Journal of the Taiwan Institute of Chemical Engineers
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2019
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IF 3.834
Yunchao Feng,Miao Zuo,Ting Wang,Wenlong Jia,Xiaoyu Zhao,Xianhai Zeng,Yong Sun,Xing Tang,Tingzhou Lei,Lu Lin
Production of 5-hydroxymethylfurfural (HMF) from glucose with high yield remains a big challenge. Thereinto, assembling catalysts with outstanding performance is the bottleneck at the current stage. In this study, effective catalysts were synthesized by loading SO 4 2− /ZrO 2 (SZ) on a series of H + zeolites to investigate the catalytic dehydration of glucose into HMF. Among all the catalysts applied, 2-SZ-HM-550 (HZSM-5 with Si/Al molar ratios of 80∼150, calcined at 550 °C) gave the yields of HMF 41.32%, 61.14%, 54.67% and 40.71% in 4 applied reaction systems, respectively. Moreover, HMF with desirable yield was obtained while other carbohydrates were dehydrated catalyzed by 2-SZ-HM-550, such as fructose, sucrose, inulin and starch.
研究领域:
化学工程
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催化科学
✓ 已验证
DOI
高影响因子
AICHE JOURNAL
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2018
·Vol. 64
·期 11
·3988-4001
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IF 3.326
Xiaowen Zhang,Jieling Hong,Helei Liu,Xiao Luo,Wilfred Olson,Paitoon Tontiwachwuthikul,Zhiwu Liang
In this work, the composite catalysts, SO 4 2 /ZrO 2 /γ-Al 2 O 3 (SZA), with different ZrO 2 and γ-Al 2 O 3 mass ratios were prepared and used for the first time for the carbon dioxide (CO 2 )-loaded monoethanolamine (MEA) solvent regeneration process to reduce the heat duty. The regeneration characteristics with five catalysts (three SZA catalysts and two parent catalysts) of a 5 M MEA solution with an initial CO 2 loading of 0.5 mol CO 2 /mol amine at 98°C were investigated in terms of CO 2 desorption performance and compared with those of a blank test. All the catalysts were characterized using X-ray diffraction, Fourier transform infrared spectroscopy, N 2 adsorption–desorption experiment, ammonia temperature programmed desorption, and pyridine-adsorption infrared spectroscopy. The results indicate that the SZA catalysts exhibited superior catalytic activity to the parent catalysts. A possible catalytic mechanism for the CO 2 desorption process over SZA catalyst was proposed. The results reveal that SZA1/1, which possesses the highest joint value of Brφnsted acid sites (BASs) and mesopore surface area (MSA), presented the highest catalytic performance, decreasing the heat duty by 36.9% as compared to the catalyst-free run. The SZA1/1 catalyst shows the best catalytic performance as compared with the reported catalyst for this purpose. Moreover, the SZA catalyst has advantages of low cost, good cyclic stability, easy regeneration and has no effect on the CO 2 absorption performance of MEA. © 2018 American Institute of Chemical Engineers AIChE J , 64: 3988–4001, 2018
研究领域:
化学工程
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催化材料
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环境科学
✓ 已验证
DOI
高影响因子
ENERGY & FUELS
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2020
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IF 3.421
Yang Qu,Yuan Zhao,Shanshan Xiong,Chenguang Wang,Shurong Wang,Lingjun Zhu,Longlong Ma
5-Hydroxymethylfurfural (HMF) and levulinic acid (LA) are two important platform compounds that can be produced by the dehydration of hexoses from hydrolysis of cellulose. In this study, glucose dehydration was catalyzed by the SO42–/ZrO2 catalyst in the NaCl–THF/H2O biphasic solvent system. Complete conversion of glucose was achieved at 160 °C. The highest HMF yield and LA yield were 61.84% and 29.68%, respectively. The results showed that the conversion and product distribution were influenced by catalyst acidity, solvent composition, temperature, and time. The SO42– load greatly changed the acidity of the catalyst, thus affecting the product distribution. By changing the composition of the catalyst and the biphasic solvent system, different yields of HMF and LA could be obtained, so as to realize directional synthesis of the target products.
