INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Zhi-Cong Wang,Pei-Gao Duan,Xiao-Jie Liu,Feng Wang,Yu-Ping Xu
The low-boiling-point distillate (LBD) via vacuum distillation of biocrude produced from hydrothermal liquefaction of soybean straw was hydrotreated to produce trace-sulfur liquid fuel. The effects of five hydrogen donor solvents (HDSs), including cyclohexene, cyclohexane, decahydronaphthalene, tetrahydronaphthalene, and Indane, on heteroatom removal efficiency were examined at 350 °C for 2 h with 6 MPa H2 added and 5 wt %(Pt/C)/feed. The LBD to HDS mass ratio was 1:1. HDSs not only could reduce the production of solid and gas and increase the yield of upgraded oil but also could favor denitrogenation, desulfurization, and deoxygenation of the upgraded oil. Among the HDSs examined, decahydronaphthalene showed the best performance for denitrogenation, and tetrahydronaphthalene was the most suitable HDS for deoxygenation and desulfurization. By employing a decahydronaphthalene and tetrahydronaphthalene mixture (w/w, 1:1) as the reaction medium, the effects of temperature (300–450 °C), time (1–6 h), H2 pressure (0.1–10 MPa), and Pt/C loading (0–20 wt %) on the product yields and quality of the upgraded oil produced from hydrotreating the LBD were examined. The upgraded oil was the dominant product fraction under all tested reaction conditions and varied between 76.7 and 87.3 wt %. The HDS mainly acted as a hydrogen transfer agent in the LBD hydrotreatment process, during which the HDS provided the hydrogen for the hydrogenation reaction, and this consumed hydrogen was resaturated by the external hydrogen source. A more positive synergistic effect was observed for the removal of N, O, and S when using the decahydronaphthalene and tetrahydronaphthalene mixture than when using decahydronaphthalene or tetrahydronaphthalene alone. N was the most difficult heteroatom to remove, followed by O and S. Catalyst loading was the most influential factor affecting the N, O, and S removal efficiencies. Under optimal reaction conditions, 93% of N, 95% of O, and 99% of S in the LBD and HDS blend were removed, which corresponded to contents of 0.05 wt %, 0.42 wt %, and 21 ppm in the upgraded oil, respectively. The equilibrium restrictions on denitrogenation, deoxygenation, and desulfurization were essential factors affecting the removal efficiencies of heteroatoms.
研究领域:
能源生物学
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化学工程
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产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Hao Bi,Zhiwei Wang,Hao Zhan,Lijian Leng,Zhiyong Zeng,Xinming Wang,Huacai Liu,Xiuli Yin,Chuangzhi Wu
Chinese herbal residue (CHR) is an association of renewable resource and hazardous waste , and high nitrogen content and low energy density are two primary obstacles to its efficient and clean thermal utilization. In this paper, acid-promoted hydrothermal was employed to probe the feasibility on CHR toward enhanced solid biofuel concerning upgradation and denitrogenation. A more excellent hydrothermal promoter (H 2 SO 4 ) was demonstrated to upgrade and denitrogenate CHR with better energy (1.125) and nitrogen densities (0.586) at optimal conditions (160 °C, 0.5 N H 2 SO 4 ), which could be attributed to the improved removal of oxygen, amino and ash during acid-promoted hydrothermal. Compared to raw feedstock or the conventional hydrochar , the acid-promoted hydrochar had enhanced compositional characteristics with higher heating value (21.00 kJ·mol −1 ), lower nitrogen (1.44 wt%) and ash (11.03 wt%) contents, thus showing more stable combustion flame with a higher comprehensive combustion index of 4.861 × 10 −8 , a higher combustion stability index of 4979.342, lower combustion alkali index of 0.026, and less nitrogen gaseous pollutant emission. Thus, acid-promoted hydrothermal would be a promising way to convert CHR into much cleaner and higher-grade solid biofuel.
