactivation. We address these challenges by developing a series of bifunctional lanthanum (La)-zirconium (Zr)-modified, hydrotalcite-derived catalysts with tailored acidity and oxygen vacancies for the selective deoxygenation of oleic acid. Detailed experimental and characterizations results revealed that La-Zr codoped magnesium oxide (MgO)-alumina (Al2O3) catalysts demonstrated the highest deoxygenation efficiency through synergistic effects, and the (1La-1Zr)/(MgO-Al2O3) catalyst exhibited 100 % conversion, 93.12 % hydrocarbon yield, and 88.39 % gasoline-range selectivity owing to elevated strong acid site density, mesoporosity (increasing accessibility), well-dispersed metal nanoparticles (small size), oxygen vacancy concentrations, and metal-support interactions (Zr4+-La3+ synergistic effect). These factors synergistically enhanced carboxyl (-COO*) adsorption and deoxygenation. Zr-rich systems favored aromatic compound and light fuel (gasoline/ aviation) formation, while La-dominated catalysts maximized diesel-range selectivity owing to the generation of abundant La-Zr alloy nanoparticles. Critically, the oxophilicity of Zr-La suppressed coke deposition, particularly reducing hard coke formation and ensuring remarkable operational stability. This study establishes a viable pathway for the industrial-scale valorization of waste vegetable oils into high-value gasoline/aviation fuel precursors through rationally designed cost-efficient catalysts.
As sustainable alternatives to fossil fuels, biomass-derived liquid fuels play a critical role in mitigating greenhouse gas emissions and diversifying energy supplies. In this study, the effect of calcination temperature (600-1000 degrees C) on the structure and catalytic performance of MnFeCoNiCu/activated carbon (AC) catalysts via in-situ carbon reduction method for the hydrodeoxygenation (HDO) of fatty acid methyl esters (FAME) to sustainable biofuels including bio-jet fuel and green diesel was systematically investigated. Results revealed that increasing calcination temperature promoted the transformation of the crystal structure from body-centered cubic (B2) to face-centered cubic (FCC), with the AC-900 catalyst (calcined at 900 degrees C) exhibiting a dominant FCC phase, enhanced metal dispersion, and optimal surface defect density. Although higher temperature reduced the specific surface area and pore volume of the AC support, the formation of a stable multimetallic solid solution and strong metal-support interactions at 900 degrees C significantly improved catalytic performance. Under optimal reaction conditions (350 degrees C, 0 MPa H-2, 2 h), the AC-900 catalyst achieved 100% FAME conversion and 97% hydrocarbon selectivity, primarily via decarbonylation/decarboxylation (DCN/DCX) pathways, favoring the production of C-15-C-17 hydrocarbons aligned with green diesel and bio-jet fuel specifications. Increasing H-2 pressure favored alkane formation by promoting olefin hydrogenation, while lower pressure enhanced C-C bond cleavage for shorter-chain hydrocarbons. Circulating stability tests indicated that the AC-900 catalyst maintained 62% FAME conversion and >80% hydrocarbon selectivity after 5 cycle. This work highlights the critical role of calcination temperature in tailoring FCC-structured multimetallic catalysts for efficient FAME conversion, providing insights into the rational design of stable, high-performance catalysts for sustainable biofuel production.
Lithium metal batteries hold immense potential for high-energy applications, yet they face significant challenges such as lithium dendrite, dead lithium formation, and volume expansion. Herein, an innovative strategy is proposed to address these issues. Specifically, a high-entropy alloy (HEA) composed of Mg, Ag, Cu, Mn, and Ni is synthesized on graphitized carbon paper via a simple impregnation and high-temperature thermal reduction method, serving as the anode for lithium metal batteries. The synergistic effects of HEA nanoparticles, LiC6, and a three-dimensional (3D) collector significantly enhance the anode's lithiophilicity, effectively guiding a uniform lithium nucleation process. Consequently, symmetric cells employing this anode exhibit outstanding cycling stability even in ester electrolytes, sustaining operation for over 2400 h at 0.5 mA cm-2/1 mAh cm-2 and exceeding 1000 h at 1 mA cm-2/1 mAh cm-2. When paired with an NCM-811 cathode, the battery exhibits a coulombic efficiency of 99.6% after 200 cycles at 0.5 C and 99.8% after 300 cycles at 1 C. These findings demonstrate that designing amphiphilic lithium sites on 3D collectors is an effective approach for optimizing lithium metal battery anodes, thereby pointing to new directions for the future development of lithium metal batteries.
