CATALYSIS LETTERS
·
2019
·Vol. 150
·期 3
·837-848
·
IF 2.372
Lu Jiqing,Liu Xing,Yu Guanqun,Lv Jinkun,Rong Zeming,Wang Mei,Wang Yue
Abstract Cyclohexanol is an important feedstock in the chemical industry and the selective hydrodeoxygenation of lignin-derived guaiacol to cyclohexanol have gained increasing research attention in recent years. In this work, a series of nanoporous metal catalysts were employed for the hydrodeoxygenation of guaiacol and nanoporous Ni (NP-Ni) exhibited high catalytic performance for the preparation of cyclohexanol. With water as solvent, 100% conversion of guaiacol and over 90% selectivity to cyclohexanol were achieved at 180 °C and 2 MPa for 4 h. In order to further promote the stability of NP-Ni, induction melting, vacuum arc melting and mechanical alloying were separately employed for the preparation of NiAl precursor alloy. Mechanical alloying seemed to be an effective method for the alloying process and the as-prepared NP-Ni could keep almost stable after 10 times recycling. Furthermore, the reaction mechanism was investigated with NP-Ni for guaiacol hydrodeoxygenation. Scanning electron microscope (SEM), Brunauer–Emmett–Teller (BET) surface area analysis, X-ray photoelectron spectroscopy (XPS), high-resolution transmission electron micrographs (TEM), energy dispersive spectrometer (EDS) and X-ray diffraction (XRD) were employed for the characterization of NiAl alloy and the optimal preparation methods of NP-Ni were acquired according to the characterization results. Graphic Abstract
研究领域:
化学工程
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材料科学
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能源化学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Dongdong Wang,Wanbing Gong,Jifang Zhang,Miaomiao Han,Chun Chen,Yunxia Zhang,Guozhong Wang,Haimin Zhang,Huijun Zhao
Catalytic hydrodeoxygenation (HDO) is one of the most promising strategies to transform oxygen-rich biomass derivatives into high value-added chemicals and fuels, but highly challenging due to the lack of highly efficient nonprecious metal catalysts. Herein, we report for the first time of a facile synthetic approach to controllably fabricate well-defined Ni-Co alloy NPs confined on the tip of N-CNTs as HDO catalyst. The resultant Ni-Co alloy catalyst possesses outstanding HDO performance towards biomass-derived vanillin into 2-methoxy-4-methylphenol in water with 100% conversion efficiency and selectivity under mild reaction conditions, surpassing the reported high performance nonprecious HDO catalysts. Impressively, our experimental results also unveil that the Ni-Co alloy catalyst can be generically applied to catalyze HDO of vanillin derivatives and other aromatic aldehydes in water with 100% conversion efficiency and over 90% selectivity. Importantly, our DFT calculations and experimental results confirm that the achieved outstanding HDO catalytic performance is due to the greatly promoted selective adsorption and activation of C=O, and desorption of the activated hydrogen species by the synergism of the alloyed Ni-Co NPs . The findings of this work affords a new strategy to design and develop efficient transition metal-based catalysts for HDO reactions in water.
