TRANSACTIONS OF TIANJIN UNIVERSITY
·
2018
·Vol. 25
·期 2
·143-151
·
IF 0
Du Jianzeng,Li Yonghong,Miao Zhenyu
Novel Ni/ZnO – HZSM-5 adsorbents were synthesized by incipient wetness impregnation. The Ni/ZnO – HZSM-5 adsorbent can achieve deep desulfurization and olefin aromatization at the same time. Thiophene sulfur was removed from 495 to less than 10 ppm via reactive adsorption desulfurization (RADS). Olefins were also converted into aromatics. HZSM-5 did not only support adsorbents but also cooperated with active Ni sites to catalyze olefins into aromatic hydrocarbons. Aromatization of 1-pentene, 2-pentene, 2-methyl-2-butene, and 1-hexene on adsorbents was investigated. The adsorbents were characterized by the Brunauer–Emmett–Teller, X-ray diffraction, temperature-programmed reduction, and temperature-programmed desorption of ammonia and thermogravimetric analysis. The experimental results showed that strong acids on the adsorbent disappeared after HZSM-5 loaded active metal sites, and almost no coke was generated on adsorbents in RADS.
研究领域:
化学工程
·
催化材料科学
✓ 已验证
产品关联
DOI
INORGANICA CHIMICA ACTA
·
2022
·
IF 3.118
Mingyan Chen,Dehua Zhang,Ziying Wang,Yao Zhang,Yucheng Liu
UiO-66 loading carboxyl and phosphotungstic acid has a good affinity to thiophene (TH). The synthesized catalyst, changed its original structure, which can increase its reactive site and enhance the interaction with thiophene (TH) in order to improve the adsorption performance. Then the structural changes were analyzed by XRD, FT-IR, SEM, BET, EDS and other characterization methods. Through static experiments of adsorption desulfurization, it is found that when the adsorption time is 240 min, the adsorption temperature is 30 ℃ and the oil-to-agent ratio is 100:1, the adsorption effect: UiO-66-(COOH) 2 (UC2) > UiO-66, the highest adsorption capacity can reach 89.99 mg/g; while PTA@UiO-66 (PAU) can reach adsorption equilibrium at 210 min, it has better desulfurization performance than UiO-66. After being recycled for 5 times, the adsorption effect is only slightly decreased: the adsorption capacity of UC2 was still 78.02% of the initial adsorption capacity, while that of PAU was 76.07% of the initial adsorption capacity. According to the adsorption kinetics, the adsorption process of thiophene on the adsorbent UC2 is more consistent with W-M model, and the adsorption of PAU is more in line with the pseudo-first order kinetic equation. In addition, it also includes the process of intraparticle diffusion and liquid film diffusion.
研究领域:
化学工程
·
材料科学
✓ 已验证
DOI
高影响因子
JOURNAL OF COLLOID AND INTERFACE SCIENCE
·
2025
·
IF 9.7
Yuting Li,Yueyang Xu,Erjian Huang,Liming Kong,Yongping Zeng
Thiophene-like sulfides present in fuel oil release sulfur oxides (SO x ) during combustion, which pose significant risks for both environmental sustainability and public health. Adsorption desulfurization (ADS) has garnered considerable attention because of its mild operating conditions, low production costs, and minimal impact on the octane number of fuels. Metal-organic frameworks used as desulfurizing adsorbents provide several advantages, including a high specific surface area and easily adjustable structures . Here, we synthesized the micro/mesoporous adsorbent CeO 2 @HP-HKUST-1 (CeO 2 @Hierarchical Porous-Hong Kong University of Science and Technology-1) through the hybridization of salicylic acid (SA) using a solvothermal method. We assessed the adsorption performance of CeO 2 @HP- HKUST-1 _ 1.5 for benzothiophene and thiophene through batch and breakthrough adsorption experiments. The adsorption capacities for thiophene and benzothiophene were measured at 21.2 mg S/g and 35.3 mg S/g, respectively. Remarkably, in competitive toluene experiments, the adsorption capacity for benzothiophene remained significant at 28.9 mg S/g, due to enhanced Ce–S bonding interactions and the exposure of unsaturated metal centers of Cu. Additionally, regeneration experiments demonstrated that CeO 2 @HP-HKUST-1 retained excellent adsorption capacities after four cycles. These findings highlight the potential of CeO 2 @HP-HKUST-1 as an effective adsorbent for desulfurization applications.
