APPLIED ENERGY
·
2022
·
IF 11.446
Tan Li,Jing Su,Huiyuan Wang,Cong Wang,Wen Xie,Kaige Wang
NiMo-doped catalysts were investigated for the conversion of lignin to drop-in fuel through catalytic hydropyrolysis. The influence of NiMo-doped catalysts with different carriers and Ni/Mo molar ratios on the hydropyrolysis product distribution were studied using both lignin and lignin model compounds. Two coefficients were proposed to qualitatively evaluate the catalytic performance of NiMo-doped catalysts. Low yield of methane (13.04c%) and high yield of condensable hydrocarbons products (25.82c%) with low selectivity of polyaromatics (4.37%) were obtained at 1.0 MPa H 2 and 400 °C catalytic temperature during lignin catalytic hydropyrolysis over Ni 1 Mo/ZrO 2 . The hydrodeoxygenation activity of Ni x Mo/ZrO 2 depends on Ni 0 , Mo 4+ , and Mo 3+ . The synergistic effect of Ni and Mo promotes the removal of the phenolic methoxy group. The increase in hydrogen pressure tends to make hydrogen to be consumed through hydrocracking and hydrogenation reactions. The influence of Ni 1 Mo/ZrO 2 on evolution of lignin hydropyrolysis volatiles was revealed. Ni shows strong activity in the removal of phenolic hydroxyl groups and benzene ring hydrogenation, while Mo tends to remove phenolic methoxy groups.
研究领域:
化学工程
·
能源科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Wenwu Zhou,Yanan Zhang,Xiujuan Tao,Yasong Zhou,Qiang Wei,Sijia Ding
The effects of gallium (Ga) modification on mesoporous Al 2 O 3 (MA) were studied, focusing on the morphology changes of the active phases and the application as catalyst support for catalytic performances for dibenzothiophene (DBT) hydrodesulfurization (HDS). MA samples with wide mesopore size distribution (MA-W), double mesopore size distribution (MA-D) and single mesopore size distribution (MA-S) were synthesized from the boehmite sol–gel via a hydrothermal synthesis method. The synthesized MA-S sample was modified with Ga 2 O 3 , and the corresponding sulfide NiMo supported catalysts were prepared. The as-synthesized samples were characterized by XRD, N 2 physisorption, NH 3 -TPD, H 2 -TPR, HRTEM and XPS. Superior catalytic performance was observed over the NiMo/MA-S-2Ga catalyst due to the moderate interaction between the active metals and the supports; the superior morphology for Ni promoted MoS 2 crystals, the highest sulfidation degree, the largest proportion of the NiMoS phase and the enhanced hydrogenation activity caused by the introduction of Ga species.
研究领域:
催化材料
·
化学工程
·
能源化学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2019
·
IF 14.229
Wenwu Zhou,Li Yang,Lang Liu,Zhiping Chen,Anning Zhou,Yating Zhang,Xinfu He,Faxiang Shi,Zegao Zhao
Highly ordered mesoporous TiO 2 -Al 2 O 3 composites with different TiO 2 mass contents (MA-xTi) were successfully synthesized via an improved solvent evaporation-induced self-assembly method and the corresponding NiMo supported hydrodesulfurization (HDS) catalysts were prepared via wetness incipient co-impregnation method. The materials were characterized by means of XRD, ICP-OES, N 2 physical adsorption-desorption, SEM, TEM, Py-FTIR, H 2 -TPR, HRTEM and XPS and the catalytic activities for 4,6-dimethyldibenzothiophene (4,6-DMDBT) HDS over the prepared NiMo/MA-xTi series catalysts were investigated. The results show that the crystal forms, crystal morphologies, pore structures, pore arrangements and acidity properties of the MA-xTi samples varied with the incorporation and increase of TiO 2 species; the interaction between the active metals and the support materials (MSI) can be modulated by the incorporation of TiO 2 species, and TiO 2 incorporation also can promote the formation of the so-called “Type II” NiMoS active phase via changing the morphology of Ni promoted MoS 2 slabs, promoting the sulfidation of both Ni and Mo species and enhancing the proportion of NiMoS phase. The catalytic evaluation results show that the enhancement in the overall HDS activity of the NiMo/MA-xTi series catalysts were mainly contributed by the enhancement in the hydrogenation desulfurization (HYDS) activity. Catalyst NiMo/MA-20Ti exhibited the superior catalytic performance due to its highly ordered mesopore arrangement, proper acidity, moderate MSI, moderate stacking and high proportion of NiMoS phase which leads to more highly active “Type II” active sites.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
APPLIED CATALYSIS A-GENERAL
·
2018
·
IF 4.521
Shilei Ding,Zhixia Li,Fuwei Li,Zhaohe Wang,Jiangfeng Li,Tingting Zhao,Hongfei Lin,Congjin Chen
Reduced NiMo catalysts were prepared by loading NiMo elements on a γ-Al 2 O 3 -β-zeolite composite support, followed by reduction with hydrogen at temperatures in the range of 400–600°C. The hydrogenation activities were investigated through treatment of stearic acid (SA), and were compared with those obtained with the composite support and the oxidized NiMo catalyst (Cox). In the tested reduction temperature range, the catalyst reduced at 450°C (T450) achieved the highest conversion (close to 100%) and C18 hydrocarbon selectivity (58.0%), which were much higher than the results obtained over the composite support and Cox. Reduction treatment contributed to production of more reducible metal species and improvement of the dispersity of metal active sites, consequently leading to high hydrodeoxygenation activity. Furthermore, the effects of H 2 pressure and the hydrogen-donor (tetralin) on the catalytic activity of T450 were investigated. Higher H 2 pressures promoted SA conversion and C18 selectivity. In contrast with dodecane as a solvent, tetralin significantly promoted the formation of C18 in a H 2 atmosphere, but improved the production of C17 and suppressed the formation of lighter hydrocarbons (≤C16) in a N 2 atmosphere. This is associated with the hydrogen-donating activity of tetralin.
