ChemCatChem
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2022
·Vol. 14
·期 12
·e202200274
·
IF 5.497
Na Ji,Shuai Cheng,Zhichao Jia,Hanyang Li,Poknam Ri,Shurong Wang,Xinyong Diao
Graphical Working together : The establishment of Co 0 -Al 2 O 3 @USY interface via in-situ growth of CoAl-LDH on USY surface rendered the high activity in HDO of lignin to naphthenes which were attributed to the synergetic effect between Co 0 sites and USY, in which Co 0 sites were responsible for hydrogenation and acid sites on USY were responsible for deoxygenation. To enhance the catalytic activity and stability of metal catalysts in the hydrodeoxygenation of lignin derivatives into naphthenes, a bifunctional Co−Al 2 O 3 @USY catalyst was fabricated by the reduction of CoAl layered double hydroxide in-situ grown on the USY zeolite. In the hydrodeoxygenation of guaiacol, a 100.0 % conversion with cyclohexane yield up to 93.6 % was achieved at 180 °C, 3 MPa for 4 h, which should be the hitherto lowest reaction temperature that has been reported over Co-based metal catalysts. This catalyst was also relatively stable with 5 runs and exhibited excellent catalytic performance in the hydrodeoxygenation of other lignin model compounds and even real lignin feedstock into naphthenes. The high-efficiency of Co−Al 2 O 3 @USY was attributed to the synergistic effect between well-dispersed small Co nanoparticles and abundant acidic sites on the USY surface, while the outstanding stability was attributed to the anchoring effect of Al 2 O 3 matrix to Co nanoparticles which avoided the leaching of Co species and particle agglomeration. This work provides a potential strategy for the design of an efficient and stable catalyst for lignin utilization.
研究领域:
催化化学
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能源化学
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材料科学
✓ 已验证
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Shanshan Shao,Laixin Ma,Xiaohua Li,Huiyan Zhang,Rui Xiao
Heavy bio-oil based carbon material (HBC) was prepared via carbonization and activation, and the basic Mg-Al-O/HBC using HBC as the carrier was synthesized for the first time for the aldol condensation of cyclopentanone to produce aviation fuel precursor. It revealed that a higher carbonization temperature and heating rate led to the decreasing production of biochar. HBC presented the highest specific surface area (2046.92 m 2 /g) and total pore volume (1.2964 cm 3 /g) at the carbonization temperature of 700 °C, the heating rate of 15 °C/min, A/C ratio of 3:1, and the activation temperature of 800 °C, in which the largest proportion of micropores was 87.19%. Compared with Mg-Al-O, a higher strength of weak and moderate basic sites was found in Mg-Al-O/HBC, which was beneficial for the aldol condensation. A higher yield of targeted condensates in the range of C9∼C16 was achieved at 87.28% in the aldol condensation of cyclopentanone over Mg-Al-O/HBC catalyst. However, the condensation performance of the composite catalysts decreased seriously in the 5th run, which was related closely to the appearance of boehmite AlO(OH) and the pore blockage of HBC. To match the basic catalyst and HBC carrier well from the viewpoint of pore property, Al ions were substituted with Zr ions, and the yield of the target condensates over Mg-Zr-O/HBC was kept stably at 72.07% at the fifth use. This study provides a unique, viable and effective method to produce porous carbon from heavy fraction of bio-oil as the carbon source, and also its good application in the production of high-valued fuels.
研究领域:
能源科学
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催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL PHYSICS LETTERS
·
2023
·
IF 2.8
Wujian Zhang,Xiangdong Zhou,Hui Sun,Zhenxiang Li,Kangjun Wang,Panpan Zhang,Wenfeng Han,Ying Li,Haodong Tang
The activated alumina with different specific surface areas and different acidity was used to catalyze the dehydrofluorination reaction of CF 3 CH 2 F (HFC-134a). The catalytic performance of the alumina catalysts was rationalized by analyzing the relationship between specific surface area and acidity before and after fluorination. A series of physiochemical techniques, including Scanning Electron Microscope (SEM), X-ray diffraction (XRD), and N 2 physical adsorption (BET), were used to investigate the changes in catalyst structure and surface morphology before and after being tested for the dehydrofluorination reaction. The Al 2 O 3 catalyst prepared from the precipitation method (Al 2 O 3 -P) demonstrated the best stability among all the Al 2 O 3 catalysts. Results from XRD techniques showed that Al 2 O 3 catalysts were fully or partially fluorinated into AlF 3 after the dehydrofluorination reaction. Al 2 O 3 -B catalyst and Al 2 O 3 -S catalyst containing mainly α-AlF 3 deactivate easier than the Al 2 O 3 -P catalyst, which has primarily β-AlF 3 . In addition, it can be concluded the high surface area Al 2 O 3 -P catalyst still has the highest specific surface area and pore size when fluorinated to AlF 3 , while forming the β-AlF 3 crystalline phase. Therefore, it has the optimum catalytic performance for dehydrofluorination of HFC-134a. This provides a new idea for designing alumina catalysts with reasonable structure.
