APPLIED CATALYSIS A-GENERAL
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2025
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IF 4.8
Kaihao Li,Yongwang Li,Yang Qin,Zheng Wang,Bingxin Zhu,Yancong Yin,Fumin Wang,Xubin Zhang
The production of high-purity hydrogen chloride from petrochemical by-product hydrogen chloride gas represents the primary industrial approach for manufacturing electronic-grade hydrogen chloride. However, trace acetylene and ethylene impurities in the feedstock severely compromise product quality. This study innovatively proposes a "stepwise conversion-deep chlorination" synergistic mechanism and successfully develops a bimetallic catalyst (10 %Fe/0.5 %Pd/AC). By tailoring the preparation processes, we precisely controlled the distribution of Fe and Pd active sites, while systematically comparing the performance between Single-metal tandem catalytic system (Pd/AC + Fe/AC) and the bimetallic catalyst. Experimental results combined with DFT calculations demonstrate the superior performance of the 10 %Fe/0.5 %Pd/AC catalyst and confirm the cascade reaction mechanism based on the synergistic tandem effect of Fe/Pd active sites: Acetylene preferentially undergoes hydrochlorination at Pd sites to form vinyl chloride, while ethylene and the resultant vinyl chloride are subsequently converted to chloroethane and more easily removable 1,1-dichloroethane at Fe sites. Under optimized conditions (120 °C, GHSV=180 h −1 ), removal efficiencies exceeding 99 % for both acetylene and ethylene were achieved, with 1,1-dichloroethane selectivity surpassing 99 %. Comprehensive characterizations demonstrated the outstanding stability of the 10 %Fe/0.5 %Pd/AC catalyst. This study presents an innovative catalytic approach for high-efficiency purification of industrial hydrogen chloride.
研究领域:
催化化学
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化学工程
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环境科学
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材料科学
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工业化学
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DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2025
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IF 7.7
Ye Li,Bai-Hang Zhao,Bao-Yu Zhang,Jia-Hang Liu,Xu-Ming Liu
Peroxymonosulfate (PMS)-based advanced oxidation processes have gained significant attention due to their strong oxidative capacity and rapid reaction kinetics. However, the development of efficient, stable, and eco-friendly catalysts remains a major challenge in realizing practical applications. To address this issue, a novel catalyst, Co 1 Ce 2 O x @PAL, was synthesized via the sol-gel method to enhance PMS activation efficiency by leveraging rare-earth doping and the carrier properties of palygorskite (PAL). Comprehensive characterization (SEM, XRD, FTIR, etc.) confirmed successful synthesis and favorable structural properties. Norfloxacin (NOR) was selected as the target contaminant to evaluate the catalytic performance of Co 1 Ce 2 O x @PAL. Under an optimal condition (30% metal loading, 0.3 g/L catalyst, 0.5 mM PMS, pH 6.2), NOR removal efficiency reached 95%, with an apparent rate constant of 0.15 min -1 . Quenching tests and electron paramagnetic resonance (EPR) analyses revealed that played a dominant role in NOR degradation. and were generated through the redox reactions between Co 2+ /Co 3+ and Ce 3+ /Ce 4+ . Furthermore, oxygen vacancies facilitated electron transfer, thereby promoting radical production and NOR degradation efficiency. DFT calculation, including electrostatic potential and frontier orbital analyses (HOMO/LUMO), identified the quinolone and piperazine rings as the most susceptible sites for radical attack. Four potential degradation pathways were proposed accordingly. The catalyst demonstrated a high stability and reusability, maintaining over 80% NOR removal after five cycles. ECOSAR predicted reduced toxicity for most transformation products. This study highlights the potential of Co 1 Ce 2 O x @PAL as an effective catalyst for sustainable water treatment by enabling efficient degradation of trace emerging contaminants and promoting water resource recycling.
