Sustainable Energy & Fuels
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2022
·Vol. 6
·期 9
·2368-2376
·
IF 6.813
Yanping Xiang,Kangyu Zhao,Shuolin Zhou,Wenguang Zhao,Zhijuan Zeng,Xiaoting Zhu,Xianxiang Liu
The catalytic transformation of biomass derived compounds into valuable liquid fuels has received considerable attention in the past few years. In this work, sulfonic acid grafted halloysite nanotubes (HNTs-SO3H) were facilely synthesized via functionalizing the halloysite nanotubes with 1,3-propanesultone, and the physico-chemical properties of the synthesized catalysts were analyzed by Fourier transform infrared spectroscopy (FT-IR), transmission electron microscopy (TEM), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), N2 adsorption isotherm techniques, etc. The characterization results revealed that the organic–inorganic mesoporous materials preserved the tubular structure of the halloysite nanotubes and were equipped with active sulfonic acid sites. The as-synthesized catalyst was employed for the catalytic conversion of 5-hydroxymethylfurfural (HMF) to biofuel 5-ethoxymethylfurfural (EMF) under solvent-free conditions. Response surface methodology (RSM) with Box–Behnken design (BBD) was used to investigate the influence of the reaction conditions such as reaction temperature, reaction time and catalyst dosage on EMF yield. An excellent EMF yield of 86.4% and HMF conversion of 99.3% could be achieved at 126 °C for 35 minutes over the HNTs-SO3H catalyst. Furthermore, the kinetics of the conversion of HMF to EMF was also studied, and the kinetic modeling results indicated that this reaction follows pseudo-first-order kinetics, and the activation energy obtained was 60.12 kJ mol −1.
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DALTON TRANSACTIONS
·
2022
·Vol. 51
·期 8
·3096-3103
·
IF 4.569
Lixia Sun,Shangyang Li,Zhuoyou Gao,Shutao Gao,Wei Gao,Xiang Cheng,Ningzhao Shang,Yongjun Gao,Chun Wang
Fabrication of biofuels and chemicals from renewable biomass is highly desirable to replace petrochemicals. Hydrogenolysis of biomass derived 5-hydroxymethylfurfural (HMF) is a promising way to obtain furanic fuels. In this paper, we describe the preparation of a CoSi-PS catalyst derived from cobalt phyllosilicate using a silica sol as the silica source. CoSi-PS exhibited excellent catalytic performance for the hydrogenolysis reaction of HMF to produce liquid 2,5-dimethylfuran (DMF) biofuel. 100% conversion of HMF and 97.5% selectivity for DMF were achieved at 170 °C and 1.5 MPa H2 for 4 h, which was superior to most of the reported catalysts. The excellent performance can be attributed to the strong interactions between the metal and support, highly dispersed cobalt nanoparticles and the Lewis acid sites induced by the coordinated unsaturated Co(II) sites in phyllosilicate.
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MOLECULES
·
2011
·Vol. 16
·期 10
·8463-8474
·
IF 1.988
Haibo Xie,Zongbao K. Zhao
A new compound was detected during the production of 5-hydroxymethylfurfural (HMF) from glucose and cellulose in the ionic liquid 1-butyl-3-methylimidazolium chloride ([Bmim]Cl) at high temperatures. Further experiments found that it was derived from the reaction of HMF with [Bmim]Cl. The structure of new compound was established as 1-butyl-2-(5’-methyl-2’-furoyl)imidazole (BMI) based on nuclear magnetic resonance and mass spectrometry analysis, and a possible mechanism for its formation was proposed. Reactions of HMF with other imidazolium-based ionic liquids were performed to check the formation of BMI. Our results provided new insights in terms of side reactions between HMF and imidazolium-based ionic liquids, which should be valuable for designing better processes for the production of furans using biomass and related materials.
