CHEMICAL ENGINEERING SCIENCE
·
2024
·
IF 4.1
Shuang Wei,Mengyue Li,Kexin Li,Sheng Zhong,Yatao Su,Ruirui Zhang,Ruixia Liu
The oxidation of cyclohexane to produce adipic acid suffered from the inefficient and polluting two-step process. We introduce the CuCo Prussian blue analogues derived in situ C, N doped CuCo composite catalysts in the selective oxidation of cyclohexane. Due to the in-situ doping of C and N elements in the form of active graphite carbon and pyridine nitrogen, the oxygen vacancy content and the ability to activate oxygen are improved. The one-step efficient catalytic oxidation of cyclohexane to adipic acid was realized due to the excellent electron transfer performance between C, N elements and metals.
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CATALYSIS TODAY
·
2024
·
IF 5.2
Jiali Zheng,Zhihui Li,Dongsheng Zhang,Xinqiang Zhao,Qian Zhao,Yanji Wang
Bio-based route for preparing adipic acid (AA) from 5-hydroxymethylfurfural is the direction for achieving green and sustainable AA production. In light of the challenges, such as corrosion and difficulties in recycling of I - containing homogeneous catalyst, large amount, high cost, and significant mass transfer resistance of ionic liquid (IL) catalyst, encountered in the current hydrodeoxygenation of 2,5-tetrahydrofurandicarboxylic acid (THFDCA) to AA process. Herein, 1-sulfobutyl-3-methylimidazolium iodide IL ([HSO 3 -b-mim]·I) was used to functionalize MIL-101-NH 2 through acid-base self-assembly approach, hence, a heterogeneous catalyst, IL/MIL-101-NH 2 was designed and applied in the hydrodeoxygenation of THFDCA to bio-based AA for the first time. When reacted at 180 °C for 2 h, the THFDCA conversion and AA yield were 100 % and 99.9 %, respectively. Moreover, IL/MIL-101-NH 2 exhibited remarkable stability and could be reused multiple times with minimal loss in activity. XRD, SEM, FT-IR, BET, XPS, and TG results revealed that the functionalization process involved the reaction between HSO 3 in the IL and NH 2 in MIL-101-NH 2 , forming a salt that chemically bonded the IL to MIL-101-NH 2 , thereby enhancing stability. The excellent hydrodeoxygenation activity was attributed to the synergistic effect of the Lewis acid site (Cr 3+ ) and the Lewis base nucleophilic site (I - ) within IL/MIL-101-NH 2 .
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CORROSION SCIENCE
·
2025
·
IF 8.5
Shiyao Du,Dongfang Jia,Lingwei Ma,Dawei Zhang
The coupling effect of adipic acid and NaCl on electrochemical migration (ECM) of SAC305 solder alloy for printed circuit boards was studied using a self-designed high-throughput preparation and electrochemical test platform. The promotion effect of 1000 ppm NaCl on anodic dissolution and ion migration steps in the electrochemical migration substantially increased the dendrite formation probability ( P dendrite ) of SAC305 solder alloy. The low P dendrite in 1000 ppm adipic acid was attributed to the enhanced resistance to ion migration step by the formation of complex precipitates. Adding 1 ppm adipic acid into 1000 ppm NaCl could effectively decrease P dendrite due to the co-formation of hydroxide and complex precipitates, while increasing adipic acid concentration (from 10 ppm to 1000 ppm) instead raised P dendrite because hydroxide precipitates could transform into dendrite source at the cathode.
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Energy Technology
·
2017
·Vol. 5
·期 8
·1322-1327
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IF 2.789
Shaolei Xie,Jinhe Sun,Shang Liu,Lipeng Han,Guixiang Ma,Yan Jing,Yongzhong Jia
An adipic acid/boric acid (AA–BA) binary eutectic mixture containing 80 wt % adipic acid and 20 wt % boric acid was investigated as a new phase change material (PCM) with high latent heat, high thermal stability, and low cost. The material′s thermophysical properties and thermal stability were studied using differential scanning calorimetry (DSC), X-Ray Diffraction (XRD), and thermogravimetric analysis (TGA). The thermal stability was investigated in situ over 100 cycles using DSC. The phase change temperature of the AA–BA binary eutectic mixture was 135.04 °C and the latent heats of the melting and crystallization process were 283.42 and 272.16 J g −1 , respectively. The latent heat of melting only dropped 4.94 % after in situ 100 cycles using DSC. Following comparison of thermal properties and price of the AA–BA eutectic mixture PCM with those of some composite PCMs, the results indicate that the newly prepared AA–BA eutectic mixture is a potential phase change material for thermal storage tanks.
