ORGANIC PROCESS RESEARCH & DEVELOPMENT
·
2014
·
IF 2.549
Kai Dong,Cheng H. Sun,Jian W. Song,Gai X. Wei,Si P. Pang
Synthesis of 2,6,8,12-tetraacetyl-2,4,6,8,10,12-hexaazaisowurtzitane (TAIW) by catalytic hydrogenolysis of 2,6,8,12-tetraacetyl-4,10-dibenzyl-2,4,6,8,10,12-hexaazaisowurtzitane (TADBIW), a key step for the synthesis of 2,4,6,8,10,12-hexanitro-2,4,6,8,10,12-hexaazaisowurtzitane (HNIW), has been first implemented under continuous flow conditions using the commercially available H-Cube Pro reactor. Several variables (i.e., reaction temperature, flow rate, and pressure) and the stability of the system have been investigated to optimize the operating conditions. The results show that a continuous flow system provides a better yield than a batch system. For instance, the yield is 99% at the optimized conditions, while the best yield from batch reactions is 92%. Continuous flow synthesis of TAIW has potential applications in improving the production technologies of HNIW for its many advantages over batch reactions.
研究领域:
化学合成
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2014
·
IF 5.039
Yong Gang Sun,Yulong Ma,Zheng Wang,Junkang Yao
A combinative pretreatment technology of steam explosion (SE) and alkali was applied to enhance hydrogenolysis conversion of corn stalk into polyol with Ni–W 2 C or Fe–Mn–K catalyst. The results showed that treatments corn stalk with 0.4 MPa SE and alkali removed 84.16 wt% of hemicellulose and 71.83 wt% of lignin and thereby increased the cellulose content from 31.54 to 80.41 wt%. But the glucose loss was insignificant during pretreatment. Data from catalytic hydrogenolysis showed that pretreatment corn stalk with 0.4 MPa SE and alkali improved the yield of polyol, and about 20.38 wt% of ethylene glycol and 52.36 wt% of glycerol were produced after catalysis with Ni–W 2 C/(coconut shell activated carbon, CSAC). Based on the yield of polyol, the catalytic performance of Ni–W 2 C/CSAC was significantly better than those of Ni–W 2 C/(coal-based activated carbon) and Fe-Mn-K/(amorphous carbon).
研究领域:
生物化学
·
可再生能源
✓ 已验证
产品关联
DOI
PubMed
高影响因子
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
ENERGY & FUELS
·
2018
·
IF 3.024
Da Wang,Yuyang Wang,Xiaoyu Li,Lei Chen,Guangci Li,Xuebing Li
In situ catalytic hydrogenolysis of lignin is an efficient method for lignin valorization. Herein, a novel in situ lignin catalytic hydrogenolysis technique in alkaline aqueous solution over a NiAl alloy catalyst under mild conditions was systematically suited. Ni served as the active phase and could be exposed by etching Al atoms with alkaline aqueous solution. Meanwhile, H2 resources could be in situ generated and easily arrived at the adjacent exposed Ni sites to be activated. The in situ lignin hydrogenolysis system exhibits attractive depolymerization results under mild conditions, with an 86.8% conversion degree and 18.9 wt % yield of aromatic monomers at 220 °C, much higher than the traditional hydrogenolysis method using a commercial Raney Ni catalyst under high pressure external H2. The mechanism studies with lignin model compounds suggest that alkaline aqueous solution could promote the cleavage of C–O–C bonds and hinder the hydrogenation of the benzene ring. In addition, a moderate amount of exposed Ni sites as well as rich active hydrogen species are determinant for efficient lignin depolymerization.
研究领域:
化学工程
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生物质能
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2021
·
IF 6.609
Ying Hu†,Haiwei Jiang†,Mei Hu,Yunyan Liu,Fenghua Zhao,Weiran Yang
As-enriched Pteris vittata L. (PVL, a kind of hyper-accumulator biomass) was converted into high-quality biofuel by the catalytic hydrogenolysis, aiming to achieve effective treatment and high-value utilization of hyper-accumulators. After pretreatment of PVL to remove lipids and lignin, more than 64% of heavy metals were transferred into water, and the As content in the solid biomass was reduced from 1328 mg/kg to 483 mg/kg. The multifunctional catalysts RhCl 3 /NaI/HCl/H 2 were used in a biphasic reaction system to convert PVL into biofuel with high selectivity. The main products are C5 and C6 furans and low oxygen content ketones, which have a high heating value (HHV) and can be directly used as biofuel. The highest yields of C5 and C6 products were obtained with 60.2% and 61.1% (based on the corresponding hemicellulose and cellulose) under the optimal reaction conditions (160 °C, 4 h, 300 psi H 2 , 4 mmol NaI, H 2 O/toluene = 1:1). The total biofuel yield based on dry PVL was 18.8 wt.%. After the reaction, more than 50% heavy metals (Cu, Pb, Zn, Cd, As) remained in the bio-char, while the heavy metals in the biofuel were less than 20% (As content was less than 55 mg/kg). Therefore, catalytic hydrogenolysis was perceived as a promising technique for PVL treatment to obtain high-quality biofuel and arsenic recovery.
