APPLIED ORGANOMETALLIC CHEMISTRY
·
2020
·Vol. 35
·期 1
·e6073
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IF 3.14
Jianyu Dong,Xiuling Chen,Fangyan Ji,Lixin Liu,Lebin Su,Min Mo,Jian-Sheng Tang,Yongbo Zhou
A simple and direct aerobic oxidative esterification reaction of arylacetonitriles with alcohols/phenols is achieved in the presence of a copper salt and molecular oxygen, which produces a broad range of aryl carboxylic acid esters in good to high yields. Copper salt plays multiple roles in the transformation, which allows the oxygenation of C H bond, cleavage of inert C C bond, and formation of C O bond in one pot without the assistance of any of the acids, bases, ligands, and so on. The reaction provides a simple, direct, and efficient protocol towards functionalized esters, especially aryl benzoates, from readily available starting materials.
研究领域:
有机化学
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合成化学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF MOLECULAR SCIENCES
·
2021
·Vol. 22
·期 16
·8668
·
IF 5.924
Jie Li,Shiyi Wang,Huayin Li,Yuan Tan,Yunjie Ding
The synthesis of ester compounds is one of the most important chemical processes. In this work, Zn-Mg-Al mixed oxides with different Zn2+/Mg2+molar ratios were prepared via co-precipitation method and supported gold nanoclusters to study the direct oxidative esterification of aldehyde and alcohol in the presence of molecular oxygen. Various characterization techniques such as N2-physical adsorption, X-ray diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectroscopy (XPS) and CO2temperature programmed desorption (TPD) were utilized to analyze the structural and electronic properties. Based on the results, the presence of small amounts of Zn2+ions (~5 wt.%) provoked a remarkable modification of the binary Mg-Al system, which enhanced the interaction between gold with the support and reduced the particle size of gold. For oxidative esterification reaction, the Au25/Zn0.05MgAl-400 catalyst showed the best performance, with the highest turnover frequency (TOF) of 1933 h−1. The active center was believed to be located at the interface between metallic gold with the support, where basic sites contribute a lot to transformation of the substrate.Keywords:gold catalyst;cluster;hydrotalcite;oxidative esterification;methyl isobutyrate
研究领域:
化学工程
·
催化材料
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2021
·Vol. 56
·期 12
·7308-7320
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IF 4.22
Hu Yongke,Xia Jiawei,Li Jin,Li Huaju,Li Yanxing,Li Shaozhong,Duanmu Chuansong,Li Bindong,Wang Xin
A highly efficient nitrogen-doped carbon black (NCB)-supported PdBi alloy nanocatalyst has been fabricated via a facile coreduction wet chemical approach. The optimal PdBi/NCB shows outstanding catalytic performance with broad substrate scope, good functional group tolerance towards direct oxidative esterification of alcohols under mild conditions in a heterogeneous catalytic system with air as the sole oxidant. A variety of benzylic and allylic alcohols were smoothly reacted with methanol and even with long-chain aliphatic alcohols, providing desired esters in good to excellent yields. Moreover, the as-prepared catalyst is easily recycled and can be reused at least five times without a significant loss of catalytic activity. Superior catalytic activity is mainly attributable to the unique structure of the catalyst, including synergetic electronic effect between Pd and Bi, as well as modulated surface character by acidification and N doping for better active components’ anchoring and dispersion, as well as reactants’ adsorption. This study provides a facial, practical, eco-friendly and efficient catalytic system for oxidative esterification of alcohols and shows promising prospect in industrial production.