研究领域:
能源与环境科学
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生物质能工程
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产品关联
DOI
高影响因子
JOURNAL OF MOLECULAR LIQUIDS
·
2022
·
IF 6.633
Chenhua Shu,Hua Cheng,Min Zhao,Dan Luo,Feng Zhu,Haijiao Xie
In this work, three deep eutectic solvents (DESs) triethylamine/formic acid ([Et 3 N/FA]), triethylamine/acetic acid ([Et 3 N/PA]), triethylamine/propionic acid ([Et 3 N/AA]) were synthesized and were used for extractive denitrogenation of model oil. Among them [Et 3 N/PA] exhibited reasonably high extraction efficiency for both indole and quinolone. Structure optimization, electrostatic potential analysis and reduced density gradient analysis were performed to explore the synthesis mechanism of DESs and extractive denitrogenation mechanism by DESs taking [Et 3 N/PA] as a representative. The structure of [Et 3 N/PA] were characterized by FTIR and NMR. Results indicate that both strong hydrogen bond and van der Waals are the major force for DESs synthesis. Both hydrogen bonds and van der Waals are responsible for indole removal, while only van der Waals is responsible for quinolone removal. The effect of factors on extraction efficiency was also investigated and results indicate that [Et 3 N]/[PA] has the advantages of short equilibrium time, ability to deal with fuel oils with a wide range of nitrogen contents, excellent performance near room temperature. The presence of olefins and aromatics in fuel oil has negligible negative influence on the extraction efficiency of indole and quinolone. Furthermore, [Et 3 N/PA] exhibits excellent regeneration performance. Consequently, [Et 3 N/PA] is a promising extractant for fuel oil denitrogenation.
研究领域:
化学工程
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环境科学
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产品关联
DOI
高影响因子
DALTON TRANSACTIONS
·
2023
·Vol. 52
·期 11
·3517-3525
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IF 4
Shihui Wang,Zhoujun He,Ling Wu,Deling Wang,Ruiru Si,Xiyao Liu,Ruowen Liang
Due to their explicit structure, metal–organic frameworks (MOFs) have been supposed to be credible platforms to research the micro-mechanism of heterogeneous photocatalysis. In this study, amino-functionalized MOFs (MIL-125(Ti)–NH2 (denoted as MTi), UiO-66(Zr)–NH2 (denoted as UZr) and MIL-68(In)–NH2 (denoted as MIn)) with three different metal centers were synthesized and applied for the denitrification of simulated fuels under visible light irradiation, during which pyridine was used as a typical nitrogen-containing compound. The results showed that MTi had the best activity among the above three MOFs, and the denitrogenation rate increased to 80% after 4 h of visible light irradiation. On the grounds of the theoretical calculation of pyridine adsorption and actual activity experiments, it can be presumed that the unsaturated Ti4+ metal centers should be the key active sites. Meanwhile, the XPS and in situ infrared results verified that the coordinatively unsaturated Ti4+ sites facilitate the activation of pyridine molecules through the surface –N⋯Ti– coordination species. The coordination–photocatalysis synergism promotes the efficiency of photocatalytic performance and the corresponding mechanism is proposed.
研究领域:
材料科学
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环境科学
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化学工程
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产品关联
DOI
PubMed
高影响因子
PETROLEUM CHEMISTRY
·
2021
·Vol. 61
·期 9
·1052-1060
·
IF 1.029
Liu Linhai,Xie Wenjing,Liu Xunzheng,Fang Hansun,Wen Yangping,Shu Chenhua
Abstract In this study a class of DESs based on triethylamine (TEA) and aromatic acids
was synthesized and used in the extractive denitrogenation of model oil fraction
firstly. The structures of DESs were characterized by nuclear magnetic resonance
and Fourier transform infrared spectrometer. The factors that influence
extraction efficiency and distribution coefficient were investigated. The
extraction performance of TEA/ o -hydroxybenzoic acid (OHBA) is better than that of TEA/benzoic acid
and TEA/ o -methylbenzoic acid. The extraction
efficiencies of quinoline and indole reach up to 99.1 and 98.3% only through two
extraction stages, respectively. The extraction efficiency is not sensitive to
reaction temperature and initial nitrogen content. The DESs based on TEA and
aromatic acids exhibit excellent regeneration performance. In summary, the DESs
based on TEA and aromatic acids are excellent extracting agents for basic and
non-basic nitrogen compounds and will become promising extracting agents for the
oil fraction denitrogenation.