研究领域:
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
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Jingjing Wang,Jinchuan Zhao,Zhihui Wen,Xinjie Wei,Junjie Liao,Liping Chang,Kechang Xie
CeY zeolite sorbent was reported to have a high adsorptive desulfurization selectivity for thiophene. However, only the cerium in the supercage, which is larger than the thiophene molecule, is effective for thiophene adsorption. In this case, regulating the cerium location to anchor it more in the surpercage of Y zeolite is an important issue. Herein, the glycine was used as a complexing agent with cerium to control its size, ensuring that the cerium precursor is in the supercage. G 0.1 CeY were prepared by ion exchange technique with glycine and cerium coordination from NaY. The adsorption capacity of sorbents was measured, and their physical and chemical properties were characterized by XRD, SEM, N 2 adsorption/desorption, NH 3 -TPD, and in situ FT − IR. The glycine complexation could effectively control the location of Ce, so that the G 0.1 CeY has the highest content of Ce located in the supercage. Moreover, in order to further explore the influence of zeolite type, HY was used as the raw material to prepared G 0.1 CeHY in the same way. G 0.1 CeHY has a higher desulfurization performance than that of G 0.1 CeY, whereas the Ce content in its supercage is lower. The NH 3 -TPD and Py-FT − IR results that the medium-strong Brønsted acid of the G 0.1 CeHY sorbent is also effectively for the improvement of desulfurization efficiency. The G 0.1 CeHY exhibits the hightest desulfurization effectiveness (51 %) and the highest breakthrough adsorption capacity of 5.42 mg/g.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2019
·
IF 8.355
Fazle Subhan,Sobia Aslam,Zifeng Yan,Ayaz Ahmad,U.J. Etim,Muhammad Naeem,Liu Zhen,Muhammad Ikram,Muhammad Yaseen
Lanthanum based adsorbents are promising in adsorptive desulfurization due to high activity. The dispersion degree of La 2 O 3 impacts desulfurization performance directly, and the development of an efficient strategy for La 2 O 3 dispersion still remained challenge. Herein, for the first time confined spaces and silanols of as-synthesized SBA-15 were used for dispersion of La 2 O 3 over mesoporous silica. The La(NO 3 ) 3 precursor is directly introduced into the confined spaces between silica walls and template of as-synthesized SAB-15 by solid state dispersion (SSD) strategy. The SSD strategy assists the formation of small sized La 2 O 3 with excellent dispersion after La precursor decomposition by the combined action of confined spaces and silanols. We also demonstrated that up to 20 wt% La 2 O 3 can be highly dispersed over as-synthesized SBA-15 (LaAS-20). Our investigations show that well-dispersion of La 2 O 3 correspond to high desulfurization activity for fuels, and the amount of thiophene captured can reach 0.12 mmol of S/g over LaAS-20, which is better than that over LaCS-20 and other La-doped reported sorbents. Furthermore, LaAS-20 adsorbent showed good stability and regeneration ability, and has potential applications to be applied in adsorptive desulfurization technology.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2023
·
IF 7.7
Xuzhao Gao,Yueyang Xu,Yan Yin,Ning Gu,Yongping Zeng