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
ChemistrySelect
·
2023
·Vol. 8
·期 10
·e202204379
·
IF 2.1
Yang Wang,Xinbao Li,Pan Li,Xinbo Zhu,Geng Chen,Yingying Zhu
Graphical Acetic acid is a main component of biomass pyrolysis oil. A high yield of hydrogen is obtained through steam reforming of acetic acid over a tungsten-modified Co/Al 2 O 3 catalyst. The interaction between the reactants and the catalyst surface is enhanced. Steam reforming of bio-oil is a promising green hydrogen production technology. Experimental and theoretical calculations have been carried out to study the performance of Co/Al 2 O 3 catalysts doped with tungsten (1–10 wt%) for bio-oil model compound acetic acid steam reforming. The maximum acetic acid conversion of 95.4 % and H 2 yield of 93.5 % were obtained over the 15Co-5W/Al 2 O 3 catalyst under the optimized reaction conditions of temperature=550 °C, steam to carbon ratio=5 and the gas hourly space velocity of 15,780 h −1 . The feeding capacity of the catalyst was improved by 2.3 times by the addition of 5 wt% W compared to that of the non-W-added Co/Al 2 O 3 catalyst. Catalyst characterizations by BET, XRD, H 2 -TPR, XPS, HRTEM, and SEM were performed. The results showed that high activities were maintained over 20 h on the 15Co-5W/Al 2 O 3 catalyst. A little filamentous coke was formed on the spent catalyst surface, and the agglomeration rate of active Co was relatively low. Density functional theory calculations confirmed that the adsorptions of CH 3 COOH and H 2 O on the catalyst were enhanced by the addition of W.
研究领域:
能源化学
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催化材料
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2019
·Vol. 21
·期 18
·5046-5052
·
IF 9.405
Ziwei Guo,Feng Zhou,Hao Wang,Xiaohao Liu,Guangyue Xu,Ying Zhang,Yao Fu
A novel and green catalytic system based on a Pd stabilized CuZnAl catalyst was designed for one-pot conversion of natural oil components to the corresponding alcohols or long-chain linear and branched alkanes with high selectivity and atom economy. When methyl decanoate was used as the model compound, a nearly full yield of n-decanol was obtained at 200 °C and 2 MPa H2 within 8 h. 100% decane was produced when acidic HZSM-5 was introduced under the same reaction conditions, and the selectivity of n-decane and i-decane could be tuned by temperature. Cu species were verified as the active sites for lipid conversion, while a small amount of Pd could stabilize the catalyst to avoid Cu leaching. The reaction pathway involved hydrogenation, where methyl decanoate can be equivalently converted to methanol and decanol or decane, and no extra CO2 or CO from decarboxylation or decarbonylation was detected. This system increases the sustainability and economy of natural oil conversion to valuable liquid fuel and chemicals.
研究领域:
催化化学
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绿色化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2022
·
IF 8.035
Rui Cao,Xueqian Wang,Ping Ning,Yibing Xie,Langlang Wang,Yixing Ma,Xiang Li,Hui Zhang,Jingye Liu
Basic sites are important to promote carbonyl sulfide (COS) and carbon disulfide (CS 2 ) hydrolysis activity while improving the oxidation resistance of hydrolysis catalysts is a challenge. Here, we report an N -doped alumina-based catalyst ( N -K@Al), where the complete hydrolysis removal of COS and CS 2 by the N -doped catalyst was extended up to 15 h at 160 °C, and the turnover frequency (TOF) value of the catalyst was increased from 0.85 × 10 -2 s −1 to 1.16 × 10 -2 s −1 . The results showed that the strong interaction between nitrogen and potassium decreased the reactive oxygen density and activated –OH, weakening the oxygen mobility. In addition, the beneficial effects of N -doped included the addition of moderately and weakly basic sites by pyridine N. The optimized N -K@Al showed good catalytic performance in the hydrolysis of COS and CS 2 removal with lower reaction temperature and higher total hydrogen sulfide yield. Density functional theory calculations revealed that N -K@Al reduced the Gibbs free energy of COS and CS 2 hydrolysis to 0.21 eV and 0.33 eV, respectively, contributing to the enhanced catalytic activity. The present study presents new strategies for developing efficient antioxidant organosulfur hydrolyzers and other practical industries.
