CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Lu Yang,Liang Zhou,Liang Yuan,Junli Ren,Chuanfu Liu,Zengyong Li
The development of efficient catalytic systems for the low-temperature oxidation of biomass-derived sugars to value-added acids remains a key challenge in sustainable biorefining. In this study, a palladium catalyst supported on amine-functionalized biochar (Pd/BC-NH 2 ) derived from corn straw for the oxidation of corn straw hydrolysate. The catalyst achieved an exceptional total sugar acid yield of 88.2% under mild conditions at 323 K with NaHCO 3 weak base. Comprehensive characterization confirmed successful amine functionalization and Pd immobilization. Kinetic and thermodynamic analyses determined an activation energy of 41.88 kJ·mol −1 and revealed endothermic, non-spontaneous reaction characteristics. DFT calculations elucidated the mechanism, identifying hydroxide ion-assisted aldehyde C − H cleavage as the rate-determining step with an energy barrier of 56.92 kJ·mol −1 . The superior performance is attributed to a synergistic mechanism where NH 2 groups enrich surface OH − concentration and electronically modulate Pd sites. The catalyst maintained excellent stability over 10 cycles. This study provides a sustainable “waste-to-wealth” strategy for biomass valorization using a straw-derived catalytic system, supported by comprehensive mechanistic insights.
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JOURNAL OF ALLOYS AND COMPOUNDS
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2026
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IF 6.7
Huimin Zhang,Zhangjian Qian,Zhiling Qiu,Ziyang Chen,Yongtao Miao,Xin Xiao,Xiangmei Wang
With the advancement of industrialization, the contamination of aquatic environments by organic pollutants has become increasingly severe, highlighting the urgent need for efficient and stable visible light-driven photocatalysts. In this study, g-C 3 N 4 /Bi 2 WO 6 composite photocatalysts were synthesized via hydrothermal synthesis method. Experimental results show that the g-C 3 N 4 /Bi 2 WO 6 composite achieves degradation efficiencies of 95.7% for Rhodamine B and 86.5% for ciprofloxacin, with reaction rate constants enhanced by factors of 1.98 to 12.8 compared to the individual components. Furthermore, the catalyst retains high activity after three consecutive cycles, indicating excellent recyclability and structural stability. Combined theoretical calculations and experimental characterizations reveal that a built-in electric field at the heterojunction interface, in synergy with interfacial orbital hybridization, promotes a direct Z-scheme charge transfer mechanism. This mechanism not only reduces the band gap, extending visible-light absorption, but also enables efficient separation of photogenerated carriers while preserving strong redox capabilities. This work establishes a robust theoretical and experimental foundation for the rational design of high-performance visible-light-responsive photocatalytic materials.
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CHEMICAL ENGINEERING SCIENCE
·
2026
·
IF 5.1
Taijia Li,Guichun He,Mengfei Liu,Zhiwen Cao,Jie Min
Selective separation of 90 Sr 2+ and 137 Cs + from nuclear wastewater is a significant challenge in the field of environmental remediation. In this paper, magnetic P-type zeolite composites loaded with Fe 3 O 4 were successfully synthesized via an alkali fusion-assisted hydrothermal method using lithium porcelain clay tailings (LPCT) as the silicon-aluminum source, achieving resource utilization of solid waste. The material exhibited excellent selective adsorption capacity for Sr 2+ : under the conditions of pH = 6 and a dosage of 2 g/L, the removal rate for Sr 2+ (100 mg/L) reached 99.4%, while that for Cs + (50 mg/L) was only 55.2%. In simulated/real seawater systems, the material maintained exceptionally high selectivity for trace Sr 2+ (with a K d value of 1.265 L·g –1 in simulated seawater). Mechanistic studies revealed that Sr 2+ undergoes specific ion exchange primarily by substituting Na + within the zeolite framework (adsorption energy: −2.37 eV), forming stable chemical bonds; in contrast, Cs + binds only through weak physical adsorption (adsorption energy: −0.85 eV), making it susceptible to displacement by competing ions. After five cycles, the Sr 2+ removal rate remained above 65%. This study presents a strategy for upcycling solid waste into high-performance functional materials and offers a promising solution for the efficient and selective separation of radioactive Sr 2+ from complex aqueous environments, highlighting its potential for practical nuclear wastewater treatment.