研究领域:
环境化学
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催化科学
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水处理技术
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材料科学
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计算化学
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污染物降解
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高级氧化过程
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高影响因子
CHEMICAL ENGINEERING JOURNAL
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2020
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IF 10.652
Ke Wang,Xin Zhang,Yongfeng Liu,Zhuanghe Ren,Xuelian Zhang,Jianjiang Hu,Mingxia Gao,Hongge Pan
High operation temperatures and slow kinetics remain big challenges for using magnesium (Mg) as a practical hydrogen storage medium. In this work, a novel graphene-guided nucleation and growth process was developed for the preparation of N-doped Nb 2 O 5 nanorods that enable remarkably improved hydrogen storage properties of MgH 2 . The nanorods were measured to be 10–20 nm in diameter. MgH 2 doped with 10 wt% of the nanorods released 6.2 wt% H 2 from 170 °C, which is 130 °C lower than additive-free MgH 2 , thanks to a 40% reduction in the kinetic barriers. About 5.5 wt% of H 2 was desorbed in isothermal dehydrogenation test at 175 °C. Reloading of hydrogen was notably completed at 25 °C under 50 atm of hydrogen pressure, which has not been reported before. Density functional theory (DFT) calculations demonstrate the extended bond lengths and weakened bond strengths of Mg-H or H-H when MgH 2 /H 2 adsorbs on the Nb-N-O/graphene model, consequently favouring lower operating temperatures and improved kinetics for hydrogen storage in MgH 2 catalyzed by the graphene-guided N-Nb 2 O 5 nanorods. Our findings provide useful insights in the design and preparation of high-performance catalysts of transition metals and rare metals for on-board hydrogen storage.
研究领域:
材料科学
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催化
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氢气储存
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纳米技术
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2026
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IF 12.5
Jinming Fu,Jun Yao,Chuiyun Tang,Tatjana Šolević Knudsen,Jian-li Liu
p-Chloroaniline (PCA), a persistent and toxic pollutant in mine tailings, necessitates cost-effective remediation strategies. This study evaluates the degradation of PCA by Fe 2+ /Fe 3+ -catalyzed sodium persulfate (SPS) and sodium percarbonate (SPC) oxidation enhanced by UVA-B irradiation. Among the systems tested, the UVA-B/Fe 2+ /SPS system achieved 96.2% PCA removal within 180 min, outperforming other configurations. Radical scavenging experiments and density functional theory (DFT) calculations suggested that SO 4 • − and •OH radicals were the primary reactive species in SPS systems, while •OH and O 2 ●- were identified as the major reactive species in SPC systems. DFT further revealed vulnerable sites on PCA for radical attack, supporting proposed degradation pathways. ECOSAR toxicity assessment revealed that although PCA acute toxicity decreased, certain intermediates (e.g., azo-compounds) retained high chronic toxicity, highlighting the importance of process optimization. This study provides novel insights into the degradation mechanisms of PCA, establishing a mechanistic foundation for designing solar-enhanced, iron-coupled advanced oxidation processes for industrial-scale remediation of halogenated aromatics in mining environments.
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BMC Chemistry
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2026
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IF 5.1
Wang Hu,Shi Hua,Guo Pengxiao,Zhang Xia,Zhou Yadong,Wang Renshu,Yin Chaochuang,Zhu Yangyang
In the present study, two Cu(II) complexes incorporating a Schiff base ligand, termed CuSBCs, were synthesized and subjected to structural characterization. The complexes are denoted as [Cu(C 10 H 8 NO 4 F)(C 10 H 9 N 3 )]·H 2 O ( C1 ) and [Cu(C 10 H 8 NO 4 F)(C 12 H 12 N 2 )]·H 2 O·CH 3 OH ( C2 ), featuring the Schiff base ligand (SBL, C 10 H 8 NO 4 F) and distinct auxiliary ligands, specifically 2,2’-dipyridylamine and 5,5’-dimethyl-2,2’-bipyridine. Within these two complexes, the central Cu(II) ion exhibits pentacoordination, binding to ONO donor sites of the SBL as well as two nitrogen donor atoms provided by the auxiliary ligand, yielding a distorted square pyramidal geometry. Theoretical computations for both complexes were performed using density