RSC Advances
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2017
·Vol. 7
·期 64
·40581-40590
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IF 3.108
Xiao Fang,Yanchun Shi,Kejing Wu,Junmei Liang,Yulong Wu,Mingde Yang
The addition of phosphotungstic acid (PTA) to the synthesis mixture of PdCu@FeIII–MOF-5 yields the direct encapsulation of PTA inside the MOF structure (i.e. PTA@PdCu@FeIII–MOF-5) through a facile solvothermal approach. The deoxygenation reaction of palmitic acid has been investigated over PdCu@FeIII–MOF-5 and PTA@PdCu@FeIII–MOF-5 under a hydrogen atmosphere in the supercritical fluid (SCF) of n-hexane. The results showed that palmitic acid can be converted completely at 240 °C on PTA@PdCu@FeIII–MOF-5 with a high selectivity of hexadecane. Owning to the improvement of acidity of the MOF catalyst by the encapsulation of PTA inside the hollow octahedral nanostructures of PdCu@FeIII–MOF-5, the selectivity for hexadecane over the PTA@PdCu@FeIII–MOF-5 catalyst is higher than that over PdCu@FeIII–MOF-5. The excellent performance in the catalytic hydrodeoxygenation (HDO) of palmitic acid is associated with the synergistic effect between yolk–shell PTA@PdCu@FeIII–MOF-5 nanostructures and SCF medium.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2021
·
IF 2.495
Haihong Xia,Jing Li,Changzhou Chen,Dichao Wu,Jurong Ren,Jianchun Jiang,Minghao Zhou
Metal-organic frameworks (MOFs) as an emerging class of porous materials exhibit some unique advantages, including controllable composition, a large surface area, high porosity, and so on. In this work, the spherical NiMo bimetal catalysts supported on porous carbon matrix were prepared using a simple wet impregnation method and studied for selective hydrogenation of furfural (FFA). Three different catalysts were investigated including Ni/C-Mo-BTC, Ni/C-Mo-DHTA and Ni/C-Mo-PTA. Of the catalysts studied the Ni/C-Mo-BTC catalyst could achieve the highest selectivity of CPL (up to 90%) under moderate reaction conditions (140 °C, 2 MPa, 2 h) in aqueous medium. In addition, other Ni-based catalysts (Ni/C-Fe, Ni/C-Zn, Ni/C-Cu, Ni/C-Ce) were also investigated to achieve yields of 20–70% under the same reaction conditions. The influence of temperature, H 2 pressure, time and solvent were investigated for the best performing catalyst. Based on the optimal reaction condition, various of furfural derivatives could also be effectively transferred to produce corresponding products. The detailed physicochemical characterization was carried out by means of XRD, SEM, TEM, XPS, NH 3 -TPD and Raman analysis. In the end, the optimal Ni/C-Mo0.4 catalyst could be recycled magnetically and efficiently applied in the next run for five consecutive recycling tests in the FFA hydrogenation to CPL. The results suggested Ni/C-Mo0.4 catalyst occurred to increasingly favor the formation of Ni-Mo alloys and suggested a metallic active site in FFA hydrogenation with the addition of element Mo. Mechanism study indicated that water was a key factor contributing to the formation of different desired products, which was responsible for the arrangement of furan compound.