The adsorption desulfurization technology presents remarkable advantages and is a promising method because of its affordability, gentle operating conditions. Metal-organic frameworks (MOFs) have garnered significant attention owing to their remarkable features, including large specific surface areas, pore volume and the designable structure. The hierarchical porous CuBTC-DMA was successfully synthesized by adding salicylic acid and using the hydrothermal method. Subsequently, Ni ions were introduced into the structure using ion-exchange method. It was found that the doping of salicylic acid and Ni ions did not significant alter the structure of the material. The new type of π-complexed adsorbent, Ni@HP-CuBTC-DMA, was prepared. The results of adsorption desulfurization experiments showed that Ni@HP-CuBTC-DMA-1.5(0.2 M) had the highest adsorption capacity, with the maximum adsorption amounts of 25.63 mg S/g and 41.06 mg S/g for thiophene and benzothiophene , respectively. In the toluene competition experiment, the adsorption amount of thiophene could still reach 19.25 mg S/g. The results of regeneration experiments demonstrate that Ni@HP-CuBTC-DMA-1.5(0.2 M) still has excellent adsorption capacity after four cycles.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2019
·
IF 3.375
Hua Song,Xiaojuan Li,Bolong Jiang,Mingyue Gong,Tianzhen Hao
A highly active and stable MOF-199-supported ionic liquid [Hnmp][H2PO4] (IL-NP) adsorbent (Py/MOF) was successfully synthesized and characterized via XRD, SEM and TEM, TG-DTG, FT-IR, BET, and XPS technologies. The effects of different sulfides and interfering components present in model oils on the adsorptive desulfurization (ADS) performance of Py/MOF were studied. The results show that the regular octahedron crystalline structure of MOF-199 was well preserved and IL-NP fixed on the surface of MOF-199 presented like a flower after grafting ionic liquid IL-NP. The Py/MOF showed highly ordered canals, which are larger than those of MOF-199. Upon introducing IL-NP to MOF-199, the ADS activities were improved, which can be attributed to the improved intimate contact between sulfur compounds and adsorbent, the additional adsorption acidic sites for slightly basic sulfur compounds, and the increased pore size with mesoporous pores appearing. The ADS activity of Py/MOF adsorbing different sulfides was in the order of DBT > BT > 3-MTP > TP > 2,5-DMTP, and the effect of interfering component on ADS performance of Py/MOF was in the order of cyclohexene > toluene > water > ethanol. After 4 times of regeneration, the DBT removal onto Py/MOF was still at 93.8%, which decreased by 4.9% as compared to that of the fresh adsorbent.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2016
·
IF 5.267
Jun Xiong,Lei Yang,Yanhong Chao,Jingyu Pang,Ming Zhang,Wenshuai Zhu,Huaming Li
Novel BN mesoporous nanowire materials with doped oxygen atoms have been controlled and prepared successfully. Multiple techniques have been employed to determine the structure, morphology, surface feature, defects, and electronic structure. It was the first time that a controlled preparation of this unique structure was applied to adsorptive desulfurization. The obtained BN mesoporous nanowires displayed outstanding adsorptive desulfurization activity for DBT (65.4 mg S g–1 adsorbent according to the Langmuir isotherm model), which was much higher than that of commercial BN and graphene-like BN. At the same time, the BN mesoporous nanowires displayed good stability and excellent adsorption performance for the 4,6-DMDBT (33.2 mg S g–1 adsorbent). The significant enhancement of adsorption desulfurization performance of BN mesoporous nanowires was ascribed to the large number of low coordinated atoms along the nanowire surface and mesopores, which could cause an interaction with DBT, and the doped oxygen atoms further strengthen the interaction.
