FUEL
·
2023
·
IF 7.4
Wenqi Zhao,Xiaowei Bai,Xiangrui Lin,Yalkunjan Tur sun,Mei Zhong,Zhenghua Dai,Jian Li
Biomass-derived furfural and its derivatives are promising feedstocks for producing valuable C 5 diols by catalytic hydrolysis. However, this process requires selective ring opening of tetrahydrofurfuryl alcohol (THFA) to 1,5-pentanediol, which is challenging. Here we report efficient route for this conversion using Ni-La(OH) 3 catalysts prepared by a green co-precipitation-hydrothermal method. We show that these catalysts can achieve up to 91.7% yield and 94.6% selectivity of 1,5-pentanediol from THFA under mild conditions. We elucidate the key role of the La(OH) 3 phase, the basic sites and the Ni n+ -O-La 3+ structure of the catalysts in promoting the selective hydrogenolysis and ring opening of THFA. We also demonstrate that the co-dehydrogenation of secondary alcohols enables lower reaction pressure and longer catalyst lifetime. Our work provides a sustainable and environmentally benign approach for producing 1,5-pentanediol from biomass-based furfural and its derivatives, which has potential applications in polymer synthesis and green chemistry.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2023
·
IF 2.6
Jian Chen,Mei Dong,Wenjing Shi,Danni Zhao,Wensheng Li,Haoran Liu,Weiping Luo
In this study, the solubility of isophthalic acid (IPA) and m-toluic acid (m-TA) in eight monobasic alcohols, methanol, ethanol, 1-propanol, iso-propanol, 1-butanol, iso-butanol, tert-butanol, and 2-butanol is measured under 101.3 kPa by the method of laser dynamics. The experimental temperature range is 294.35–360.75 K. The measured data showed that the solubility of IPA and m-toluic acid increased with the increase of temperature in the measured temperature range. At the same temperature, the solubility of m-toluic acid in the same pure solvent is higher than that of IPA. The solubility of IPA and m-toluic acid in eight solvents decreased with the increase of the number of carbon atoms of the solvent. At the same temperature, the solubility ratio of m-toluic acid to IPA in iso-butanol is the highest in the same solvent, and the ratio was greater than 70, making it the best solvent for separating IPA and m-toluic acid. The Apelblat model, the Buchowski–Ksiazczak λh model, and the modified nonrandom two-liquid activity coefficient model were used to correlate the experimental data, and the calculated solubility was in good agreement with the measured result. The calculated solubilities were in good fit with the measured results. The thermodynamic properties were calculated, and the main contributor of the standard molar Gibbs energy of IPA and m-toluic acid in eight alcohols is enthalpy, about 55.40 to 82.86%.
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Electrocatalysis
·
2022
·Vol. 13
·期 6
·818-829
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IF 2.933
Dong Zhichen,Wu Jian,Guo Xingjia
In this work, we prepared cubic nickel oxide (NiO) nanosheets and constructed NiO with oxygen defects induced by halogen Cl ions (NiO-Vo1). Cubic nickel oxide nanosheets were used as catalysts for electrocatalytic oxygen evolution reaction (OER) and oxidation of chiral 2-butanol. Under artificial simulated sunlight, NiO-Vo1 exhibited good photo-electrocatalytic OER activity and catalytic stability. The high catalytic activity is mainly attributed to the activation of nickel active sites by the halide ion-induced oxygen defect and the enhancement of photoinduced electron–hole separation efficiency. Furthermore, the electrocatalytic performance of oxygen-deficient nickel oxide for the oxidation of chiral 2-butanol was investigated. The results show the catalytic activity of NiO-Vo1 for electrocatalytic oxidation of 2-butanol to butanone compared with NiO. Interestingly, there is no significant difference in the electrocatalytic activity of NiO for (R)-(-)-2-butanol and (S)-( +)-2-butanol oxidation. When NiO-Vo1 was used as the catalyst, the catalytic oxidation reaction rate of (R)-(-)-2-butanol alcohol was significantly higher than that of (S)-( +)-2-butanol alcohol. At 1.77 V vs RHE voltage, the (R)-(-)-2-butanol alcohol has obvious oxidation reaction while the (S)-( +)-2-butanol alcohol is almost absent, realizing the selective electrocatalytic oxidation of (R)-(-)-2-butanol alcohol. This may be attributed to the difference in the interaction strength of chiral molecules with the surface defects of NiO after applying a voltage during the catalytic process, resulting in different catalytic activities. Here, our proposed strategy through the synergistic effect of applied voltage and surface defects provides a new approach for chiral molecule synthesis and efficient chiral resolution. The halide ion-induced defect-catalyst provides a new strategy for the preparation of efficient electrocatalytic water splitting OER and alcohol-selective oxidation catalysts. Graphical Abstract