functional theory (DFT) with the B3LYP functional via the Gaussian 16 program. The computational results are in good agreement with experimental observations. Notably, both complexes exhibited significant inhibitory activity against jack bean urease (UA), with C1 (IC 50 = 4.79 ± 0.77 µM) outperforming C2 (IC 50 = 6.83 ± 1.19 µM) and the reference inhibitor acetohydroxamic acid (AHA). Molecular docking (MOD) and molecular dynamics (MD) simulations reveal that the superior activity of C1 originates from its better steric matching and more stable interactions with the enzyme active site, providing structural evidence for the experimental activity trend. In addition, ADME predictions indicated that both complexes possess favorable drug-like properties and promising bioavailability. These findings highlight the promising therapeutic potential of Cu(Ⅱ) Schiff base complexes as UA inhibitors. Graphical
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Food Chemistry-X
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2025
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IF 8.2
Pengxun Gao,Shang Wang,Baomin Feng,Chunying Liu,Yi Wang,Shaohua Dou,Liang Dong
The composition of volatile compounds generated by the thermal decomposition of Amadori rearrangement products (ARPs) in the Maillard reaction between glucose and alanine was investigated by using a combination of thermal desorption cryo-trapping system and gas chromatography–mass spectrometry. A total of 25 volatile compounds were detected and identified, including 15 pyrazines, 3 pyridines, 1 pyrrole, and 6 complex nitrogen-containing compounds. The results indicated that pyrazines are the predominant products of the thermal decomposition of ARPs, and the specific formation temperatures of the various volatiles were determined. Additionally, density functional theory (DFT) was employed to study the formation mechanism of 3-ethyl-2,5-dimethylpyrazine in depth, and the structures of the reactants, transition states, and products were elucidated. Furthermore, by comparing the rate constants and reaction energy barriers of the different reactions, it was concluded that the synthesis of deoxyglucosones and the ring-forming reaction of pyrazines are the key reactions in the generation pathway of 3-ethyl-2,5-dimethylpyrazine.
研究领域:
食品科学
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化学
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DOI
PubMed
高影响因子
Journal of Environmental Chemical Engineering
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2025
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IF 7.2
Dongting Huang,Huixin You,Lirong Chen,Yongjing Liu,Hua Li
This study extends the development of a Graphene oxide@Zirconium-based metal-organic framework@Deep eutectic solvents (GO@MOF-808@DESs) through hydrothermal self-assembly using zirconium chloride and 1,3,5-benzenetricarboxylic acid (H 3 BTC), subsequently functionalized with four carbon-tailored fatty acid-based deep eutectic solvents (DESs) via ultrasonic impregnation. Comprehensive characterization of GO@MOF-808@DES confirmed the successful surface modification via DES. A dispersive micro-solid phase extraction(D-μSPE) method was established employing GO@MOF-808@DESs as an adsorbent for efficient removal of residual entacapone (ETCP) and tolcapone (TCP) from water. Optimization of the D-μSPE method revealed optimal conditions at pH 9.0, with a sample volume of 40 mL, an adsorbent dosage of 20 mg, and an adsorption time of 60 min. Under these conditions, the method achieved a significant adsorption capacity of 86.50 ± 4.79 mg/g for ETCP and 126.21 ± 2.72 mg/g for TCP. Mechanistic investigation revealed chemically dominated adsorption kinetics through pseudo-second-order modeling and Langmuir isotherm fitting. Concurrently, density functional theory (DFT) studies demonstrated that the synergistic effect between carboxyl-mediated hydrogen bonding and hydrophobic interactions led to enhanced adsorption performance. The engineered GO@MOF-808@DESs based D-μSPE method demonstrated superior performance in removing ETCP and TCP from river water matrices, achieving 99.67 % and 99.24 %, respectively. Meanwhile, a sensitive and reliable method for trace-level monitoring of ETCP and TCP residues in environmental waters was successfully proposed, employing GO@MOF-808@DESs-based D-μSPE coupled with liquid chromatography-tandem mass spectrometry (LC-MS/MS). This study presents a robust strategy for fabricating high-performance GO@MOF-808@DESs composite materials, demonstrating significant potential for practical applications.
