JOURNAL OF COLLOID AND INTERFACE SCIENCE
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2022
·
IF 9.965
Xiaofeng Wang,Chengcheng Zhang,Zuyi Zhang,Yaoming Gai,Qingbo Li
The interface site between metal and support possess unique electronic and morphological structure, providing distinct active centers for favorable reaction in catalytic conversion of biomass derivatives to valuable chemicals. In this study, a series of Cu-Co/CeO x catalysts were prepared for hydrogenolysis of 5-hydroxymethylfurfural (HMF) to 2,5-dimethylfuran (DMF) via reduction of the corresponding layered double hydroxide precursors. The characterizations indicated the formation of CoCe-Vö interface (Vö denotes oxygen vacancy) and the effect of hydrogen spillover from Cu species to CoCe-Vö interface. Furthermore, the experiments and theoretical calculations verified that CoCe-Vö interface could activate the C O bond. The optimized catalyst showed a DMF yield of > 90% at 180 °C and 1.5 MPa H 2 with no deactivation in the cycling tests. This study reveals the interfacial effects of the nanocatalysts, including the oxygen vacancies and hydrogen spillover, on hydrogenolysis of HMF, which provided a simple and efficient approach for synthesis of high-performance non-noble metal nanocatalysts applied to the hydrogenolysis of various biomass derivatives.
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SEPARATION AND PURIFICATION TECHNOLOGY
·
2021
·
IF 7.312
Fuzhen Liu,Xue Wang,Zhengzhi Liu,Fei Miao,Yin Xu,Hui Zhang
Zinc oxide supported on granular activated carbon (ZnO-GAC) was synthesized for the photocatalysis of Reactive Black 5 (RB5) with the presence of peroxymonosulfate (PMS). RB5 removal was improved with increasing temperature and dosage of PMS or catalyst, but declined with increasing pH and RB5 concentration. The reaction followed first-order kinetic model and the activation energy was determined to be 16.15 kJ mol −1 . After 60 min treatment, 43.6% of TOC was removed and further extending the reaction time to 90 min resulted in 51.9% TOC removal. The evolution profile of ammonium and nitrate ions was monitored during the treatment, and the organic degradation products of RB5 oxidation were identified by LC-MS analysis with a plausible degradation pathway being proposed. Quenching experiments indicated that electron hole (h + ) and reactive radicals (e.g. HO • /SO 4 •− ) were mainly responsible for RB5 removal in the UV/ZnO-GAC/PMS system. The catalyst reuse experiment shows that ZnO-GAC had no obvious deactivation after four cycles, which implied the reusability and stability of the prepared catalyst. Response surface methodology (RSM) with Box-Behnken design (BBD) was used to evaluate the effect of operating conditions, including PMS concentration, reaction temperature and initial pH on the removal rate of RB5. The result of adequacy check indicated the proposed RSM model was reliable and accurate to analyze the operating parameters of the UV/ZnO-GAC/PMS system.
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TALANTA
·
2021
·
IF 6.057
Qian Wang,Huanshun Yin,Jia Ding,Xi Fang,Yunlei Zhou,Shiyun Ai
The endogenous epigenetic marker 5-formylcytosine (5 fC) is introduced by 5-methylcytosine (5 mC) oxidation under action of enzyme oxidation, and plays an important role in many life activities. Since the content of 5 fC in mammalian tissues and cells is very low, it is necessary to exploit a sensitive and specific detection method to further understand the function of 5 fC. In this work, a sensitively and selectively photoelectrochemical (PEC) biosensor was developed for 5-formyl-2′-deoxycytidine (5fdC) detection. CuBi 2 O 4 /ZnPc@WS 2 was used as photoactive material, where the formed ternary heterojunction structure greatly enhanced the PEC response and increased the detection sensitivity. Positively charged polyethyleneimine (PEI) was employed as 5fdC recognition and capture unit, where the amine group on PEI specifically reacted with aldehyde group of 5fdC to form stable amide bond. 4-Carboxyphenylboronic acid (4-CPBA) was adopted as crosslinker for 5fdC and amino functionalized CuBi 2 O 4 based on the covalent interaction between 1,3-diol bond on 5fdC and boric acid structure on 4-CPBA, and the covalent interaction between –COOH on 4-CPBA and –NH 2 on amino functionalized CuBi 2 O 4 . On the basis of the positive synergistic effect of ZnPc and CuBi 2 O 4 on improving the photoelectric performance of WS 2 , the separation of photo-generated electron-hole pairs in semiconductors were promoted, and the examination range was expanded from 0.1 to 500 nM, and the detection limit was 0.0483 nM (3σ). Based on the unique covalent reaction between –NH 2 and –CHO, the PEC biosensor has excellent detection sensitivity, and can even separate 5fdC from 5-methylcytosine deoxyribonucleoside and 5-hydroxymethylcytosine deoxyribonucleoside. The effect of antibiotics and heavy metals on the 5fdC content in wheat tissue genome has also been further investigated using this sensor.