研究领域:
催化化学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2014
·Vol. 2
·期 29
·11091-11098
·
IF 0
Lina Li,Hao Ren,Ye Yuan,Guangli Yu,Guangshan Zhu
Currently, synthesis of most porous organic frameworks (POFs) requires noble metals as the main catalyst. Herein we report a low-cost and straightforward synthetic strategy to develop porous aromatic frameworks (PAFs). With AlCl3 as the catalyst, the Scholl coupling reaction could occur between the phenyl rings of aromatic compounds. Using 3-dimensional monomers, such as triphenylamine, tetraphenylmethane, tetraphenylsilane, and tetraphenylgermane, we successfully obtained a series of PAFs with moderate Brunauer–Emmett–Teller (BET) surface areas ranging from 515 m2 g−1 to 1119 m2 g−1. Among the obtained PAF materials, PAF-41 exhibited the best CH4 and CO2 sorption capacity with CH4 (1.04 mmol g−1) and CO2 (3.52 mmol g−1) at 273 K. In addition, PAF-43 demonstrated its comparably high isosteric heat of adsorption at 34.8 kJ mol−1 for CO2 and 29.7 kJ mol−1 for CH4. It is also worth mentioning that the developed approach also overcomes typical flaws of some classic PAFs, such as high cost and complexity of precursor preparation.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
FUEL
·
2022
·
IF 8.035
Miao Zuo,Xinyu Wang,Wenlong Jia,Yanzhong Zhu,Xianhai Zeng,Lu Lin
As one of the essential building blocks for bio-chemicals and bio-fuels, the 5-Hydroxymethylfurfural (HMF) production is still challenging in a green and cheap way. This work developed a bio-derived aqueous-natural deep eutectic solvent (A-NADES) to synthesize HMF using α-Al 2 O 3 or Al(OH) 3 as robust catalysts, obtaining high yields of 67.1% and 63.6% HMF from glucose under mild reaction reactions, respectively. Different kinds of starches and starchy food waste also exhibited high conversion efficiency in the A-NADES system. The mechanistic study indicated that the in-situ formed Al (III) site of α-Al 2 O 3 during the reaction was critical for converting glucose-based carbohydrates. A-NADES could be effectively reused six times with a more convenient direct reuse method without significant activity loss. This study suggested a novel A-NADES reaction media in the synergistic reaction with robust aluminum-based catalysts for HMF synthesis, and proposed a novel process of food waste utilization in green solvents.
研究领域:
生物化学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
RENEWABLE ENERGY
·
2022
·
IF 8.634
Yuewen Shao,Jie Wu,Zhiyuan Zheng,Mengjiao Fan,Kai Sun,Félix Mérimé Bkangmo Kontchouo,Lijun Zhang,Shu Zhang,Guangzhi Hu,Xun Hu
Production of cyclopentanone (CPO) from biomass-derived furfural is attractive but challenging, as deep hydrogenation or ring-opening of furan ring in furfural over Co-based catalysts hinders the formation of the targeting products. In this study, alloying Co with Fe species in Co–Fe–Al catalysts is proposed for selective conversion of furfural to CPO in water. The formation of CoFe alloy in Co–Fe–Al catalyst weakened the interaction between Co species and the alumina carrier, lowered the adsorption/activation of H 2 , suppressed the formation of especially Brønsted acidic sites, facilitated the electron transfer from Co 0 to Fe species, increased the activation energy for hydrogenation of furfural (from 17.2 kJ mol −1 over Co–Al to 33.4 kJ mol −1 over 1.5Co-1.5Fe-1.0Al), and weakened the adsorption of C C and C–O–C functionalities in furan ring of furfuryl alcohol (FA) on metallic sites. These factors together suppressed deep hydrogenation of furan ring in FA or ring-opening of FA to diols, producing CPO and CPL with total yield of 91.5%, which was attributed to the synergy between hydrogenation and Brønsted acidic sites. In addition, the presence of Fe in Co–Fe–Al catalysts also enhanced the structural stability of Co species, preventing the phase transformation and aggregation of Co species, and rendering the catalyst with superior reusability .