The capacity degradation characteristics of 18650 NCA lithium battery under different working conditions were investigated. Experiments were carried out at 45℃, and the direct effects of charge-discharge ratio and cut-off voltage on capacity degradation were analyzed. The results show that when the charge-discharge ratio is 2C, the capacity degradation rate is significantly higher than 1C and 1.5C. The degradation of battery capacity is more obvious in high cut-off voltage and high temperature environment. Through XRD and XPS characterization, it was found that high temperature resulted in the formation of lithium dendrites and the destruction of material structure, which affected the crystal state and chemical composition of the battery surface. The comprehensive analysis shows that the charge-discharge ratio and cut-off voltage are the key factors affecting the capacity degradation of 18650 NCA lithium battery. Optimizing these conditions can effectively delay the capacity decline and improve the service life and stability of the battery.
The structure of hard carbon somehow determines the Na storage mechanism and directly affects its rate capability and initial Coulombic efficiency (ICE) in Na-ion batteries. Herein, we fabricate hierarchical graphitized carbon fibers via flash Joule heating within seconds. The fiber presents a uniform graphitized shell layer and a disordered core layer, which can maximize the Na intercalation capacity and reversibility. Combined with advanced spectroscopic techniques, we clearly observe that metallic Na clusters are uniformly stored in the outer layer at a low-voltage plateau. Such Na storage mechanism shortens ion transport distance and enhances reaction kinetics. As a result, the carbon fiber exhibits the highest ICE (97.7% at 50 mA g-1) and fast charging capability (4 mins charging). A single-layer pouch cell with a low N/P ratio can be cycled stably 1000 times at 1C. To our knowledge, this Na+ storage is reported for the first time, providing new insights into the rational design of hard carbon.
Silicon (Si)-based anodes have emerged as promising candidates for the next-generation lithium-ion batteries (LIBs) due to their high theoretical capacity (4200 mAh g−1). However, their further application is hindered by critical challenges, including severe volume expansion (∼300 %), formation of unstable solid electrolyte interphase (SEI), and inherently low conductivity. While extensive research has sought to alleviate the substantial internal stress caused by volume expansion through the rational design of Si-based anode structures, the underlying mechanisms that govern these improvements remain insufficiently understood, leaving significant gaps in mechanical and interface electrical failure. To build a comprehensive understanding relationship between structural design and performance enhancement of Si-based anodes, this review first analyzes the characteristics of various Si-based anode structures and their associated internal stresses. Subsequently, it summarizes effective strategies to optimize the performance of Si-based anodes, including doping design, novel electrolyte design, and functional binder design. Additionally, we assess emerging technologies with high commercial potential for structural design and interfacial modification, such as porous carbon carriers, chemical vapor deposition (CVD), spray granulation, and pre-lithiation. Finally, this work provides perspectives on the structural design of Si-based anodes. Overall, this review systematically summarizes modification strategies for Si-based anodes through structural regulation and interface engineering, thereby providing a foundation for advanced structural and interfacial design.
The production of sustainable biofuels via lipid deoxygenation relies heavily on efficient catalysts, but conventional tube-furnace calcination often leads to excessive metal grain growth and limited active sites, restricting catalytic performance. Herein, we report the synthesis of MnFeCoNiCu/C catalysts using a rapid Joule heating method to address these limitations, aiming to enhance lipid deoxygenation for efficient sustainable fuel production. Compared with the traditionally calcined catalyst (AC-900), the Joule -heated catalyst (AC-900 J) exhibits distinct structural advantages: smaller metal crystallites (23.31 nm vs. 41.91 nm), a higher specific surface area (1050 m2/g), and abundant moderate-strong basic sites, which are attributed to ultra-fast heating that suppresses grain growth and promotes uniform metal dispersion. Catalytic tests at 350 °C under atmospheric pressure H2 show that both catalysts achieve near-complete conversion of fatty acid methyl esters (FAME), while AC-900 J demonstrates superior bio-jet fuel selectivity (65.1% vs. 57.5% for AC-900). Its versatility is validated across diverse feedstocks (e.g., palmitic acid, oleic acid, soybean oil), maintaining 100% conversion and >94% hydrocarbon selectivity despite structural variations in substrates. Additionally, AC-900 J exhibits favorable cyclic stability, retaining 84.7% conversion and 49.2% bio-jet fuel selectivity after 4 cycles. This work highlights rapid Joule heating as a robust strategy to fabricate MnFeCoNiCu/C catalysts with tailored nanostructures, effectively enhancing lipid deoxygenation and enabling efficient production of sustainable biofuels.