研究领域:
材料科学
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热力学
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能源存储
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化学工程
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功能材料
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Journal of Inorganic and Organometallic Polymers and Materials
·
2021
·Vol. 31
·期 11
·4195-4208
·
IF 3.543
Wang Lulu,Zeng Xiangrui,Wang Haiyan,Wang Yujia
Abstract A series of porous confined ionic liquid phosphotungstate were synthesized by encapsulated of N-(3-sulfopropyl)morpholinium phosphotungstate ([C 3 SO 3 Hnhm] 3 -PW 12 O 40 ) into MIL-101. Then the aforementioned porous confined ionic liquid phosphotungstate as heterogeneous catalyst will be used together with H 2 O 2 for the catalytic synthesis of adipic acid from cyclohexene. During the experiment, the effect of weight content of [C 3 SO 3 Hnhm] 3 PW 12 O 40 on the catalytic performance was investigated in detail. And the chemical structure of the catalyst was also characterized by XRD, FT-IR, 1 H-NMR, SEM–EDX and N 2 adsorption–desorption isotherms. Experimental results revealed that the desired products has been successfully prepared, and the best catalytic performance (81.2% yield of the adipic acid) was obtained under the dose of [C 3 SO 3 Hnhm] 3 PW 12 O 40 was 31wt%, which was almost close to the catalytic activity of original [C 3 SO 3 Hnhm] 3 PW 12 O 40 (85.3% yield of the adipic acid), which was also proved the strategy of packaging ionic liquid phosphotungstate with MIL-101 in this research is feasible. Furthermore, recycled catalytic performance of the catalyst under repeat 6 times was evaluated and the result revealed that the yield in adipic acid was still higher than 80.0%, which also proved that the catalytic active component was stable in the catalyst. Graphic Abstract
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JOURNAL OF COORDINATION CHEMISTRY
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2015
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IF 2.012
Cui-Cui Wang,Jin-Hua Wang,Gui-Mei Tang,Yong-Tao Wang,Yue-Zhi Cui,Seik Weng Ng
Three new metal coordination polymers constructed from adipic acid and 2-(pyridin-3-yl)-(1H)-benzimidazole ligands, [M(ADP)(3PBI)2(H2O)2]·2H2O (M = Ni and Co for 1 and 2, respectively) and [Cd(ADP)(3PBI)(H2O)] (3) [ADP = adipic acid dianion; 3PBI = 2-(pyridin-3-yl)-(1H)-benzimidazole], have been synthesized by hydrothermal reactions and were characterized by X-ray single-crystal diffraction, elemental analyses, IR, powder X-ray diffraction, and thermogravimetry. Complexes 1 and 2 are isostructural. Both form a 1-D linear chain structure, which is further assembled into a 3-D supramolecular framework by π⋯π stacking and hydrogen bonding interactions. Complex 3 possesses a binuclear unit and displays a 2-D layer which is further extended to a 3-D supramolecular architecture via hydrogen bonding and other weak packing interactions. The luminescent properties of 3 were investigated in the solid state at room temperature.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2016
·
IF 2.567
Jian Jian,Kuiyi You,Qing Luo,Hongxu Gao,Fangfang Zhao,Pingle Liu,Qiuhong Ai,He’an Luo
Developing an economic and efficient approach for the production of adipic acid is a grand challenge in the chemical industry. Toward this goal, we report a simple method for selective synthesis of adipic acid from cyclohexane with NO2 by using Ni–Al–VPO/MCM-41 as catalyst. The physical-chemical properties of supported Ni–Al–VPO/MCM-4 catalysts were characterized, the reaction conditions were optimized, and the reusability of the catalyst was examined. The results showed that the supported 30%Ni–Al–VPO/MCM-41 catalyst exhibited excellent catalytic performance with 65.1% of cyclohexane conversion and 85.3% of selectivity toward adipic acid, especially, its catalytic performance was still stable after five runs. Maybe this developed method has potential industrial application prospects for production of adipic acid.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