研究领域:
催化化学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2017
·
IF 3.752
Huan Liu,Quanzhen Liu,Jianzhong Zhang,Changlong Yin,Yuxin Zhao,Shumeng Yin,Chenguang Liu,Wanfu Sun
The effect of polyvinyl pyrrolidone (PVP) on the physicochemical properties and catalytic activities of unsupported NiMo catalysts was studied. The NiMo catalyst precursors were synthesized by a PVP-assisted chemical precipitation method, by adding various contents of PVP to a Ni- and Mo-containing solution. A series of techniques, including CHSN analysis, XRF , XRD, N 2 adsorption-desorption, FT-IR, SEM, TG-DSC, TPR, and XPS, were used to characterize the NiMo oxide precursors and sulfided catalysts, and the catalytic activities were tested in the hydrodesulfurization (HDS) of dibenzothiophene (DBT). The characterization results revealed that PVP was efficiently removed due to low contents in the synthesis and high solubility in water. The pore properties and hysteresis loop , the agglomeration of the nanoparticles , and the reducibility of the NiMo precursor were affected by the introduction of PVP, while the phases of the precursors and the thermal stabilities were little changed. Ni 3 S 2 and MoS 2 phases were observed in the sulfided catalysts. The catalysis results revealed that the hydrogenation pathway was predominant in the HDS of DBT. A NiMo catalyst synthesized with 0.5 g PVP showed a higher conversion of DBT than the other NiMo catalysts, possibly due to efficient formation of the ‘NiMoS’ active phase. This facile, scalable, and cost-effective route to prepare unsupported NiMo catalyst with enhanced HDS activities would be attractive in industrial applications.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2018
·Vol. 8
·期 32
·18059-18066
·
IF 2.936
Kaihong Xie,Yanxiong Fang,Baoyu Liu,Chengchao Li
Novel composites made from monodispersed porous Al-glycolate spheres (NiMo/Al-SP) were synthesized through alcoholysis or hydrolysis treatments. The obtained samples were characterized by a complementary combination of X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), N2 physisorption, scanning electron microscopy (SEM), transmission electron microscopy (TEM), hydrogen temperature-programmed reduction (H2-TPR), and pyridine Fourier transform infrared spectroscopy (Py FT-IR). In addition, the catalytic performances of the resultant catalysts were evaluated in the simultaneous HDS of dibenzothiophene (DBT) and HYD of naphthalene (DBT and naphthalene represent the sulfur-containing compounds and polycyoalkanes, respectively). The experimental results showed that, 71.22% DBT and 88.28% naphthalene were converted by NiMo/Al-SP(H) under the conditions of 270 °C temperature, 5 MPa H2 (initial pressure at room temperature) and 10 h reaction time. The design and preparation of NiMo/Al-SP provide an effective and novel pathway for the development of high-performance catalysts and production processes.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
RSC Advances
·
2021
·Vol. 11
·期 60
·37932-37941
·
IF 3.361
Ge Guo,Wenzhi Li,Tauseef Ahmed,DuoDuo Hu,Ru Cui,Baikai Zhang,Xia Zhang
Non-noble bimetallic NiMo supported on zeolitic imidazolate framework-derived porous carbon (NiMo@FDC) catalyst for lignin depolymerization has been successfully developed. The synergism between Ni and Mo species in NiMo@FDC catalyst could promote the catalytic cleavage of C–O linkages in Kraft lignin. At a low reaction temperature of 240 °C and under 4 MPa H2, the lignin liquefaction yield was 98.85 wt% and minimum coke yield was 1 wt%, particularly when using 10%NiMo@FDC catalyst. Additionally, at a high reaction temperature of 300 °C and under 2 MPa H2, there was an overall yield of 86 wt% of liquid product and 42 wt% of petroleum ether soluble product. The higher heating value (HHV) increased from 27.65 MJ kg−1 to 34.11 MJ kg−1. In the cycling experiment, the bifunctional catalyst also demonstrated reversability and stability. The synergy of Ni hydrogenation sites and Mo coupled adsorption sites identified a possible mechanism path, which could offer considerable potential for lignin depolymerization.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
DOI
PubMed
高影响因子
JOURNAL OF MATERIALS SCIENCE
·
2022
·Vol. 57
·期 6
