RENEWABLE ENERGY
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2022
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IF 8.634
Yifan Nie,Qidong Hou,Hengli Qian,Xinyu Bai,Tianliang Xia,Ruite Lai,Guanjie Yu,Mian Laiq Ur Rehman,Meiting Ju
Sulfonated carbon material is an important class of catalysts, but controllable preparation of high-performance materials for biomass transformations is still challenging. Here, we demonstrate an effective strategy to prepare mesoporous sulfonated carbon materials from chicken bones to convert carbohydrates to 5-ethoxymethylfurfural (EMF). The carbonization of chicken bones without using additional templates gave hierarchical porous carbon materials. The subsequent sulfonation by chemical reduction approach introduced 2.33 mmol/g of -PhSO 3 H group, reserved abundant mesopores but blocked micropores. The sulfonated carbon materials afforded EMF yields of 94.7% and 68.6% from 5-hydroxymethylfurfural (HMF) and fructose in ethanol within 1.5 h and 2 h, respectively, without using high boiling point co-solvents. Furthermore, the apparent activation energies for HMF and fructose conversion were 29.1 and 49.5 kJ/mol, respectively. The catalyst could be reused four times with EMF yield decreasing from 68.6% to 62.7%.
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ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Jiahuan An,Guohan Sun,Haian Xia
An efficient method for the catalytic aerobic oxidation of 5-hydroxymethylfurfural (HMF) to 5-hydroxymethyl-2-furancarboxylic acid (HMFCA) was developed using size-controlled Ag nanoparticles (NPs) in an aqueous solution. A series of AgNPs catalysts stabilized by poly(vinylpyrrolidone) (PVP) supported on ZrO2with different Ag loadings were prepared. XRD, TEM, XPS, and FT-IR techniques were used to characterize the nature of these catalysts. The impact of the Ag loading, the molar ratio of PVP to Ag, the reaction temperature and time, and the base type on the conversion of HMF and yield of HMFCA was investigated. The reaction results show that Ag–PVP/ZrO2 catalysts with a bigger particle size (>10 nm) exhibited superior catalytic activity and HMFCA selectivity compared to Ag/ZrO2 with a smaller particle size (ca. 8.5 nm), indicating that the addition of PVP has a promoting effect on the aerobic oxidation of HMF into HMFCA. The 2.5%Ag–PVP/ZrO2(1:1) catalyst presents an excellent activity with 100% conversion of HMF and 98.2% yield of HMFCA in oxygen flow at 20 °C for 2 h.The basicity is also very critical to obtain a high HMFCA yield, especially for the use of high concentration of HMF; i.e., Ca(OH)2 afforded a higher selectivity toward HMFCA compared to the use of NaOH or Na2CO3 under an identical reaction condition. It is revealed for the first time that the presence of a capping agent (PVP) can effectively modulate the metal–support interaction. Interestingly, it is found that the relatively weak interaction between Ag NPs and the ZrO2 support has a beneficial effect on the conversion of HMF. This work provides new insights into the relationship between the metal–support interaction mediated by PVP molecule and the activity and selectivity of the oxidation reaction.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
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2014
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IF 2.063
Yongshen Ren,Bing Liu,Zehui Zhang,Jintao Lin
Three kinds of silver-exchanged phosphotungstic acid catalysts were prepared and used for the synthesis of potential biofuel 5-ethoxymethylfurfural (EMF). It was found that the partially silver exchanged phosphotungstic acid (Ag 1 H 2 PW) showed the best catalytic activity among silver exchanged phosphotungstic acids prepared. The highest EMF yield of 88.7% was obtained from 5-hydroxymethylfurfural (HMF) at 100 °C after 10 h. Furthermore, Ag 1 H 2 PW also showed high catalytic activity for the one-pot conversion of fructose into EMF with a yield of 69.5%. In addition, Ag 1 H 2 PW could be reused several times without a significant loss of its catalytic activity.