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JOURNAL OF CATALYSIS
·
2024
·
IF 6.5
Hongbing Wang,Yifei Yang,Shixiang Yu,Beibei Zhang,Junzhong Xie,Jun Chen,Dongping Wang,Bomin Feng,Changyin Zhong,Linsen Zhou,Wei Cui,Ding Ma,Yunxi Yao
Liquid-phase hydrogen isotopes exchange between hydrogen and water is a promising route for the hydrogen isotopes separation from water, catalyzed by the metal Pt with hydrophobic coating to surmount the flooding of reactive sites. However, poor water activation ability on Pt has limited the catalytic efficiency of Pt-based catalysts and hindered their application. Herein, we report a bifunctional Pt/ZSM-5 catalyst with hydrophobic modification by surface silylation for H 2 -HDO isotope catalytic exchange. The integration of metallic Pt and Brønsted acid (BA) sites in the microporous ZSM-5 boosts the catalytic efficiency of deuterium extraction by two orders of magnitude compared to commercial Pt-C at the optimum condition. In-situ spectroscopic and theoretical studies demonstrated that HDO-H 2 O preferentially adsorbs on BA sites (-Si-OH-Al) to form protonated water clusters stabilized by hydrogen-bonded network or to undergo the proton exchange to leave deuterium on zeolite framework as a new acidic site ([AlO 4 D]). Under the attractive interaction, the dissociated hydrogen on Pt clusters releases partial electrons to form positively-charged hydrogen, which further transfers to the [AlO 4 D] sites or protonated water clusters by interfacial spillover to produce the overcharging intermediates. These intermediates cleave their O-D bonds to form positively charged D, which ultimately spills back to Pt cluster and combines with the remaining electron to desorb in the form of HD. The synergistic effect between Pt and BA sites creates a new pathway of hydrogen transfer, which enables the more efficient hydrogen-water isotope exchange on the bifunctional Pt/ZSM-5 catalyst.
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FUEL
·
2022
·
IF 8.035
Puxiang Yan,Haiyong Wang,Yuhe Liao,Pengyao Sun,Chenguang Wang
Catalytic valorization of biomass into chemicals and fuels plays a key role in order to achieve net-zero greenhouse gas emissions. Herein, a series of hierarchical ZSM-5 zeolites were synthesized by the post-treatment method to transform furfural alcohol (FAL) to levulinic acid (LA). ZSM-5 obtained from tandem alkaline treatment (0.2 M NaOH) and acid washing (0.1 M HCl), denoted as ZSM-5-OH 0.2 -H, exhibited the highest activity, affording 76.2% LA yield in 9:1 acetone–water mixed solvents at 393 K for 0.5 h. The enhanced adsorption capacity and acid accessibility of FAL on zeolite mediated by the introduction of mesopores, as well as the reduced secondary reactions of the generated LA due to few Al atoms in straight and sinusoidal channels (as confirmed by UV–vis diffuse reflectance), were responsible for the outstanding catalytic performance of ZSM-5-OH 0.2 -H. The structure–activity relationship revealed that regulating the porous structure and Al distribution of ZSM-5 was an effective strategy to enhance its hydrolytic performance of FAL to LA. Moreover, ZSM-5-OH 0.2 -H could be reused for three reaction cycles without significant loss in catalytic activity.
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FLUID PHASE EQUILIBRIA
·
2019
·
IF 2.514
Yameng Wan,Haixia He,Pengshuai Zhang,Rui Zhao,Jiao Sha,Tao Li,Baozeng Ren
Mole-fraction solubility of 5-norbornene-2,3-dicarboximide (NODI) in eleven solvents including methanol (MtOH), ethanol (EtOH), 2-ethoxyethanol, methyl acetate (MAC), ethyl acetate (EAC), n-propyl acetate (NPAC), isopropyl acetate (IPAC), n-butyl acetate (NBAC), acetone (DMK), N,N-dimethylformamide (DMF) at (278.15–323.15) K and 1,4-dioxane at (288.15–323.15) K was experimentally measured by laser monitoring technique under 0.1 MPa. Solubility of NODI increased with the increasing temperature. Hansen Solubility Parameter was employed to explain the solubility behavior. The Kamlet-Taft parameters were calculated to investigate the solvent effect based on linear solvation energy relationships concept. Thermodynamic modeling including the Two-Suffix Margules model, Wilson model, NRTL model, NRTL-SAC model and UNIQUAC model were employed to correlate the experimental solubility. Wilson model and NRTL-SAC model were more suitable in correlation with solubility data. Furthermore, thermodynamic properties of mixing process (Δ mix G , Δ mix H , Δ mix S , ln γ 1 ∞ , H 1 E,∞ , ζ TS and ζ H ) were discussed based on Wilson equation.
