CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Yongxiao Tuo,Wanli Liu,Qing Lu,Xingzhao Wang,Jiabing Luo,Shutao Wang,Yan Zhou,Min Wang,Xiaohui Sun,Xiang Feng,Mingbo Wu,De Chen,Jun Zhang
The most difficulty of efficient CO 2 electroreduction lies in the activation step that turns CO 2 into the CO 2 − radicals or other intermediates that can be further converted. To overcome this bottleneck, many efforts have been devoted to develop electrocatalysts to lower the overpotential of CO 2 activation, but they inevitably involve complicated or/and unscalable synthesis methods. Here we reported that the SO 4 2− ion modified metal foils, including Zn, Ag, Au and Cu, demonstrated ∼6.5, 1.4, 14 and 2.5 times of CO faradaic efficiency in K 2 SO 4 electrolyte compared to KHCO 3 electrolyte at −1.05 V vs. RHE. According to both experimental and DFT studies, the electron-rich metal-SO 4 adlayer can activate CO 2 by bending the linear molecule of CO 2 through donating electrons to the antibonding orbital of CO 2 , thus facilitating the formation of key intermediate *CO 2 − . Moreover, the adsorption of H + on metal sites is restrained by the metal-SO 4 adlayer, leading to a suppressed H 2 evolution activity. From a broader perspective, many catalysts can benefit from this approach to achieve more efficient CO 2 electrochemical reduction.
研究领域:
材料科学
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电化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Analytical Methods
·
2024
·
IF 2.7
Kang Shen,Caili Bi,Haifan Yang,Miaowen Xu,Lili Huang,Youwei Wang
Based on the coordination principle of Lewis acid, the 4-mercaptophenylboronic acid (4-MPBA)-modified novel dumbbell-shaped Au-Ag nanorods (4-MPBA@DS Au-AgNRs) substrate has been developed, which could be combined with the surface-enhanced Raman scattering (SERS) technique to detect SO42- with high sensitivity and specificity. DS Au-AgNRs synthesized in this paper with dumbbell particular structure have been verified by finite-difference time domain (FDTD) simulation to be capable of stimulating strong localized electromagnetic enhancement (EM) at nano-edge, gap, generating a large number of “hot spots” exhibiting excellent SERS performance. The 4-MPBA modified on its surface could specifically recognize SO42-, producing a change in the spectral peak at 1382 cm-1, thus realizing highly sensitive and specific sensing of SO42-. Under optimized conditions, this SERS sensor responded rapidly to SO42- within 2 minutes and demonstrated uncommon immunity. Ratio calculation by the ratio of the characteristic peaks at 1382 and 1070 cm-1 (I1382/I1070) enabled quantitative detection of SO42- in the range of 1 × 10-8-1 × 10-3 M, and the detection threshold was as low as 1 nM, which was superior to that of similar detection methods. Importantly, the utility and reliability of this SERS substrate for the determination of SO42- in actual samples were evaluated using ion chromatography as the gold standard, and there was no significant difference between the two protocols (P > 0.05), and the RSD was less than 6% with a satisfactory recovery rate (97.6-102.3%). Therefore, the present protocol has the advantages of simplicity and rapidity, high sensitivity, specificity, stability, and practicability in the determination of SO42- in aqueous solution, providing a reliable solution for tracing SO42- in the field of food safety and environmental testing.
研究领域:
分析化学
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环境科学
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食品安全
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of the Taiwan Institute of Chemical Engineers
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2019
·
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
·
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
FUEL
·
2024
·
IF 6.7
Renjie Ji,Defu Yin,Yao Chen,Like Ma,Fanglin Lv,Yuhao Zhang,Zhen Jia,Jingyun Zhang,Mingya Liu,Shitao Yu,Yue Liu
A core–shell catalyst mZSM-5@SO 4 2- /mSiO 2 composed of mZSM-5 core and SO 4 2- /mSiO 2 shell was prepared by the soft template method. Core-shell structure could promote the building of Brønsted -Lewis (B-L) acids interface and significantly improve the synergistic effect of B-L. In this paper, the Brønsted/Lewis (B/L) of mZSM-5@SO 4 2- /mSiO 2 was targeted regulating by innovatively introducing Brønsted acid (BA) sites into the shell. The optimal mZSM-5@SO 4 2- /mSiO 2 catalyst (B/L = 0.142) could achieve 72.1 % furfural yield at 140 ℃ for 1 h. In addition, 70.2 % furfural yield could be obtained after the catalyst was recycled and regenerated for 5 times. Combining In-situ IR and 13 C NMR, the reaction path was revealed in detail: xylose was first isomerized to xylulose and then dehydrated to furfural. This paper provides a research idea for the directional regulation of dual active sites of cascade reaction catalysts.
