Molecular Catalysis
·
2025
·
IF 4.9
Weitao Wang,Kang Wang,Huan Wang,Jiaqi Zhu,Zhen-Hong He,Zhao-Tie Liu
Selective oxidation of benzyl alcohol to benzaldehyde with molecular oxygen is a typical oxidation in synthetic chemistry. In present, Mn-Cu bimetal oxide spinel catalyst was prepared and characterized. The content of surface oxygen vacancies can be adjusted by the molar ratio of Cu to Mn during the preparation process and oxygen vacancies were found positively related to the activity of entitled reaction. The solvent effect on the reaction is investigated. The reaction conditions of the entitled reaction were optimized and the conversion of benzyl alcohol can reach 98.5 % with 100 % selectivity to benzaldehyde at 70°C for 8 h. The catalyst is stable and can be reused for 5 times without any significant decrease in its catalytic performance. In addition, the reaction was studied from the aspect of kinetic to reveal the reason of high selectivity.
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ChemSusChem
·
2025
·
IF 6.6
Ari F. Fischer,Teseer Bahry,Zhangyue Xie,Roberto Batista da Silva Junior,Kaicheng Qian,Renhong Li,James Kwan,François Jerome,Sabine Valange,Wen Liu,Prince N. Amaniampong,Tej S. Choksi
Graphical Ultrasound irradiation generates hydroxyl radicals from water to drive the fragmentation of aqueous aromatic compounds. These fragmentations form superoxide as a byproduct, which propagates further oxidation towards biodegradable endpoints through nucleophilic additions. Harnessing these superoxide reactions improves the efficiency of advanced oxidation processes for water treatment. The abatement of aromatic pollutants in water requires their oxidation to nontoxic products by resource-intensive reactions with hydroxyl radicals (⋅OH). We elucidate the mechanisms of ⋅OH-induced aromatic ring degradation by combining kinetic measurements, electron paramagnetic resonance spectroscopy, density functional theory calculations, and kinetic modelling. We demonstrate that benzyl alcohol (a model aromatic compound) is oxidized by ⋅OH radicals, generated by ultrasonic irradiation in an O 2 -rich environment, into aromatic compounds (benzaldehyde and phenol derivatives) and C1−C2 oxygenates (formic acid, glyoxal, and oxalic acid). Through pathways akin to atmospheric chemistry, these ⋅OH radicals de-aromatize and fragment benzyl alcohol, producing 5-hydroxy-4-oxo-pentenal and other dicarbonyl products. Unique to the aqueous phase, however, superoxide (⋅O 2 − ) forms by ⋅OOH deprotonation, which is generated by ultrasound (alongside ⋅OH) and as a byproduct of ⋅OH-benzyl alcohol reactions. ⋅O 2 − acts as a nucleophile, oxidizing 5-hydroxy-4-oxo-pentenal into oxalic acid and C 1 oxygenates via aldehyde and ketone intermediates. This process regenerates ⋅O 2 − and does not consume ⋅OH, thereby further degrading ring fragmentation products while preserving ⋅OH to activate the refractory aromatic ring of benzyl alcohol. These nucleophilic ⋅O 2 − reactions can therefore reduce the energy and number of chemical initiators needed to degrade aromatic compounds, thus advancing ⋅OH-based oxidation processes in water treatment.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Lihao Liu,Suiqin Li,Kai Li,Jiahui He,Yuhang Wang,Jieyu Wang,Ying Chen,Yinjie Xu,Mengxin Wang,Yongyong Cao,Xing Zhong,Jianguo Wang
The selective electrocatalytic oxidation of alcohols (EOA) to aldehydes under weak alkaline conditions offers sustainable synthetic routes. However, a deficiency in basicity inevitably leads to diminished electrocatalytic efficiency, and the dynamic reconstruction mechanism of the electrocatalyst remains insufficiently researched. Herein, the NiMoO x -COOH electrocatalyst/4-acetamido-TEMPO (ACT) synergistic system was employed for the efficient EOA under weak alkaline. In situ studies reveal electric double layer-driven metal/ligand co-leaching induces in situ dissolution-redeposition of metal, forming active Ni 2 (CO 3 )(OH) 2 . Experimental and Density functional theory (DFT) studies confirm a synergistic electrocatalytic mechanism between NiMoO x -COOH and ACT. The reconstructed Ni 2 (CO 3 )(OH) 2 promotes ACTH surface adsorption, thereby facilitating the turnover cycle of ACT. Therefore, outstanding EOA electrocatalytic performance has been achieved (500 mA/cm 2 , 96 % high yield, maintaining 30 cycles for benzyl alcohol oxidation, 15 substrate examples and 100 g scales synthesis). This work offers a promising approach to achieving high-performance EOA under weak alkaline.