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高影响因子
CATALYSIS TODAY
·
2015
·
IF 3.893
Jing Xing,Liang Song,Cong Zhang,Mingdong Zhou,Li Yue,Xuebing Li
Upgrading of lignin derived bio-oil is a very promising way to relieve humankind's dependence on traditional fossil fuels. Eugenol, a model compound for lignin monomers with a methoxyl group and a hydroxyl group, was hydrodeoxygenated in aqueous phase with Pd/C as hydrogenation catalyst and ZSM-5 zeolite as hydrolysis and dehydration catalysts. The bulky lignin monomers had difficulty in accessing the acid sites of the micropores of ZSM-5 zeolite, thus we introduced mesopores via alkaline treatment under various conditions. Alkali-treated ZSM-5 zeolites showed higher conversion and hydrocarbon selectivity compared to the parent ZSM-5 zeolite. When ZSM-5 zeolite was treated at 338 K, the conversion and the hydrocarbon selectivity increased by 21% and 24%, respectively. In addition, much more weak acid sites of ZSM-5 zeolites after alkaline treatment also promoted the hydrolysis and dehydration process.
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Journal of Biobased Materials and Bioenergy
·
2018
·Vol. 12
·期 4
·321-329
·
IF 2.993
Liao Longfei,Liu Ying,Wu Shubin
A series of V2O5/SBA-15 catalysts with various loadings of 5, 10, 15 and 20% (by weight) V2O5 have been prepared by molecular designed dispersion (MDD) method and are characterized by N2 adsorption–desorption, Fourier Transform-Raman
spectroscopy (FT-Raman), transmission electron microscopy (TEM), low angle and wide-angle XRD, H2 temperature programmed reduction (TPR), inductively coupled plasma-optical emission spectrometry (ICP-OES), and Ultraviolet-visible diffuse reflectance spectroscopy (UV-Vis, DRS) techniques.
Among V2O5/SBA-15 catalysts, the 10% V2O5/SBA-15 catalyst exhibited 88.6% 5-hydroxymethylfurfural (HMF) conversion with 57.9% yield of 2,5-diformylfuran (DFF) when molecular oxygen (0.28 MPa) and toluene were employed as green oxidant and organic
solvent respectively at 110 °C. The remarkable performance of 10% V2O5/SBA-15 catalyst is owing to the isolated distribution of uniform sized nanovanadium species which are dispersed on the pore surfaces of the hexagonally well-ordered mesoporous material SBA-15 silica
support.
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Journal of Materials Chemistry A
·
2018
·Vol. 6
·期 42
·21178-21185
·
IF 9.931
Hao Chen,Xu Shi,Jianfang Liu,Kecheng Jie,Zihao Zhang,Xiaobing Hu,Yimei Zhu,Xiuyang Lu,Jie Fu,He Huang,Sheng Dai
Zeolite materials play a significant role throughout the oil refining and petrochemical industry. Microporous ZSM-5 has a high degree of crystallinity but low mass transfer, while hierarchical ZSM-5 shows a low degree of crystallinity as well as acidity. In this work, we first report the synthesis of ZSM-5 with a new morphological structure, which has nanocrystalline ZSM-5 particles on the surface of an intact ZSM-5 zeolite. This not only improved the mass transfer in microporosity but also overcame disadvantages of hierarchical ZSM-5 including low degrees of crystallinity and acidity. This new and very efficient structure with both intracrystal microporosity and intercrystal macroporosity, formed by secondary crystallization after the intact ZSM-5 zeolite was synthesized, was verified by transmission electronic microscopy, N2 adsorption and desorption, and X-ray diffraction. The obtained ZSM-5 zeolite showed a uniform size (∼200 nm), high crystallinity acidity, and a suitable hierarchical structure that exhibited excellent properties in the catalytic fast pyrolysis of cellulose to produce aromatics.
