NEW JOURNAL OF CHEMISTRY
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2023
·Vol. 47
·期 9
·4337-4345
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IF 3.3
Zhangbin Liao,Yunlong Duan,Liying Guo,Rongrong Zheng,Liyan Wang,Yanming Chen,Linnan Zhang,Xin Qian
Five titanium-centered heteropoly acids with different metal vacancies were prepared first, and then combined with an ionic liquid by ion exchange to prepare heteropoly acid ionic liquid catalysts Bmim4–6[M(H2O)TiMo11O39] (M = Cu2+, Fe2+, Pb2+, Ti4+, and Zn2+). The structure and thermal properties of each catalyst were tested and analyzed by Fourier transform infrared (FTIR) spectroscopy, ultraviolet (UV) spectroscopy, X-ray powder diffraction (XRD), apparent morphology analysis, and thermogravimetric analysis (TGA). Five heteropoly acid ionic liquids were investigated by using waste mineral water bottles as samples for performance in the catalytic degradation of bottle-grade polyethylene terephthalate (PET), and the degradation product, bis(2-hydroxyethyl) terephthalate (BHET), was analyzed for the chemical structure. The results showed that the five heteropoly acid ionic liquid catalysts were successfully prepared, with good thermal stability. Of these catalysts, Bmim4[Ti(H2O)TiMo11O39] showed the optimal catalytic performance. It achieved an alcoholysis rate of 100% and a yield of BHET of 84.73% with a catalyst dosage of 0.6% (percentage in the total mass of the raw materials) at 190 °C for 5 h. Moreover, after six cycles of use, the alcoholysis rate was still as high as 94.36%, and the yield of BHET was 75.65%. The above results indicated that the prepared heteropoly acid ionic liquid catalysts showed good performance in the catalytic degradation of bottle-grade PET, presenting a promising prospect for development.
研究领域:
化学
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材料科学
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环境科学
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产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2024
·Vol. 26
·期 4
·2170-2182
·
IF 9.3
Zhuosen He,Yucui Hou,Jian Wei,Shuhang Ren,Weize Wu
Formic acid (FA) is a bulk chemical and a promising hydrogen energy carrier. The development of FA production from renewable biomass instead of multiple-step production from diminishing fossil resources is attractive. Formaldehyde (FAld) is another bulk chemical but industrial production requires high temperatures (250–600 °C). Herein, efficient oxidation of biomass to FA coupled with low-energy FAld production was developed using heteropoly acids as catalysts. Biomass and derivatives were oxidized to FA in yields of up to 88.6% while methanol was selectively oxidized to FAld at 90–190 °C with a markedly enhanced reaction rate. The synergistic mechanism has been unveiled that biomass activates methanol oxidation by boosting the catalytic redox cycle to form hydroxyl radicals and methanol scavenges the hydroxyl radicals to inhibit the overoxidation of biomass. This work opens up a promising direction for efficient FA production from biomass coupled with low-energy oxidation of alcohols to aldehydes.
研究领域:
化学工程
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可再生能源
✓ 已验证
产品关联
DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2024
·
IF 5.6
He Wan,Xiuqiang Chen,Kuiyuan Cao,Yongwei Han,Xixin Duan,Zhong Sun,Junyou Shi
Formic acid (FA) plays a key role in various chemical processes and industrial procedures. Attractively, FA can be produced from renewable biomass instead of fossil resources. In this paper, FA was successfully prepared with the help of isopolyacid Na 6 [ α -Mo 6 V 2 O 26 ] (Mo 6 V 2 ), which is superior to Keggin-type heteropoly- acids containing vanadium because its stronger oxidizing ability endows Mo 6 V 2 with better ability to break C-C bonds. Some carbohydrates and biomass, including glucose, fructose, xylose, hemicellulose, cellulose, corn stover, and birch, acted as sources to prepare FA in aqueous solution in the presence of Mo 6 V 2 . For monosaccharides, Mo 6 V 2 can accelerate the reaction rate and obtain the highest FA yield of 62 % from xylose. For hemicellulose, the yield of FA reaches up to 54 % in only 8 min. In the case of insoluble biomass materials, the combination of p -toluenesulfonic acid (TsOH) and Mo 6 V 2 can boost the catalytic performance of the system, with the FA yield being 47 % from cellulose, 37 % from corn stover, and 41 % from birch. Therefore, Mo 6 V 2 can be valued as an universital and promising catalyst for transforming renewable waste biomass to high-value chemicals.