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Catalysts
·
2025
·Vol. 15
·期 5
·442
·
IF 4
Zhe Wang,Xiaoliang Li
A series of Pd/g-C3N4catalysts were synthesized using different graphitic carbon nitride precursors, and were found to exhibit significant variations in catalytic performance for solvent-free selective catalytic oxidation of benzyl alcohol. Through comprehensive characterization (XRD, N2-BET, ICP-AES, TEM, and XPS), the experimental results found that the nitrogen chemical configuration and surface Pd2+concentration critically determined the catalytic efficiency. Among the various nitrogen species, N-(C)3-type nitrogen demonstrated the strongest influence on catalytic activity, which was positively correlated with its abundance in g-C3N4matrices. In particular, g-C3N4derived from dicyandiamide contained the highest N-(C)3type nitrogen content. When serving as Pd nanoparticle support, this material simultaneously achieved the best Pd2+surface concentration and catalytic performance compared to the other g-C3N4-supported catalysts.
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APPLIED CATALYSIS A-GENERAL
·
2025
·
IF 4.8
Huan Wang,Weitao Wang,Shuang Yue,Yang Liu,Jiaqi Zhu,Yiqian Yao,Zhen-Hong He
Developing highly efficient and stable non-precious metal oxide catalysts for selective oxidation reactions remains a key challenge in the field of heterogeneous catalysis. This study synthesized a series of manganese oxide catalysts with distinct structural characteristics by controlling the calcination temperature of the precursors. The results indicate that the calcination temperature significantly influences the catalyst's crystal structure, the distribution of manganese valence states, and the surface defect concentration. Among these, the manganese oxide calcined at 400 °C exhibits optimal catalytic performance due to its unique structural characteristics, which include residing at a phase transition boundary, a partial transition of Mn ion valence states, and the resulting abundance of surface oxygen vacancies. These structural features collectively regulate the catalyst's electronic structure, effectively promoting the adsorption, and activation of molecular oxygen. This generates superoxide radicals (·O 2 – ) as key reactive oxygen species, thereby driving an efficient oxidation reaction cycle. This work elucidates the structure–activity relationship of manganese oxides in oxidative catalysis, providing important insights for designing metal oxide catalysts with specific surface defects and electronic properties.
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Journal of Environmental Chemical Engineering
·
2025
·Vol. 14
·期 1
·120879
·
IF 7.2
Chengzhao Liu,Tao Liu,Suhua Liu,Xiufang Zhang,Guanlong Wang
Recently, it was reported photocatalytic H 2 O 2 generation performed in biphasic system could significantly increase the H 2 O 2 yield. Aiming to further improve the H 2 O 2 yield, hydrophobic heterojunction of α-S and vacancy-rich g-C 3 N 4 (CNN) was constructed. H 2 O 2 production performance tests demonstrated the 0.2α-S/CNN composite achieved H 2 O 2 yields 1.72 and 1.99 times higher than pristine CNN and α-S, respectively. N-(C) 3 bonded nitrogen(N 3 C ) promoted oxygen activation, and heterojunction facilitated the separation of photogenerated holes and electrons. These contributed more effective photocatalytic synthesis of H 2 O 2 . The optimal 0.2α-S/CNN achieved a production rate of 2218 μmol g −1 , with an impressive apparent quantum yield (AQE) of 6.92 % under 455 nm monochromatic light, outperforming the state-of-the-art catalysts. The proposed mechanism suggested that photogenerated electrons migrated from α-S to CNN, reducing adsorbed O 2 to form •O 2 − radicals. These radicals subsequently reacted with water in the aqueous phase to generate H 2 O 2 via 2e − ORR. Due to the strong hydrophobicity of the catalyst, most •O 2 − radicals were generated in benzyl alcohol (BA) phase, while H 2 O 2 predominantly formed in the aqueous phase. This spatial separation delayed H 2 O 2 decomposition, facilitating its accumulation and enhancing overall yield.