研究领域:
生物化学
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催化化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
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2020
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IF 3.421
Chenglong Wen,Jundong Xu,Xueman Wang,Yu Fan
A novel SO42–/ZrO2@SAPO-11 (SZ@SA-11) composite was synthesized via a two-step method, and the corresponding SZ@SA-11 supported Pt catalyst was applied to catalyze n-heptane hydroisomerization. First, UiO-66@SAPO-11 is produced by the growth of UiO-66 on SAPO-11 due to the covalent bonds between Zr and the oxygen in the hydroxyl groups of SAPO-11. Then, UiO-66@SAPO-11 is decomposed to form ZrO2@SAPO-11 via calcination in air, and the SZ@SA-11 composite is obtained by the impregnation of ZrO2@SAPO-11 with (NH4)2SO4 and subsequent calcination. Compared with the physical mixture of SO42–/ZrO2 and conventional SAPO-11 (SZ+SA-11), SZ@SA-11 possesses smaller ZrO2 particles and more tetragonal ZrO2. Moderate and strong Brønsted acid sites (MSBAS) are produced only via interactions between tetragonal ZrO2 and sulfate, so SZ@SA-11 with more tetragonal ZrO2 has a greater amount of MSBAS than SZ+SA-11. These advantages of SZ@SA-11 endow the corresponding Pt/SZ@SA-11 catalyst with a better performance for n-heptane hydroisomerization compared to Pt/(SZ+SA-11). In addition, compared with the other counterparts such as Pt/SZ and Pt/SA-11, Pt/SZ@SA-11 presents higher selectivity for total isomers (91.5%), higher selectivity for multibranched isomers (22.6%), and a lower cracking selectivity (8.1%) in n-heptane hydroisomerization. The strategy proposed herein provides a new insight into the acidity adjustment of the molecular-sieve-based catalysts for hydrocarbon hydroisomerization.
研究领域:
催化化学
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能源化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CLAY SCIENCE
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2019
·
IF 3.89
Haiyan Yang,Yang Zhou,Dongshen Tong,Miao Yang,Kai Fang,Chunhui Zhou,Weihua Yu
Cellulose is the most abundant form of biomass on earth, and is considered as an alternative for fuels and chemicals. The hydrolysis of cellulose to platform compounds, such as reducing sugars (RS), is one of the most important ways for the utilization of cellulose. In this study, the solid acid catalysts of SO 4 2− -ZrO 2 /montmorillonite (SZ-Mt) were prepared by coupling SO 4 2− with ZrO 2 and then introducing into the interlayer of Mt using the coprecipitation method. Meanwhile, the catalytic performance of the SZ-Mt catalysts for the hydrolysis of cellulose to RS in water was studied. The catalysts were characterized by XRD , FT-IR, BET, SEM(EDS), NH 3 -TPD and XPS . The catalytic results showed that the SZ-Mt composite calcined at 500 °C with the molar ratio of S/Zr of 0.3 showed the highest total reducing sugars yield of 30.1%. The characterization results revealed that the surface S O bonds of sulfated zirconium oxide could gradually change from O=S-OH groups (type I, -HSO 4 ) to O=S=O groups (type II, -S 2 O 7 ). It was concluded that the surface S-OH groups in type I were responsible for the hydrolysis of cellulose in the low molar ratio of S/Zr and the new S-OH bonds formed by breaking the S-O-S bonds in type II were contributed to the conversion of cellulose in the high molar ratio of S/Zr. Finally, the mechanism of cellulose hydrolysis on the SZ composites was suggested.
研究领域:
化学工程
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材料科学
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生物化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
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IF 9.136
Sitan Wang,Xuan Meng,Naiwang Liu,Li Shi
Sulfated zirconia, as a promising catalyst in various acid-catalytic reactions, still suffer from unsatisfactory catalytic stability and regeneration performance due to severe leaching of sulfur species, while aluminum modification can effectively overcome these drawbacks. Unfortunately, the limited acceptability of aluminum content by co-precipitation and milling methods remains a critical issue. Herein, an effective strategy of coating sulfated zirconia on the surface of γ-Al 2 O 3 was developed to synthesize the novel Al 2 O 3 @SO 4 2- /ZrO 2 catalyst with high aluminum content. The synthesis variables were investigated and systematically optimized. The structural and acidic properties of Al 2 O 3 @SO 4 2- /ZrO 2 were determined by XRD, HR-TEM equipped with EDX, N 2 adsorption-desorption isotherms, EA, FT-IR, NH 3 -TPD and Py-FTIR. Results indicated that the unique structure constructed by sulfated zirconia coated on γ-Al 2 O 3 not only realized the stabilization of favorable tetragonal zirconia phase even at exceedingly high aluminum content but also promoted Brønsted acid sites. Accordingly, the optimal Al 2 O 3 @SO 4 2- /ZrO 2 - 50% performed outstanding catalytic activity and stability, given the olefins conversion of 98%-75% during the continuous reaction experiment. Owing to the alleviation of sulfur loss by Al-promoting effects, excellent regeneration performance, with olefins conversion only slightly declining after 4 consecutive reaction-regeneration cycles, was also obtained. The mechanistic pathway for the alkylation of olefins with aromatics over Al 2 O 3 @SO 4 2- /ZrO 2 was also investigated and proposed by GC–MS analysis.