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Separation Science Plus
·
2022
·Vol. 5
·期 9
·513-519
·
IF 0
Yanni Huang,Jia Chen,Gafang Fu,Chi Zhang,Hongdeng Qiu
This work reported the preparation and evaluation of a 2D porous graphene as the stationary phase for gas chromatography with high-resolution performance from non-polar to polar structural isomers. As a result, the dynamically coated porous graphene capillary column has a film thickness of about 16 μm. After aging treatment at different temperatures, the porous graphene capillary column exhibited high thermal stability up to 300°C. In addition, the porous graphene capillary column has good column repeatability and reproducibility. The retention time RSDs are 2.61–3.90% ( n = 3) during the days and 4.58–4.78% ( n = 3) column-to-column. This work demonstrates the advantageous separation performance of a good potential for the porous graphene as a new stationary phase for gas chromatography analysis.
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Journal of Coatings Technology and Research
·
2022
·Vol. 19
·期 4
·1233-1241
·
IF 2.339
Wang Tian-Yu,Yang Wei,Hui Hao-Hao,Lei Xiang-Yang,Zhang Qing-Hua,Wang Jian,Xu Qiao,Deng Xue-Ran
The sol–gel method is an important process for the preparation of laser frequency conversion components, such as dihydrogen phosphate (KDP), which are often employed in high-power laser facility. Methyltriethoxysilane (MTS) precursor is a typical matrix to prepare polysiloxane under hydrolysis and polycondensation process. Further coating and curing procedure is applied to obtain desired polysiloxane coating which acts as the moisture-proof and refractive index matching layer. Subsequently, an antireflective coating is prepared over this polysiloxane coating (a bilayer coating system) to realize ultrahigh transmission at desired wavelengths. Due to the low curing temperature (limited by the phase transition temperature of KDP), current MTS-polysiloxane coating could not be completely cured and inter-coating permeation between this bilayer coating system would lead to deterioration of coating properties. Thus, copolymerization of MTS and tetraethylorthosilicate (TEOS) is adopted to fabricate the polysiloxane coating with improved curing property (denser structure and higher hardness after curing). It is found that under certain molar ratio of MTS to TEOS, the structure of modified polysiloxane coating could be effectively densified and the coating hardness increases significantly. Meanwhile, the bilayer coating system still exhibits excellent transmission, high laser-induced damage threshold as well as satisfactory moisture resistance.
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CHEMICAL ENGINEERING JOURNAL
·
2022
·
IF 16.744
Xiao Xiao,Yajie Zhao,Ping'an Ma,Ziyong Cheng,Jun Lin
Sonodynamic therapy (SDT), one of the rising non-invasiveness methods relying on ultrasound-stimulated reactive oxygen species (ROS), has emerged as a cancer therapeutic approach aiming to eliminate deep-seated solid tumors. It remains challenging for the integration of sensitive US responsivity, high quantum yield for ROS, low toxicity and appropriate bio-degradability into one sonosensitizer. Here, the two-dimensional (2D) boron-based B-OH@Cy5-PEG-NH 2 nanosheets (BOP NSs) as a new type of sonosensitizer are synthesized via liquid exfoliation technology and adopted in SDT therapy. These BOP NSs expose an elevated US-stimulated severance of electron (e - )-hole (h + ) pairs, attributing to the narrower band gap than other nano-sonosensitizers. Moreover, we investigate other undeveloped features of BOP NSs such as attractive peroxidase-like activity and beneficial biological effects of biodegradation. Experiments both in vitro/vivo exhibit significant therapeutic effects against tumor growth due to the elevated ROS generation by the combination treatment of US-based SDT and enzyme catalytic reaction. It is believed that such BOP NSs highly united with multifunctionality and great biodegradability can be wildly directed at cancer therapy and expand a brand new route for the utility of 2D boron NSs.