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ENERGY & FUELS
·
2024
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IF 5.2
Jia-yuan Tian,Jun Hu,Feng Lin,Yu-long Ma,Yong-gang Sun,Ying-bo Zhu,Jin-peng Wei,Yi-ting Lei,Jing-jing Wu
The catalytic selective hydrodeoxygenation of guaiacol to value-added cyclohexane is one of the sustainable biomass utilization pathways for which the Ru/HZSM-5 support catalyst has been considered as promising. However, the effect of the catalyst morphology on the catalytic properties must be further investigated. Four Ru catalysts with different support morphologies, two-dimensional nanosheets (Ru/HZSM-5-P), brick-shaped (Ru/HZSM-5-G), cross-shaped (Ru/HZSM-5-J), and irregular particles (Ru/HZSM-5-D), were prepared by the impregnation method to investigate the effects of catalyst morphology and acidity on the conversion efficiency of lignin-derived guaiacol to cyclohexane. The catalytic activity data showed that Ru/HZSM-5-P exhibited the best catalytic performance among the four catalysts with a conversion rate of 99.9% for guaiacol and a yield of 99.9% for cyclohexane. The characterization results showed significant differences among the four catalysts in terms of accessibility (thickness and pore volume), acidity, metal particle size, and reduction temperature. The Ru/HZSM-5-P catalyst with a two-dimensional nanosheet structure showed the best accessibility, smaller metal particle size, reasonable metal–support interaction, and appropriate B/L. The relatively strong acid centers facilitate the activation of C–C and C–O bonds. Besides, the reduced Ru species on the Ru/ZSM-5 catalyst exhibited high H2 adsorption activity, which was beneficial for the adsorption of guaiacol. This indicates that the difference in catalyst morphology could greatly affect its catalytic activity, thereby altering the conversion rate of reactants and selectivity of the products.
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MOLECULAR CRYSTALS AND LIQUID CRYSTALS
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2025
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IF 0.7
Yang Yun-Xia,Fu Shi-Huia,Ma Xiao-Na,Guo Ying-Wa,Wu Xiang-Xiang
In this article, two novel complexes with 5-[[4-(2H-Tetrazol-5-yl)phenyl]methoxy]-1,3-benzenedicarboxylic (HL) as ligand were synthesized under solvothermal conditions: [Co2L(H2O)2]∙2H2O (1), [Zn2L(H2O)2]∙2H2O (2). However, these two complexes are very unstable because they tend to lose their water molecules under room temperature. Single crystal X-ray diffraction analysis under low temperature show that these two complexes are isomorphic and the Schleffli symbol of the topological structure is {322.416.57}{341.468.511}. Interestingly, two unique Co atoms link with one water molecules to form a binuclear cluster, then the cluster further coordinates with the organic ligand and water molecules to infinitely extend to be one-dimensional chain, and the chains are connected with four nitrogen atoms of the ligands to form a two-dimensional layer structure, which are further connected to generate the final three-dimensional framework.
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Chemical Science
·
2024
·Vol. 15
·期 28
·11043-11052
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IF 7.6
Xingyu Lu,Ke Qi,Xueya Dai,Yunlong Li,Di Wang,Jing Dou,Wei Qi
The biomass-derived HMF oxidation reaction (HMFOR) holds great promise for sustainable production of fine chemicals. However, selective electrooxidation of HMF to high value-added intermediate product 5-formyl-furan-2-formic acid (FFCA) is still challenging. Herein, we report the electrocatalytic HMFOR to selectively produce FFCA using carbon paper (CP) supported polyaniline (PANI) as a catalyst. The PANI/CP non-metallic hybrid catalyst with moderate oxidation capacity exhibitsoptimized FFCA selectivity up to 76% in alkaline media, which has reached the best performance in reported literature studies. Identification and quantification of active sites for the HMFOR are further realized via linking the activity to structural compositions of PANI; both polaronic-type nitrogen (N3) and positively charged nitrogen (N4) species are proved responsible for adsorption and activation of HMF, and the intrinsic activity of N4 is higher than that of N3. The present work provides new physical–chemical insights into the mechanism of the HMFOR on non-metallic catalysts, paving the way for the establishment of structure–function relations and further development of novel electrochemical synthesis systems.