研究领域:
化学工程
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可再生资源转化
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产品关联
DOI
高影响因子
ChemistrySelect
·
2024
·Vol. 9
·期 40
·e202403878
·
IF 1.9
Haifeng Liao,Jianwei Guo
Graphical Three kinds of heteropoly acid-based ionic liquids with different Hammett acidity were prepared for the catalytic conversion of cellulose to levulinic acid, and the effects of different solvent systems on the catalytic reactions were investigated. The results showed that higher Hammett acidity was beneficial to increase the yield of levulinic acid, and GVL/H 2 O bi-phase solvent system was helpful to extract the product to the organic phase and promote the formation of levulinic acid. Levulinic acid is an important chemical intermediate, which has many applications in organic synthesis, industry, agriculture, and medicine. In this word, three kinds of heteropoly acid based ionic liquids ([IMPS]H 2 PW 12 O 40 、[PyPS] H 2 PW 12 O 40 [TEAPS] H 2 PW 12 O 40) were used to catalyze the one-pot conversion of cellulose to levulinic acid. [IMPS]H 2 PW 12 O 40 has the highest catalytic activity due to its strong Hammett acidity ( H 0 ). In addition, the effect of biphasic solvent systems on the conversion of cellulose to levulinic acid was also studied. The results showed that the GVL/H 2 O system could effectively promote the conversion of cellulose and increase the yield of levulinic acid. The yield of levulinic acid could reach 52.6% and the conversion rate of cellulose was 91.2% at 180 °C for 180 min under the GVL/H 2 O volume ratio of 1:1 with [IMPS]H 2 PW 12 O 40 as a catalyst at 1 Mpa N 2 and cellulose as raw material. And [IMPS]H 2 PW 12 O 40 can be recycled up to five times without significant performance loss. This study provides a promising method for efficiently converting cellulose and other biomass resources to levulinic acid extraction.
研究领域:
化学工程
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生物质能
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有机合成
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产品关联
DOI
高影响因子
FUEL PROCESSING TECHNOLOGY
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2020
·
IF 4.982
Chaonan Tao,Lincai Peng,Junhua Zhang,Liang He
Efficient production of fuels and chemicals from lignocellulosic biomass is the main goal of biorefinery processes. Herein, the metal-modified heteropolyacids with tunable Lewis and Brønsted acid sites were designed as the monolithic multifunctional catalyst for valorizing cellulose and lignocellulosic biomass to alkyl levulinate, a versatile platform molecule. Among them, Al-exchanged two protons of H 4 SiW 12 O 40 (Al 2/3 H 2 SiW 12 O 40 ) was found to be uniquely effective. The kinetic behavior describing the conversion of cellulose to ethyl levulinate was investigated to monitor the process, and compared between parent H 4 SiW 12 O 40 and Al 2/3 H 2 SiW 12 O 40 to understand the mechanistic role of Al 3+ . The introduction of Al 3+ substantially facilitated cellulose depolymerization and glucose-to-fructose isomerization , leading to a high rate and product selectivity. The estimated activation energies for cellulose degradation and glucopyraoside alcoholysis decreased by 50.6 kJ/mol and 40.9 kJ/mol, respectively. 50–72% yields of ethyl levulinate were accomplished from cellulosic biomasses such as pine wood, eucalyptus, bamboo, bagasse and Napier grass. Al 2/3 H 2 SiW 12 O 40 allowed cellulose conversion in various linear alcohols producing high-yield alkyl levulinate, and could be reused multiple times with a good stability. This study opens a reliable and promising avenue for one-pot transformation of cellulose and raw lignocellulosic biomass to ester compounds.