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2017
·
IF 2.323
Xiangji Liao,Xiuqing Li,Yujun Han,Jun Song,Yingjie Gao,Ao Yang,Yan Zhu,Weiping Luo
In this work, the solubilities of adipic acid and succinic acid in glutaric acid + cyclohexanone and glutaric acid + acetic acid mixtures were measured respectively by using the laser dynamic method under atmospheric pressure, in which the temperature ranged from 296.15 to 340.85 K and the mass fraction of glutaric acid in the binary solvent mixtures ranged from 0.00 to 0.30. The effects of glutaric acid on solubility of adipic acid and succinic acid have been discussed. It is found that the effects of glutaric acid on the solubility of adipic acid and succinic acid were negative and that with the increasing mass fraction of glutaric acid in the mixtures the solubilities of adipic acid and succinic acid would decrease. With the gradual increase of temperature, the measured solubility of adipic acid and succinic acid in glutaric acid + cyclohexanone and glutaric acid + acetic acid mixtures would increase at the constant proportion of solvent mixtures. Then the experimental data were well-correlated by the modified Apelblat equation and the modified nonrandom two-liquid (NRTL) activity coefficient models, in which the average relative deviation (ARD) were less than 2.50%, and the values of the solubility calculated showed good agreement with the experimental observation. The interaction parameters of AA and GA and SA and GA were determined first in this work.
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CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Zhiyang Zhang,Mi Hu,Qingfeng Gui,Jing Gu,Wenlong Xu,Qingbo Xiao,Wei Huang
Adipic acid is a valuable chemical used to product Nylon-66, and one of the greenest ways to synthesize it is catalyzing the oxidation of cyclohexane by molecular oxygen in the absence of any other chemicals. However, it is challenging to convert cyclohexane effectively with high selectivity to adipic acid using the available catalysts. In response to the dilemma of achieving satisfactory conversion and selectivity at the same time, a remarkable Au@NaX catalyst is proposed using an improved in-situ crystallization method that exhibits Au clusters surrounded by X-zeolite channels. A 29.5% conversion of cyclohexane and an 85.6% selectivity to adipic acid can be obtained in a one-pot oxidation of cyclohexane at 140 °C, 20 bar O 2 , far exceeding most published results. Since determined by detailed characterizations and DFT calculations, the effective dynamic collaboration between Au clusters and zeolite inner micro-environment is the decisive role for superior catalytic performance. Specifically, the surrounding zeolite channel encourages the adsorption and activation of cyclohexane over the confined Au clusters, resulting in an unprecedented activity. The continuous oxidation of cyclohexanol and cyclohexanone to adipic acid is also vulnerable on the enclosed Au clusters, and the subsequent adipic acid can be further stabilized as a result of the strong interaction of –COOH with Na ± in zeolite channels surrounding enclosed Au clusters. It prevents AA from poisoning active sites and generates a higher selectivity for the desired adipic acid. Our study highlighted the critical significance of the dynamic interaction between metal clusters and the zeolite channel microenvironment. It would shed light on the further high-performance catalysts designs for selective oxidation.
