FUEL PROCESSING TECHNOLOGY
·
2024
·
IF 7.2
Xiequan Chen,Qi Zhang,Song Li,Haiyong Wang,Xinghua Zhang,Lungang Chen,Longlong Ma,Jianguo Liu
Acidic promoters are significant in the hydrodeoxygenation (HDO) of bioderived furans into alkanes over metal-acid bifunctional catalysts. Here, a supported Pd/HPW-SiO 2 catalyst was prepared to investigate the promotion effect of phosphotungstic acid (HPW) on the HDO of HMF-acetone adduct (H-Ac). Characterizations suggested that an intimate contact between Pd and HPW was established in Pd/HPW-SiO 2 . HPW promoters significantly reduced the reduction temperature of Pd oxides with enhanced hydrogenation and HDO capability. Particularly, in-situ DRIFTS confirmed that Pd-HPW sites significantly weakened the π CO η 2 adsorption mode (ν 3 (C=O)) of C=O group on Pd surfaces. Thereby, the HDO efficiency was synergistically improved through releasing more Pd metal sites to activate hydrogen for hydrogenation and HDO with HPW promoters. Eventually, >90% yield of nonane was efficiently achieved at 160 °C. This work is applicable to explore the structure-activity relationship of bifunctional catalysts in the efficient HDO of complicated oxygenated bioderived furans.
研究领域:
化学工程
·
催化科学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2020
·
IF 10.652
Yuling Ma,Airong Li,Cheng Wang,Xingbo Ge
Phosphotungstic acid (H 3 PW 12 O 40 , HPW) exhibits a good desulfurization performance towards the oxidative desulfurization (ODS) of oil-derived fuels. However, it presents two drawbacks: a small specific surface area and poor recovery. In this work, HPW was loaded on the support UiO-66 with a stable structure and large specific surface area, and a family of HPW@UiO-66 catalysts was prepared. Based on the structure and property analyses of powder FT-IR, ICP-OES, XRD, SEM, TG and BET, 0.5-HPW@UiO-66 with defects possessed a high crystallinity, regular morphology, stable structure and dispersed HPW clusters. The removal efficiency of DBT reached 100% and was maintained at 94.70% after 12 times of repeated use under the optimal reaction conditions. The results showed that the catalytic performance of HPW@UiO-66 catalyst for model oil desulfurization was improved when the defects existed.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF WUHAN UNIVERSITY OF TECHNOLOGY-MATERIALS SCIENCE EDITION
·
2021
·Vol. 36
·期 3
·338-346
·
IF 0.957
Shan Hailin,Du Yue,Du Xiaodi,Lei Jiaheng
In order to reduce the emission of SO x in the environment, sulfur compounds must be removed efficiently from fuels. Three-dimensional highly ordered meso-macroporous HPW/TiO 2 (3DO m/M HPW/TiO 2 ) materials were synthesized successfully by sol-gel method and applied as oxidative desulfurization catalyst for the model fuel. The characterization results displayed the existence of highly ordered meso-macroporous structures and the Keggin type of HPW was highly dispersed in TiO 2 framework. The effect of catalyst on desulfurization under different reaction conditions was studied systematically. The results showed that the catalyst exhibited excellent desulfurization performance in the hydrogen peroxide oxidation system, which could be explained by the unique meso-macroporous structure of catalyst. In addition, the catalyst showed good cycling performance and the removal rate of DBT still reached 96.1% even after 6 cycles, providing a feasible method for the development and application of fuel deep desulfurization catalysts.