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高影响因子
ChemCatChem
·
2015
·Vol. 7
·期 9
·1470-1477
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IF 4.556
Fenghua Xu,Zehui Zhang
Graphical Take baby steps: Polyaniline-grafted vanadyl acetylacetonate shows high catalytic activity for the oxidation of 5-hydroxymethylfurfural (HMF) under atmospheric oxygen pressure. A high HMF conversion of 99 % and a 2,5-diformylfuran (DFF) yield of 86 % are obtained after 12 h. More importantly, the synthesis of DFF directly from fructose is also realized with two binary catalysts: Amberlyst-15 and polyaniline–vanadyl acetylacetonate. Herein, polyaniline-grafted vanadyl acetylacetonate [VO(acac) 2 ] was prepared and used as an effective catalyst for the oxidation of 5-hydroxymethylfurfural (HMF) under atmospheric oxygen pressure. A high HMF conversion of 99.2 % was obtained after 12 h at 110 °C, and 2,5-diformylfuran (DFF) was obtained in 86.2 % yield. More importantly, the one-pot conversion of fructose into DFF was also realized with two binary catalysts: Amberlyst-15 and polyaniline–VO(acac) 2 . Amberlyst-15 was used for the acid-catalyzed dehydration of fructose into HMF, followed by the in situ oxidation of HMF catalyzed by polyaniline–VO(acac) 2 . DFF could be obtained in a yield of 42.1 % from fructose by using the one-pot reaction, whereas two consecutive steps gave a higher DFF yield of 71.1 %. Owing to the facile catalyst preparation and low cost, this method showed a promising potential for the synthesis of DFF from abundant carbohydrates.
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SCIENCE OF THE TOTAL ENVIRONMENT
·
2020
·
IF 6.551
Srinivasan Vinju Vasudevan,Xianghai Kong,Mengjie Cao,Mei Wang,Hanping Mao,Quan Bu
Tungstophosphoric acid (TPA) encapsulated dendritic fibrous silica KCC-1 was prepared via a microemulsion system with the simple reflux method using cetyltrimethylammonium bromide as a structure-directing agent. The TPA impregnated on KCC-1 (ITPA-KCC-1) was also prepared for comparative. Various physicochemical techniques were used to characterize the synthesized materials and their activity evaluated in the 5-hydroxymethylfurfural (HMF) formation from carbohydrates derivatives of fructose, glucose and cellulose . The effect of various factors such as catalyst to substrate ratio, different solvents and temperature were investigated on the formation of HMF. The resultant encapsulated catalyst was very active in fructose dehydration with the yield of 92% HMF and full conversion of fructose at 120 °C for 30 min under the microwave heating condition without any salt additive in the THF solvent system as well as 95% in MIBK solvent. The HMF yield was achieved by 58% and 16.2% from glucose and cellulose in the DMSO solvent, respectively. The TPA-KCC-1 can be separated easily after reaction from the reaction mixture and reused atleast five times without substantial loss in catalytic activity. This study provides an easy encapsulation method for TPA in dendritic fibrous silica KCC-1 as a heterogeneous catalyst , and it should have great application potential in other biomass valorization processes.
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Green Chemical Engineering
·
2023
·
IF 0
Jian Yang,Jia Zhang,Enrico Benassi,Xuemei Li,Hailong Liu,Weiguo Fang,Junying Tian,Chungu Xia,Zhiwei Huang
Al 2 O 3 -supported monometallic Ni, Co, and bimetallic Ni–Co nanocatalysts originated from layered double hydroxide precursors were synthesized by co-precipitation method, and used for the synthesis of useful 5-amino-1-pentanol (5-AP) and 1,5-pentanediol (1,5-PD) by reductive amination (RA) or direct hydrogenation of biofurfural-derived 2-hydroxytetrahydropyran (2-HTHP), respectively. In both reactions, the yield of the target products decreased monotonously with the increasing amounts of Co in the NiCo/Al 2 O 3 catalysts, owing probably to the replacement of highly reactive Ni by Co component with inferior hydrogenation activity at the low reaction temperature of 60 °C. However, the incorporation of Co could improve the reducibility of the NiCo/Al 2 O 3 bimetallic catalysts and promote the reaction stability of the catalysts, especially for Ni 2 Co 1 /Al 2 O 3 , in both reactions with over 180 h time-on-stream. Characterization of the catalysts before and after the reaction showed that the incorporating Co could inhibit the sintering of metal particles and hinder the surface oxidation of the more reactive Ni 0 species, thanks to the formation of Ni–Co alloy in the bimetallic catalysts. DFT-based modeling of the reaction mechanisms is also performed, supporting the reaction pathway proposed previously and also the much higher activity of Ni in the RA of 2-HTHP as compared with Co.