研究领域:
催化化学
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生物质转化
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
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2020
·
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
RSC Advances
·
2014
·Vol. 4
·期 29
·15216-15224
·
IF 3.708
Chong-Wen Jiang,Xin Zhong,Zheng-Hong Luo
5-Hydroxymethylfurfural (5-HMF) which can be produced from cellulose is considered as one of the promising green platform chemicals. In this work, the conversion of cellulose to 5-HMF was carried out through hydrolysis in a batch reactor using the SO42−/Ti-MCM-41 catalyst at a temperature of 463–503 K. Two analytical techniques including the 3,5-dinitrosalicylic acid (DNS) method and high performance liquid chromatography (HPLC) were employed to track the time evolution of the main reagents, i.e., cellulose, 5-HMF and reducing sugar. Based on the typical kinetic experiments for the cellulose hydrolysis, a comprehensive hydrolysis mechanism was introduced to describe the heterogeneous hydrolysis of cellulose to 5-HMF. A corresponding kinetic model was proposed on the basis of the hydrolysis mechanism and the mass balance law. The results show that the predicted data obtained via the suggested model agree well with the experimental results. In addition, some data from the open reports were referred for further model verification in this work. The kinetic model suggested in this work is a mechanism model for the heterogeneous catalytic cellulose hydrolysis process, which is different from the previous first-order kinetic model.
研究领域:
化学工程
·
可再生化学
✓ 已验证
产品关联
DOI
高影响因子
ENERGY & FUELS
·
2020
·
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
·
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
·
材料科学
·
生物化学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Environmental Chemical Engineering
·
2025
·
IF 7.2
Changhao Wu,Xudong Yu,Nan Zhang,Jing Li,Qi Li,Yousheng Yang,Ke Chen,Bo Yang,Shuang Wang,Yiping Liu,Zhenwen Xing
To solve the massive accumulation of gypsum generated from polyhalite leaching and secondary gypsum, this study investigated phase equilibria of the ternary system NH 4 + , Ca 2+ // SO 4 2- - H 2 O at 323.2 K and 348.2 K. The phase diagrams included 2 invariant points, 3 univariate curves, and 3 crystallization regions corresponding to (NH 4 ) 2 SO 4 , CaSO 4 ·2H 2 O, and double salt koktaite (NH 4 ) 2 Ca(SO 4 ) 2 ·H 2 O. As temperature increased, the crystallization region of CaSO 4 ·2H 2 O contracted, whereas those of (NH 4 ) 2 SO 4 and koktaite expanded, indicating that the temperature-enhanced was beneficial to improve the crystallization efficiency of koktaite. Guided by multitemperature phase diagram, the influencing factors and optimal conditions of the comprehensive utilization process of phosphogypsum were explored. The synthesis of koktaite achieved maximum efficiency under conditions of 1: 1.5 molar ratio, 348.2 K reaction temperature, 90 min duration, and 250 rpm agitation. Concurrently, under solid-liquid ratio of 1: 0.5 and after three leaching cycles of 30 seconds each, the yield of CaSO 4 ·2H 2 O production reached 99.80% with a purity of 99.52%. However, the purity and yield of product decreased due to the accumulation of impurities during the cycles, stabilizing after 6 cycles (koktaite yield: 98.50%; purity: 95.69%; (NH 4 ) 2 SO 4 yield: 97.69%; purity: 95.42%). Granulated koktaite released NH 4 + through layer-by-layer dissolution, which prolonged the dissolution time, and the complete dissolution time was 6 times and 24 times longer than that of ungranulated koktaite and (NH 4 ) 2 SO 4 . This work integrates theoretical phase behavior analysis with process engineering to establish a circular resource recovery strategy for synthesizing high-value products from phosphogypsum.
研究领域:
物理化学
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化学工程
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材料科学
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环境科学
·
无机化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2022
·
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
·
化学工程
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
RSC Advances
·
2015
·Vol. 5
·期 128
·106053-106060
·
IF 3.84
Jie Wang,Ting Qu,Minsi Liang,Zhenbo Zhao
In this work, we investigated the dehydration of fructose into 5-hydroxymethylfurfural using solid catalysts with microwave assistance in dimethyl sulfoxide. Five kinds of solid catalyst ZrO2, WOx/ZrO2, MoOx/ZrO2, SO42−/WOx–ZrO2 and SO42−/MoOx–ZrO2 were prepared and characterized by XRD, UV-DRS, FTIR, XPS, TEM, TPD, BET, and Raman and the surface acid amount was obtained by combining pyridine adsorption and UV spectrometry. The SO42−/WOx–ZrO2 catalyst was found be the most active catalyst, and a fructose conversion of 95.80% with 83.90% 5-HMF yield was obtained at 150 °C in a relatively short reaction time of 5 min. The value of the activation energy was comparable with previous values reported in the literature, implying that SO42−/WOx–ZrO2 was efficient for the dehydration of fructose to 5-HMF and that microwave radiation heating had a remarkable accelerating effect on the fructose conversion.
研究领域:
化学工程
·
催化科学
✓ 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）