研究领域:
催化材料
·
环境科学
·
能源化工
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2024
·
IF 4.7
Xiaofei Li,Lili Geng,Haifeng Shi,Songshou Ye,Ley Boon Sim,Jinbao Zheng,Nuowei Zhang,Binghui Chen
In this study, we utilized a sol-gel method to prepare Ni-HPW/SiO 2 catalysts with varying citric acid (CA):Ni molar ratios ranging from 0 to 5.0. The catalysts demonstrated different levels of activity in the hydrogenation of ethylbenzene , which correlated to their respective CA:Ni ratios. Introducing citric acid in the preparation process of nickel-based catalysts yielded mesopore formation and reduced NiO particle size, producing a more uniform NiO dispersion on SiO 2 , which was confirmed by BET, XRD, and TEM analyses. The results of H 2 -TPR, H 2 -TPD, NH 3 -TPD, and Py-IR analyses suggested that the addition of citric acid augmented the interaction between phosphotungstic acid (HPW), Ni species, and SiO 2 . Citric acid improved Ni species and HPW dispersion, fostering increased HPW-Ni species formation. This, in turn, generated additional electron-deficient Ni ions , stemming from semi-reduced HPW-Ni species, which acted as Lewis acid sites, enhancing Ni + species effectiveness in activating aromatic rings. The better-dispersed, non-HPW-bound NiO, which, upon complete reduction to Ni, led to a substantial rise in H 2 bond cleavage, thereby facilitating more hydrogen spillover. Overall, the infusion of citric acid into fabricating Ni-HPW/SiO 2 catalysts sparked a significant surge in their aromatic hydrogenation ability.
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
CHEMICAL ENGINEERING SCIENCE
·
2023
·
IF 4.7
Yakun Liu,Shennan Yang,Chengxiang Shi,Lun Pan,Xiangwen Zhang,Ji-Jun Zou
Simmons-Smith cyclopropanation commonly promoted by CF 3 COOH is one important method for transforming olefin into high-energy–density cyclopropyl fuel, but it brings problems such as high cost and harm to environment. In this work, a series of highly active solid acid catalysts HPW/MCM-41 is prepared by impregnation method for the cyclopropanation of dicyclopentadiene. The composition, structural and acidity of catalyst were characterized by TEM, XRD, NH 3 -TPD, etc. The 5 % HPW/MCM-41 contains more Dawson-type P 2 W 18 (H 6 P 2 W 18 O 62 ) and defective-type P 2 W 21 (H 6 P 2 W 21 O 71 ) that can provide the most abundant acid sites. This catalyst shows the best catalytic activity, the conversion and bicyclic product selectivity for cyclopropanation of dicyclopentadiene are 93.4 % and 55.7 %, respectively, both higher than that of CF 3 COOH. Moreover, such catalyst shows good catalytic activity for several olefin substrates, and can be recycled in several runs. This work provides a green and efficient catalyst for cyclopropanation reactions for synthesis of high-energy–density fuel, pesticide and medicine.
研究领域:
催化化学
·
能源化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2023
·
IF 7.4
Yibo Zhang,Wei Wang,Chunlai Liu,Peihang Shen,Zelong Liu,Jianglei Hu,Fengwei Shi
In this work, we successfully synthesized a novel composite (HPW@MOF-199/SBA-15C, PMS-15C) in which MOF-199 encapsulated HPW catalyst (named HPW@MOF-199) was confined in SBA-15C, which is the carboxy-functionalized SBA-15. Physicochemical properties of the composites PMS-15C were systemically characterized by N 2 adsorption–desorption isotherms, wide-angle and low-angle XRD, XPS, FT-IR, SEM, and TEM. The results exhibited that HPW@MOF-199 had been successfully synthesized and embedded into the SBA-15C pores by COOH on the surface of SBA-15C. Meanwhile, the composites PMS-15C exhibited high activity and excellent reuse properties in the esterification reaction of acetic acid and ethanol, and no evidence of aggregation, leaching, or inactivation of HPW@MOF-199 during repeated use. The good dispersion of HPW within the MOF-199 cage and the interaction between HPW@MOF-199 and SBA-15C may be responsible for the good catalytic activity as well as the high stability of PMS-15C.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF APPLIED POLYMER SCIENCE
·
2023
·Vol. 140
·期 25
·e53978
·
IF 3
Xiaocan Zhang,Huixiao Ma,Tong Pei,Ruochen Zhang,Yiran Liu