研究领域:
环境科学
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能源科学
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植物学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
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2020
·
IF 6.274
Guanyi Chen,Juping Liu,Xiangping Li,Jianguang Zhang,Han Yin,Zhenping Su
In this work, HZSM-5, Al-SBA-15 and Al-SBA-15/HZSM-5 were adopted as supporting materials for the nickel-based catalysts used in hydrodeoxygenation process. Incipient wetness impregnation method was employed to load nickel species onto these materials. The physicochemical characterization was carried out using advanced instruments. The effect of composition of nickel-based catalysts on hydrodeoxygenation (HDO) reaction was studied. Support materials of nickel-based catalyst have a significantly impact on HDO activity. The highest selectivity (67.9%) of propyl-cyclohexane was obtained over nickel based Al-SBA-15/HZSM-5 catalyst, and nearly all the eugenol was completely hydrodeoxygenated after reaction. The impact of light fractions existed in bio-oil on phenols upgrading process was investigated. The conversion of eugenol mixed with light fractions reached nearly 100% for all the reactions. Eugenol mixed with light fractions as reactant could reduce ring break reaction during hydrodeoxygenation process. The selectivity of alkanes remained nearly unchanged after adding ethylene glycol into the reactant. However, the selectivity of propyl-cyclohexane was significantly decreased by mixing furfural or acetic acid with eugenol as reactant.
研究领域:
化学工程
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能源科学
✓ 已验证
DOI
高影响因子
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
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2024
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IF 7.7
Haonan Xue,Haihong Xia,Hui Li,Fei Ge,Wei Xu,Xiaohui Yang,Minghao Zhou
Lignin represents a significant source of aromatic hydrocarbons in the natural world. The production of high-value chemicals from lignin has the great potential to effectively address the issue of fossil energy scarcity. In this study, complex sulfides of nickel‑cobalt bimetallic catalysts were prepared via hydrothermal synthesis and subsequently employed in the catalytic hydrogenolysis of C O bonds present in lignin. A series of complex sulfides Ni 3 S 2 /Co 3 S 4 -CS n -x-T derived from lignin-MOF ( n = 0.5, 1, 1.5 and 2; x = 2, 4 and 6; T = 400, 500, 600 and 700 °C), were prepared under different conditions and subsequently employed in the catalytic hydrogenolysis of lignin model compounds. The optimal catalyst Ni 3 S 2 /Co 3 S 4 -CS 1 –4-500 exhibited the highest conversion rate of benzyl phenyl ether (BPE) (about 97.3 %), and the yields of toluene and phenol produced were 49.5 % and 43.6 %, respectively with isopropanol as the reaction solvent and no external H 2 . The introduction of element sulfur in catalysts could effectively inhibit the further hydrogenation of generated aromatic chemicals. The catalysts were well characterized, and the results demonstrated that the catalysts exhibited high catalytic activity with an increased loading of active components. This study provided some novel findings for the construction of biomass-based catalysts and the production lignin-derived aromatic chemicals.
研究领域:
生物质化学
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催化材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Reaction Chemistry & Engineering
·
2021
·Vol. 6
·期 3
·465-470
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IF 4.239
Hang Zhang,Shimin Kang,Jinxia Fu,Yunbing He,Xiangxuan Huang,Jie Chang,Yongjun Xu
Poly(butylene succinate) (PBS), a biodegradable plastic, is expected to have a huge consumer product market in the near future. In this work, PBS was found to be an excellent source of producing valuable tetrahydrofuran (THF), through a solvent-less catalytic hydrogenolysis process over a Pd/C catalyst. A high THF yield, 59.5 wt%, was achieved via a simple one-pot reaction under mild temperature conditions (240 °C). This technique provides a distinctive but important method for the green production of THF from spent PBS.
研究领域:
化学工程
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环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ENVIRONMENTAL POLLUTION
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2022
·
IF 9.988
Zhigang Zhao,Zheng Li,Xiangkun Zhang,Tan Li,Yuqing Li,Xingkun Chen,Kaige Wang
The catalytic hydrogenolysis of a typical model compound of mulching film waste, polyethylene, was investigated as a potential way to improve economic efficiency of mulching film recycling. Nickel-based heterogeneous catalysts are proposed for polyethylene hydrogenolysis to produce liquid hydrocarbons. Among catalysts supported on various carriers, Ni/SiO 2 catalyst shows the highest activity which may due to the interactions between nickel and silica with the formation of nickel phyllosilicate . As high as 81.18% total gasoline and diesel range hydrocarbon was obtained from the polyethylene hydrogenolysis at relatively mild condition of 280 °C, and 3 MPa cold hydrogen pressure. The result is comparable to what have been reported in previous studies using noble metal catalysts. The gasoline and diesel range hydrocarbon are n-alkanes with a distribution at a range of C 4 –C 22 . The gas products are primarily CH 4 along with a small amount of C 2 H 6 and C 3 H 8 . High yield of CH 4 as much as 9.68% was observed for the cleavage of molecule occurs along the alkane chain.