研究领域:
化学工程
·
石油加工
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DOI
高影响因子
INTERNATIONAL JOURNAL OF REFRACTORY METALS & HARD MATERIALS
·
2025
·
IF 4.6
Zhongyou Que,Xingyu Li,Lin Zhang,En Mei,Chenguang Guo,Haishen Sun,Junming Liu,Mingli Qin,Gang Chen,Xuanhui Qu
The in-situ synthesis of finely dispersed second phases with high melting points and thermal stability is an effective strategy to address the high cost, inadequate high-temperature performance, and reduced thermal conductivity of tungsten‑rhenium (W Re) alloys. In this study, we employed a novel nitridation-denitridation (NDN) process to synthesize W-10Re-HfN nano powder, in-situ synthesizing nano HfN particles to strengthen and toughen the W Re alloy. Compared to W 10Re, the hardness of W-10Re-2HfN increased significantly from 604 HV to 977 HV, the compressive strength was improved from 1366 MPa to 2181 MPa, and fracture strain increased from 3.6 % to 32 %. Statistical results indicate that HfN particles within the grains or with sizes below ∼36 nm exhibit completely coherent interfaces with the W Re matrix. By combining in-situ synthesis of nitrides with a two-step sintering process, we successfully retained 63 % of HfN particles within the grains and controlled the average particle size of HfN particles at the grain boundaries to be 36 nm, thereby enhancing grain boundary strengthening and coherent interface strengthening. This study innovatively incorporates finely dispersed and highly stable nitrides into W Re alloys through in-situ doping, offering a novel strategy for reinforcing refractory metals.
研究领域:
材料科学
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机械工程
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产品关联
DOI
高影响因子
CATALYSIS TODAY
·
2016
·
IF 4.312
Peigao Duan,Caicai Zhang,Feng Wang,Jie Fu,Xiuyang Lü,Yuping Xu,Xianlei Shi
This study examined a two-stage (noncatalytic pretreatment followed by catalytic upgrading) hydrothermal processing of crude bio-oil produced from the hydrothermal liquefaction of duckweed. The activities of six activated carbons (ACs)-pine wood AC, coconut shell AC, bamboo stem AC, apricot pit AC, peach pit AC, and coal AC-toward the deoxygenation and denitrogenation of the pretreated duckweed bio-oil were determined in supercritical water at 400 °C for 1 h with the addition of 6 MPa of H 2 and 10 wt% AC. All of the ACs exhibited activity similar to Ru/C toward the denitrogenation and deoxygenation of the pretreated duckweed bio-oil. Of the ACs tested, bamboo stem AC produced an upgraded bio-oil with the highest yield (76.3 wt%), the highest fraction (90.13%) of material boiling below 350 °C, and the highest energy density (44.1 MJ/kg). Decreased ash and acidic groups in the pre-treated AC disfavored the production of upgraded bio-oil but aided denitrogenation and desulfurization. The ACs are suspected to leach ions and weak acids into the reaction solution, which would catalyze denitrogenation and desulfurization. The gases mainly consisted of unreacted H 2 , CO 2 and CH 4 together with small amounts of C x H y ( x ≤ 5, y ≤ 12) hydrocarbon gases produced from the cracking of the upgraded bio-oil.
研究领域:
能源植物学
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环境科学
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DOI
高影响因子
RSC Advances
·
2020
·Vol. 11
·期 2
·700-710
·
IF 3.119
Shurong Gao,Jiaxin Jin,Masroor Abro,Ruozhen Song,Miao He,Xiaochun Chen
Extractive denitrification (EDN) of shale oil using ionic liquids (ILs) as the extracting agent has good industrial prospects. In such processes, ILs with higher selectivity to N-compounds and lower solubility in shale oil are desired to improve the EDN efficiency, and reduce the loss of ILs and the contamination of shale oil. In the present study, we employed COSMO-RS to calculate the selectivity of 70 ILs to the typical N-compounds (pyridine, quinoline and indole). The influence of the IL structural characteristics, composition of shale oil and properties of N-compounds are investigated from a micro-level view with the σ-surface and σ-profile. The selectivity strongly depends on anionic species and it is greatly influenced by hydrogen bonding (HB) and π–π interaction between N-compounds and ILs. ILs composed of [H2PO4]− and [MeSO3]− with larger HB donor energy show higher selectivity to the basic N-compounds, while ILs composed of [Ac]− with larger π-electron cloud density show higher selectivity to the non-basic N-compounds. Anions with stronger polarity have lower solubility in shale oil. Moreover, experimental determinations of EDN indicated that [C4py][H2PO4]/[C4mim][H2PO4] and [C2mim][Ac]/[C2py][Ac] have good EDN performance for quinoline/pyridine with efficiency of 100% and for indole with efficiency of 91%, respectively. This work presents a theoretical basis to design and select ILs having higher selectivity for N-compounds and lower solubility in shale oil for use in denitrification.