研究领域:
化学
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材料科学
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催化
✓ 已验证
DOI
高影响因子
Sustainable Energy & Fuels
·
2024
·
IF 5
Xueyang Ren,Jie Zheng,Jinxian Zhao,Jun Ren,Yanhong Quan
The one-step oxidative esterification of ethylene glycol (EG) is an effective and promising route for methyl glycolate (MG) synthesis, during which the development of efficient catalysts is critically crucial. Herein, Au/ZnO catalysts were prepared using impregnation (IM), colloidal-deposition (CD), deposition-precipitation (DP) and co-precipitation (CP) methods, respectively. The catalytic activities results revealed that the Au/ZnO-DP catalyst was far superior than the other three catalysts, achieving an EG conversion rate of 90.4% and a selectivity towards MG of 93.8%. Catalysts were systematically characterized by N2 adsorption-desorption, XRD, TEM, XPS, H2-TPR, EPR, O2-TPD and CO2-TPD. The results showed that the large number of Au-ZnO interfaces facilitated the adsorption and activation of O2. Moreover, it is found that the basic sites promoted the cleavage of O-H bonds in the EG molecules, and the acidic sites are responsible for the selectivity of MG. This work offers a simple strategy for design of gold catalysts in EG oxidative esterification.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Industrial Chemistry & Materials
·
2022
·Vol. 1
·期 1
·106-116
·
IF 0
Wen Yao,Chenghong Hu,Yajie Zhang,Hao Li,Fengliang Wang,Kui Shen,Liyu Chen,Yingwei Li
Nitrogen-rich zeolitic imidazolate frameworks (ZIFs) are ideal precursors for the synthesis of metal single atoms anchored on N-doped carbon. However, the microporous structures of conventional ZIFs lead to low mass transfer efficiency and low metal utilization of their derivatives. Here, we construct a composite of Co single atoms anchored on nitrogen-doped carbon with a three-dimensional ordered macroporous structure (Co-SA/3DOM-NC) by two-step pyrolysis of ordered macro/microporous ZnCo-ZIF. Co-SA/3DOM-NC shows high activity in the oxidative esterification of furfural, achieving a 99% yield of methyl 2-furoate under mild reaction conditions, which is significantly superior to the microporous and the Co-nanoparticle counterparts. The high activity of Co-SA/3DOM-NC should be attributed to the CoN4 centers with high intrinsic activity and the ordered macroporous structure, promoting the mass transfer of reactants and accessibility of active sites.
Keywords: Heterogeneous catalysis; Hierarchical pores; Ordered macropore; Oxidative esterification reaction; Single-atom catalysts.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
Reaction Kinetics Mechanisms and Catalysis
·
2013
·Vol. 110
·期 2
·437-448
·
IF 1.104
Cui Wenjing,Jia Meilin,Ao Wulan,Zhaorigetu Bao
Nano-gold catalysts were prepared by the liquid reduction method and employed in the oxidative esterification of alcohols under ambient conditions. The effects of the supports and gold loading on the catalytic behavior were investigated. The catalysts were characterized by transmission electron microspectroscopy, X-ray diffraction, X-ray photoelectron microspectroscopy and atomic absorption spectrometry. The results indicated that nano-scale metallic state gold was highly dispersed on the support. 95 % methyl benzoate yield was obtained over 3 wt% Au/ZrO 2 catalyst at 30 °C under air atmosphere. Under optimized reaction conditions, benzyl alcohols with electron-withdrawing groups could give high selectivity to the corresponding methyl ester at moderate conversion of alcohols. However, when a benzyl alcohol with electron-donating group was used, high conversion of alcohol but low selectivity of the corresponding methyl ester was obtained. Low yields were obtained with aliphatic alcohols as substrates even at high temperature. The kinetic analysis of the oxidation from benzyl alcohol to benzaldehyde and from benzaldehyde to methyl benzoate was also described. The facile and simple procedure was a great option for direct synthesis of methyl esters from alcohols.