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JOURNAL OF CATALYSIS
·
2025
·
IF 6.5
Xiangyu Jia,Xiaoming Li,Shiying Li,Kai Yuan,Xiaoqing Gao,Shanhui Zhu,Mei Dong,Weibin Fan
Metals embedded nitrogen-doped carbon (M/NC) materials have garnered substantial attention due to the catalytic active centers provided by their transition metals. Here, the ZIF-67 derived Co/NC hollow structure catalyst (Co/NHC-4) exhibited remarkable performance in the hydrogenation of biomass-based 5-hydroxymethylfurfural (HMF) to valuable 2,5-dihydroxymethylfuran (DHMF). Under mild conditions of 60 °C and 2 MPa H 2 , the conversion of HMF reached nearly 100 %, with DHMF selectivity >99 %. Through the integration of advanced characterization techniques, such as TEM, XPS, XAFS, Raman spectroscopy, vapor adsorption curve, H 2 -TPD and in situ FTIR spectroscopy, it was demonstrated that the superior hydrogenation performance of hollow-structured catalysts primarily stems from unique morphology. Specifically, the hollow morphology facilitates the adsorption and diffusion of HMF on Co surface, which substantially enhances the hydrogenation efficiency. DFT calculation reveals the preferential parallel adsorption geometry of HMF and the energetically favorable hydrogenation pathway.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Fuxin Wang,Guojun Lv,Jiande Hu,Zixiang Li,Xupeng Yang,Shengnan Xu
Heterogenization of Co-based catalyst can effectively solve the catalyst recovery problem encountered by homogenous catalyst Co(OAc) 2 , but there may generate an obvious performance decrease for the heterogenized cobalt site ascribed to the increased mass transfer resistance. Hence, how to alleviate or eliminate the performance decline for Co-based heterogeneous catalyst is an intriguing scientific question. In this study, we reported the application of crystal engineering strategy on Co 3 O 4 to bridge the performance gap between homogeneous catalyst and heterogeneous catalyst in the selective oxidation of toluene into benzaldehyde. Four distinct spinel Co 3 O 4 catalysts, predominantly exposing the {220}, {222}, {440}, and {311} crystal facets respectively, were prepared and utilized as heterogeneous catalysts. The Co 3 O 4 -P sample predominantly exposing the {220} facets exhibited the optimal catalytic activity for toluene oxidation, achieving a toluene conversion of 56.1 % and a benzaldehyde selectivity of 67.6 %, which was significantly superior to that of homogenous catalyst Co(OAc) 2 . The enhanced performance of this material is primarily attributed to the abundant reversible Co 2+ /Co 3+ redox couples on its surface, which maintains sufficient Co 2+ active sites throughout the catalytic process and facilitates toluene oxidation reactions. In addition, Co 3 O 4 -P also exhibited the maximum specific surface area, the highest Co 2+ /Co 3+ ratio, and the greatest oxygen vacancy density, which together give rise to its best catalytic performance. Density functional theory (DFT) calculations further corroborated these findings. According to quenching experiments and in-situ FTIR characterizations, the possible selective toluene oxidation mechanism over Co 3 O 4 -P catalyst was proposed. Moreover, the recycled Co 3 O 4 -P sample could be reused for more than five consecutive reactions, demonstrating its eminent re-usability.
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JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Wenping Shi,Xiao Yang,Haitao Li,Chunxia Zhao,Jing Zhou,Yuli Xiong,Wen Chen
Covalent organic frameworks (COFs) with tunable redox activity have emerged as promising electrochromic (EC) materials owing to their structural diversity, tunable bandgaps, interlayer π-π electron delocalization and ordered porosity. However, most imine-linked COF-based EC materials suffer from weak interlayer interactions and inefficient charge transport, leading to poor long-term cycling stability. Herein, we present an efficient linkage conversion strategy, where an imine-linked COF (Im-COF) is oxidized to an amide-linked COF (Am-COF), resulting in a significant improvement in the long-term EC cycling stability of COF films. The Am-COF shows 94.6 % retention after 550 cycles, compared to 81.4 % retention after 480 cycles for Im-COF. Such performance disparity is attributed to differences in interlayer interactions, charge separation, and charge transfer efficiency, as confirmed by characterizations and theoretical calculations. Additionally, at 1050 nm, the Am-COF film exhibits a high optical contrast of 87 %, a rapid response time of 0.6/1.1 s (coloration/bleaching), and a high coloration efficiency of 275 cm 2 C −1 . This work highlights linkage engineering as an effective approach to optimize the charge transfer and redox reversibility of COF-based EC materials, providing a viable pathway for their practical application in advanced optoelectronic devices.