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High Voltage
·
2026
·Vol. 11
·期 2
·577-588
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IF 5.7
Kai Zhang,Yudan Tang,Zhengyong Huang,Jian Li
Free radical reactions are crucial in the thermal oxidation of natural esters, yet the underlying elementary reaction pathways and oxidation mechanisms remain unclear. This study uses density functional theory to systematically investigate these mechanisms. The interaction between triglyceride free radicals and oxygen during the initial thermal oxidation stage was examined. Structural and thermodynamic data for 16 reactions were evaluated, proposing a cyclic model for the involved free radicals. Most reactions are exothermic, releasing 35.06–166.59 kJ/mol. Initial reactions (R1 and R2) are thermodynamically favourable for heat accumulation and peroxyl radical formation. Peroxyl radicals initiate cyclic pathways and react with C–C double bonds, forming new active sites and alkoxy radicals (RO·), depleting reactive groups and oxygen. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) data corroborate the computational predictions, confirming the approach’s precision. This study suggests eliminating key active groups (R·, ROO·, RO· and ·OH) to prevent premature oxidative failure of natural esters by terminating the cyclic chain reaction. This insight could guide the development of more stable natural ester-based products.
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CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Wende Yi,Xiaodong Jin,Binbin Wang,Xiaoqing Xiong,Hua Yang,Xin Zhou,Jieru Xiong,Zhijun Zhang,Zhihong Peng,Zhihan Peng,Wufei Tang
While ammonium polyphosphate (APP) has been widely investigated for enhancing the flame retardancy of polylactic acid (PLA), its practical application remains constrained by inherent limitations, such as poor compatibility with the polymer matrix, limited flame-retardant efficiency at lower loadings, and the tendency to aggravate deterioration of mechanical properties. To address these issues, we synthesized a novel modified APP (MAPP) via reaction with piperazine, cyanuric chloride, and Tris reagent, resulting in an all-in-one intumescent flame retardant (IFR) that integrates acid, gas, and carbon sources within a single structure. PLA/MAPP composites achieved self-extinguishing behavior in the UL-94 test, with remarkably improved flame retardant efficiency and limiting oxygen index (LOI) compared to state-of-the-art studies. TGA analysis revealed a char residue of 8.9% at 800 °C, exceeding both the theoretical value and the char yields of conventional PLA composites. The flame-retardant mechanism indicated that MAPP mainly endowed PLA with excellent flame retardancy through the solid phase. Notably, density functional theory (DFT) calculations combined with experimental characterizations validated MAPP's synthesis and enabled in-depth elucidation of the flame-retardant mechanism. Through DFT simulations, MAPP was rationally designed as an innovative flame retardant that simultaneously provided an acid source, gas source, and carbon source. These calculations further elucidated its key properties and validated the enhanced thermal stability of the overall system, which aligned with the core theme of this research. Meanwhile, PLA/MAPP exhibited outstanding tensile strength among all samples, exceeding that of PLA by 20.8% and PLA/APP by 63.3%. This work provides a viable strategy for developing high-performance PLA composites with well-elucidated flame-retardant mechanisms, holding promising implications for advanced flame-retardant polymer materials.
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CHEMICAL ENGINEERING JOURNAL
·
2026
·
IF 12.5
Min Zhou,Guanjun Chen,Ningbo Yu,Zhiwu Liang,Hongxia Gao
DMSO promotes primary/secondary amines and sustains tertiary amine kinetics. • DMSO enhances amine nucleophilicity by restructuring solvation shells and modulating N H interactions. • Destabilized transition states in DMSO lower activation barriers, promoting reaction activity. • Provides molecular insights for designing efficient water-lean CO 2 capture systems. The high energy demand associated with regeneration poses a significant bottleneck for conventional aqueous amine absorbents, rendering the R&D (Research and Development) of water-lean systems crucial for energy-efficient CO 2 capture. This study employs an integrated approach combining stopped-flow apparatus with multi-scale simulations to systematically investigate the intrinsic kinetic behavior of AP, EAE and MDEA in DMSO-H 2 O mixed solvents ([H 2 O]: 0–55 M for AP and EAE, 5–55 M for MDEA). Experimental results revealed distinct solvent-response profiles for the three amines: the intrinsic rate constant k 0 of AP increased monotonically with decreasing water content, peaking in pure DMSO; EAE exhibited a non-monotonic U-shaped trend with a kinetic minimum at 20 M water; whereas MDEA maintained a relatively stable kinetic profile. Molecular dynamics (MD) simulations indicated that DMSO restructures solvation shells to alleviate steric shielding effects and enhanced the electron density of the amine nitrogen, thereby improving local reactivity. Density functional theory (DFT) calculations further corroborated that DMSO lowered reaction activation barriers by destabilizing transition states through the attenuation of hydrogen-bond stabilization. This work elucidates the cooperative regulation mechanism involving DMSO solvent effects and electronic properties, providing a theoretical basis for the rational design of efficient water-lean CO 2 capture systems.