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高影响因子
Environmental Science-Nano
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2025
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IF 5.1
Lu Wang,Siyuan Zhang,Jukun Xiong,Meicheng Wen
Formaldehyde (HCHO), a prevalent indoor volatile organic compound, poses significant health risks to humans even at very low concentrations. As a result, its efficient degradation at room temperature is of utmost importance. However, the detailed mechanism for catalytic oxidation of formaldehyde remains unclear, particularly regarding the role of water vapor, which has been subject to considerable debate. In this study, we synthesized Pt-supported TiO2 glass fiber catalysts (Pt/TiO2 GF) via NaBH4 reduction to investigate the reaction pathways and clarify the influence of water vapor on the oxidation process. The reaction mechanism and intermediates were systematically studied at room temperature using in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), kinetic isotope effect (KIE) analysis, and density functional theory (DFT) calculations. Results revealed a clear reaction pathway of HCHO → DOM → HCOO− → CO2, with formate C–H bond cleavage (HCOO−* + O* → CO2 + OH*) identified as the rate-determining step. Both experimental KIE results and theoretical calculations confirmed that water vapor substantially reduces the activation barrier for this step, significantly promoting formate decomposition and subsequent CO2 formation. This work provides critical insights into the role of water in enhancing formaldehyde oxidation and offers theoretical support for developing efficient catalysts suitable for humid environments.
研究领域:
环境化学
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催化
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材料科学
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表面科学
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DOI
高影响因子
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
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2016
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IF 3.958
Lei Zhao,Baoyue Zhang,Xin Xiao,Feng Long Gu,Rui-Qin Zhang
Active species such as holes, electrons, hydroxyl radicals ( OH), and superoxide radical anions ( O 2 − ) involved in the photocatalytic oxidation of benzyl alcohol (BA) into benzaldehyde (BAD) on TiO 2 under ultraviolet (UV) light were investigated by adding corresponding scavengers. The experimental results show that the oxidation of BA into BAD is driven mainly by the holes and OH radical. The role of dissolved O 2 was studied by bubbling N 2 through the reaction. The results show that the dissolved O 2 is, to some extent, the source of OH. Additional density functional theory (DFT) calculations identified two H-abstraction pathways ( R abs OH and R abs α). The structure of the R abs OH product is less stable and tends to transfer resulting in the R abs α product. The holes are the main driving force for the abstracting of H from BA. The OH radical combines with the H-abstract product to form a precursor of product BAD, detected by LC–MS technique ( m / z 123), which then undergoes an intramolecular dehydration reaction to form BAD. The results will help to select the optimal active species for the photocatalytic oxidation of BA into BAD on TiO 2 under UV light.
研究领域:
物理化学
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光催化
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环境化学
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材料化学
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理论计算化学
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DOI
高影响因子
APPLIED SURFACE SCIENCE
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2026
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IF 6.6
Wenmei Wuxia,Yu Chen,HuanHuan Li,Ning Ma,Lengyuan Niu,Yinyan Gong,Can Li
Zr 4+ incorporation drives a complete transition to an amorphous phase and increases the electrochemically active surface area. • Zr 4+ incorporation induces a downward shift in the core-level binding energies of Fe, Co, and Ni sites. • Optimized S-CrMnFeCoNiZr 1.5 specimen achieves overpotentials of 240/287 mV at 10/100 mA/cm 2 . • S-CrMnFeCoNiZr 1.5 specimen exhibits outstanding stability and a 16-fold enhancement in TOF relative to S-CrMnFeCoNi specimen. Developing efficient and durable electrocatalysts for oxygen evolution reaction (OER) is pivotal to advancing renewable energy conversion technologies. Herein, a series of amorphous CrMnFeCoNi-based high-entropy compounds (HECs) with varied Zr content were synthesized, and the role of Zr doping in modulating the atomic/electronic structures were investigated, as well as the OER activity. Experimental characterization reveals that Zr 4+ incorporation drives a complete transition to an amorphous phase, increases the electrochemically active surface area, and induces a downward shift in the core-level binding energies of Fe, Co, and Ni. Relative to the Zr-free analogue, the optimized catalyst