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ACS Sensors
·
2025
·
IF 9.1
Changle Pei,Muhammad Hamza Nadeem,Nan Li,Jun Fu,Nan Xu,You Wang,Adrian Carl Stevenson,Guang Li,Ruifen Hu
The complexity of in situ volatile organic compounds (VOCs) detection demands high selectivity and anti-interference capability of electronic noses (E-noses). Multivariant virtual sensor array (VSA) is a new generation of E-noses under research to overcome the insufficient VOCs selectivity limitation of existing electronic noses and alleviate the issue of sensor drifts. In this paper, a frequency-amplitude dual-parameter modulation strategy is presented on a wireless electrodeless quartz crystal microbalance with dissipation (WE-QCM-D) to realize the recognition and analysis of VOC mixtures and complex real-world analytes with a single multivariant VSA E-nose, by probing the gas dynamic sorption in a sensitive film at various scales of oscillating shear displacements and obtaining multiple partially independent responses to VOCs. Ten VOC analytes from alcohols, esters, and aromatic hydrocarbons were classified with accuracies of above 95% for both interclass and intraclass discriminations. Additionally, a discriminating accuracy of 95% has been achieved on VOC mixtures, and their component concentrations were predicted with coefficients of determination above 0.9. For practical testing, the system was exposed to the headspace VOCs of banana, pineapple, and mango under different concentrations. It recognized different fruits and identified the ripen state of bananas based on the detection of their volatiles. The dual-parameter modulated WE-QCM-D paves a promising multivariant way to realize online real-time VOCs monitoring with high performance on selectivity and quantitative analysis.
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AICHE JOURNAL
·
2025
·
IF 4
Qi Liu,Yan Ouyang,Tong Luo,Qinlan Luo,Min Xiao,Hongxia Gao,Zhiwu Liang
Blending is a common method to improve the performance of amine solution for CO 2 capture. While the amine will degrade at elevated temperatures or so-called thermal degradation, the mixing of multiple amines could change the thermal degradation behavior and it is critical to reveal them before implementing the CO 2 capture at large scale. Herein, the thermal degradation performance of blended amines was studied via experimental and computational methods. In comparison with single amine solution, the effect of an additional tertiary amine N,N -dimethylethanolamine (DMEA) was analyzed. The thermal degradation experiments were carried out at multiple temperatures. The temperature threshold was identified for the blended solution after which the degradation rate increases dramatically. Based on the obtained degradation products, the degradation mechanism of the blended amine is proposed. The energy barrier of key reactions in thermal degradation was obtained and the interaction of primary amine and tertiary amine is clarified.
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JOURNAL OF HAZARDOUS MATERIALS
·
2025
·
IF 11.3
Yidong Zhou,Zhijian Ke,Jiazhuo Zhang,Wenbin Chang,Yarong Cui,Yimiao Chen,Yirui Huang,Chunli Xia,Wenjia Zhong,Zifa Deng,Dayong Jin
Microorganisms are constantly evolving to resist the toxicity of artificial antibiotics and preservatives released into the environment. Parabens, a group of alkyl and aryl esters of p -hydroxybenzoate, are a class of widely used antimicrobial preservatives, particularly effective against Gram-positive bacteria and fungi. Previous studies have reported the degradation of parabens by numerous Gram-negative strains and activated sludge, with degradation processes often involving transesterification. However, the physiological significance of transesterification has received little attention. Here, a Gram-positive bacterium, Microbacterium sp. S1037 was isolated and characterized for its ability to degrade eight parabens and completely mineralize them through p -hydroxybenzoate and protocatechuate ( β -ketoadipate pathway). Moreover, strain S1037 also possesses the ability of paraben-transesterification. Alcohols compete with water molecules for the active center of enzymes, accelerating the transesterification of parabens and inhibiting hydrolysis. Considering that the fate of the transesterification product is still hydrolysis, we speculated and proved that such a “superfluous” mechanism is a detoxification strategy, and could be used in the bioremediation of parabens in wastewater. Microbial transesterification of parabens has been reported worldwide, and we speculated that it might be a common detoxification choice in the evolution of microorganisms worldwide.
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