CaO-supported Ni catalysts have been extensively applied in lipids deoxygenation due to their cost-effectiveness and efficiency. However, excessive C-C bond cracking induced by strong base sites and metallic Ni activity limited their practical application. Herein, CaO-MgO supported Ni catalysts with variable MgO content was synthesized via sol-gel method and applied for selective catalytic deoxygenation of fatty acid (saturated and unsaturated) and lipid (edible oil and non-edible oil) for generation high-valuable hydrocarbon-range biofuel in free-H-2 conditions. Additionally, the possible catalytic reaction pathways, deactivation mechanism, reusability and broad applicability were also elucidated. Ni-Ca-Mg catalyst demonstrated exceptional performance in conversion fatty acid and lipids into hydrocarbon fuels, and achieving 86.70 % hydrocarbon (HCs) yield and 56.01 % gasoline selectivity over Ni-Ca-Mg (20:1 mass ratio) catalyst. Detailed characterizations revealed that oxygen vacancies and enriched Lewis acid sites facilitated to -COO* adsorption and dehydration hydrodeoxygenation reaction. More importantly, NiO-MgO solid solution formation significantly stabilized support structure and boosted cycling stability (>85 % activity retention after 4 cycles) and coke position resistance. Besides, catalyst deactivation primarily owing to coke deposition, pore blockage; reductive dissolution and surface oxidation of Ni0 active sites as well as weaken of strong metal-support interaction (SMSI) at Ni-support interfaces. This study establishes a novel, low-cost synthesis strategy for high-efficiency Ca-based catalysts, demonstrating significant potential for valorizing carboxylic-rich biomass feedstocks into premium fuels and chemicals.
Carbon based anodes that rely solely on Li-ion storage are inherently limited in energy density, whereas systems dominated by Li-metal storage suffer from poor reversibility and short cycle life. Hybrid Li-ion/Li-metal batteries (LIB/LMBs), enabled by carbon-based Li-free anodes, offer a promising pathway by integrating Li-ion intercalation and Li-metal plating/stripping within a single framework. Despite rapid progress, the practical implementation of hybrid LIB/LMBs remains hindered by low Coulombic efficiency, unstable solid electrolyte interphase, dendrite growth, and large volume fluctuations. These challenges are fundamentally associated with irreversible Li loss and interfacial instability, which limit long-term cycling and energy efficiency. In this review, we systematically summarize recent advances in carbon-based Li-free anodes for hybrid LIB/LMBs, with a focus on (i) the hybrid storage mechanism, (ii) rational design of carbon materials, (iii) interface engineering strategies, (iv) mechanistic insights from in situ characterization, and (v) critical perspectives toward practical deployment. Particular emphasis is placed on the relationship between Coulombic efficiency, Li inventory retention, and system-level performance. This review provides a unified framework for understanding hybrid storage chemistry and offers strategic guidance for the development of next-generation high-energy-density batteries.
Accurate long-horizon prediction of state of charge (SOC) and battery temperature is critical for safe operation of large-scale battery energy storage systems (BESS). However, owing to strong electro-thermal coupling, cell heterogeneity, and time-varying operating conditions, existing data-driven and physics-informed methods may exhibit substantial error accumulation and limited transferability under long-horizon and distribution-shifted conditions. A Physics-Dominated Structured Evolution Framework (PDSEF) is proposed to model battery states as a constrained evolution process rather than direct observation-to-state regression. The state-transition backbone is governed by physical laws, including charge conservation and thermal dynamics, while adaptive physical parameters are inferred from recent historical observations during deployment, thereby characterizing cell-level heterogeneity without requiring explicit offline parameter calibration. Constrained neural residuals are further introduced to compensate for unmodeled nonlinear behaviors, and temporal, hierarchical spatial, and operating semantic representations are integrated to capture long-horizon dependencies, inter-cell interactions, and dynamic operating variations. The proposed framework is validated on a real-world BESS containing 384 cells under multi-condition charge-discharge operations. A 30-step recursive rollout is repeatedly propagated over more than 10,000 evolution steps to evaluate long-horizon prediction stability. The results demonstrate stable SOC and terminal temperature predictions with minimal error accumulation. The cross-condition mean SOC NMAE reaches 0.02299 and 0.02279 under zero-shot and fine-tuned settings, respectively, while terminal temperature NMAE improves from 0.16786 to 0.08999 after adaptation. Comparative and ablation studies confirm that the proposed physics-dominated evolution mechanism enhances generalization and long-horizon stability compared with existing baselines. Overall, the framework provides a reliable approach for proactive state monitoring and safety-oriented management of large-scale BESS.
