FUEL
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2021
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IF 6.609
Xinyue Zhang,Bo Zhang,Yanjun Chen,Lei Li,Houxiang Sun,Xuandong Liu,Rong Guo,Bo Meng,Peng Liu,Weiyu Song,Qiaoxia Guo,Baojian Shen
Electronic structure tuning is an effective strategy to activate transition metals. In this study, silica-promoted γ-Al 2 O 3 -supported Fe-based hydrodesulfurization catalysts of Fe species with electron loss were successfully prepared by transferring electrons from Fe to Si. The characterization results showed that the Fe-based hydrodesulfurization catalyst with the addition of silica modulated the structure and properties of the active metal, which not only improved the degree of sulfidation of the active metal but also promoted the generation of Fe(III)-S. The hydrodesulfurization rate of dibenzothiophene showed a remarkable rise from 38.4 to 83.2% at 673 K. Importantly, the formation of Fe(III)-S greatly stretched the bond length of Fe-S bonds, exhibiting an increase of approximately 21%, this facilitating the generation of coordinatively unsaturated active site. Finally, the HDS reaction performance of the Fe-based hydrodesulfurization catalysts was mainly influenced by the Fe(III)-S/Fe(II)-S ratio, with the most significant enhancement in the direct desulfurization reaction path. The results of this study provide a promising approach for the design and development of environmentally friendly and economical Fe-based catalysts in the field of clean fuels.
研究领域:
催化
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化学工程
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材料科学
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环境化学
✓ 已验证
DOI
高影响因子
JOURNAL OF HAZARDOUS MATERIALS
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2023
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IF 13.6
Haoran Yu,Changmin Liu,Shuo Liu,Yu Gu,Shuya Wang,Ali Yaraş,Linchao Hu,Wenyi Zhang,Mingguo Peng,Hasan Arslanoğlu,Linqiang Mao
Spent petroleum refining catalyst is regarded as the important secondary resource for valuable metals. However, common recycling strategies, including soda roasting, acid and alkaline solutions leaching and chemically precipitation, produced large quantities of high salinity wastewater. This study proposed an efficient method to recovery of Mo and Ni from the spent hydrodesulfurization (HDS) catalyst via O 2 -rich roasting and organic acid leaching with the advantage of less salinity wastewater production. The transformation of Mo(IV) into soluble Mo(VI) was enhanced by O 2 -rich atmosphere roasting, and 98.64% of Mo(IV) was oxidized at 650 ℃ for 2 h in atmosphere containing 30% of O 2 . The oxidation process of Mo(IV) was agreed with the shrinkage pore model, and regulated by surface reaction and internal diffusion. 97.97% of Mo(VI) was leached from roasted product by oxalic acid , separated with complexation extraction agent of Ala-TBP and recovered as (NH 4 ) 8 Mo 10 O 34 and (NH 4 ) 2 Mo 3 O 10 by evaporative crystallization. Ni was leached out from spent catalyst with 1 mol/L acetic acid, and precipitated as NiC 2 O 4 with oxalic acid . 95.92% of Mo and 96.77% of Ni were recovered from spent HDS catalyst with this recycling route. This study provided a high-efficient and eco-friendly method to recovery of valuable metals from spent catalyst.
研究领域:
环境科学
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冶金工程
✓ 已验证
DOI
PubMed
高影响因子
ANALYTICAL CHEMISTRY
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2020
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IF 6.785
Shu-Jian Zheng,Jie Zheng,Cai-Feng Xiong,Hua-Ming Xiao,Shi-Jie Liu,Yu-Qi Feng
Identification of metabolites at the trace level in complex samples is still one of the major challenges in untargeted metabolomics. One formula in the metabolomic database is always corresponding to more than one candidate, which increases the difficulty and cost in the subsequent process of standard compound matching. In this study, we developed an effective method for amine metabolite identification by hydrogen–deuterium scrambling (HDS) based on chemical isotope labeling coupled with liquid chromatography–mass spectrometry (HDS–CIL–LC–MS). After d4-4-(N,N-dimethylamino)phenyl isothiocyanate (d4-DMAP) labeling, the labeled amine metabolites can produce HDS under collision-induced dissociation (CID). The HDS can effectively reflect the number of labile hydrogen atoms in amine metabolites and thus distinguish amine isomers with different functional groups. The developed HDS–CIL–LC–MS method was applied to the determination of amine metabolites in mice feces, in which the amine candidates obtained by the database based on chemical formula searching were reduced by 64% on average, which greatly reduces the cost of standard compound matching. Taken together, the developed HDS–CIL–LC–MS analysis was demonstrated to be a promising method for untargeted metabolomics and a novel strategy for deciphering tandem mass spectrometry (MS2) spectra.