研究领域:
化学工程
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材料科学
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产品关联
DOI
PubMed
高影响因子
Micro & Nano Letters
·
2019
·Vol. 14
·期 13
·1287-1292
·
IF 0.975
Feng Wang,Jie Li,Long Xu,Feng Jiang,Jianfeng Zhang
In this work, the study of synthesis and denitrogenation of magnetic polymeric ionic liquids (PILs) for N-compounds in simulated oils and diesel are reported. Three functionalised magnetic particles, Fe 3 O 4 @SiO 2 @PILs with side alkyl chain of C2, C4 and C6, respectively, were prepared by grafting PILs on the surface of silica-coated Fe 3 O 4 . Fourier transform infrared spectra, thermogravimetric analysis, X-ray diffraction and scanning electron microscopy were carried out to characterise the structure of Fe 3 O 4 @SiO 2 @PILs. It has shown that Fe 3 O 4 @SiO 2 @ PILs possess precious merits for sorbents, such as regular morphology, good stability and magnetic properties. Denitrogenation experiments of simulated oils demonstrate that Fe 3 O 4 @SiO 2 @ PILs show better denitrogenation efficiency of basic N-compounds than neutral N-compounds. The effects of temperature, reaction times, ratio of reagent to oil on denitrogenation for simulated oils were explored, and 92.1% denitrogenation efficiency was obtained to remove quinoline from simulated oils. Denitrogenation of Fe 3 O 4 @SiO 2 @PILs in diesel leads to 84.3% denitrogenation efficiency, and it can remain 82.5% denitrogenation efficiency after five times of recycles. Compared with other similar sorbents, Fe 3 O 4 @SiO 2 @PILs show competitive performances to eliminate organic N-compounds. It is hopeful that Fe 3 O 4 @SiO 2 @PILs can be promising sorbents for purification of liquid fuel by adsorptive denitrogenation.
研究领域:
化学工程
·
材料科学
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产品关联
DOI
高影响因子
TOPICS IN CATALYSIS
·
2017
·Vol. 60
·期 12
·987-996
·
IF 2.486
Wang Wei,Li Xiang,Wang Anjie,Sun Zhichao,Chen Yongying
A series of mixtures of NiCl 2 , hypophosphites (NaH 2 PO 2 and NH 4 H 2 PO 2 ), and additives were used as precursors (denoted as x additive: y hypophosphite: z NiCl 2 , where x, y , and z represents the molar ratios of the compounds) for the synthesis of Ni 2 P both in N 2 and H 2 plasma. The catalytic performances of the obtained catalysts were evaluated by the hydrodenitrogenation (HDN) of quinoline (Q) and decahydroquinoline (DHQ). Ni 2 P was stoichiometrically synthesized by the treatment of 1.0NH 4 H 2 PO 2 :2.0NiCl 2 with N 2 plasma at a low total power input of 8 W (40 V × 0.2 A). In H 2 plasma, the precursor was over-reduced to a mixture of Ni and Ni 2 P, with Ni 2 P as the minor phase. The over-reduction can be inhibited by the addition of proper amount of alkali-metal chloride (NaCl or KCl) or P 2 O 5 . CaCl 2 facilitated the reduction of nickel salts to Ni. KCl was the best among the additives investigated. Both the surface and bulk over-reduction of 1.0NH 4 H 2 PO 2 :2.0NiCl 2 was inhibited by KCl, while P 2 O 5 mainly inhibited the bulk over-reduction. The addition of KCl strongly suppressed the hydrogenation of Q to DHQ, but facilitated the HDN of DHQ. On the other hand, not only the hydrogenation of Q but also the dehydrogenation of DHQ was substantially inhibited by P 2 O 5 .