Studies on the solid electrolyte interphase (SEI) formed via selective electrocatalysis often pay too much attention to LiF content while neglecting that the continuous accumulation of LiF severely limits fast-charging capability due to its inherently low electrical conductivity. Herein, we propose a tailored core-shell composite (Si@Fe3C-NC) comprising Si nanoparticle cores encapsulated by a partially graphitized nitrogen (N)-doped carbon shell embedded with uniform Fe3C nanoparticles. The synergistic effect of N-doping and Fe-induced partial graphitization of the carbon layer constructs efficient electron/ion transport pathways. Additionally, self-encapsulated Fe3C nanoparticles not only selectively catalyze the formation of a thin and LiF-rich SEI but also mitigate the conductivity loss caused by LiF accumulation. Consequently, the Si@Fe3C-NC anode exhibits outstanding electrochemical performance, delivering an ICE of 90.2%, a high specific capacity of 1750.8 mAh g-1 after 300 cycles at 1 A g-1, and excellent fast-charging durability (858.8/539.2 mAh g-1 after 500/2000 cycles at 5 A g-1). Moreover, the 1 Ah pouch cells assembled with the Si@Fe3C-NC anode and LFP/NCM811 commercial cathodes exhibit excellent fast-charging performance and cycling stability over 200 cycles at 2 C. This study reveals the "dual role" of a LiF-rich SEI and presents a promising strategy for its formation on Si anodes.
Accurate prediction of the State of Health (SOH) of lithium-ion batteries under diverse operating conditions remains a significant challenge, primarily due to heterogeneous usage patterns, compositional variations, and the scarcity of labeled data. To address these challenges, a Transferable SOH Prediction (TSP) framework is proposed for robust cross-domain generalization. The proposed TSP framework integrates one-dimensional convolutional neural networks (1D-CNNs) with multi-head attention mechanisms to simultaneously capture local and global degradation characteristics. A physics-informed dual-stage loss function is developed to enforce monotonic SOH degradation and facilitate domain-invariant feature learning across different battery chemistries and temperature conditions. Extensive cross-domain evaluations on NCM and NCA batteries across varying temperatures (25 degrees C, 35 degrees C, 45 degrees C) and C-rates (0.25C, 0.50C) demonstrate that the TSP model consistently achieves low RMSE (e.g., 0.0142 +/- 0.0003 for NCA at 35 degrees C and 0.0153 +/- 0.0045 for NCM at 25 degrees C) and exhibits high statistical reliability (p-values > 0.89), outperforming state-of-the-art benchmarks including Physics-Informed Neural Networks (PINN) and other deep transfer learning models. Ablation studies confirm the critical contribution of each component to the overall performance. These findings highlight the potential of TSP to enable reliable and data-efficient SOH estimation for next-generation battery management systems operating under diverse and uncertain conditions.