研究领域:
化学工程
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催化材料科学
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DOI
高影响因子
ACS Applied Nano Materials
·
2024
·
IF 5.3
Yu Liu,Xuanzhi Wang,Xingyu Lu,Di Wang,Wenze Li,Yu Fu,Wei Qi
Addressing the critical scientific challenge of enhancing the catalytic efficiency of transition metal-based metal–organic framework (MOF) materials in the two-electron oxygen reduction reaction (2e– ORR) for the electrochemical synthesis of H2O2 is of paramount importance in a related field. In this context, we had developed an interface synthetic strategy for constructing a series of bimetallic Ni–M (M = Co, Fe, Cu) center MOFs. This approach capitalized on the strong synergy among metallic ions, effectively regulating the electronic structure and thereby improving the catalytic activity of Ni active sites. Notably, the proposed Ni–Co MOF catalyst demonstrated exceptional 2e– ORR activity, achieving a remarkable H2O2 selectivity of up to 96%. This performance significantly surpassed that of Ni–Fe (54%) and Ni–Cu (67%) MOFs, as well as many other reported transition metal catalysts. Detailed studies on the structure–function relationship at the atomic level unveiled that Ni species in a high oxidation state, effectively regulated and stabilized by adjacent Co2+ ions, played a pivotal role in ensuring the superior 2e– ORR activity of the Ni–Co MOF. These physical-chemical insights into the reaction mechanism and structure–function relationships offer valuable guidance for the rational design of highly efficient MOF-based catalysts and reaction systems for on-site electrochemical synthesis of H2O2 via a 2e– ORR process.
研究领域:
材料科学
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电化学
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催化反应
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产品关联
DOI
高影响因子
Sustainable Chemistry and Pharmacy
·
2023
·
IF 6
Qiuyun Zhang,Yanting Lei,Luyan Li,Jiao Lei,Mengmeng Hu,Taoli Deng,Yutao Zhang,Peihua Ma
A novel Bi-based metal-organic framework impregnated phosphomolybdic acid (PMA@Bi-MOF) catalyst has been fabricated via a simple hydrothermal procedure, and successfully applied in the preparation of biodiesel using oleic acid (OA) as the raw material. The PMA@Bi-MOF composites were exhaustively characterized with the help of FTIR , XRD, TPD-NH 3 , SEM-EDX, N 2 -physisorption, TGA , and XPS analyses. Experimental findings showed that the PMA@Bi-BTC exhibited a higher activity than that of PMA@Bi-BDC and Bi-BTC, attributed to its textural property, the presence of more acid sites with higher strength, and synergistic catalytic effects between PMA and Bi-BTC. The optimum conditions for esterification of OA, with a conversion of up to 92.5%, were found to be a molar ratio of methanol to OA of 20:1 and 0.15g PMA@Bi-BTC catalyst at 160 °C in 3 h. Meanwhile, reused studies indicated that the OA conversion reached more than 80% after seven reaction cycles. Furthermore, the activation energy of esterification catalyzed by PMA@Bi-BTC was also calculated as 54.8 kJ/mol. It is expected that our study provides an efficient route to biofuel production involving polyoxometalates/MOF synergistic catalysts.
研究领域:
催化化学
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能源科学
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材料科学
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产品关联
DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2023
·
IF 6
Li Wang,Ji-Xiang Guo,Xiao-Jun Zhang,Chen-Hao Gao,Rui-Ying Xiong,Wyclif Kiyingi,Dan Luo
Oil shale is of increasing interest as it is considered an essential alternative to traditional energy sources due to its abundant reserves. In this research, nanoscale Co/MOF and Ni/MOF were prepared by modified methods, and the catalytic pyrolysis mechanism of oil shale was studied using structural characterization and pyrolysis experiments. The TG and DTG curves show that MOF catalysts increase the total weight loss rate of oil shale pyrolysis and decrease the temperature corresponding to the initial temperature, final temperature, and maximum weight loss rate of oil shale pyrolysis. Kinetic analysis shows that Co/MOF and Ni/MOF catalysts reduce the activation energy of oil shale pyrolysis reaction by 32 KJ/mol and 25 KJ/mol, respectively. The change in the yield and composition of the products before and after catalytic pyrolysis was compared through the dry distillation experiment. It was found that MOF had a good catalytic effect, and the shale oil output was significantly increased. The FT-IR and GC/MS analysis of the catalytic pyrolysis of shale oil shows that the addition of Co/MOF and Ni/MOF catalysts is conducive to the increase of aromatics, olefins , and alkanes and the decrease of oxygen-containing compounds. The effect of the catalysts on the nature of the products and on the yields suggests that the Lewis and Bronsted acid groups on the surfaces of the MOF catalysts and that these can induce positive charges on carbon atoms in alkanes, alkenes etc to promote pyrolysis generate more oil.