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JOURNAL OF CHEMICAL AND ENGINEERING DATA
·
2021
·
IF 2.694
Yangyi Huang,Lin Zhang,Mengqi Yan,Qinan Huang,Yuning Zhang,Yanqun Ren,Weiping Luo
In this research, the solubilities of adipic acid in sec-butyl alcohol (SBA), isobutyl alcohol (IBA), and n-octyl alcohol (NOA); glutaric acid in n-propyl alcohol, isopropyl alcohol, n-butyl alcohol, SBA, IBA, tert-butyl alcohol (TBA), and NOA; and succinic acid in SBA, IBA, TBA, and NOA were determined by the dynamic laser method from 302.65 to 352.95 K at atmospheric pressure (101.3 kPa). Furthermore, the solubilities of three dibasic acids in straight-chain alcohols of different lengths and alcohol isomers were compared. Meanwhile, X-ray diffraction was used to detect the change of the crystal form before and after dissolution. Additionally, the experimental data were correlated by two models (Apelblat model and the modified nonrandom two liquid activity coefficient model), showing that the model matched well with the experimental data. The most accurate model is selected for every system after calculating the Akaike information criterion of each model.
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2021
·
IF 3.764
Shahid Hussain,Haifeng Dong,Yanqiang Zhang,Guoxiong Zhan,Shaojuan Zeng,Huifang Duan,Xiangping Zhang
The efficient capture of carbon dioxide (CO2) has industrial, economic, and environmental significance. Here, CO2 capture performance in terms of CO2/CH4 selectivity for the zeolitic imidazolate framework (ZIF-8) is enhanced by impregnation of 1-n-butyl-3-methylimidazolium dicyanide [BMIM][DCA]. The preparation of ionic liquids (ILs)/ZIF-8 composites, their comprehensive characterization, and the impact of IL impregnation are all investigated. The crystal structure and morphology of ZIF-8 remained intact even after the impregnation of ILs, according to X-ray diffraction and scanning electron microscopy studies. The infrared spectroscopy known as Fourier transform infrared spectroscopy determines the interaction between ILs and ZIF-8 in the composite. The isotherm fitting was also performed by dual site Langmuir models, which showed good agreement with the experimental results. The CO2/CH4 selectivity results demonstrated that the ideal selectivity for the IL-impregnated ZIF-8 composite has five times higher selectivity than pristine ZIF-8 at 0.05 bar which is the highest reported selectivity. The normalized selectivity of this type of IL/ZIF-8 composite is also higher. This study suggested that the IL/MOF composite with a tunable structure have a strong potential for enhanced acid gas separation performance to meet the environmental challenges.
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ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Guoxing Liu,Huai Liu,Junhua Zhang,Rui Zhang,Heng Zhang,Yong Sun,Lincai Peng
Catalytic conversion of concentrated carbohydrates and raw biomass into 5-hydroxymethylfurfural (HMF), an important and value-added platform chemical, is highly desirable for industrial applications but challenging. In this work, the tin pyrophosphate-oxide (SnP2O7–SnO2) catalyst has been designed to efficiently produce HMF from various concentrated carbohydrates and raw biomass. Especially, a high HMF yield of 67.8% was implemented over the SPC4 catalyst from concentrated glucose (36 wt %) in a biphasic solvent system of water and methyl isobutyl ketone. Moreover, the SPC4 catalyst disclosed a wide range of universality for converting various concentrated carbohydrates and raw biomass to HMF with satisfactory yields (45.9–79.5%). To the best of our knowledge, this is the first example of accomplishing appreciable HMF yields from carbohydrates and raw biomass at such a high substrate concentration. It has been demonstrated that the superior catalytic performance of the catalyst should originate from its balanced Lewis and Brønsted acidity and superhydrophilicity property. This work invents a highly promising heterogeneous catalyst for efficiently valorizing renewable lignocellulose-related compounds into versatile furans.