研究领域:
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
AICHE JOURNAL
·
2022
·Vol. 69
·期 4
·e17933
·
IF 4.167
Wei Xie,Yiping Guo,Jianping Li,Honglai Liu,Jun Hu
Metal organic frameworks (MOFs) have shown promising adsorptive desulfurization (ADS) capacity yet remains great challenges to maintain excellent performance in presence of water. Guided by the density function theoretical (DFT) calculations, we select bromine modified linkers with different substitution degrees to construct MIL-47-xBr to regulate the porosity and hydrophobicity. The optimized MIL-47-Br exhibits the highest saturation dibenzothiophene (DBT) capacity of 179.2 mgS g −1 from the hydrous oil, surpassing the record of all ADS adsorbents. Meanwhile, the excellent selectivity, adsorption kinetics, and recycle stability endow MIL-47-Br with superior ADS performance from the commercial hydrous gasoline. With the DBT capacity decreases by only 12.3% from the commercial gasoline, a continue flow ADS is successfully achieved on the fixed-bed of MIL-47-Br column. Therefore, this facial strategy of simple substitution can fully exploit the functions of open metal sites for enhancing the task-specific selectivity, and has a promising application prospect in industrial ADS.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2017
·
IF 3.091
Wenfeng Li,Yingjie Li,Yong Chen,Qingnan Liu,Yingzhou Lu,Hong Meng,Chunxi Li
Carbon-based materials are a kind of promising sorbent for the desulfurization of fuel oils, especially for polycyclic aromatic sulfur heterocycles (PASHs), and development of new sorbents is of great significance. In this paper, six alkynyl carbon materials (ACM-1 to ACM-6) were prepared for the first time through mechanochemical reaction of calcium carbide with six full halogenated hydrocarbons, i.e., CCl4, C2Cl6, C2Cl4, C6Cl6, C6Br6, and C14H4Br10, respectively. Their carbon content and specific surface areas (SSAs) were analyzed, and their adsorption performance for thiophenic sulfurs was studied. The ACMs are mesoporous materials with relatively high SSAs and favorable adsorptive performance for PASHs with the order of DBT > BT > 3-MT. Their adsorptivity is virtually consistent with the SSA values and follows the order of ACM-6 > ACM-5 > ACM-4 > ACM-1 > ACM-3 > ACM-2. ACM-6 has the highest SSA (712 m2 g–1) and saturated adsorbance of 21.1 mg-S·g–1 for DBT in octane, as well as 6 mg-S·g–1 for real diesel. As a whole, ACM-6 represents the best ADS sorbent among all mesoporous carbon materials and may be applicable for real oils after some further modification.
研究领域:
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2018
·
IF 4.908
Xiong-Fei Zhang,Zhongguo Wang,Yi Feng,Yuxia Zhong,Jiaqiang Liao,Yaquan Wang,Jianfeng Yao
Metal organic frameworks (MOFs) have recently emerged as promising candidates for efficient removal of sulfur-containing compounds (SCCs) from liquid fuels. In this study, adsorptive desulfurization (ADS) is performed by adsorbing thiophene (TP) and benzothiophene (BT) from model fuels over pristine and functionalized UiO-66 (Zr). The introduction of amino ( NH 2 ) and carboxylic ( COOH) groups reduces the porosity of UiO-66. However, the adsorption capacities of functionalized UiO-66 improved remarkably. Especially for the adsorbent functionalized with amino moieties (UiO-66-NH 2 ), its maximum adsorption capacities for TP (29.5 mg S/g) and BT (35.7 mg S/g) are 1.7 and 1.8 times to that of bare UiO-66. The superior performance of UiO-66-NH 2 is ascribed to the higher availability of hydrogen-bond donor sites in the surface and the favorable interactions between H atoms of NH 2 and sulfur species. UiO-66-COOH is beneficial for the adsorption of SCCs than that of pristine UiO-66 because of the existence of acid-base interactions. Moreover, the reusability of UiO-66-NH 2 is confirmed by regenerating it via a simple solvent washing.
研究领域:
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
FUEL
·
2015
·
IF 3.52
Yawei Shi,Xiangwen Zhang,Guozhu Liu
Both activation and surface oxidation were employed to tailor the textural and surface properties of a typical ordered mesoporous carbon (CMK-3) for better adsorptive desulfurization performance. The amount of small micropores increased dramatically upon activation, while abundant surface functionalities were introduced by surface oxidation. Thanks to the abundant mesopores present in the carbons, a quasi-equilibrium situation for DBT adsorption from model fuels could be reached rapidly in less than 30 min, and the adsorption amounts at 5 min were equal to more than 95% of the equilibrium values. Moreover, the adsorption amount of DBT was increased by up to 121% with the introduction of small micropores and surface functionalities. Further experiments were designed to demonstrate that the adsorption amount is depended on both textural and surface properties.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子