Ammonium-ion asymmetric supercapacitor (AASC) has emerged as promising candidates for next-generation energy storage systems due to their environmental benignity, cost-effectiveness, and high safety. However, achieving efficient interfacial charge transfer and robust interfacial kinetics remains a critical challenge for highperformance AASC. Herein, we design a high-quality NiCo2S4/Fe2O3 heterojunction electrode with tailored interfacial engineering to address these issues. The results show that NiCo2S4/Fe2O3 heterojunction forms charge transfer via NH4+ mediation, including Co center dot center dot center dot N-H coordination bond and N-H center dot center dot center dot O hydrogen bond. The bridges coupled with a built-in electric field (BIEF) induced by the work function difference at the p-n heterointerface, synergistically accelerate NH4+ diffusion and reduce charge transfer barrier. As a result, NiCo2S4/Fe2O3 exhibits a remarkable specific capacitance of 838.7 F g- 1 and excellent interfacial durability with 96.6 % capacitance retention after 10,000 cycles. A braided coaxial NiCo2S4/Fe2O3//AC@CNT AASC is constructed to achieve a wide voltage window of 1.8 V and a high energy density of 135.5 Wh kg- 1, along with superior mechanical flexibility and cycling stability (92.5 % retention over 2500 cycles). Our study provides a rational strategy for designing interface-bonding heterojunctions to manipulate charge carriers, paving the way for advanced AASCs in wearable and flexible electronics.
Two-dimensional materials featuring active sites have the potential to replace platinum as scalable oxygen reduction reaction (ORR) catalysts. Transition metal carbon-nitrogen frameworks (TM-C9N10), owing to their distinct electronic and geometric configurations along with numerous active sites, have emerged as a focal point in contemporary catalytic studies. However, constrained by lengthy experimental cycles and the high costs associated with traditional computational methods, the influence of different central atom compositions in TM-C9N10 monolayers on their ORR catalytic activity remains largely unexplored, significantly impeding the progress of this material. In this research, combining density functional theory (DFT) and high-throughput screening, we systematically investigated ORR catalytic mechanisms in various TM-C9N10 monolayers. Computational results show d-band center tuning optimizes intermediate binding, while TM-C9N10-intermediate coupling dictates ORR efficacy. From 38 candidates, Fe-C9N10 and Mn-C9N10 emerged as the most promising, with Fe-C9N10 achieving an impressively low overpotential of 0.24 V and Mn-C9N10 showing 0.45 V, both exhibiting excellent thermodynamic and electrochemical stability. This study provides key insights for designing high-performance ORR catalysts and elucidates TM-C9N10's catalytic mechanisms.
This study investigated the catalytic upgrading of oleic acid in the presence of Ni-Ce-Zr catalysts to evaluate its potential for the synthesis of hydrocarbon fuels. For this purpose, a series of Ce-Zr and Ni-Ce-Zr catalysts were synthesized via different methods (mechanical mixing (Mix), ball milling (BM), incipient impregnation (ImP), and coprecipitation (CoP)) and systematically characterized via various techniques to elucidate their structure-property relationships. Then, the effects of the synthesis methods on the product yield, hydrocarbon distribution, possible reaction pathways and catalytic deactivation mechanism were carefully determined. Detailed characterization and control experiments revealed that the catalytic activities of various Ni-Ce-Zr catalysts were in the following order: ImP-Ni > CoP-Ni > Mix-Ni > BM-Ni. ImP-Ni exhibited superior catalytic deoxygenation capacity and obtained a 100 % conversion rate, 86.22 % HCs yield with 82.43 % green diesel selectivity due to good dispersion of Ni and Ce species, abundant metal-to-acid sites, abundant oxygen vacancies and defects, high concentrations of Ni-0 and the interaction of Ni-0/Ni2+ and Ce3+/Ce4+ redox pairs. Additionally, the samples exhibited outstanding reusability and coke resistance after the fourth cycle (HCs remained above 90 %, mass loss of 1.73 %). Ni addition notably enhanced hydrodeoxygenation activity toward diesel-range fuels compared with support catalysts with higher decarbonylation/decarboxylation selectivity. Furthermore, Ni was the main hydrodeoxygenation reactive site because it created more Lewis acid sites and provided active hydrogen atoms via the dissociation of H-2. Ce functions as a decarbonylation/decarboxylation reactive site with abundant oxygen vacancies to adsorb and activate COO*. This approach provides a straightforward and effective method for designing catalysts that are structurally tailored to the production of green diesel-range fuels via the waste-to-resource strategy.