研究领域:
生物化学
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可再生资源工程
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DOI
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2018
·
IF 5.667
Di Zhu,Dongxuan Guo,Lulu Zhang,Lichao Tan,Haijun Pang,Huiyuan Ma,Mo Zhai
Heteropolyacids (PMo 6 W 6 ) and ferrocene (Fc) were assembled on the glassy carbon electrode for the first time by electrodepositon method, and further combined with reduced graphene oxide (RGO) through the layer-by-layer self-assembly technology, developing a novel non-enzymatic nanocomposite for xanthine (XA) detection. The detection signal of XA was greatly amplified on the Fc-PMo 6 W 6 /RGO nanocomposite modified electrode due to coexist of these three active components. As ferrocene and PMo 6 W 6 all have relatively good electrochemical reversibility, fast electron transfer ability and generation of stable redox forms, meanwhile RGO can enlarge the active surface area of the electrode, increase the conductivity and load of ferrocene and PMo 6 W 6 . Under the optimized conditions, the developed nanocomposite modified electrode displayed superb sensing property towards xanthine with a widely linear range from 5.00 × 10 −8 ∼ 2.03 × 10 -3 M, along with a relatively low detection limit of 1.01 × 10 -8 M. The modified electrode has good stability as it is prepared by the smart combination electrodeposition and layer-by-layer self-assembly. Additionally, the nanocomposite was applied in detecting xanthine in actual samples with acceptable results, demonstrating the feasibility of Fc-PMo 6 W 6 /RGO nanocomposite in routine testing xanthine to some extent.
研究领域:
分析化学
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生物医学工程
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DOI
高影响因子
BIORESOURCE TECHNOLOGY
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2021
·
IF 9.642
Haichuan Zhang,Hui Zhang,Shenglong Tian,Shiyu Fu
In this work, near-complete conversion of lignocellulosic biomass and high products yields were achieved through catalytic transfer hydrogenolysis (CTH) in isopropanol using a heteropoly acid SiW 12 synergistic with Pd/C catalyst at a relatively mild condition. The performances of various heteropoly acids and catalytic conditions were extensively examined. The results confirmed that SiW 12 exhibited the highest activity on disrupting C–C linkages and C-O linkages than H 2 WO 4 , PW 12 , and PMo 12 . 34.91 wt% and 43.55 wt% monophenols were achieved for hydrogenolysis of bagasse and eucalyptus, respectively, at their optimal temperature for 5 h. Characterization studies on the lignin oil revealed that the notable structural changes were observed including the breaking of the side chain alkyl-aryl ether bonds and glycosidic bonds, while methoxyl groups were retained. Additionally, particle size of feedstock also has significant impact on the distribution and yields of the monophenols.
研究领域:
生物化学
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可再生资源与环境工程
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2021
·
IF 5.645
Sansan Bao,Chen Shen,Xiaodan Wu,Jingsong Cao,Chunjian Zhao,Wei Wang,Liping Yao,Xiqing Wang,Yujie Fu
An active and recyclable magnetic biobased heteropolyacid catalyst (HPW-MCMs) was prepared for the high yield of transesterification of Pistacia chinensis seed oil (PCO). The magnetic cellulose microspheres (MCMs) were used as the supporter, and the phosphotungstic acid (HPW) was synthesized in surface and micropores via in-situ reaction. Fourier transform infrared spectra (FT-IR), scanning electron microscopy (SEM), Energy-dispersive X-ray spectroscopy (EDX) and diffraction of X-ray (XRD) were fully used to characterize the catalyst. Furthermore, the conditions of 600 W of microwave power, 65 °C of temperature, 6 wt. % of catalyst amount, 8 of methanol/oil ratio and 30 min of reaction time were selected as the optimal conditions. Under the conditions, a high conversion of 96.6 % could be obtained. The HPW-MCMs could also be recovered conveniently and efficiently recycled for six cycles. Therefore, the prepared HPW-MCMs would be potentially useful for the efficient and economic transesterification reaction of PCO.
研究领域:
化学工程
·
可再生资源利用
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DOI
高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
·
2024
·
IF 4.4
Xiaohui Yang,Qi Ye,Fei Ge,Minghao Zhou
Lignin, as an important biomass resource, has significant research value in its oxidative cleavage process. Nickel-based metal catalysts could selectively depolymerize lignin. A series of heteropolyacid doped nickel based bimetallic catalysts Ni 4 Mo 1 -MOF-x（x represented heteropolyacid）were prepared by hydrothermal method, which were calcined to catalyze the oxidative cleavage of lignin model compound (2-phenoxy-1-acetophenone). The catalyst Ni 4 Mo 1 -MOF-SiWA-0.1(500) showed the best catalytic performance in methanol solvent under conditions of 160 °C, 4 h, 0.5 MPa oxygen pressure, where the conversion rate was nearly 100 % and the yields of phenol and benzoic acid were 54.5 % and 23.3 %, respectively. The catalysts were well characterized to explore the catalytic performance during the oxidation of lignin dimer. This study could provide some interesting and useful information for the catalytic oxidation of lignin to biomass-derived chemicals.
研究领域:
生物质化学
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催化化学
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）