S-CrMnFeCoNiZr 1.5 delivers a 57/69 mV reduction in overpotential at 10/100 mA cm −2 , exhibits a 17-fold higher turnover frequency, and maintains exceptional operational stability over 72 h. This OER activity outperforms most previously reported HECs. Density functional theory calculations corroborate these observations, demonstrating that Zr doping upshifts the d-band centers of Fe, Co, and Ni, thereby strengthening adsorption of intermediates and optimizing the free-energy profile for the rate-determining steps. Collectively, this study establishes a rigorous structure–electronic property–performance correlation and demonstrates Zr-mediated electronic modulation as a rational, scalable strategy for engineering high-entropy electrocatalysts. Download: Download high-res image (70KB) Download: Download full-size image
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JOURNAL OF ALLOYS AND COMPOUNDS
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2025
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IF 6.3
Haihong Liu,Yumin Zhang,Huiping Shao,Zheng Yan,Xin Ke
In this work, the co-precipitation method was used to prepare Fe-doped BiOCl-modified materials for visible photocatalytic degradation of ofloxacin in water by taking advantage of the property that the acidic nature of FeCl 3 ·6H 2 O dissolved in water can improve the surface structure of the materials. In order to improve the problems of BiOCl’s poor absorption of visible light and high compounding rate of electron-hole pairs, the transition atom Fe is introduced to add impurity energy levels in BiOCl, which effectively reduces the bandgap width of the material and promotes the photogenerated electron migration of the material, and it is calculated that after modification, the band gap of the material can be reduced to 2.79 eV, which is a decrease of 0.32 eV compared to the original BiOCl (3.11 eV). Fe acts as an electron trap to capture electrons in electron-hole pairs and slows down their complexation with holes, effectively enhancing the stability of carrier separation in the material. Through free radical quenching experiments and ESR assays, it is understood that superoxide radicals are one of the free radicals needed in that act in the reaction process, indicating that the efficient electron capture enables the electrons to better react with adsorbed oxygen to generate superoxide radicals, which enhances the oxidizing ability of the system. Meanwhile, the degradation ability of modified materials on ofloxacin has been studied. Compared to the original BiOCl, under the condition of adding 50 mg/100 mL, the degradation ability of modified materials on ofloxacin has significantly improved. After 100 min of light exposure, the degradation efficiency of OFL·(10 mg/L) increased from 26.10% to 88.02%.
研究领域:
环境科学
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材料化学
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光催化
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水处理
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计算化学
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产品关联
DOI
高影响因子
ENVIRONMENTAL RESEARCH
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2022
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IF 8.431
Qi Han,Mingming Wang,Feiyun Sun,Boping Yu,Zijun Dong,Pu Li,Jingwen Luo,Mu Li,Xingliang Jin,Zhiguang Dai
Bisphenol A (BPA), one of the widely known endocrine-disrupting chemicals, can be effectively degraded by advanced oxidation processes in water because of the powerful reactive oxygen species . In this study, Fenton , UV/Fenton, and metal ion/peroxymonosulfate (PMS) processes were compared to investigate BPA degradation efficiency and pathways initiated by hydroxyl radicals and sulfate radicals. In contrast to the Fenton system, which only degraded 60% of BPA within 15 min, the UV/Fenton system could degrade greater than 80% of BPA, because more hydroxyl radicals (•OH) were generated under the reduction of Fe 3+ to Fe 2+ . The optimized parameters of the UV/Fenton system were as follows: 8 μmol/L of Fe 2+ , 80 μmol/L of H 2 O 2 , and a pH value of 3.0. As for the metal ion/PMS system, the BPA degradation efficiency was closely associated with the applied metal ions, and the order was as follows: Co 2+ /PMS (∼100%) > Fe 2+ /PMS (∼80%) > Cu 2+ /PMS (∼79%). The degradation pathways of BPA were theoretically interpreted through density functional theory prediction and degradation products during various processes. Two major initial reaction sites (4C and 6C) for •OH initiated using the UV/Fenton system and one initial reaction site (4C) for sulfate radicals (SO 4 •− ) using the metal ion/PMS system were recognized for BPA degradation processes. The degradation products by •OH showed a larger average molecular weight than those by SO 4 •− . These studies are instructive for the application of different advanced oxidation systems in the treatment process of BPA in wastewater.
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高影响因子
危险品化学品经营许可证（带存储）