APPLIED CATALYSIS B-ENVIRONMENTAL
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2019
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IF 14.229
Junhua Zou,Zhitong Wang,Wei Guo,Binbin Guo,Yan Yu,Ling Wu
ZnTi-LDH nanosheets have been synthesized as photocatalysts for selective oxidation of benzyl alcohol (BA) to benzaldehyde (BAD) under visible light irradiation. Based on UV–vis DRS, in-situ FTIR and XPS results, it was revealed that BA would be efficiently chemisorbed and activated on ZnTi-LDH forming the surface coordination species, which contributed to harvesting visible light and induced the photocatalytic reaction. The ESR spectra suggested that oxygen vacancies would be produced in ZnTi-LDHs after the adsorption of BA molecules. More exposed surface OH groups would induce more oxygen vacancies, which would serve as the centers for capturing photoelectrons from the photoexcited surface coordination species and act as active sites for enhanced O 2 adsorption and activation, resulting outstanding photocatalytic activity. Finally, a possible mechanism was proposed to illustrate the photocatalytic process which mediated by surface coordination species formed by the interaction between ZnTi-LDH and BA.
研究领域:
材料科学
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化学工程
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DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
·Vol. 48
·期 36
·15839-15845
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IF 2.7
Tao Wang,Mengyao Shi,Changyan Guo,Jide Wang
ZIF-67 has garnered much attention in the field of photocatalytic water splitting due to the advantages of MOFs and zeolite sieves. However, post-modification and composite strategies have emerged as effective approaches to enhance its photocatalytic performance, particularly in enabling bi-functionality for oxidation-coupled reduction reactions. In this study, 2-mercaptobenzimidazole (MBI) modified ZIF-67 and cadmium sulfide (CdS) composites were prepared to investigate their application in photocatalytic oxidation-coupled hydrogen evolution reactions. The results demonstrated an enhancement in hydrogen production performance over CdS@ZIF-67-MBI, with an increase from 2.39 mmol g−1 h−1 to 4.49 mmol g−1 h−1 upon the introduction of MBI. Moreover, the conversion efficiency of benzyl alcohol reached an improved value of 58.5%. The study findings revealed that the heterogeneous coupling between ZIF-67 and CdS, along with the effective charge transfer facilitated by the anion S, played a decisive role in promoting charge–hole separation of composite materials and improving carrier transport efficiency. This demonstrates the viability of utilizing ZIF-67 in a bifunctional photocatalytic reaction system, thereby paving the way for broader applications of ZIF-67.
研究领域:
材料科学
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化学工程
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环境科学
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DOI
高影响因子
Molecular Catalysis
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2025
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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.
研究领域:
催化化学
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材料科学
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高影响因子
Molecular Catalysis
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2020
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IF 3.687
Qian Wang,Meiling Ge,Yuheng Dou,Fu Yang,Junkai Wang,Yuyang Shao,Agen Huang
Polymer supports play an important role in noble metal loaded catalysts. In this study, palladium clusters stabilized by several polyamides have been widely studied in the oxidation of benzyl alcohol under airflow. The different kinds of polyamides (PADs) were synthesized with aromatic diamines and trimesoyl chloride by mechanical grinding method and solvent-heat method. Polyamide support was synthesized through mechanical grinding method. And the laminar structure and abundant amide bonds of polyamide can help obtain ultrafine Pd clusters with a mean particle size of 1.76 nm. The Pd 0.5 @PAD-2-M effectively catalyzed benzyl alcohol into benzaldehyde with a conversion of 96.1 % and turnover number (TON) of 1441 under 90 °C in water which was 2.5 times higher than the commercial Pd/C catalyst. High TON value of 6505 was also achieved in solvent-free system. This work reveals the advantages of laminar structure of polyamide in dispersing Pd clusters and promoting benzyl alcohol conversion. Besides, the carrier properties of amphipathy and substrate adsorption were also investigated to illustrate the significance of interfacial effect for laminar catalyst in heterogeneous catalysis.
研究领域:
材料科学
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催化化学
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DOI
高影响因子
Reaction Kinetics Mechanisms and Catalysis
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2013
·Vol. 109
·期 2
·551-562
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IF 1.104
Cui Wenjing,Zhu Huaiyong,Jia Meilin,Ao Wulan,Zhang Yulin,Zhaorigetu Bao
Imines were synthesized from benzyl alcohol and amines by using catalysts of gold nanoparticles supported on ZrO 2 (Au/ZrO 2 ). The effects of reaction time, temperature, gold loadings and base were investigated. High yields were achieved under moderate conditions (60 °C) in the presence of KOCH 3 . For instance, the yield of N -benzylidenebenzylamine produced from benzyl alcohol and benzylamine on 3 wt% Au/ZrO 2 is 87 %. The synthesis of imine involves two reaction steps: selective oxidation of benzyl alcohol to benzaldehyde and the coupling reaction of amines with benzaldehyde. In the first step, the base promotes the selective oxidation. The reactions of benzyl alcohol with three different amines, aniline, n -butylamine and benzylamine, were conducted to produce corresponding imines. The results show that the amine with stronger nucleophilicity has better ability to react with benzaldehyde in the second step, resulting in higher yield of the corresponding imine. We proposed a tentative mechanism for the synthesis process.