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SENSORS AND ACTUATORS B-CHEMICAL
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2026
·
IF 8.3
Liyong Du,Jiayi Li,Enhui Liu,Shuli Wei,Qing Lu,Guoli Yang
In this work, hollow double-shelled ZnSnO 3 /SnO 2 heterojunctions are fabricated via a straightforward self-sacrificing template route. The crystal structure, microstructure, elemental composition, surface chemical states, optical properties and oxygen vacancies of the as-prepared materials are systematically characterized. Gas sensing tests reveal that the ZnSnO 3 /SnO 2 -2 sample exhibits a high response of 104.5 toward 100 ppm triethylamine (TEA) with a rapid response speed of 1 s at a relatively low operating temperature of 160°C, along with good selectivity, repeatability and long-term stability. The enhanced gas sensing mechanism is elucidated from the perspectives of electronic structure and surface reaction by combining density functional theory (DFT) calculations and in-situ Fourier transform infrared (FTIR) spectroscopy. Furthermore, preliminary monitoring of pork freshness during storage using the ZnSnO 3 /SnO 2 -2 sample demonstrates its potential in practical applications. This study provides a theoretical foundation and experimental support for the design of high-performance and low-power TEA gas sensors.
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COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
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2025
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IF 5.4
Yongxing Shang,Jian Xiong,Shuo Chen,Junjie Zhu,Xiaodie Zhao,Bitao Xiong,Xing’ao Li
Acid Orange 7 (AO7) is a recalcitrant contaminant exhibiting persistent resistance to degradation in aquatic environments. Materials based on graphitic carbon nitride (
) demonstrate significant potential in removing pollutants like AO7 through synergistic interactions with oxidants, utilizing their exceptional catalytic properties and high surface area for adsorption. However, their effectiveness is limited by a relatively large band gap, which hinders their catalytic performance. This study reveals that Ni/O dual-doped
(NiOCN) effectively optimizes the structure and catalytic performance of
. Experimental results indicate that the NiOCN/peroxymonosulfate (PMS) system exhibits optimal AO7 degradation performance, achieving 92.3% degradation within 10 min while maintaining 80% efficiency in simulated aqueous matrices. Quenching experiments further identified superoxide anion radicals ( ⋅ O 2 − ) as the predominant reactive species governing AO7 degradation. Using density functional theory (DFT) calculations, we confirmed that Ni/O dual-doping narrows the band gap and boosts catalytic activity. Our findings mechanistically demonstrate that Ni/O dual-doping augments PMS activation performance by introducing impurity energy levels, increasing adsorption sites, and accelerating electron migration kinetics.
研究领域:
环境化学
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材料科学
·
催化反应
·
污染物处理
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理论计算
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水污染控制
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INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
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2026
·
IF 8.3
Tianyun Zhao,Qiuwan Shen,Jicang Si,Jinliang Yuan,Shian Li
Configurational entropy engineering was employed to design perovskite catalysts for efficient hydrogen production via methanol steam reforming (MSR). The optimized medium-entropy perovskite, LaCo 1/3 Fe 1/3 Cu 1/3 O 3 , achieves an exceptionally high oxygen vacancy concentration (42.11 %), which dramatically enhances its catalytic performance. It demonstrates stable operation for over 40 h at 600 °C with high methanol conversion and hydrogen selectivity. Combined experimental and DFT studies reveal that the superior activity and low CO selectivity originate from a unique surface mechanism on the (110) facet: a high energy barrier for ∗CO desorption suppresses CO release, while a low barrier steers the reaction toward the water-gas shift pathway, favoring H 2 and CO 2 production. This work underscores the promise of entropy-engineered perovskites for durable and selective hydrogen generation.