·4180-4196
·
IF 4.682
Yu Xiaohang,Dong Yanzeng,Jia Haining,Li Xin,Wang Zhiheng,Liu Yanyan,Gao Ruiyao,Yao Songdong
Multilayered, spatially ordered and highly permeable three-dimensional cross-network porous carbons were prepared from waste superabsorbent polymer (SAP) and were used as supports for NiMo hydrodesulfurization (HDS) catalysts. The acidified SAP-based carbon support and the corresponding catalyst were characterized by FT-IR, XRD, N 2 adsorption–desorption, NH 3 -TPD, TG, SEM, TEM, XPS and H 2 -TPR. The results show that the acidification of the SAP-based carbon support optimizes the pore structure, increases the acidic surface functional groups, enhances the interaction between the metal and the support, and significantly improves the catalytic hydrodesulfurization performance of the catalyst. Liquid phase acidification can produce defects and wrinkles on surfaces of carbon material and form interconnected voids on spongy catalyst. Further acidification with nitric acid vapor is helpful to form a three-dimensional cross-network structure with multilayer, spatial order and high permeability. Under the same metal Mo loading and high reaction temperature, HDS performance of DBT and 4,6-DMDBT of the NiMo catalyst supported on acidified SAP is better than that of the commercial NiMo catalyst. Graphical Abstract
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Hao Zhang,Qing Zhang,Guang-Ren Qian,Hong Liu,Yang Yue
In this research, a bimodal mesoporous AlMCM-41 (B-AM41) material was prepared and applied to support NiMo catalysts for the hydrodesulfurization (HDS) of 4,6-dimethyldibenzothiophene. Additionally, catalysts supported on smaller and larger single-pore AlMCM-41 (S-AM41 and L-AM41) were also prepared as reference catalysts. Detailed characterizations show that the proportion, stacking degree, and length of the MoS 2 active phase on the different catalysts are distinct. As a result, HDS evaluation indicates that the NiMo/B-AM41 catalyst exhibited better catalytic activity with a reaction rate constant of 10.4 × 10 −8 mol g −1 s −1 and a turnover frequency of 7.0 × 10 −4 s −1 , significantly surpassing the S-AM41 and L-AM41 supported catalysts. The superior activity of the NiMo/B-AM41 catalyst can be attributed to a high sulfidation degree that provides sufficient highly dispersed type Ⅱ MoS 2 phases with minimal stacking and moderate slab length. Moreover, the bimodal mesoporous structure promotes the diffusion of 4,6-DMDBT and benefits its contact with active sites.
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
ACS Catalysis
·
2017
·
IF 10.614
Wenwu Zhou,Meifang Liu,Qing Zhang,Qiang Wei,Sijia Ding,Yasong Zhou
Mesoporous MY-xGa zeolites exhibiting both crystallized pore walls and narrowly dispersed mesopores with different Ga content were successfully synthesized. The synthesized samples were characterized by XRD, N2 adsorption desorption isotherms, SEM, TEM, XPS, FTIR, 29Si MAS NMR, 71Ga MAS NMR, and Py-FTIR methods. The results show that the synthesized samples exhibit unique open channel like mesopore systems and outstanding crystallite natures; no nonframework Ga species were observed over the MY-xGa series samples, and their acidic properties can be modulated by varying the Ga/Al ratio in the initial synthesis gel. The corresponding NiMo/HMY-xGa catalysts were prepared via the incipient wetness coimpregnation method; the morphologies of the sulfide catalysts were characterized by HRTEM, and the covalent states of the active metals were characterized by XPS. The catalytic activities of the investigated catalysts for the 4,6-DMDBT HDS reaction were assessed, and the collected products were analyzed by GC and GC-MS methods. The catalyst NiMo/HMY-0.5Ga showed the highest catalytic activity due to the synergistic effect of modulated acidic properties, excellent morphology, highest sulfidation degree, and proper proportion of NiMoS phase. More importantly, 4-MDBT, DBT, and BP were observed and identified as the products of the 4,6-DMDBT HDS reaction, designated as the demethylation pathway (DM) for the 4,6-DMDBT HDS reaction. Finally, a reaction network including DDS, HYD, ISO, and DM pathways for the 4,6-DMDBT HDS reaction over catalyst NiMo/HMY-0.5Ga was proposed.