研究领域:
催化化学
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材料科学
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有机合成
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
·
2019
·
IF 3.674
Cuncun Zuo,Yun Tian,Yanxia Zheng,Lei Wang,Zhongjun Fu,Tiantian Jiao,Ming Wang,Haofei Huang,Yuchao Li
Series of gold and ceria supported γ-Al 2 O 3 catalysts were developed for the oxidative esterification of methacrolein with methanol. All the catalysts were prepared through one step deposition-precipitation method, and K 2 CO 3 and urea were used as precipitant, respectively. Au, CeO 2 and γ-Al 2 O 3 could self-assemble unique particle morphology during co-precipitation process and form semi-core shell or core shell structure after calcination . The relationship between catalytic reactivity and structural characteristics were analyzed by SEM, TEM, EDS, BET, XRD, XPS, etc. Among Au-CeO 2 /γ-Al 2 O 3 (K 2 CO 3 ), Au-Ce/γ-Al 2 O 3 (Urea) and Au/γ-Al 2 O 3 (Urea) catalysts with different active components and precipitant, the last two exhibited higher catalytic activity. Moreover, the Ce-doped catalysts shown higher stability than just Au supported on pure alumina. The active stability of the optimum Au-Ce/γ-Al 2 O 3 catalyst was evaluated with seven-time cyclic reactions exhibiting high stability and activity with the yield of MMA above 90%.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2023
·
IF 2.8
Chen Yao,Li Shuyue,Li Yuchao,Zheng Yanxia,Zuo Cuncun,Ge Tingting,Xu Rui,Huang Haofei,An Jiutao
Nano-Au particles are commonly used as an active component in oxidation esterification reactions. To inhibit the agglomeration of nano-Au particles, a series of highly stable Au@CeO 2 /MnO x core–shell structured catalysts were synthesized using inverse microemulsion technology for the oxidative esterification to prepare methyl methacrylate (MMA). The core–shell structured catalysts were prepared by using two different surfactants (CTAB and CO-520) and adjusting the molar ratio of water to oil (ω). XRD, Raman, N 2 adsorption, ICP−MS, TEM, UV–vis, FT-IR, XPS, and H 2 -TPR were applied to characterize the samples. The nano-Au particles were encapsulated by CeO 2 , forming a core–shell structure confirmed with TEM. The Au@CeO 2 /MnO x -C-ω = 10 catalyst prepared with CTAB as the surfactant has the best activity. The Au@CeO 2 /MnO x -C-ω = 10 catalyst has the highest hydrogen consumption and Ce 3+ content, indicating that the catalyst has the strongest interaction among Ce, Au, and Mn and more active oxygen. Active oxygen is beneficial to methanol activation and hemiacetal dehydrogenation, accelerating the formation of esters. The active oxygen content, Ce 3+ content, and H 2 consumption were correlated with the catalytic performance positively. After the catalyst was reused 10 times, the activity remained unchanged and the Au nanoparticles did not agglomerate due to the core–shell structure. Graphical Abstract
研究领域:
催化化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2019
·
IF 4.914
Yan Wan,Congcong Zheng,Xianchi Lei,Mengqi Zhuang,Jinhan Lin,Wenda Hu,Jingdong Lin,Shaolong Wan,Yong Wang
ABSTRACT Acetol is a major light oxygenate and readily produced from staged or fast pyrolysis of lignocellulose biomass. Herein we report that acetol can be selectively converted to methyl pyruvate, an important fine chemical, through oxidative esterification over Au-based catalysts. Detailed experimental studies showed that Au on amphoteric supports with appropriate strength and balanced ratio of acid and base sites can facilitate the desired oxidative-esterification pathway without accelerating undesired aldol-condensation or Cannizzaro reactions. In particular, hydroxyapatite (with a Ca/P ratio of 1.62) supported Au achieved 87% selectivity to methyl pyruvate at an acetol conversion of 62%.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
Catalysts
·
2021
·Vol. 11
·期 2
·162
·
IF 4.146
Huayin Li,Yuan Tan,Xingkun Chen,Wenshao Yang,Chuanqi Huang,Jie Li,Yunjie Ding