研究领域:
分析化学
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代谢组学
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质谱
✓ 已验证
产品关联
DOI
PubMed
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2025
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IF 9.7
Hongyang Lv,Fengyu Tian,Xingxing Cui,Zhenkun Chen,Guangzheng Sun,Yuan Pan,Yichuan Li,Bin Dong,Bin Liu,Yongming Chai,Chenguang Liu
With the trend of heavy and inferior crude oil, the design of hydrodesulfurization (HDS) catalysts with excellent activity and high active metal utilization is an inevitable trend for the upgrading of refining technology. In this study, a highly dispersed Mo catalyst confined within nitrogen-doped porous carbon (xMo@NC) was prepared using an in situ encapsulation-pyrolysis approach and used in the HDS reaction of dibenzothiophene (DBT). The methods of XRD, HRTEM, HAADF-STEM, N 2 physisorption, FT-IR, Raman, and XPS were used to carry out thorough microstructural characterization. The results demonstrated that the Mo species in xMo@NC were highly dispersed, exhibiting superior intrinsic HDS activity compared to MoS 2 /NC* catalysts and conventional supported catalyst MoS 2 /Al 2 O 3 . The xMo@NC catalyst exhibited significant direct desulfurization (DDS) pathway in the HDS reaction of DBT. Differential charge density and bader charge suggested that significant electron transfer between the sulfur atom of DBT and the Mo species of xMo@NC, which weakened the C S bond and made it easier to remove sulfur via DDS pathway during the HDS reaction. This work presents a new catalytic material with high intrinsic activity and enhanced DDS desulfurization selectivity, providing fresh perspectives on the creation of high-performance HDS catalysts.
研究领域:
催化化学
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化学工程
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材料科学
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石油炼制
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表面化学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
FUEL
·
2024
·
IF 6.7
Guosheng Li,Yu Ding,Xiaohan Li,Kunhong Li,Xinrui Yin,Liang Zhao,Shenyong Ren,Chunming Xu,Baojian Shen
Regulation of electronic structure of metal active phase for catalysts has been known as efficient in promoting its catalytic activity; however, manipulating the activity of catalysts via controllable metal active phase electronic structure is still challenging. A non-equilibrium electronic structure Fe-based bulk catalyst has been developed via controllably adding P species, where the non-equilibrium electronic structure of Fe species is formed through the electron transfer from the Zn species through the P electronic channel. As a result, the catalytic activity of the modified Fe-based bulk catalysts has increased by 24.4–50.4%. Meanwhile, the sulfurization degree (SD) of the modified Fe-based bulk catalysts has increased by 5.6–25.9%. In addition, the HDS reaction rate constant ( k HDS ) has increased by about 2.0 times, and the DDS reaction rate constant ( k DDS ) has increased by about 2.4 times. The P modifying can regulate the directional transfer of unpaired free electrons between Fe and Zn species to form a more non-equilibrium electronic structure of Fe species, which can reduce the energy barrier of the C–S bond adsorbed on the P-modified Fe-based bulk catalysts. Importantly, the P species can be used as an active site to adsorb S-containing compounds in the modified Fe-based bulk catalysts, which is conducive to generating more coordinatively unsaturated sites (CUSs). The former can promote the formation of the more non-equilibrium electronic structure of Fe species, and the latter can adjust the adsorption active site of S-containing on the catalyst surface. Therefore, an electron transfer channel is formed among Fe, Zn, and P species, and another one is formed among Fe, P, and S-containing compounds, which form a dual-channel electron transfer behavior. Furthermore, the specific surface area, total pore volume, and reducibility of the modified Fe-based bulk catalysts have also shown varying degrees of improvement via the controllable addition of P species.
研究领域:
催化
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材料科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
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