研究领域:
能源化学
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催化材料科学
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DOI
高影响因子
Materials Research Express
·
2019
·Vol. 6
·期 12
·125101
·
IF 1.449
Kai Huang,Lin Lin Guo,Dong Fang Wu
Different from the traditional aldimine condensation reaction, N-containing ligand: pyridine-2-formaldehyde was selected as the source of aldehyde group, and NH2-MIL-53(Al) containing a large number of amino functional groups was took as the carrier, transition metal Cu2+ coordinated with N-containing ligand to prepare a new and more stable MOFs catalyst named Cu@Al-MIL-53-P21. The catalyst exhibited a cross-linked nanorod morphology. The effect of the morphology on the catalytic oxidation activity of styrene was studied, the results showed that the catalyst could not only promote the production of benzaldehyde, but also inhibit the production of benzoic acid and phenylacetaldehyde. In addition, the optimal reaction conditions and the reaction mechanism were also discussed in this paper.
研究领域:
材料科学
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催化化学
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产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2023
·
IF 22.1
Xuejiao Wang,Jing Yang,Ming Zhang,Qian Hu,Bai-Xue Li,Jin Qu,Zhong-Zhen Yu,Dongzhi Yang
We design a spontaneously super-hygroscopic alkaline microreactor by photoinduced integration of Zr-MOF catalyst and alkaline poly(dimethylaminoethyl acrylate) onto LiCl-salinized poly(N-isopropylacrylamide) gel, generating a microenvironment with non-volatile polymeric base and non-bulk water for detoxification of a typical nerve agent simulant, dimethyl 4-nitrophenyl phosphate (DMNP), in atmospheric environments. The super-hygroscopic gel with directional microchannels facilitates the absorption, transport and storage of water under different humidities, and exhibits fast hygroscopic efficiency with a high moisture absorption capacity of 6.4 g g −1 . The integrated microreactor achieves simultaneous water uptake and catalytic hydrolysis of DMNP in an atmospheric environment with an initial half-life of ∼1.9 h and a final conversion of 95.5%, which is attributed to the synergistic catalytic microenvironment of the exposed Zr-MOF catalyst, the polymeric base, and the water from moist air. This work provides a feasible strategy for designing spontaneously hygroscopic microreactors for detoxifying nerve agent simulants in atmospheric environments.
研究领域:
材料科学
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
·
2024
·
IF 7.7
Changzhou Chen,Jie Jiang,Yajun Liu,Xialin Ji,Mengqing Zhou,Jun Zhao,Jianchun Jiang
The enhanced utilization of biomass-derived chemicals for the generation of high value aromatics through an advanced catalytic strategy has captured considerable attention within the realm of eco-friendly manufacturing. This work presented four innovative three-dimensional rod-shaped mesoporous Ce-based MOF materials, which were coupled with a H-donor solvent to facilitate vanillin hydrodeoxygenation and macromolecular lignin. Under the optimized conditions (30 mg CoCe@C catalyst, 2 MPa N 2 pressure, 15 mL isopropanol, 190 °C, and 5 h), the CoCe@C catalyst achieved nearly complete conversion of vanillin and demonstrated 87.8 % selectivity in the hydrogen-donor solvent. The characterization findings suggested that the synergy between metallic Co and oxygen vacancy sites enabled the effective activation of CHO group in vanillin, leading to formation of reactive product MMP . In addition, the optimal CoCe@C catalyst could also achieve macromolecular lignin hydrodeoxygenation to obtain high yield of lignin oil products with narrower molecular weight distribution . This study presented a viable approach for the concurrent utilization of lignin derivatives in the generation of high value fuels and chemicals.
研究领域:
化学工程
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生物质能利用
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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