研究领域:
催化化学
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有机合成
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高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2022
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IF 4.326
Wen-Shuang Zhu,Dai Sun,Ling-Li Yu,Shao-Qi Zhi,Yu-Dong Shan,Yi-Fang Lu,Hai-Tao Ren,Song-Hai Wu,Yong Liu,Xu Han
In this study, Bi2.15WO6 with different morphologies was successfully synthesized and used for the selective photooxidation of benzyl alcohol to benzaldehyde in aqueous solutions. High conversion (85%) and selectivity (85%) can be simultaneously achieved under alkaline conditions by adding ethylenediamine to protect the produced benzaldehyde from overoxidation. In the oxidation process, ≡Bi–OO• and ≡Bi–OOH on Bi2.15WO6, instead of OH• and O2•–, are the primary oxidizing species to sequentially abstract two H (H+ + e–) from benzyl alcohol, accompanied by the formation of H2O2. Meanwhile, h+ and OH– also minorly contribute to the selective oxidation of benzyl alcohol via the H-abstraction pathway. This study enriches our understanding of the oxidizing species involved in the selective photooxidation of benzyl alcohol to benzaldehyde.
研究领域:
材料科学
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催化化学
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环境科学
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2024
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IF 3.8
Da Sheng,Qing He,Zhong-Hua Cao,Lun-Bo Chen,Song-Hai Wu,Yong Liu,Hai-Tao Ren,Xu Han
Although photooxidation of benzyl alcohol to benzaldehyde in aqueous solution is an important chemical process, its selectivity cannot be readily controlled due to the overoxidation of benzaldehyde. In this study, a series of Bi–Mo/CN photocatalysts are synthesized, and their reactivity in photooxidation of benzyl alcohol under visible light is compared. Bi–Mo/CN-2 exhibits high photocatalytic reactivity in the conversion of benzyl alcohol (51%) with a high selectivity toward benzaldehyde of 99.9%. In this process, the formed ≡Bi–OO• and ≡Bi–OOH selectively oxidize benzyl alcohol to benzaldehyde via the H-abstraction pathway after O2 is photoreduced on Bi–Mo/CN, accompanied by the formation of H2O2. Meanwhile, the doped Mo utilizes the produced H2O2 or ≡Bi–OOH to produce ≡Mo–O2 peroxo, which not only contributes to the selective oxidation of benzyl alcohol to benzaldehyde but also effectively prevents overoxidation of benzaldehyde. This work provides new insight into designing novel photocatalysts for selective oxidation of organic substrates.
研究领域:
化学
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材料科学
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高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2020
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IF 16.683
Qiong Lin,Yue-Hua Li,Ming-Yu Qi,Jing-Yu Li,Zi-Rong Tang,Masakazu Anpo,Yoichi M.A. Yamada,Yi-Jun Xu
The photocatalytic coupling reaction can be conducted in one pot to realize the simultaneous utilization of electrons and holes, thereby obtaining value-added fine chemicals and fuels. Herein, we report a binary nickel modified ZnIn 2 S 4 (Ni:ZIS) for highly efficient photocatalytic selective oxidation of benzyl alcohol (BA) to benzaldehyde (BAD) integrated with hydrogen (H 2 ) evolution, in which Ni can promote photogenerated charge transfer for enhancing photoactivity. Particularly, the products of converting BA to aromatic compounds over blank ZnIn 2 S 4 (ZIS) and Ni:ZIS show a marked difference under the same reaction conditions. Hydrobenzoin (HB) is the primary product over blank ZIS. After the introduction of Ni, the formation of HB is dramatically suppressed, resulting in higher selectivity of BAD, because the introduction of Ni facilitates the α-H abstraction. In addition, an analogous phenomenon has been observed on Ni-based compounds modified ZIS, such as Ni x P and NiS. It is hoped that this work would provide a feasible paradigm for modifying the surface of photocatalysts to tune the selectivity of product-oriented alcohols oxidation coupled with H 2 evolution in water.