Methyl methacrylate (MMA) is an important monomer in fine chemicals. The synthesis of MMA by one-step oxidative esterification from methacrolein with methanol over a heterogeneous catalyst with high activity, selectivity and stability is highly desirable. Herein, Zn-Al-hydrotalcites (HTs)-supported atomically precise Au25nanoclusters with different molar ratios of Zn2+/Al3+were prepared and used as the precursors for this reaction. They exhibited good performances in comparison with the gold catalysts prepared by the deposition precipitation method. The structural and electronic properties were evaluated by various characterization technologies, including X-ray diffraction (XRD), high-resolution transmission electron microscopy (HRTEM), in situ diffuse reflectance infrared Fourier-transform spectroscopy (DRIFTS) of CO adsorption, X-ray photoelectron spectroscopy (XPS), and CO2temperature-programmed desorption (TPD). The combined characterization results suggested that the adsorption property of gold and the basicity of the catalyst contributes to their high activities. Substrates extended experiments and stability tests implied the potential application of Zn-Al-mixed oxides supported gold catalysts, which paves a new way for supported gold catalyst in the one-step oxidation esterification reaction.Keywords:gold cluster;hydrotalcite;methacrolein;methyl methacrylate;oxidative esterification
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
CATALYSIS TODAY
·
2022
·
IF 6.562
Linhao Yu,Hong Chen,Yingying Li,Zhe Wen,Yongdan Li
The metallic cobalt supported on nitrogen dopped carbon material was employed as an efficient catalyst in the oxidative esterification of 5-hydroxymethylfurfural (HMF) to furan-2,5-dimethylcarboxylate (FDMC). The carbonization temperature has a significant effect on the morphology and structure of Co/N-C samples. The Co/N-C calcined at 900 °C exhibits the best catalytic performance and a 73.8% FDMC yield at 91.7% HMF conversion is measured at 130 °C for 20 h with K 2 CO 3 under 1 MPa O 2 . The catalytic activity of Co/N-C was benefited by the synergistic effect between the metallic cobalt and nitrogen-doped carbon material. The reaction mechanism of FDMC formation was proposed.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2025
·
IF 4.3
Yaping Liu,Chao Pan,Xianjie Li,Hailin Zhang,Zhijie Shang,Hongbing Song
Oxidation, a pivotal process in organic synthesis, is essential for the conversion of various biomass derivatives, including 5-hydroxymethylfurfural (HMF), into valuable chemicals. This research employs poly(ionic liquid)s (PILs) as supports to fabricate Au/PILs catalysts, which are subsequently utilized in the oxidative esterification of HMF to produce dimethyl 2,5-furandicarboxylate (FDMC). The modification of PILs demonstrates that catalyst’s performance is optimized when the PILs anion (IL: EGDMA = 1: 4) is [Tf 2 N - ]. The presence of the [Tf 2 N - ] group is essential for charge transfer between the carrier and the active metal Au, thereby enhancing the catalytic reaction. Thermogravimetric analysis (TG) reveals the exceptional thermal stability of the 2 % Au/PILs-Tf 2 N-14 catalyst. The efficient conversion of HMF to FDMC is achieved using the 2 % Au/PILs-Tf 2 N-14 catalyst at 120°C, 12 h, with CH 3 ONa (0.75 equiv.) and 2 MPa O 2 , yielding a HMF conversion ( C HMF ) of 96.41 % and a FDMC selectivity ( S FDMC ) of 100 %. The heterogeneous catalyst 2 % Au/PILs-Tf 2 N-14 maintains high catalytic activity after multiple cycling experiments. A catalyst based on precious metal-loaded PILs was utilized to achieve efficient and selective conversion of HMF to FDMC under low loading conditions. This approach not only offers valuable insights for future research but also promotes the shift towards renewable energy sources. Additionally, the adsorption behavior of O 2 on Au 8 clusters and the interaction between the reaction substrate HMF and [Tf 2 N - ] were examined through density functional theory (DFT) calculations, providing theoretical backing for further investigation.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）