研究领域:
催化化学
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生物质能
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Omega
·
2020
·
IF 2.87
Ning Shi,Qiying Liu,Ying Liu,Lijun Chen,Hongyan Zhang,Longlong Ma
The soluble byproducts formed during the hydrothermal conversion of cellulose catalyzed by solid tungstated alumina (AlW) were analyzed by LC–MS and LC–MS2 to determine their formulas and possible structures. These identified soluble compounds could be roughly divided into four species of carboxylic acids, α-carbonyl aldehydes, carbocyclic compounds, and furanic compounds with molecular mass in the range of 90–220 Da. Compared with the noncatalytic condition, the addition of AlW could increase the selectivity of carboxylic acids (especially α-hydroxy acid) from cellulose and suppress the formation of furanic compounds, carbocyclic compounds, and hydrochar. Based on the product distribution, the hydrothermal conversion route of glucose was proposed by regarding the formed α-carbonyl aldehydes as the key intermediates for formation of carboxylic acids, carbocyclic compounds, and furanic compounds.
研究领域:
化学工程
·
生物质能
·
催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
ENVIRONMENTAL SCIENCE AND POLLUTION RESEARCH
·
2014
·Vol. 21
·期 21
·12563-12568
·
IF 2.757
Shen Shuguang,Li Meina,Li Binbin,Zhao Zhijun
In order to find an effective method for treating urea wastewater, the experiments on the hydrolysis of urea in wastewater were conducted in a fixed bed reactor with different aluminas (α-Al 2 O 3 , γ-Al 2 O 3 , and η-Al 2 O 3 ) as catalysts respectively in contrast with inert ceramic particle. The results indicate that the three alumina catalysts show obvious catalytic activity for urea hydrolysis at 125 °C. The order of activity is η-Al 2 O 3 > γ-Al 2 O 3 > α-Al 2 O 3 , and the activity difference increases with increasing temperature. According to the characterization results, surface acidity has little impact on the activity of catalyst. However, it was found that surface basicity of alumina catalyst plays an important role in catalytic hydrolysis of urea, and the activity of catalyst may be also influenced by the basic strength. With η-Al 2 O 3 as catalyst, the urea concentration in wastewater is reduced to 4.96 mg/L at a temperature of 165 °C. Moreover, the η-Al 2 O 3 shows a good stability for urea hydrolysis. The hydrolysis of urea over η-Al 2 O 3 catalyst can evidently reduce the reaction temperature and is promising to replace industrial thermal hydrolysis process.
研究领域:
环境科学
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催化化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CELLULOSE
·
2022
·Vol. 29
·期 4
·2257-2272
·
IF 6.123
Shi Ning,Zhu Yuju,Qin Bangzhi,Liu Ying,Zhang Hongyan,Huang Hongsheng,Liu Yunhua
A simple and efficient biphasic system comprising H 2 O, tetrahydrofuran (THF), cyclohexane (CHX) and Al 2 (SO 4 ) 3 was employed to convert cellulose into 5-hydroxymethylfurfural (HMF). The volume ratio of the organic phase to the aqueous phase (V org /V aque ), concentration of Al 2 (SO 4 ) 3 in the aqueous phase (C[Al 2 (SO 4 ) 3 ] aque ) and concentration of Al 2 (SO 4 ) 3 in the organic phase (C[Al 2 (SO 4 ) 3 ] org ) of the biphasic system played critical roles in the conversion of cellulose into HMF. In the biphasic systems with H 2 O/THF/Al 2 (SO 4 ) 3 of 4/18/0.4 and H 2 O/THF/CHX/Al 2 (SO 4 ) 3 of 3/16/3/0.4, > 80% of the added H 2 O was dissolved in the organic phase, whereas most of the added Al 2 (SO 4 ) 3 remained in the aqueous phase under the reaction temperature, jointly leading to high V org /V aque , high C[Al 2 (SO 4 ) 3 ] aque and low C[Al 2 (SO 4 ) 3 ] org in the biphasic system. All of these results yield the excellent performance of these biphasic systems in the conversion of cellulose into HMF. The addition of CHX into the biphasic system can decrease the solubility of Al 2 (SO 4 ) 3 in the organic phase, thus improving the stability of HMF in the reaction system. The influences of catalyst usage, reaction temperature and time, and cellulose/solvent ratio were all explored, and a high HMF yield of 71.2% was obtained in the H 2 O–THF–CHX biphasic system with an H 2 O/THF/CHX volume ratio of 3/16/3 under optimized conditions. Graphical abstract
研究领域:
化学工程
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生物质能
✓ 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）