研究领域:
催化
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化学工程
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Natural Gas Chemistry
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2012
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IF 1.348
Lincai Peng,Junping Zhuang,Lu Lin
Effects of Zr/Ti molar ratio in SO 2− 4 /ZrO 2 -TiO 2 solid acid catalyst calcined at different temperatures on its surface properties and catalytic activity were thoroughly investigated in this paper. The physicochemical characteristics of prepared samples were determined by N2 adsorptiondesorption, XRD, NH3-TPD and XPS techniques, respectively. It was found that the crystallization temperature of the samples increased after the combination of ZrO 2 and TiO 2 ; and phase transformations from the anatase to the rutile of TiO 2 species and the tetragonal to the monoclinic of ZrO 2 species were effectively suppressed at higher temperature. The sample with a Zr/Ti molar ratio of 3/1 calcined at 450 °C showed the highest surface area and the most acid sites among all the tested samples. The acid site densities of samples were relatively closed to each other if they were calcined at the same temperature, however, decreased with the calcination temperature. The result indicates that the sulfur content in samples is a crucial factor to control the acid site density. Calcining the sample at 650 °C and higher temperatures resulted in a significant desorption of sulfate ion on the samples. The synthesized samples were evaluated as a potential catalyst for glucose conversion under the near-critical methanol conditions (200 °C/4 MPa). The results suggested that the relatively weaker acid sites of the catalyst were more favorable for the accumulation of methyl glucosides, while the moderate acid sites were responsible for the formation of methyl levulinate. The catalytic activity for methyl levulinate production almost increases linearly with the catalyst acid site density. The catalyst deactivation is due to the loss of sulfate ion and the two catalysts with Zr/Ti molar ratios of 3/1 and 1/3 could effectively alleviate the deactivation caused by sulfate solution in the reaction medium and can be reused after calcination with the reuse rate of over 90% in terms of the methyl levulinate selectivity.
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
Catalysts
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2021
·Vol. 11
·期 12
·1464
·
IF 4.146
Su Yang,Xiaoxuan Guo,Xiaomei Pan,Liuyu Gu,Xueping Liu,Lijing Gao,Guomin Xiao
Concentrated sulfuric acid is generally used as a catalyst for producing brominated alkanes in traditional methods, but is highly corrosive and difficult to separate. This work reports the preparation of bromopropane from n-propanol based on a reactive distillation strategy combined with alumina-modified sulfated zirconia (Al2O3/SO42−/ZrO2) as a heterogenous catalyst. As expected, under the optimum reaction conditions (110 °C), the yield of bromopropane was 96.18% without side reactions due to the reactive distillation strategy. Meanwhile, the microscopic morphology and performance of Al2O3/SO42−/ZrO2were evaluated by X-ray diffraction (XRD), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), Brunner–Emmet–Teller (BET), Fourier transform infrared spectroscopy (FT–IR), and other characterization methods. The results confirmed that the morphology of zirconia sulfate is effectively regulated by the modification method of alumina, and more edges and angles provide more catalytic acid sites for the reaction. Furthermore, Al2O3/SO42−/ZrO2exhibited high stability and remarkable reusability due to the strong chemical bond Zr–Al–Zr. This work provides a practical method for the preparation of bromopropane and can be further extended to the preparation of other bromoalkanes.Keywords:sulfated zirconia;modification of alumina;bromopropane;catalytic distillation
研究领域:
化学工程
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催化
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有机化学
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
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2019
·
IF 8.426
Zain Ali Saleh Bairq,Hongxia Gao,Yufei Huang,Haiyan Zhang,Zhiwu Liang
A significant impediment to the widespread adoption of amine-based post-combustion technique for CO 2 capture from flue gas is the huge energy demand for amine solvent regeneration. In this study, five novel bifunctional heterogeneous catalysts e.g., SO 4 2− /ZrO 2 /SiO 2 with different molar ratios of zirconia and SO 4 2− /ZrO 2 as a parent catalyst were synthesized and applied to evaluate their effectiveness in enhancing the CO 2 desorption and solvent regeneration of 5M monoethanolamine solution with CO 2 loading of 0.5 ± 0.01 mol CO 2 /mol monoethanolamine at 97 °C. The catalysts were characterized by Fourier transform-infrared spectrometry, pyridine-infrared spectroscopy, X-ray diffraction, N 2 -adsorption-desorption, and ammonia-temperature programmed desorption. The results demonstrated that these catalysts can significantly reduce the heat duty for CO 2 desorption by 36.48% compared to without catalyst and enhance desorption rate by 35.1%. The results also showed that SO 4 2− /ZrO 2 /SiO 2 15% presented the highest efficiency compared to the other SO 4 2− /ZrO 2 /SiO 2 ratios and the super solid acid catalyst SO 4 2− /ZrO 2 . Additionally, to investigate if the catalysts induce any unfavorable effects on the amine, the absorption of CO 2 by regenerated amine solvent was studied. Finally, a reaction mechanism for the amine solvent regeneration with the synthesized catalyst e.g., SO 4 2− /ZrO 2 /SiO 2 was suggested.