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APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Sheng-Li Lv,Kuan Wang,Song-Song Li,Xin-Peng Li,Tong-Le Dang,Zhen-Hong He,Huan Wang,Weitao Wang,Yang Yang,Zhao-Tie Liu
Photothermal catalytic oxidation of cyclohexane was found to be an effective and green strategy for the production of cyclohexanol and cyclohexanone (KA oil). However, such strategy existed some obstacles, which hindered its application in the one-step synthesis of adipic acid (AA), necessitating further breakthroughs. Herein, a p-n heterojunction of Fe 8 Ce 2 O x /WO 3 was constructed by a simple combination of solvothermal and impregnation methods, enabling the one-step synthesis of AA via the photothermal cyclohexane oxidation under solvent-free and visible light conditions. Remarkably, the Fe 8 Ce 2 O x /WO 3 nanocomposites exhibited outstanding catalytic performance, achieving a conversion of cyclohexane reached 9.67% with the 92.45% selectivity towards AA (solid, 59.46%) and KA oil (liquid, 32.99%). The Fe 8 Ce 2 O x /WO 3 composites also demonstrated exceptional stability in the production of AA, further highlighting its potential as a catalyst for industrial applications. The exceptional catalytic properties of Fe 8 Ce 2 O x /WO 3 composites can be attributed to the promoted electronic excitation capability, enhanced separation and migration of electron-hole, suppressed charge complexation, broaden visible-light absorption, and effective photo-thermal co-catalytic effects. Furthermore, the Fe 8 Ce 2 O x /WO 3 composites possess a strong adsorption capacity for oxygen and suitable specific surface area, which can be effectively facilitate the interaction between O 2 and cyclohexane, enabling the full utilization of oxygen in the oxidation of cyclohexane to form AA. The proposed approach offers a novel methodology for the design and fabrication of photothermal catalysts to achieve the direct synthesis of AA via the cyclohexane oxidation under solvent-free and visible light conditions in industry.
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JOURNAL OF CATALYSIS
·
2026
·
IF 6
Kexin Li,Bin He,Huanghao Ning,Ruiyi Yan,Ruirui Wang,Ruirui Zhang,Ruixia Liu
The highly selective and direct oxidation of cyclohexane to adipic acid (AA) using molecular oxygen under solvent-free conditions represents a “dream reaction” in industrial catalysis, yet is severely hampered by the inherent chemical inertness of C-H bond and the challenging activation of O 2 . Addressing this grand challenge, we report a non-metal heterointerface engineering strategy to construct an advanced B/F-doped h-BN/g-C 3 N 4 heterojunction catalyst (known as BN/CN-BF 4 ) via a facile synergistic ultrasonication and thermal treatment utilizing the ionic liquid. The resulting BN/CN-BF 4 exhibits a powerfully ability to regulate interfacial electronic microenvironment, as evidenced by spectroscopic, electrochemical analysis, and DFT calculations, which reveal a type-II staggered band alignment and an internal electric field (IEF) formation across the heterojunction. This precisely engineered heterointerface achieved a remarkable breakthrough in catalytic performance, yielding a high cyclohexane conversion of 18.8% with an unprecedented selectivity for AA reaching 51.3% (a significant advancement over the typical 3%-5% conversion) in solvent-free system. Mechanistic investigations established a multi-step synergistic catalytic mechanism that B-N sites and H-bonding facilitate the initial C-H bond adsorption and activation; simultaneously, the IEF-driven directional electron transfer and C-F bond formation significantly accelerate the activation of O 2 to generate highly reactive oxygen species, steering the reaction pathway directly towards the terminal product, adipic acid. This work provides a novel strategy for enhancing industrial selective oxidation by manipulating the interfacial electronic microenvironment with IEF, offering a promising route for advanced solvent-free and metal-free selective oxidation catalysts.
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JOURNAL OF MOLECULAR STRUCTURE
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2022
·
IF 3.841
Lulu Wang,Jing Lu,Yujia Wang,Haiyan Wang,Jilin Wang,Tieqiang Ren
In this study, a series of MIL-101-X catalysts were prepared by confining acidic ionic liquid phosphotungstate in MIL-101 nanocages using the organic electron-rich N-heterocyclic compound as a chemical bridge and the aforementioned catalysts were used for the oxidation of cyclohexene to adipic acid. During the aforementioned process of post-synthetic modification, a Bronsted acidic ionic liquid phosphotungstate ([C 3 SO 3 Hnhm] 3 PW 12 O 40 ) was synthesized in the nanocage of MIL-101. The research results reveal that the yield of adipic acid for the cyclohexene oxidation catalyzed by the constructed MIL-101-X catalyst was up to 78.16% in solvent-free condition. And its catalytic activity is not significantly reduced after six cycles. The novel catalyst synthesized in this paper combines the common advantages of ionic liquid phosphotungstate and MIL-101 nanocage microenvironment to facilitate the diffusion of reactants and their interaction with the catalytic activity center. This research will provide a new idea to solve the problem in terms of the shortage of efficient catalysts in the field of catalytic oxidation of cyclohexene to adipic acid.
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危险品化学品经营许可证（带存储）