Incorporating phosphotungstic acid (HPW) in proton exchange membranes (PEMs) is an effective way to improve proton conductivity, but its leakage remains a problem. It can be solved by immobilizing acid in membranes to enhance the stability of PEMs. Herein, we proposed a novel sulfonated poly(ether ether ketone) (SPEEK) composite membrane (SPEEK/HPW@MIL) that was prepared by blending amino-modified MIL-101(Cr) to anchor HPW. In this work, HPW was anchored through hydrogen bond to minimize its leakage and enhance the overall compatibility. The incorporation of MIL-101(Cr)-NH 2 also helped lower the swelling ratio and improve the dimensional stability. Compared with pristine SPEEK and SPEEK/MIL membrane, the proton conductivity of the SPEEK/HPW@MIL composite membrane increased by 26% and 14%, respectively. The superior performance recommended a promising conception for anchoring HPW in PEMs.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Chongfu Wu,Zhenhua Sun,Changshen Ye,Zhaoyang Qi,Jie Chen,Zhixian Huang,Ting Qiu
The development of catalysts with excellent performance in oxidative desulfurization (ODS) at room temperature will greatly facilitate the advancement of desulfurization technology. An efficient novel strategy, 4-aminopyridine molecular bridging combined with manual grinding, was presented to encapsulate HPW into UiO-66 for achieving stable loading of PW and to produce abundant defects that contribute to the formation of active complexes with strong oxidation ability. The prepared catalyst showed outstanding catalytic activity in the ODS system, achieving full desulfurization in 15 min at room temperature and a low O/S molar ratio. Further investigations reveal that the synergistic catalytic effect of the faulty UiO-66 and PW is mostly responsible for superior catalytic performance. UiO-66 rich in defects promote the decomposition of H 2 O 2 into radicals, and PW can combine with the radicals to form more stable active peroxide intermediates, then exerting the catalytic ability of ODS at room temperature. Such a synergistic catalytic mechanism provides a guide to improving the oxidation ability of PW-based catalysts at room temperature.
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
Molecular Catalysis
·
2025
·
IF 4.9
Yibo Zhang,Yang Liu,Wei Wang,Chunlai Liu,Hongyu Zhou,Na Wang,Jianglei Hu,Fengwei Shi
Metal-organic framework (MOF)-based composites have received significant attention for catalytic applications and are believed excellent heterogeneous catalysts. In this article, we prepared a new type of material, HPW@MOF-199/SBA-15C (PMS-15C). For this material, the MOF-199 encapsulating Keggin-type phosphotungstic acid (HPW) was grown inside the pores of the SBA-15 functionalized by carboxylic acids. The N 2 adsorption-desorption isotherms and pore size distributions, X-ray powder diffraction, transmission electron microscopy, and scanning electron microscopy analyses showed that the PMS-15C composites had an ordered two-dimensional hexagonal mesoporous structure, in which HPW encapsulating by MOF-199 loaded into the SBA-15C. Fourier-transform infrared spectroscopy and X-ray photoelectron spectroscopy indicated that HPW was successfully loaded, and the Keggin structure of HPW in PMS-15C remained unchanged. With the reaction of acetic acid and ethanol, the catalytic performance of PMS-15C was studied. Under the optimal conditions, ethyl acetate yield reached 81.4 %. The forward reaction rate was 0.432 mL mol −1 min −1 , and the activation energy was 38.35 kJ mol −1 . And the data were found to be consistent with the second-order reversible reaction kinetic model. The catalytic activity of the PMS-15C-0.2 composites remained stable after five catalytic cycles. In addition, the esterification of n-octanol/acetic acid and ethanol/oleic acid were studied using PMS-15C-0.2 as the catalyst. The results suggested that the catalytic activity of PMS-15C-0.2 was weakened upon increasing the substrates’ alkyl chain length.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
NEW JOURNAL OF CHEMISTRY
·
2022
·Vol. 46
·期 27
·13047-13053
·
IF 3.925
Feng Xu,Chao Liu,Jia-Xin Li,Cai-Zhen Zhan,Qi-Ning Xun,Wen-Shen Zhang,Wen-Fang Xing,Gang-Gang Chang