研究领域:
催化化学
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材料科学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
Russian Journal of Physical Chemistry A
·
2024
·Vol. 98
·期 10
·2219-2232
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IF 0.7
Guiling Wu,Zhao Wenli,Yang Xinyue,Niu Xiaopo,Guo Zhen,Liu Danni,Wang Qingfa
Abstract Producing high-density fuel of alkylated decalins from hydrodeoxygenation (HDO) of naphthalene derivatives is an environmentally friendly but still challenging method. Herein, a bifunctional Ru/HZSM-5 catalyst was fabricated by acid treatment (citric acid, oxalic acid, nitric acid) to effectively synthesize the alkylated decalins via HDO of naphthalene derivative. Acid treatment adjusted the acidic site distribution of Ru/HZSM-5. Nitric acid treatment (NA) resulted in more abundance of weak acidic sites which was beneficial for the dehydration process in HDO, and the lowest ratio of BAS/LAS to promote the hydrogenation of alkylated octalins, the rate-determining step of HDO. NA-treated Ru/HZSM-5 showed the highest HDO activity with the highest selectivity of 1,2-dimethyldecalin (74%). Besides, it also presents good HDO activity of naphthalene derivatives to produce high-density hydrocarbons. Therefore, Ru/HZ5-NA is a promising catalyst for the production of alkylated decalins and other high-value biofuels and chemicals.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
ACS Catalysis
·
2024
·
IF 11.3
Fengli Gan,Xia Jiang,Ziheng Jin,Mingwu Tan,Xindi Xie,Qin Peng,Guangmei Cao,Shenggui Ma
Mass transport in conventional microporous zeolite catalysts can be enhanced by introducing secondary mesopores during hydrodeoxygenation (HDO). However, the impact of the macropore architecture with intrinsic mass transfer advantages over mesopores on HDO performance remains elusive. In this study, a macroporous zeolite monolith catalyst without a template and binder was synthesized using a crystal space-confined growth method. This catalyst exhibited a 1.3 times higher macropore volume (0.566 m3/g) than a conventional zeolite catalyst, while the microporous structure was similar. Moreover, the high degree macropore connectivity was directly visualized and quantified with an advanced nanocomputed tomography technique. The macroporous catalyst achieved a higher guaiacol conversion rate of 93% and better coke resistance (3.2 wt % coke) than the conventional zeolite catalyst, which showed a 90% guaiacol conversion rate and 5.6 wt % coke. This improvement was primarily due to faster diffusion rates and an increased number of acid sites in the macropores.
研究领域:
化学工程
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催化材料科学
✓ 已验证
产品关联
DOI
高影响因子
Frontiers of Chemical Science and Engineering
·
2021
·Vol. 16
·期 4
·443-460
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IF 4.204
Shi Yinteng,Ai Lin,Shi Haonan,Gu Xiaoyu,Han Yujun,Chen Jixiang
Carbon-coated Ni, Co and Ni-Co alloy catalysts were prepared by the carbonization of the metal doped resorcinol-formaldehyde resins synthesized by the one-pot extended Stöber method. It was found that the introduction of Co remarkably reduced the carbon microsphere size. The metallic Ni, Co, and Ni-Co alloy particles (mainly 10–12 nm) were uniformly distributed in carbon microspheres. A charge transfer from Ni to Co appeared in the Ni-Co alloy. Compared with those of metallic Ni and Co, the d -band center of the Ni-Co alloy shifted away from and toward the Fermi level, respectively. In the in-situ aqueous phase hydrodeoxygenation of methyl palmitate with methanol as the hydrogen donor at 330 °C, the decarbonylation/decarboxylation pathway dominated on all catalysts. The Ni-Co@C catalysts gave higher activity than the Ni@C and Co@C catalysts, and the yields of n -pentadecane and n -C 6 - n -C 16 reached 71.6% and 92.6%, respectively. The excellent performance of Ni-Co@C is attributed to the electronic interactions between Ni and Co and the small carbon microspheres. Due to the confinement effect of carbon, the metal particles showed high resistance to sintering under harsh hydrothermal conditions. Catalyst deactivation is due to the carbonaceous deposition, and the regeneration with CO 2 recovered the catalyst reactivity.
研究领域:
化学工程
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催化材料科学
✓ 已验证
DOI
高影响因子
ChemSusChem
·
2017
·Vol. 10
·期 7
·1436-1447
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IF 7.226
Jiang Li,Jun-ling Liu,He-yang Liu,Guang-yue Xu,Jun-jie Zhang,Jia-xing Liu,Guang-lin Zhou,Qin Li,Zhi-hao Xu,Yao Fu
Graphical Selective and stable Fe : Selective catalytic hydrodeoxygenation of 5-hydroxymethylfurfural to 2,5-dimethylfuran over heterogeneous Fe catalysts is demonstrated in batch and continuous flow fixed-bed reactors. The Fe catalyst exhibited excellent stability, which is probably a result of the well-preserved active species and the pore structure of the Fe catalyst in the presence of H 2 . This work provided the first example of selective hydrodeoxygenation of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) over heterogeneous Fe catalysts. A catalyst prepared by the pyrolysis of an Fe-phenanthroline complex on activated carbon at 800 °C was demonstrated to be the most active heterogeneous Fe catalyst. Under the optimal reaction conditions, complete conversion of HMF was achieved with 86.2 % selectivity to DMF. The reaction pathway was investigated thoroughly, and the hydrogenation of the C=O bond in HMF was demonstrated to be the rate-determining step during the hydrodeoxygenation, which could be accelerated greatly by using alcohol solvents as additional H-donors. The excellent stability of the Fe catalyst, which was probably a result of the well-preserved active species and the pore structure of the Fe catalyst in the presence of H 2 , was demonstrated in batch and continuous flow fixed-bed reactors.