The production of bio-jet fuel via the hydrodeoxygenation (HDO) process of lipids emerges as a highly promising strategy for alleviating environmental pollution within the aviation sector. However, conventional catalysts typically require complex preparation procedures and depend on high pressure hydrogen, thereby increasing production costs and limiting their widespread application. This study presents a novel one-step in-situ preparation of nickel-iron (Ni/Fe) bimetallic catalysts supported on carbon, specifically designed to enable efficient bio-jet fuel production under solvent-free and low hydrogen pressure conditions. Using methyl palmitate (MP) as a model feedstock, the effects of Ni/Fe ratio, reaction temperature, hydrogen pressure, and Ni/ZSM-5 addition on the hydrodeoxygenation conversion and bio-jet fuel selectivity were systematically investigated. Remarkably, the NiFe/C catalyst optimized with a Ni/Fe ratio of 1:1 demonstrated extraordinary performance, attaining a complete conversion of 100 % and high selectivity of 97 % towards bio-jet fuel at 375 degrees C and a relatively modest 2 MPa hydrogen pressure. Despite a moderate decrease in conversion (to 53.65 %) and selectivity (to 83.06 %) after five cycles- attributed to carbonaceous deposition-the NiFe/C catalyst demonstrated robust durability and exceptional versatility with respect to different feedstocks. Decarboxylation (DCX) and decarbonylation (DCN) were identified as the dominant reaction pathways in the NiFe/C-catalyzed hydrodeoxygenation process. Notably, combining NiFe/C with Ni/ZSM-5 enriched product composition with aromatic hydrocarbons, isoalkanes, and cycloalkanes, thereby improving the overall quality of the bio-jet fuel. This innovative approach provides a cost-effective and high-efficiency pathway for the advancement of bio-jet fuel preparation technology.
Hydrogen and bioderived fuels are central for decarbonizing energy systems, yet catalyst deactivation and inefficient synthesis methods remain major bottlenecks. Herein, we report a rapid strategy to synthesize graphite-encapsulated NiMn heterostructured nanoparticles via a rapid high-temperature carbothermal shock (HCS). Structural characterization reveals a dual-phase architecture comprising Mn-incorporated face-centered cubic Ni (fcc-Ni) and MnO phase, synergistically enhancing bond cleavage within complex reactions. The optimized catalyst achieves an 18.7-fold increase in hydrogen yield (8.4 +/- 0.3 mmol/gbiomass-daf, 40.3 +/- 0.9 vol %) compared to noncatalytic pyrolysis, while simultaneously enabling complete conversion of various lipid feedstocks, particularly fatty acid methyl ester (FAME), into biojet and diesel-range hydrocarbons via dominant decarboxylation (DCO2) pathways. The catalyst maintains over 80% efficiency over seven cycles, and its catalytic activity can be effectively restored through a rapid shock-based regeneration strategy. Mechanistic studies further reveal that the heterostructure design and shell structure modulation enhance bond activation and promote reaction kinetics. This work demonstrates the effectiveness of HCS as a platform for engineering Ni-based nanomaterials, potentially bridging biomass-to-hydrogen conversion with biofuel upgrading for integrated biorefineries.
In the context of global energy transition and carbon neutrality goals, developing sustainable technologies for converting biomass waste into high-value green hydrogen (H-2) is critical for advancing cleaner production and a circular economy. This study presents a novel approach to synthesizing carbon-supported ultrasmall FeCoNiCuZn high-entropy alloy (HEA) nanoparticles via flash Joule heating (FJH) carbothermal shock, enabling efficient catalytic valorization of poplar sawdust waste into H-2. The FJH process at 1000 degrees C suppresses volatile metal (e.g., Zn) loss and promotes rapid reduction, yielding high-density active sites with enhanced metallic states. Structural characterizations confirm the formation of a single-phase face-centered cubic HEA structure, uniformly dispersed on nitric acid-modified biochar with strong metal-support interactions, stabilized by oxygen-containing functional groups. The synergistic effects of ultrasmall particle size (<5 nm), high specific surface area (1636 m(2)/g), and graphitized carbon framework significantly boost catalytic efficiency in ex situ biomass pyrolysis. The optimized catalyst (FeCoNiCuZn/C-8-HNO3) achieves a H-2 yield of 23.56 mmol/g(biomass-daf) (48.66 vol %), which is 37-fold higher than noncatalytic pyrolysis and 1.3-fold higher than conventional tube furnace-synthesized catalysts. This work establishes a sustainable pathway for converting low-value biomass waste into green H-2 using cost-effective, high-performance HEA catalysts, addressing key challenges in cleaner production, resource utilization, and carbon-neutral energy systems.