γ-Valerolactone (GVL) is an important lignocellulosic platform molecule with huge potential for various industrial and chemical applications, which is usually produced using levulinic acid (LA) or its esters as raw materials. However, a two-step reaction process in which hydrogenation of the carbonyl groups on metal sites and subsequent lactonization catalyzed by acidic sites over multiple catalysts has generally been needed to realize this synthesis. In this work, a hierarchically multifunctional single catalyst of Ru/phosphotungstic acid/hierarchically porous UiO-66 (Ru/HPW/HP-UiO-66), simultaneously integrated with acidic and metal sites, has been fabricated via a simple strategy and successfully applied in the one-pot synthesis of GVL using methyl levulinate (ML) as the raw material. The hierarchically porous and nanosized (∼15 nm) HP-UiO-66 can not only provide sufficient space for the mass transfer of substrates but also favors the loading of bulk HPW molecules, which can effectively mediate the catalytic activities and stability of Ru NPs using the confined pore effect of UiO-66 and the strong interaction between HPW and Ru. When applied in the one-pot synthesis of GVL, the hierarchical Ru/HPW/HP-UiO-66 catalyst showed excellent catalytic activity (>97% yield) and stability (maintained after 7 successive cycles) for GVL. More importantly, the hierarchical catalyst also exhibited an extraordinary performance in the hydrogenation of different unsaturated hydrocarbons in aqueous solution. It is expected that our study offers a novel route to biomass upgrades involving metal/acid bifunctional synergistic catalysts.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Peng Wei,Yang Sui,Dong Huang,Bensheng Zhu,Xiaoyu Meng,Qiong Zhou
Sulfonated poly ether ether ketone (SPEEK) was used to fabricate proton exchange membrane (PEM) due to its adaptable proton conductivity. However, PEM cannot simultaneously enhance its conductivity and stability. To solve the problem mentioned above, phosphotungstic acid (HPW) with strong inherent proton conductivity was chosen to add to the SPEEK matrix, but it still faces the leaky problem. NH 2 -UiO-66 (NU6) with a large surface area and chemical stability was synthesized in situ on the surface of polyimide (PI) nanofiber to create NU6@PI nanofiber, which can be used to anchor HPW. Meanwhile, the stability of proton transport channel may be further enhanced by the sandwich structure, which may be advantageous for proton transport. The NU6@PI/SPEEK + HPW-20 exhibited a conductivity of 174.9 mS·cm −1 and a swelling ratio of 19 % at 60 °C and 100 % RH. After 6 weeks of testing, its conductivity decreased to 151.2 mS·cm −1 which was 24 % higher than that of SPEEK, while the swelling ratio increased to 31 % which was lower than that of SPEEK. The outcome demonstrates that the sandwich-structure NU6@PI/SPEEK + HPW membrane may really boost proton conductivity and stability at the same time. By using XPS and TEM, it is possible to confirm the acid-base interaction and acid-rich layer that exist at the interfaces of NU6@PI nanofiber and HPW/SPEEK matrix. After 6-weeks of usage, the sandwich-structure composite membrane with nanofiber at both the top and bottom of PEM can still maintain high proton conductivity and high stability, offering a novel research idea for resolving the issue that PEM cannot simultaneously achieve significant proton conductivity as well as elevated stability.
研究领域:
材料科学
·
化学工程
·
电化学
·
纳米技术
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 89
·73083-73090
·
IF 3.84
Kuiyi You,Renjie Deng,Jian Jian,Pingle Liu,Qiuhong Ai,He’an Luo
Developing a new environmentally friendly process for benzene nitration to nitrobenzene has been highly desirable for a long time. In this work, NO2 was used as a nitration agent to replace traditional nitric acid, and different mesoporous SiO2 and their supported heteropoly acid (salt) were employed to catalyze benzene nitration to nitrobenzene. Several typical catalysts were characterized using XRD, BET and FT-IR, and the acid amounts of the various catalysts were determined. The effects of various factors such as different catalysts, the molar ratio of benzene to NO2, reaction temperature, reaction time, HPW loading, the acid amounts of the catalyst and the reuse of the catalyst on the nitration reaction have also been systematically examined. The results indicate that the supported HPW/MCM-41 catalysts exhibit a remarkably synergistic catalytic performance on the nitration reaction of benzene to nitrobenzene. In particular, the 50%HPW/MCM-41 catalyst gives the best results with 73.4% benzene conversion and 98.8% selectivity to nitrobenzene under the optimal reaction conditions. Moreover, the mesoporous structure of MCM-41 was retained under the high loading of HPW. The possible reaction mechanism for the nitration reaction of benzene with NO2 over HPW/MCM-41 is suggested in the present work. This method provides a promising strategy for the preparation of nitro-aromatic compounds from a catalytic nitration reaction by using NO2 as the nitration reagent.
研究领域:
化学工程
·
环境科学
✓ 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）