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JOURNAL OF THE ENERGY INSTITUTE
·
2019
·
IF 3.774
Xiaohua Li,Wenbin Dong,Jin Zhang,Shanshan Shao,Yixi Cai
The Fe-, Co-, Cu-loaded HZSM-5 zeolites were prepared via impregnation method. The upgrading by catalyst on biomass pyrolysis vapors was conducted over modified zeolites to investigate their catalytic upgrading performance and anti-coking performance. The Brønsted acid sites amount on Cu-,Co-loaded HZSM-5 decreased sharply, while that of Lewis both increased. The yield of liquid fraction and refined bio-oil over metal loaded ZSM-5 catalysts decreased, while that of char almost kept constant. The physical property of refined bio-oil was promoted in terms of pH value, dynamic viscosity and higher heating value (HHV). FT-IR analysis revealed that the chemical structure of refined bio-oil obtained over Fe-, Co-, Cu-loaded HZSM-5 zeolites was highly similar. The yield of monocyclic aromatic and aliphatic hydrocarbon over Fe-,Co-loaded HZSM-5 were boosted by around 2.5 times compared with original ZSM-5 zeolites. Data analysis revealed that Cu/HZSM-5 presented the worst deoxygenation ability. The anti-coking capability of Fe/HZSM-5 was obviously better, i.e., the coke content showed an approximate decrease of 38%. Thus, this study provided an efficient Fe/HZSM-5 catalysts for preparation of bio-oil derived from catalytic upgrading of biomass pyrolysis vapor.
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JOURNAL OF HAZARDOUS MATERIALS
·
2024
·
IF 12.2
Zuhao Chen,Yongyou Hu,Guanglei Qiu,Donghui Liang,Jianhua Cheng,Yuancai Chen,Xiaoqiang Zhu,Guobin Wang,Jieyun Xie
The effects of antibiotics, such as tetracycline, sulfamethoxazole, and ciprofloxacin, on functional microorganisms are of significant concern in wastewater treatment. This study observed that Acinetobacter indicus CZH-5 has a limited capacity to remove nitrogen and phosphorus using antibiotics (5 mg/L) as the sole carbon source. When sodium acetate was supplied (carbon/nitrogen ratio = 7), the average removal efficiencies of ammonia-N, total nitrogen, and orthophosphate-P increased to 52.46 %, 51.95 %, and 92.43 %, respectively. The average removal efficiencies of antibiotics were 84.85 % for tetracycline, 39.32 % for sulfamethoxazole, 18.85 % for ciprofloxacin, and 23.24 % for their mixtures. Increasing the carbon/nitrogen ratio to 20 further improved the average removal efficiencies to 72.61 % for total nitrogen and 97.62 % for orthophosphate-P (5 mg/L antibiotics). Additionally, the growth rate and pollutant removal by CZH-5 were unaffected by the presence of 0.1–1 mg/L antibiotics. Transcriptomic analysis revealed that the promoted translation of aceE , aarA , and gltA genes provided ATP and proton -motive forces. The nitrogen metabolism and polyphosphate genes were also affected. The expression of acetate kinase, dehydrogenase, flavin mononucleotide enzymes, and cytochrome P450 contributed to antibiotic degradation. Intermediate metabolites were investigated to determine the reaction pathways.
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JOURNAL OF INDUSTRIAL AND ENGINEERING CHEMISTRY
·
2019
·
IF 4.978
Huai Liu,Xuejuan Cao,Ting Wang,Junnan Wei,Xing Tang,Xianhai Zeng,Yong Sun,Tingzhou Lei,Shijie Liu,Lu Lin
The conversion of concentrated 5-hydroxymethylfurfural (HMF) or fructose to 2,5-furandicarboxylic acid (FDCA), a renewable alternative to petroleum-derived terephthalate acid, is highly desirable but challenging for FDCA production in an industrial scale. In this contribution, DMSO/H 2 O mixture was demonstrated as an effective medium for the production of FDCA from high concentration of HMF or fructose. For example, FDCA yield up to 93% was achieved at 10 wt% HMF concentration in DMSO/H 2 O over commercially available Ru/C (2 equiv. NaHCO 3 , 130 °C, 4 MPa O 2 and 12 h). Furthermore, an overall FDCA yield of 65% was achieved from concentrated fructose (19 wt%) through a facile two-step process. Notably, it is so far the highest HMF or fructose concentration employed for FDCA formation. As compared to pure water or DMSO , DMSO/H 2 O mixed system is able to stabilize HMF in an alkaline environment, which allows the efficient oxidation of HMF at high concentrations.
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危险品化学品经营许可证（带存储）