研究领域:
化学
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材料科学
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高影响因子
ChemSusChem
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2025
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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.
研究领域:
环境科学
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化学工程
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水处理技术
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DOI
PubMed
高影响因子
NEW JOURNAL OF CHEMISTRY
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2024
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IF 2.7
Yufen Wang,Yantao Wang,Yongqing Ma,Asma Mohmmad Elsharif,Chen Zhang,Weiran Yang,Christophe Len
A new transition-metal-free catalytic system which uses sodium iodide as the catalyst with formic acid as the hydrogen donor in a biphasic medium was reported for the reduction of the hydroxyl group and various unsaturated groups such as CC, CC, CN and CO. Using the same catalytic system, reductive N-formylation of nitroarenes with formic acid was explored to produce the corresponding amide in high selectivity. Moreover, the catalyst stability was evaluated and reaction mechanisms were studied and proposed for the three model reactions.
研究领域:
有机化学
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催化化学
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高影响因子
JOURNAL OF CATALYSIS
·
2021
·
IF 7.92
Shuhui Yang,Xi Ke,Qizan Chen,Runda Huang,Weizhe Wang,Kunqiang Wang,Kaixiang Shu,Chen Tu,Zhaoqiang Zheng,Dongxiang Luo,Haowei Huang,Menglong Zhang
Constructing mixed dimensional materials have been regarded as an outstanding approach to maximum the advantages from materials of different dimensions. In this work, we prepared a mixed dimensional photocatalyst based on Formamidinium lead bromide (FAPbBr 3 ) perovskite and 2D materials (2DMs). The aim of this work is to utilize distributions of the active sites in 2DMs, through growing FAPbBr 3 on the different position of 2DMs, the concentration of photogenerated charges is manipulated, thus conducting different reactions. A pre-treatment using HBr to increase the unsaturated bonds in MoS 2 presents significant influence on the FAPbBr 3 growth and its photocatalytic product. The scanning electron microscopy (SEM), transmission electron microscopy (TEM) and energy dispersive spectroscopy (EDS) confirm that the perovskite nanoparticles were well loaded on the 2D materials. The photocatalytic process and the heterojunction arrangement are demonstrated by X-ray photoelectron spectroscopy (XPS), time-resolved photoluminescence (TRPL), electron paramagnetic resonance (EPR) and surface photovoltage microscopy (SPVM). By adjusting the weight ratios and growth of FAPbBr 3 on the top of 2DMs, the optimized composite photocatalyst (with 30 wt% of FAPbBr 3 ) exhibits remarkable photoactivity for oxidation of benzyl alcohol into benzaldehyde (30 wt% FAPbBr 3 @WS 2 performed 75.9% conversion in 4 h, approximately 9-fold than the pure 2DMs). Meanwhile, by growing FAPbBr 3 on the edge of 2DMs, benzoic acid is obtained as the product. Although longer reaction time is needed, the photocatalyst performs outstanding activity (30 wt% FAPbBr 3 @MoS 2 reached 84.5% conversion in 5 h).
研究领域:
材料科学
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催化化学
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DOI
高影响因子
ENERGY & FUELS
·
2025
·
IF 5.3
Shengqi Lin,Hailong Huang,Jieyi Fan,Chunhe Li,Kuankuan Ren,Weidong Dou
Photocatalytic conversion of biomass-derived compounds into value-added chemicals coupled with hydrogen production presents a promising strategy to address energy and environmental challenges. In this study, a series of NiB/ZnIn2S4 nanocomposites were synthesized via a facile two-step hydrothermal approach. The designed system enables the simultaneous utilization of photoexcited electrons and holes in redox reactions, achieving efficient benzyl alcohol oxidation and hydrogen evolution. The optimized 3%-NiB/ZnIn2S4 nanocomposite demonstrates exceptional photocatalytic performance, exhibiting a hydrogen evolution rate of 7223.2 μmol g–1 h–1 in 1.50 vol % benzyl alcohol solution, representing 2889.3-fold and 4.8-fold enhancements over pristine NiB and ZnIn2S4, respectively. Furthermore, the system maintains robust stability over 14 photocatalytic cycles, achieving 71.7% conversion efficiency and 86.8% selectivity toward benzaldehyde production. The enhanced performance originates from the formation of Z-scheme heterojunctions between NiB and ZnIn2S4, which facilitates efficient charge carrier separation and transport, as evidenced by improved photocurrent response and reduced electrochemical impedance. This work provides valuable insights into the photocatalytic valorization of biomass-derived platform chemicals under visible light irradiation.
研究领域:
材料科学
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环境科学
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化学工程
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DOI
高影响因子
危险品化学品经营许可证（带存储）