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高影响因子
ACS Applied Materials & Interfaces
·
2021
·
IF 9.229
Chao Du,Di Zhou,Shu-Zhao Hao,He-Tuo Chen,Jian Zhang,Shi-Kuan Sun,Tao Zhou,Ming-Zhao Dang,Shao-Fei Wang,Hai-Wen Liu,Long Li,Zhuo Xu
Transparent material has been widely used in product design and has seen a large increase in its use. In this paper, a kind of aesthetically decorative 5 GHz Wi-Fi dielectric resonator antenna (DRA) of aluminum oxynitride (AlON) transparent ceramic has been designed. High-quality-factor AlON transparent dielectric ceramics were fabricated by presintering at 1780 °C and further cold isostatic pressing (CIP) under a 200 MPa argon atmosphere. For a 9.0 mm thick specimen, the in-line light transmittance reached 83%. Optimum dielectric constant (εr = 9.32), quality factor (Qf = 47 960) and temperature coefficient (TCF = −51.7 ppm/°C) was achieved in the AlON transparent ceramic by cold isostatic pressing. As a result, the proposed aesthetically decorative DRA can achieve an impedance bandwidth of 32% (4.48–6.19 GHz), a high radiation efficiency of 85%, and a low cross-polarization discrimination (XPD) of −30 dB. To achieve a broad bandwidth, the proposed antenna was excited in its dominant TE111x mode and higher-order TE113x mode. The proposed antenna is thus an excellent candidate for an indoor decoration Wi-Fi antenna.
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Journal of Energy Chemistry
·
2025
·
IF 14.9
Zehua Liu,Caiyi Liu,Shenghe Si,Ying-Ao Liu,Xuhui Shao,Dong Liu
Photoelectrochemical (PEC) oxidation provides a promising strategy to convert solar energy into high-value-added products. The oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to 2,5-furandicarboxylic acid (FDCA) is of particular interest, but efficient PEC conversion remains challenging due to the limitations of selectivity, stability, and energy conversion efficiency. Although n-type silicon offers the highest theoretical photocurrent, its practical application is hindered by insufficient photovoltage and sluggish interfacial catalysis. Here, we report a NiO x /Ga 2 O 3 /n-Si photoanode integrated with a Ni(OH) 2 cocatalyst for efficient HMF oxidation. The ultrathin Ga 2 O 3 interlayer facilitates the built-in electric field, thus leading to enhanced photovoltage and enabling superior HMF oxidation performance. When coupled with a commercial Pt/C cathode, the system achieves stable, bias-free FDCA production under simulated solar illumination. This work highlights the potential of engineered silicon photoanodes for sustainable light-driven biomass valorization.
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高影响因子
CHINESE JOURNAL OF CHEMICAL ENGINEERING
·
2024
·
IF 3.7
Xin Li,Yue Ma,Xuning Wang,Jianguo Wu,Dong Cao,Daojian Cheng
The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an important reaction in the field of biomass hydrogenation, because it is a bridge between biomass resources and chemical industry. Here, we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method. By changing the reduction temperature, catalysts with different oxidation state could be precisely constructed. Moreover, the important correlation between the ratio of Pd 0 /Pd 2+ and catalytic activity is revealed during the selective hydrogenation of HMF. The Pd/g–C 3 N 4 –300 catalyst with a Pd 0 /Pd 2+ ratio of 3/2 showed the highest catalytic activity, which could get 96.9% 5-hydroxymethylfurfural conversion and 90.3% 2,5-dihydroxymethylfuran selectivity. Further density functional theory calculation revealed that the synergistic effect between Pd 0 and Pd 2+ in Pd/g–C 3 N 4 –300 system could boost the adsorption of the substrate and the dissociation of hydrogen. In this work, we highlight the important correlation between metal oxidation state and catalytic activity, which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
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Carbon Letters
·
2025
·
IF 5.8
Xiao Xinyu,Li Mingyue,Chen Guangmeng,Zhou Weihua,Zhao Weiwei,Liu Xiaoqing