研究领域:
化学工程
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催化材料
✓ 已验证
产品关联
DOI
PubMed
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
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2021
·
IF 19.503
Tianci Xiao,Xiaohao Liu,Guangyue Xu,Ying Zhang
Crystal structure of catalyst support has great influence on its surface and electronic properties. Thus, tuning the crystal phase may adjust the catalytic activity. Herein, we prepared a series of monoclinic, tetragonal and mixed phase of Co/ZrO 2 catalysts, denoted as Co/m-ZrO 2 , Co/t-ZrO 2 and Co/Mix-ZrO 2 . They showed different hydrogenation and hydrogenolysis activities in conversion of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF). The characterization and catalytic performance indicated that the interaction between cobalt and t-ZrO 2 resulted in cobalt electron-deficiency and higher concentration of Zr(III) species, which contributed to the higher hydrogenation activity of carbonyl on Co/t-ZrO 2 than Co/m-ZrO 2 . While the hydrogenolysis of C OH group showed higher efficiency on Co/m-ZrO 2 , which was determined by the acid concentration on the surface of catalysts. The combination of both high hydrogenation and hydrogenolysis activities in Co/Mix-ZrO 2 achieved the highest yield of DMF (90.7 %) under mild conditions of 130 °C and 1 MPa H 2 .
研究领域:
催化化学
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材料科学
✓ 已验证
DOI
高影响因子
Bioresource Technology Reports
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2018
·
IF 0
Hao Li,Zhiling Liu
Hydrodeoxygenation (HDO) is one of the most promising technologies for the biomass pyrolysis oil upgrading, but substantial challenges for the development of efficient HDO catalysts still remain. In this work, the nickel catalysts supported on carboxylic carbon nanotube (Ni/CCNTs-X, X = 1, 2, 3, 4 and 5) with different diameter have been synthesized for the HDO of model compound (vanillin) to p -creosol. As the tube diameters of Ni/CCNTs-X catalysts increased, the catalytic activity increased firstly, and then decreased. The conversion of vanillin over Ni/CCNTs-4 catalyst reached up to 90.0% under mild reaction condition, with a concomitant 87.7% selectivity of p -creosol. The transformation pathway for the HDO of vanillin over Ni/CCNTs-X catalysts involve in hydrogenation, hydrogenolysis and etherification .
研究领域:
催化化学
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能源化学
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生物质转化
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可再生能源
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环境化学
✓ 已验证
DOI
Jove-Journal of Visualized Experiments
·
2019
·
IF 1.108
Weixiang Guan,Chuang Li,Xiao Chen,Xiao-Ying Lu,Chi-Wing Tsang,Haoquan Hu,Hongxu Qi,Changhai Liang
We herein present a method for the synthesis of HNbWO6, HNbMoO6, HTaWO6 solid acid nanosheet modified Pt/CNTs. By varying the weight of various solid acid nanosheets, a series of Pt/xHMNO6/CNTs with different solid acid compositions (x = 5, 20 wt%; M = Nb, Ta; N = Mo, W) have been prepared by carbon nanotube pretreatment, protonic exchange, solid acid exfoliation, aggregation and finally Pt particles impregnation. The Pt/xHMNO6/CNTs are characterized by X-ray diffraction, scanning electron microscopy, transmission electron microscopy and NH3-temperature programmed desorption. The study revealed that HNbWO6 nanosheets were attached on CNTs, with some edges of the nanosheets being bent in shape. The acid strength of the supported Pt catalysts increases in the following order: Pt/CNTs < Pt/5HNbWO6/CNTs < Pt/20HNbMoO6/CNTs < Pt/20HNbWO6/CNTs < Pt/20HTaWO6/CNTs. In addition, the catalytic hydroconversion of lignin-derived model compound: diphenyl ether using the synthesized Pt/20HNbWO6 catalyst has been investigated.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2020
·
IF 4.939
Yanxia Zhu,Ze Zhang,Jun Cheng,Hao Guo,Weijuan Yang