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MICROPOROUS AND MESOPOROUS MATERIALS
·
2023
·
IF 5.2
Pingping Li,Lei Han,Donghun Kim,Kemal Celebi
The demand for high aspect ratio zeolite crystals has been increasing dramatically for many applications, ranging from catalysis to membrane separations . However, manufacturing such platelike crystals usually requires energy-intensive and time-consuming synthesis procedures. Here, by employing a thin-wall tubular reactor, we report for the first time a fast synthetic strategy that yields preferentially- b -oriented platelike MFI crystals within minutes of hydrothermal treatment . Various synthesis conditions such as hydrolysis, precursor aging, chemical compositions, etc. can be quickly optimized within days. Such optimization resulted in highly crystalline platelike crystals with lateral dimensions up to ∼5 μm length in c -axis or ultra-thin crystals with ∼25 nm thickness. Meanwhile, non-platelike MFI crystals can even reach 135 μm lateral size in 24 h. This fast synthetic strategy can be further generalized for the preparation and optimization of diverse important materials including MOFs , COFs , and other zeolites, benefiting both fundamental research and practical applications.
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FUEL
·
2023
·
IF 7.4
Shuangshuang Cen,Lijun Wang,Cong Wan,Xinyan Chai,Lei Li,Wensheng Linghu
Zr 4+ −O 2− pairs in MOFs and macromolecule − Zr(IV) complexes have proved one of the ideal catalytic components for catalytic transfer hydrogenation of biomass-derived furfural. However, restricted by limited adjustability of Zr 4+ −O 2− coordination environment and the complex design and creation of ligand defects, currently, there are only a few efficient low-temperature (<100 °C) catalytic systems. In this work, oxygenated groups enriched polyolefin − Zr(IV) complexes were prepared and fixed on/in mesoporous silica aerogel support. The complexes possessed a stable structure with C C bonds as the connecting skeleton of each oxygenated group, and the types and densities of oxygenated groups ( COOH, SO 3 H, and OH) could be easily adjusted by using different monomers. In the catalytic transfer hydrogenation reaction of furfural and 2-propanol, the catalyst synthesized using dicarboxylic maleic acid as a monomer of polyolefin exhibited the best catalytic performance in low temperatures, the main product furfuryl alcohol with a high yield of 96.0 % and a high selectivity of 98.2 % was obtained at 85 °C for 8 h. In 6 cycles of reactions at 85 °C, the furfuryl alcohol yield decreased gradually from 96 % in the 1st cycle to 84.0 % in the 4th cycle and further restored to 90.9 % and 89.3 % in the 5th and 6th cycles, respectively, by refreshing the used catalyst with methanol washing, and there was almost no leaching of Zr 4+ species in the reaction medium. The catalyst poisoning experiment with acidic and basic sites shielded by pyridine and boric acid, respectively, showed that the catalytic activity was more sensitive to the shielding of basic sites, and the isotope experiments revealed that two H of the product furfuryl alcohol are transferred from 2-propanol. Hereby, the oxygenated group-bearing polyolefin − Zr(IV) complexes with stable structure, variable functional groups and the corresponding various Zr 4+ −O 2– coordination pairs, are ideal catalyst candidates for the selective transfer hydrogenation of furfural to furfuryl alcohol.
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APPLIED CATALYSIS A-GENERAL
·
2021
·
IF 5.706
Weizhong Mao,Junhua Liu,Bingqian Yin,Deyu Kong,Shiwen Miao,Fang Wang
We propose a simple preparation route that converting biomass-derived furfural (FUR) to furfuryl alcohol (FOL) over a series of Ni-Mg-Al catalysts (NMA-n) with different molar ratios. Yield of FOL can reach 96.8 % over NMA-2 catalyst under the mild reaction conditions. There are three reasons for this high yield of FOL: (1) The introduction of different amounts of Mg and Al causes the synergistic effect to adjust the acidity and basicity of catalyst, optimal acid-base ratio (0.73:1) and Ni metal site achieve multi-centers collaborative catalysis. (2) Mesoporous structure of this catalyst provides a large number of adsorption sites. Furthermore, the highest O defect /O lattice ratio (1.79:1) create more oxygen vacancies, and then increase the adsorption sites of reactants, thereby making the catalytic activity of NMA-2 higher than most reported Ni-based catalysts. (3) Through kinetic studies, this excellent catalytic performance is related to activation energy (51.8 kJ/mol), which is lower than most reported CTH catalysts.
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