研究领域:
化学工程
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材料科学
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环境科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2019
·
IF 4.507
Chen Zhu,Jing-Pei Cao,Xiao-Yan Zhao,Tao Xie,Ming Zhao,Xian-Yong Wei
The synergistic catalysis in the catalytic hydrogenolysis (CH) of lignin and its model compounds over a Ni-Ru/AC bimetallic surface was well established. The Ni-Ru/AC exhibits excellent activity and stability for catalytic hydrogenolysis of lignin and its model compound. The additions of Ru into supported Ni/AC can not only improve the overall reactants conversion, but also modify the product distribution. The apparent activation energy (E a ) of BPE hydrogenolysis over Ni-Ru/AC is measured approximately to be 18.3 kJ/mol. This value is considerably lower than the values measured for monometallic Ni/AC (42.4 kJ/mol). Additionally, the turnover frequency (TOF) of Ni-Ru/AC (62.7 h −1 ) was much higher than that of Ni/AC (5.1 h −1 ). In case of CH of lignin, Ni-Ru/AC gave better total liquid yield and higher relative content of main aromatic monomers . The enhancement in the overall hydrogenolysis activity of reactants over bimetallic Ni-Ru/AC is related to the synergistic effect of Ni and Ru. Various characterization methods (XRD, XPS , TEM-EDS, SEM-EDX and BET) are performed to elucidate the formation of synergistic effect. This synergistic effect could originate from the generation of additional surface active sites, small size of metal particles and high dispersion of metal particles.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
BIOMASS & BIOENERGY
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2025
·
IF 5.8
Chunyang Han,Zhen Dong,Yahui Zhang,Haian Xia
Ethylene glycol (EG) and 1,2-propylene glycol (1,2-PG) are very important chemicals that are produced mainly from fossil resources at present. Catalytic hydrogenolysis of biomass (such as cellulose and sugar alcohols) to diols has attracted much attention in recent years. However, compared to sugar alcohols, sugars such as xylose have been scarcely used for the production of EG and PG until now due to their instability and low selectivity of diols. Xylose is an abundant and readily available bio-chemicals that can be produced from the hydrolysis of hemicellulose, but its catalytic hydrogenolysis into diols with high yields remains a great challenge. Herein, bimetallic Ru-Re/CZO(Ce 0.7 Zr 0.3 O 2 ) catalysts were synthesized and used to catalyze the hydrogenolysis of xylose to EG and PG. The nature of the catalysts is thoroughly characterized by XRD, XPS, BET, TEM, etc. It is found that Ru and Re nanoparticles are uniformly distributed on CZO alloy support formed by Ce and Zr. A very high total yield (65.0 %) of EG and 1,2-PG was achieved on the 4 %Ru-1 %Re/CZO catalyst under optimal conditions. Recycling experiments demonstrate that high xylose conversion and diol yields are maintained over four successive cycles under optimal conditions, despite a slight increase in Ru nanoparticle size observed via TEM analysis. The mechanistic study shows that xylose is first isomerized into xylulose, which undergoes retro-aldol cleavage to generate the intermediates, followed by further hydrogenation to EG and 1,2-PG. This work provides a new research avenue for the efficient preparation of diols from xylose.
研究领域:
化学工程
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生物质转化
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催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2025
·
IF 7.3
Mengdi Li,Anyan He,Liheng Deng,Qingmao Yang,Haodong Chu,Chun Shen,Tianwei Tan
Catalytic conversion of cellulose in biomass into 2,5-hexanedione is a significant step for the production of biobased p-xylene (PX), and a precise understanding about the effect of the coexisting hemicellulose and lignin components is extremely essential and desirable, but still severely deficient. Herein, we investigate the above issue by catalytic tests, structural characterizations, and composition analysis. Catalytic tests confirm that the coexisting hemicellulose does not affect cellulose conversion and could be converted into 5-chloro-2-pentanone, while the lignin component plays a detrimental role. Lignin and the oligomers from lignin hydrogenolysis can block the catalytic active sites via deposition due to the strong interaction between lignin and Pd/C catalyst. Meanwhile, there is noncovalent interaction between lignin and cellulose, reducing the accessibility of cellulose to the catalytic active sites including the Pd/C and acidic sites. Basic treatment by NaOH aqueous solution could result in simultaneous removal of lignin and fracture of the biomass structure and hence higher accessibility for the Pd/C catalyst. When the biomass is treated by NaOH with the concentration of 1.0 wt %, the amount of lignin (8.3 wt %) is low enough and the structure is fractured enough to achieve the yield of HDO and DMF comparable to that using sole cellulose as the reactant.
研究领域:
生物质化学
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催化化学
✓ 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）