To improve catalytic performance of metal active sites in hydrodeoxygenation and hydrocracking conversion of methyl palmitate into high-quality jet biofuel, Ni-1,3,5-benzenetricarboxylate (Ni-BTC) metal-organic framework loaded on MCM-41(Mobil Composition of Matter No. 41) was prepared to enhance the accessibility of Ni active sites, facilitating hydrodeoxygenation to increase alkane yield with suitable arene content. The distance (0.98 nm) between Ni active sites within Ni-BTC structure, which was much larger than that (0.20 nm) within Ni nanoparticles , enabled methyl palmitate with maximum molecule width of 0.68 nm to go through Ni-BTC crystalline plane and get access to Ni active sites more easily. Ni-BTC nanosheets newly assembled in pore channels of MCM-41 were beneficial to effectively screen chain molecules of alkane products. With the largest BET surface area of 1014.2 m 2 /g, the Ni-BTC@MCM-41 catalyst with 2.5 wt% nickel (2.5Ni-BTC@MCM-41) reduced the nickel metal consumption by 75% comparing to nickel nanoparticle loading (10Ni@MCM-41), but achieved the best catalytic performances through hydrodeoxygenation on Ni active sites and hydrocracking on -SiOH acid sites. The alkane yield increased from 23.3% to 33.9%, while arene yield reduced from 22.4% to 6.5% in jet biofuel products. This resulted in an overall jet biofuel yield of 53.2% with uniform distribution along carbon numbers . The higher heating value of jet biofuel products thus increased to a peak of 45.90 MJ/kg.
研究领域:
催化材料
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能源化学
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纳米技术
✓ 已验证
产品关联
DOI
高影响因子
LANGMUIR
·
2020
·
IF 3.557
Qicheng Zhang,Danyun Xu,Junmei Liang,Qianqian Lin,Wenchao Peng,Yang Li,Fengbao Zhang,Xiaobin Fan
Hydrodeoxygenation (HDO) of bio-oil is a crucial step for improving the bio-fuel quality, but developing highly dispersed Pt-based catalysts with high selectivity for target alkanes remains a great challenge. This study presents a fast surfactant-free method to prepare the MoS2-supported Pt catalyst for HDO. Ultrafine Pt nanoparticles with sizes of <5 nm can be readily grown on chemically exfoliated MoS2 nanosheets (NSs) via the direct microwave-assisted thermal reduction. The obtained Pt NPs/MoS2 composites show excellent catalytic performance in the conversion of palmitic acid, and the best selectivity (also the yield) of hexadecane and pentadecane is 80.56 and 19.43%, respectively.
研究领域:
材料科学
·
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 110
·108217-108228
·
IF 3.289
Lujiang Xu,Zheng Han,Ying Zhang,Yao Fu
The vapor phase hydrodeoxygenation (HDO) of lignin-derived phenols under H2 atmosphere has great significance for producing high-quality fuels and commodity chemicals. Herein, we reported a simple, green method to prepare molybdenum oxide@N-doped carbon (MoOx@NC) via in situ pyrolysis of molybdenum precursor preloaded cellulose and demonstrated its catalytic performance for vapor phase HDO of lignin-derived phenols. When the pyrolysis temperature was at 600 °C, the catalyst (MoOx@NC-600) exhibited the best catalytic performance in vapor phase HDO of guaiacol. Through systematically investigating the parameters, such as: reaction temperature, WHSV, residence time, and concentration, the optimal reaction conditions for vapor phase HDO of guaiacol were 450 °C and 1 h−1 with atmospheric H2. The concentration of the feed was 20% in mesitylene, and the residence time was about 3.3 s. The carbon yield of aromatic hydrocarbons was 83.3%, with 65.7% benzene, 15.5% toluene and 2.1% alkylbenzenes. In addition, other lignin-derived phenols were also investigated and desired results were achieved with the MoOx@NC-600 catalyst. Furthermore, MoOx@NC-600 showed good stability due to the N-doped carbon formed on the surface of the MoOx particles. The catalysts were characterized using elemental analysis, AAS, BET, XRD, XPS, TEM, and EDS mapping. The high catalytic performance of MoOx@NC-600 toward lignin-derived phenols HDO can be attributed to the synergistic effect of the carbon supports and Mo5+ (molybdenum oxynitrides), Moδ+ (Mo2N) and Mo4+ on the surface of the MoOx particles.
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
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