Improving the oxygen evolution reaction (OER) performance or replacing OER with the value-added conversion of biomass is of great significance for the green hydrogen energy production. In this work, bimetallic species-decorated laser-induced graphene (LIG) was fabricated and demonstrated as the self-supported electrodes towards efficient OER and 5-hydroxymethylfurfural oxidation reaction (HMFOR). Three-dimensional LIG was obtained via one-step irradiation process under ambient conditions, and active metal species were then introduced through electrodeposition, with Ni-based catalyst as the primary catalytic material and Fe and Co as modified metals. Among, LIG-NiFe electrode achieved an extremely low overpotential of 241.7 mV at a current density of 20 mA/cm 2 for OER and demonstrated long-term stability. This could be attributed to the promoted formation of Ni 3+ active centers by Fe modified and the intrinsic porous structure of LIG providing an enhanced surface area. As for LIG-NiCo, due to the low onset potential of Co for HMF, it could achieve 99.6% HMF conversion and yielded value-added 2, 5-furandicarboxylic acid (FDCA) with a selectivity of 87.1%. Coupled with the merit of facile fabrication of LIG framework, this study demonstrates that LIG-based electrodes assume great practical application value in electrocatalytic reactions. Graphical abstract
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BIOCHEMICAL PHARMACOLOGY
·
2025
·
IF 5.6
Dapeng Lu,Lin Ma,Qingyue Zhang,Chengzhong Xing,Yanke Li
5-Fluorouracil (5-FU) is an effective drug in the treatment of colorectal cancer (CRC); however, the development of acquired resistance to 5-FU poses a great challenge in clinical practice. Through the analysis of public datasets, we found that reduced 3-Hydroxybutyrate Dehydrogenase 2 (BDH2) expression in CRC tissues predicted poor survival in CRC patients. Low expression of BDH2 in clinical CRC tissue samples predicted a higher degree of malignancy. In addition, public dataset analysis showed that GLI Pathogenesis Related 1 (GLIPR1) expression was elevated in CRC patients following 5-FU treatment, contrasting with the expression pattern of BDH2. We reported that in 5-FU-resistant CRC cell lines (LOVO/5-FU and HCT15/5-FU), BDH2 was downregulated, while the expression of GLIPR1 was increased. To explore the regulatory relationship between BDH2 and GLIPR1 in 5-FU resistance, BDH2 and GLIPR1 overexpression plasmid vectors were constructed to transfect 5-FU resistant CRC cell lines. BDH2 led to enhanced 5-FU sensitivity in 5-FU-resistant CRC cell lines and inhibited the malignant behavior of CRC-resistant cells in vitro . In nude mice with subcutaneous tumors and intraperitoneal injections of 5-FU, tumor tissues formed by BDH2-overexpressing cells exhibited slower growth and increased apoptosis. Mechanistically, the upregulation of BDH2 increases GLIPR1 promoter methylation, mediated by DNA methyltransferases, thereby inhibiting GLIPR1 expression. High expression of GLIPR1 reduces 5-FU sensitivity in 5-FU-resistant CRC cell lines, which abolished the impact of BDH2 expression. These results suggest that BDH2 inhibits GLIPR1 expression by increasing GLIPR1 promoter methylation, thereby enhancing 5-FU sensitivity of 5-FU-resistant CRC cell lines and inhibiting CRC progression.
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PubMed
高影响因子
Journal of Energy Chemistry
·
2024
·
IF 14
Haoyu Zhan,Baixue Cheng,Yankun Lu,Danning Xing,Xingshuai Lv,Huining Huang,Thomas Frauenheim,Tao Wang,Peng Zhou
Co 3 O 4 possesses both direct and indirect oxidation effects and is considered as a promising catalyst for the oxidation of 5-hydroxymethylfurfural (HMF). However, the enrichment and activation effects of Co 3 O 4 on OH − and HMF are weak, which limits its further application. Metal defect engineering can regulate the electronic structure, optimize the adsorption of intermediates, and improve the catalytic activity by breaking the symmetry of the material, which is rarely involved in the upgrading of biomass. In this work, we prepare Co 3 O 4 with metal defects and load the precious metal platinum at the defect sites (Pt-Vco). The results of in-situ characterizations, electrochemical measurements, and theoretical calculations indicate that the reduction of Co–Co coordination number and the formation of Pt–Co bond induce the decrease of electron filling in the antibonding orbitals of Co element. The resulting upward shift of the d -band center of Co combined with the characteristic adsorption of Pt species synergically enhances the enrichment and activation of organic molecules and OH − species, thus exhibiting excellent HMF oxidation activity (including a lower onset potential (1.14 V) and 19 times higher current density than pure Co 3 O 4 at 1.35 V). In summary, this work explores the adsorption enhancement mechanism of metal defect sites modified by precious metal in detail, provides a new option for improving the HMF oxidation activity of cobalt-based materials, broadens the application field of metal defect based materials, and gives an innovative guidance for the functional utilization of metal defect sites in biomass conversion.
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