研究领域:
催化化学
·
材料科学
✓ 已验证
DOI
高影响因子
CHEMISTRY-A EUROPEAN JOURNAL
·
2017
·Vol. 23
·期 39
·9369-9382
·
IF 5.317
Wenwu Zhou,Yasong Zhou,Qiang Wei,Lin Du,Sijia Ding,Shujiao Jiang,Yanan Zhang,Qing Zhang
Graphical Desulfurization : The effects of gallium modified HUSY zeolite acidic co-supports on the hydrodesulfurization (HDS) activity and isomerization selectivity of highly refractory organosulfur compounds such as 4,6-dimethyldibenzothiophene have been investigated. The effects of metal-modified acidic co-supports on the hydrodesulfurization (HDS) activity and isomerization selectivity of highly refractory organosulfur compounds such as 4,6-dimethyldibenzothiophene have been investigated. Y zeolite crystals with high Si/Al ratios and small crystallite sizes were successfully synthesized by a new hydrothermal synthesis approach. The synthesized Y zeolite crystals were ion-exchanged and stabilized. The prepared samples were then modified with different gallium contents using an impregnation method to adjust their acidity properties, and these modified samples were used as co-supports for NiMo sulfide HDS catalysts. The catalyst containing 10 wt.% zeolite Y modified by 2 wt.% gallium (NiMo/2GaY-ASA-A) exhibited the highest HDS activity, with 4,6-dimethyldibenzothiophene (4,6-DMDBT) conversion nearly double the rate of the catalyst without zeolite at 563 K, 4.0 MPa and liquid hourly space velocity (LHSV) of 40 h −1 . NiMo/2GaY-ASA-A also exhibited superior isomerization ability, with 3,4′-DMBP, 4,4′DMBP, and 3,6-DMDBT as the main products, indicating that the isomerization pathway was the main reaction route over NiMo/2GaY-ASA-A. The superior catalytic performance is related to the synergistic effect of the proper amount of medium and strong Brønsted acid sites. The compounds 3,6-DMDBT and 3,7-DMDBT (isomers of 4,6-DMDBT) and 3,4,6-TMDBT and tetra-methyl-DBT (transmethyl products) were detected simultaneously in the HDS product of 4,6-DMDBT for the first time over NiMo/GaY-ASA-A catalysts. Finally, a new reaction network over NiMo/2GaY-ASA-A was proposed.
研究领域:
催化化学
·
材料科学
·
能源化工
✓ 已验证
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·
IF 9.3
Shan Jiang,Riyang Shu,Anqi Wang,Zhuoli Deng,Yuhong Xiao,Jiajin Li,Qingwei Meng,Qian Zhang
High-quality liquid biofuels can be produced from renewable lignin-derived phenolic compounds through the efficient hydrodeoxygenation (HDO) process, in which the traditional catalysts usually include metal site and acid site that catalyzes hydrogenation and deoxygenation procedures respectively. This work presented a novel acid-free NixMoyN/C catalyst from the perspective of green chemistry, providing a new pathway for HDO of lignin-derived phenolic compounds that involves hydrogenation, deoxygenation and hydrogenolysis at the same time. A series of NixMoyN/C catalysts were prepared by varying Ni and Mo molar ratio, where the Ni1Mo3N/C catalyst showed the best HDO performance. Guaiacol was completely converted at 260 °C after 4 h, with 95.8% cyclohexane selectivity. And a small amount of benzene can be obtained as a valuable fuel additive by-product by altering the conventional HDO reaction path. By shortening the reaction time, benzene can be obtained as the intermediate products with a relative high selectivity. Based on the characterizations of XRD, BET, SEM, TEM, XPS, H2-TPD and EPR, the results demonstrate that the multiple active components of Ni1Mo3N/C catalyst allow it to efficiently catalyze the hydrogen activation and C-O bond cleavage even under acid-free condition. The existence of the active phase of Ni, Ni2Mo3N and β-Mo2C, as well as the interaction between Ni and Mo metals, contributes together to achieve an efficient HDO performance. Not only for the various phenolic model compounds, the feasibility of Ni1Mo3N/C catalysts for upgrading raw lignin-oil was also demonstrated, with the hydrocarbon content increasing from 5.7% to 88.4%. Notably, arenes account for 18.2% in the hydrocarbon products, which confirms the occurrence of hydrogenolysis in the catalytic process. This work provides a novel route for the conversion of lignin-derived phenolic compounds to the production of high-quality hydrocarbon liquid biofuels, especially the direct production of arene component.
研究领域:
化学工程
·
催化
·
可再生能源
·
绿色化学
✓ 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）