研究领域:
化学工程
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环境科学
✓ 已验证
DOI
高影响因子
Surfaces and Interfaces
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2021
·
IF 4.837
Ikram Ullah,T.A. Taha,Asma M. Alenad,Ikram Uddin,Asif Hayat,Ashiq Hayat,Muhammad Sohail,Ahmad Irfan,Javid Khan,Arkom Palamanit
In this study, sulfated zirconia with loading of platinum (Pt) and platinum alumina (PA-Al 2 O 3 ) promoted sulfated zirconia (SZ) catalysts were synthesized by hydro-thermal route. The samples were characterized by XRD, BET, FT-IR, NH 3 -TPD, and TGA. The catalytic efficiency of all the synthesized catalysts was tested on the isomerization of n -butane. The results indicated that the conversion of n -butane (71.04%), selectivity to i -butane (98.96%), and yield of i -butane (70.30%) is significantly high for PA/SZ sample than that of Pt modified SZ and bare SZ. The results of this study suggest that the SZ modified by Pt/Al 2 O 3 (PA) provided better catalytic performance and higher stability (within 25 h of TOS), when compared with SZ, and Pt-modified SZ.
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
FUEL
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2022
·
IF 8.035
Xiaodi Li,Shan Ren,Lian Liu,Xiangdong Xing,Lin Chen,Jiangling Li,Jian Yang,Qingcai Liu
The serious deactivation of denitration catalysts caused by heavy metals still a thorny issue in the practical application of selective catalytic reduction of NO x with NH 3 . Herein, we proposed a novel anti-poisoning strategy by designing SO 4 2− /ZrO 2 superacid supported CeO 2 /ZrO 2 catalyst, and the effect of SO 4 2− /ZrO 2 supported CeO 2 /ZrO 2 for PbO-resistance NO x catalytic reduction was investigated. It was worthy to note that the introduction of solid superacid SO 4 2− /ZrO 2 significantly enhanced catalytic performance over the entire temperature range, with an exceptionally high NO x removal efficiency over 98 % during 250–500 °C. When 2 wt% PbO was deposited on the fresh catalyst, the catalytic activity of CeO 2 /ZrO 2 catalyst decreased obviously, while CeO 2 /ZrO 2 -S catalyst can still maintain a higher NO x conversion over 90 % from 275 to 500 °C. The characterization results confirmed that the introduction of solid superacid SO 4 2− /ZrO 2 enhanced the surface acidity and promoted the transformation from Ce 4+ to Ce 3+ . The results of in situ DRIFTS implied that the Eley-Rideal (E-R) mechanism was obeyed over CeO 2 /ZrO 2 catalyst, and both Eley-Rideal (E-R) and Langmuir-Hinshelwood (L-H) mechanisms were followed over CeO 2 /ZrO 2 -S catalyst in the SCR process. With regard to poisoned catalysts, the NH 3 adsorption was inhibited to some extent, while the reaction mechanism wasn’t changed by PbO poisoning.
研究领域:
催化
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环境科学
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化学工程
✓ 已验证
产品关联
DOI
高影响因子
APPLIED ENERGY
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2024
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IF 10.1
Yingjie Niu,Ting Li,Ali Hassan Bhatti,Jiaqi Qu,Xin Zhou,Li Luo,Francesco Barzagli,Chao'en Li,Rui Zhang
The use of solid acid catalysts for sorbent regeneration is an emerging approach to improve the energy efficiency of CO 2 capture processes. In this study, fly ash (FA), an industrial byproduct rich in acid/base sites, was chosen as a support material for the solid acid SO 4 2− /ZrO 2 (SZ) in the preparation of SZ@FA composite catalysts. Three catalysts with different mass ratios between SZ and FA were synthesized and evaluated in the regeneration process at 88 °C of a CO 2 -saturated MEA solution. Their desorption performance, expressed as CO 2 desorption rate, amount of CO 2 desorbed , and heat duty, was then compared with that obtained with unmodified FA, ZrO 2, and in the absence of catalysts (blank), under identical operating conditions. Compared to the uncatalyzed system, the SZ@FA composite catalysts showed significantly better desorption performance. In particular, SZ@FA-1/2 provided the highest values of desorption rate and cyclic capacity while reducing energy consumption by 45.4% compared to the blank system. It also demonstrated stability over 20 consecutive absorption-desorption cycles. Comparison with other reported catalysts highlighted the high performance of SZ@FA-1/2, particularly in terms of relative heat duty reduction, positioning it as a cost-effective and environmentally friendly choice for post-combustion capture applications.
研究领域:
化学工程
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环境科学
✓ 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）