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APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Jiping Zhao,Youlong Xu,Shiheng Liu,Xiangdong Ding
Adsorption of oxygen-containing species on the surface of tantalum (Ta) electrode significantly affects its electrochemical corrosion behavior. Density-functional theory (DFT) is employed to investigate the adsorption energies, structural properties and electronic structures of atomic oxygen (O) and molecular water (H 2 O) on Ta (1 1 0) surface. The adsorption behavior of H 2 O at room temperature is also studied based on ab initio molecular dynamics (AIMD). We find the passivation of Ta metal is mainly attributed to the strong adsorption of oxygen atoms. Thermodynamic results show that bulk Ta 2 O 5 is easily formed at room temperature, which is the fundamental reason for the spontaneous passivation of Ta (1 1 0) surface. The formation of an oxygen monolayer (1.00 ML) on Ta (1 1 0) surface dramatically increases the work function, making the equilibrium potential of Ta electrode move in the positive direction, thus slowing down the corrosion rate of Ta metal. However, the adsorption of H 2 O causes a negative work function change, which promotes its anodic dissolution. The electrochemical impedance spectra (EIS) of tantalum foil in three different NH 4 F-methanol electrolytes (pure, 0.01 M water and oxygen saturated) shows that the charge transfer resistance increases in the sequence R H2O < R pure < R oxygen , which can be well explained by the results of DFT calculations.
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JOURNAL OF CATALYSIS
·
2018
·
IF 6.759
Xiaolong Liu,Qingzhen Han,Wenbo Shi,Cheng Zhang,Erwei Li,Tingyu Zhu
In this work, ruthenium-based bimetallic catalysts of 1Ru-5 M/TiO 2 (M = Co, Ce, Fe, Mn, Cu, Ni) were prepared and evaluated in ethyl acetate oxidation. It was found that 1Ru-5Cu/TiO 2 gave the highest catalytic activity. The influence of CuO content and the preparation method on the catalytic activity was also studied. 1Ru-5Cu/TiO 2 showed great catalytic stability in the on-stream reaction test. The influence of H 2 O on the catalytic activity is presented. The bimetallic catalyst 1Ru-5Cu/TiO 2 showed better catalytic performance than the monometallic catalysts 1Ru/TiO 2 and 5Cu/TiO 2 . XRD, TEM, HAADF-STEM, H 2 -TPR, and XPS characterizations were conducted, and the synergistic effect between Ru and Cu was well presented. In situ FTIR studies were also conducted, and the reaction intermediates were revealed on the catalyst surface. The theoretical calculations suggested that ethyl acetate is more easily adsorbed on the CuO surface, while it reacts more easily on the RuO 2 surface . Accordingly, a reaction mechanism for the catalytic oxidation of ethyl acetate over a Ru-Cu bimetallic catalyst is proposed.
研究领域:
催化化学
·
环境化学
·
表面科学
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材料化学
·
物理化学
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ENVIRONMENTAL SCIENCE & TECHNOLOGY
·
2021
·
IF 9.028
Shuaiying Zhai,Yuetan Su,Xiaole Weng,Renna Li,Haiqiang Wang,Zhongbiao Wu
Vanadium-based catalysts have been extensively applied for the synergistic control of NOx and chlorinated organics. However, how the vanadia species affect the reaction activity and products distribution, and what are the dominant reaction sites of these vanadia species are still unknown. Herein, we investigated the reaction characteristics of monomeric and polymeric vanadate domains for the catalytically synergistic elimination of NOx and chlorobenzene (CB). Density functional theory (DFT) calculations and experimental investigations have been combined to clarify the effects of different vanadyl species on the synergistic reaction. It was noted that the main adsorption site of CB on the monomeric domain was V–OH bond, and that on the polymeric one was V═O bond. The monomeric vanadyl was favorable for converting the Lewis V═O into Brønsted V–OH, which provided sufficient H protons for HCl formation, whereas the polymeric species could effectively retain the V4+/V5+ redox cycle, and yielded superior activity in CB catalytic oxidation (CBCO) reaction. However, the abundant oxygen vacancies and the inclined accumulation of Cl by forming the V–Cl bands led to significant polychlorinated byproducts on the polymeric vanadyl catalysts. Our work gives the first insight into different vanadate domain effects on the synergistic reaction, and is expected to provide theoretical basis for efficient design of the vanadium-based catalysts toward multipollutants elimination.
研究领域:
催化化学
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环境化学
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材料科学
·
计算化学
·
污染物控制
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