研究领域:
材料科学
·
催化化学
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DOI
高影响因子
ACTA PHYSICO-CHIMICA SINICA
·
2013
·Vol. 29
·期 11
·2422-2428
·
IF 0.869
WANG Zhao-Yang,LI Gang,SUN Zhi-Guo
Sulfonic acid functionalized MIL-101(Cr) (S-MIL-101(Cr)) are obtained by sulfonation of MIL-101(Cr) (Cr3F(H2O)2O[(O2C)-C6H4-(CO2)]3·nH2O (n~25)) using triflic anhydride
and sulfuric acid. The amount of sulfonic groups in the framework can be controlled by changing the molar ratio of MIL-101(Cr), triflic anhydride, and sulfuric acid. The sulfonated samples were characterized by X-ray diffraction (XRD), Fourier transform infrared (FTIR) spectroscopy, nitrogen
physical adsorption/desorption, acid-base potentiometric titration, and thermogravimetric analysis (TGA). The results show that the sulfonated samples retain the general structure of MIL-101(Cr), but the specific areas and pore diameters decrease. The sulfonated samples formed with between
0.21 and 0.42 mmol·g-1 of sulfonic acid groups. The adsorptive denitrogenation of a model fuel by different S-MIL-101(Cr) samples was investigated in batch adsorption experiments. Sulfonation can strengthen the interactions between nitrogen-containing compounds (NCCs) and
the adsorbent. The sample obtained using a molar ratio of n(MIL-101(Cr)):n(H2SO4):n(Tf2O)=1:3:4.5 had the largest adsorption capacity for quinoline and indole. Compared with the bare MIL-101(Cr), this sulfonated material showed enhancement
of the maximum adsorption capacity by 12.2% and 6.3% for quinoline and indole, respectively. Regeneration of the used adsorbent was conducted by washing with ethanol, and the adsorptive capacity for NCCs from the model-fuel showed no obvious decrease after three cycles of use.
研究领域:
化学工程
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材料科学
✓ 已验证
DOI
高影响因子
RSC Advances
·
2016
·Vol. 6
·期 18
·14993-15001
·
IF 3.289
Mu Li,Yinguang Chen,Yinglong Su,Rui Wan,Xiong Zheng
The influences of three fulvic acids, referred to as SAFA (purchased from Shanghai Aladdin Reagent Company), SRFA (Suwannee River Fulvic Acid from International Humic Substances Society (IHSS)) and PPFA (Pahokee Peat Fulvic Acid from IHSS), with different chemical composition, structure, hydrophobicity and aromaticity degree on biological wastewater denitrification were investigated. It was found that SAFA remarkably enhanced the denitrification performance, while SRFA and PPFA had no obvious effect. Mechanistic study revealed that SAFA remarkably improved the metabolism of a carbon source (glucose) by stimulating the activities of key enzymes (hexokinase, 6-phosphofructose kinase, glyceraldehyde-3-phosphate dehydrogenase (GAPDH), and pyruvate kinase) involved in glycolysis. The increase of glucose utilization resulted in the increase of intracellular NADH/NAD+ ratio that favored microbial denitrification. Meanwhile the bacterial growth was significantly improved in the presence of SAFA. Further studies revealed that SAFA also increased the activities of key denitrifying enzymes, including nitrate reductase (NAR), nitrite reductase (NIR), nitric oxide reductase (NOR), and nitrous oxide reductase (N2OR), thus enhancing the reduction of nitrate and transformation of its intermediates, especially nitrite and nitrous oxide. All the above positive effects posed by SAFA might be attributed to its lower molecular weight, less complex aromatic structures with predominantly aliphatic carbons and higher hydrophilicity than SRFA and PPFA, which lead to a more active interaction with denitrifying microorganisms via metabolism process regulation. A better knowledge of the relationship between molecular structure of fulvic acids and microbial denitrification activity may be of practical interest in the nitrogen cycle in nature's niches.
研究领域:
环境科学
·
微生物学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）