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PubMed
高影响因子
Sustainable Chemistry and Pharmacy
·
2024
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IF 5.5
Zhi-Gang Zhang,Yan Yi,Jia-Chun Lin,Dong Chen,Xiao-Jun Ji
2, 5-furandicarboxylic acid (FDCA) is a versatile bio-based building block that can be used for the synthesis of degradable polymers. Recently, developing green and sustainable catalytic processes for producing FDCA from renewable platform chemical molecules has attracted continuing attention. In this study, we proposed a green and sustainable one-pot, two-step biocatalytic process for the sequential oxidation of biomass-derived 5-hydroxymethylfurfural (HMF) to form FDCA with good yield and excellent selectivity. The initial step involves the oxidation of HMF to 2, 5-diformylfuran (DFF) and 5-formyl-2-furancarboxylic acid (FFCA) catalyzed by recombinant E. coli cells expressing a 5-hydroxymethylfurfural oxidase . The second step is to convert DFF and FFCA into FDCA final product via aldehyde oxidation reaction catalyzed by Deinococcus wulumuqiensis R12 whole cells . Combining the two different whole-cell biocatalysts , 180 mM of HMF could be easily converted into FDCA with a yield of 99% under optimized reaction conditions. This study offers an efficient and sustainable approach for the valorization of biomass-based HMF to form value-added FDCA.
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CHEMICAL ENGINEERING SCIENCE
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2025
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IF 4.3
Lin Zhou,Zhanghong Guo,Jingxuan Guo,Haining Cui,Jinxin Ma,Chan Wang,Qijun Song
2, 5-furandicarboxylic acid (FDCA) is an eco-friendly polyester monomer that holds great promise for the production of biodegradable plastics. FDCA can be prepared by the oxidation of 5-hydroxymethylfurfural (HMF), but the transformation was usually achievable only in alkaline conditions, resulting in a millimolar level reaction and complicated product purification. In present work, a series of iridium nanozymes with an average size of 2 nm were synthesized by using tartaric acid (TA) or other structurally similar small molecular ligands as the stabilizing agents. The different ligands significantly affect the Ir 4f binding energy, with TA exhibiting superior electron donation effect to the Ir center, thus facilitates the electron transfer and the enhancement in enzymatic efficiency. In the presence of H 2 O 2 , the TA-Ir nanozymes can directly catalyze the conversion of molar level HMF to FDCA in acidic condition (pH 4), achieving 99.8% HMF conversion and ∼ 90% FDCA yield.
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PREPARATIVE BIOCHEMISTRY & BIOTECHNOLOGY
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2017
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IF 1.361
Xiaoyan Li,Chen Qi,Peilian Wei,Lei Huang,Jin Cai,Zhinan Xu
Uridine 5′-diphosphate N-acetylglucosamine (UDP-GlcNAc) is a natural UDP-monosaccharide donor for bacterial glycosyltransferases, while uridine 5′-diphosphate N-trifluoacetyl glucosamine (UDP-GlcNTFA) is its synthetic mimic. The chemoenzymatic synthesis of UDP-GlcNAc and UDP-GlcNTFA was attempted by three recombinant enzymes. Recombinant N-acetylhexosamine 1-kinase was used to produce GlcNAc/GlcNTFA-1-phosphate from GlcNAc/GlcNTFA. N-acetylglucosamine-1-phosphate uridyltransferase from Escherichia coli K12 MG1655 was used to produce UDP-GlcNAc/GlcNTFA from GlcNAc/GlcNTFA-1-phosphate. Inorganic pyrophosphatase from E. coli K12 MG1655 was used to hydrolyze pyrophosphate to accelerate the reaction. The above enzymes were expressed in E. coli BL21 (DE3) and purified, respectively, and finally mixed in one-pot bioreactor. The effects of reaction conditions on the production of UDP-GlcNAc and UDP-GlcNTFA were characterized. To avoid the substrate inhibition effect on the production of UDP-GlcNAc and UDP-GlcNTFA, the reaction was performed with fed batch of substrate. Under the optimized conditions, high production of UDP-GlcNAc (59.51 g/L) and UDP-GlcNTFA (46.54 g/L) were achieved in this three-enzyme one-pot system. The present work is promising to develop an efficient scalable process for the supply of UDP-monosaccharide donors for oligosaccharide synthesis.
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PubMed
高影响因子
SENSORS AND ACTUATORS B-CHEMICAL
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2017
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IF 5.401
Danyang Ji,Yahui Du,Hongmin Meng,Lin Zhang,Zhongming Huang,Yalei Hu,Jianjun Li,Fei Yu,Zhaohui Li
In this work, cobalt oxyhydroxide nanoflakes (CoOOH nanoflakes) were reported to possess a high oxidizability toward TMB for the first time and based on which we have developed a new strategy for qualitative and quantitative detection of ascorbic acid (AA). In our design, CoOOH nanoflakes can directly oxidize 3,3′,5,5′-tetramethylbenzidine (TMB) to oxTMB with an obvious blue color emerging, and AA can selectively inhibit the oxidation of TMB to oxTMB by resolving CoOOH nanoflakes to Co 2+ , resulting in a decrease in the absorbance of oxTMB and bleaching of blue color. As such, the concentration of AA could be identified very easily by UV–vis spectroscopy and bare eyes. Under optimal conditions, this sensing platform showed a highly sensitive response to AA with a detection limit of 142 nM and a short assay time of 5 min. This assay was also successfully used to quantify AA in human serum samples and practical food samples. Importantly, using this fabricated sensing strategy, we have further developed a paper-based strip sensor for AA detection with satisfactory results, showing its great potential for point of care applications.
研究领域:
分析化学
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医学诊断
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食品科学
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JOURNAL OF PHYSICAL CHEMISTRY A
·
2017
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IF 2.847
Zhongneng Zhou,Xueyao Zhou,Xueli Wang,Bin Jiang,Yongle Li,Jinquan Chen,Jianhua Xu
Excited state dynamics of 5-azacytosine (5-AC), 2,4-diamino-1,3,5-triazine (2,4-DT), and 2-amino-1,3,5-triazine (2-AT) were comprehensively investigated by steady state absorption, fluorescence, and femtosecond transient absorption measurements. Time-dependent density functional theory (TDDFT) calculations were performed to help assign the absorption bands and understand the excited state decay mechanisms. The experimental results of excited singlet state dynamics for 5-AC, 2,4-DT, and 2-AT with femtosecond time resolution were reported for the first time. Two distinct decay pathways, with ∼1 ps and tens of picosecond lifetimes, were observed in 5-AC. Only one decay pathway with 17 ps lifetime was observed in 2,4-DT while an emissive state was found in 2-AT. TDDFT calculations suggest that 5-AC has a dark nπ* (S1) state below the first allowed ππ* (S2) state, which leads to the ultrafast decay of the ππ* state. In 2,4-DT, there is no dark nπ* state below the bright ππ* (S1) state and the 17 ps lifetime is assigned to the relaxation from the ππ* (S1) state to ground state. Two dark nπ* states (S1 and S2) were found in 2-AT, which exhibits much more complex excited state dynamics compared with the other two. Photoluminescence in 2-AT has been confirmed to be fluorescence emission from its bright ππ* (S3) state. Our results strongly suggest that electronic structures are very sensitive to the substitution on the triazine ring and that the photophysical properties of nucleic acid analogues depend highly on their molecular structures.
研究领域:
物理化学
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光化学
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计算化学
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分子光谱学
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核酸类似物
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2022
·
IF 9.136
Yonghou Xiao,Jiahui Fu,Heyang Zhu,Qidong Zhao,Liang Zhou
The diffusion limitation owing to the long and narrow pore structure in traditional ZSM-5 zeolite could restrain the adsorptive desulfurization performance towards thiophene sulfur compounds from fuels. Herein, ZSM-5 zeolite nanocrystals were successfully fabricated using steam-assisted gel crystallization strategy to control the size of zeolite particles within 70 ∼ 160 nm. Compared to traditional micron ZSM-5, ZSM-5 zeolite nanocrystals could effectively reduce the diffusion pathway, enlarge the specific surface area, and increase exposure of adsorption sites, which could enhance the desulfurization performance. ZSM-5 nanocrystals with a mole ratio SiO 2 /Al 2 O 3 of 200 exhibited a satisfactory desulfurization efficiency, and the breakthrough capacity attained 0.0509 mmol S/g adsorbent. After ZSM-5 nanocrystals were ion-exchanged with NH 4 + and Ag + , both mesoporous characteristics and the Lewis acid (L-acid) sites were enhanced, which promoted the adsorption desulfurization performance. Furthermore, nanocrystalline ZSM-5 and Ag/ZSM-5 also exhibited acceptable regeneration performance. This study is expected to provide an effective strategy and a facile method to prepare nanocrystalline ZSM-5 based adsorbents for the development of efficient desulfurization materials.
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