JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
·
2024
·
IF 2.8
Chenwei Liu,Ran Jing,Yue Li,Daolai Sun,Jianhua Lv
Background Succinic acid is a vital platform chemical derivable from lignocellulosic biomass. Various non-noble metal catalysts were used to hydrogenate succinic acid and produce 1,4-butanediol in this study. Among them, Co-loaded SiO 2 with a moderate mean pore size of 10 nm exhibited a superior catalytic performance. Results The high catalytic activity of Co-loaded SiO 2 , which was prepared by an impregnation method, was demonstrated in the hydrogenolysis of succinic acid to provide 1,4-butanediol. The Co/SiO 2 catalyst reduced at 400 °C and calcined at 300 °C existed in the form of Co 2+ and Co 0 , exhibiting a high catalytic activity. The production of 1,4-butanediol from succinic acid was significantly enhanced at a temperature of 200 °C and an H 2 pressure exceeding 5 MPa. At 200 °C and 7 MPa H 2 pressure, a 1,4-butanediol selectivity of 67.8% and a full succinic acid conversion were obtained over Co/SiO 2 . Conclusion The Co-loaded SiO 2 with a moderate mean pore size of 10 nm was conducive to the efficient generation of 1,4-butanediol from succinic acid. The Co/SiO 2 catalyst reduced at 400 °C existed in the form of Co 0 and Co 2+ . It was suggested that the efficient synthesis of 1,4-butanediol from succinic acid was facilitated by the cooperative action of Co 0 and Co 2+ . © 2024 Society of Chemical Industry (SCI).
研究领域:
化学工程
·
催化材料
✓ 已验证
产品关联
DOI
高影响因子
APPLIED CATALYSIS B-ENVIRONMENTAL
·
2023
·
IF 22.1
Xuan Liu,Jianying Wang,Zhongying Fang,Shuaiqi Gong,Dengke Xiong,Wei Chen,Deli Wu,Zuofeng Chen
Herein, an ultrafast electro-corrosion approach is developed for activating Ni foam (NF) into an efficient electrocatalyst for upcycling polybutylene terephthalate (PBT) waste plastic. The electro-corrosion process assisted by Cl − is completed by only 6 CV cycles (∼3 min) and the activity of the treated NF (T-NF), characterized by the integrated Ni 2+ /Ni 3+ peak area is enhanced by 150 times. The T-NF electrode exhibits excellent catalytic activity toward 1,4-butanediol oxidation , delivering a current density of 50 mA cm − 2 at 1.36 V (vs. RHE). This allows the electrocatalytic reforming of 1,4-butanediol component in PBT hydrolysate into succinate with a high Faraday efficiency 93%. The in-situ Raman and FTIR spectroscopies combining density functional theory calculations identify catalytically active centers, critical intermediates, and favorable pathway for 1,4-butanediol oxidation to succinate. This work provides an ultrafast one-step surface engineering strategy to turn pristine Ni foams into high-performance electrocatalysts for upcycling PBT plastic and other electrochemical applications.
研究领域:
材料科学
·
环境科学
·
化学工程
✓ 已验证
DOI
高影响因子
Catalysis Science & Technology
·
2024
·
IF 4.4
Kai Cui,Jiaming Yang,Yuli Jing,Junwen Chen,Chen Zhao,Peng Wu,Xiaohong Li
Sustainability issues have led to a gradual market expansion for the 1,4-butanediol (BDO) monomer of the biodegradable plastics to replace conventional plastics. Maleic anhydride (MA) can be derived from the oxidation of bio-based furfural or fructose. Although the hydrogenation of MA can produce a series of products, including succinic anhydride (SA), γ-butyrolactone (GBL), BDO and tetrahydrofuran (THF), the one-pot deep hydrogenation of MA to BDO or THF under mild conditions has been rarely reported in the literature until now. Herein, we report the production of BDO from the one-pot deep hydrogenation of MA over a Cu–0.03Mo/SiO2 catalyst, achieving 100% MA conversion and 88.3% BDO yield. The Cu–0.03Mo/SiO2 catalyst also showed good long-term stability without obvious loss in activity or BDO selectivity during a 160 h time-on-stream test. Doping Mo to Cu/SiO2 catalysts in an optimal amount adjusted the distribution of Cu0/Cu+ species and modulated the interaction of Cu–SiO2 and surface acidity, so that the activation of hydrogen, MA and relevant intermediates can become balanced, in addition to the restriction of side-reactions. This study provides potential for the green synthesis of BDO with non-precious Cu-based catalysts.
研究领域:
化学工程
·
可持续发展
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Wenlong Pang,Bin Li,Yufeng Wu,Qing Zeng,Jun Yang,Yu Zhang,Shaonan Tian
Biodegradable plastics such as Poly (butylene adipate-co-terephthalate) (PBAT) have been extensively utilized in numerous fields. However, post-consumption, PBAT tends to pollute the environment and waste resources. Herein, a novel approach employing a 1,4-butanediol-alkali combined method for the hydrolysis of PBAT is introduced. At 130 °C, with a reaction time of 60 min, the hydrolysis rate of PBAT exceeds 99 %. Subsequently, a two-step synthesis rapidly produces a foam nickel-supported NiOOH catalyst for the electrocatalytic reformation of the PBAT hydrolysate into higher-value chemicals (succinate salts) at an impressive current density of 100 mA cm −2 at 1.43 V (vs. RHE) and a Faradaic efficiency of 97.6 %. Experimental results and density functional theory calculations have elucidated the active state changes of the foam nickel-supported NiOOH catalyst and the intermediates in the oxidation of 1,4-butanediol to succinate, alongside the reaction mechanism. This study offers a viable approach for the degradation of PBAT plastic through a 1,4-butanediol-alkali method and the rapid preparation of a foam nickel-supported NiOOH electrocatalyst, achieving the upgraded recycling of post-consumer biodegradable PBAT plastic.
研究领域:
环境科学
·
材料科学
·
电化学
✓ 已验证
产品关联
DOI
高影响因子
Heliyon
·
2024
·
IF 3.4
Yuan Lv,Linrong Wu,Jiangyu Yan,Zhisen Shen,Junjun Zhang,Xiaoqin Zhang,Tian Li
Perforation of the tympanic membrane (TM) is a common condition that often requires a scaffold as a support for surgery. However, because of the external environment of the auditory canal, the scaffold could become bacterially infected and prevent the TM from healing. As a result, the perfect scaffold should have both antibacterial and biomimetic qualities. In this study, the biodegradable biomaterial poly(1,4-butylene carbonate) (PBC) films containing levofloxacin (LEV) was successfully prepared for the first time. The results showed that the hydrophilicity of the LEV/PBC film was improved after the addition of LEV, and the tensile strength was also complied with the requirements of the standard. The created antibacterial film demonstrated excellent antibacterial properties. In vitro hemolysis experiments revealed no risk of hemolysis for the new material, and the cytotoxicity study further confirmed its non-cytotoxic nature. Overall, LEV was a good component of PBC/LEV film, which is expected to be used for TM repair in the future.
研究领域:
生物材料学
·
耳科学
·
抗菌材料研究
✓ 已验证
产品关联
DOI
PubMed
高影响因子
CHEMICAL RESEARCH IN CHINESE UNIVERSITIES
·
2018
·Vol. 34
·期 4
·578-583
·
IF 1.248
Song Menglu,Yang Xiangui,Wang Gongying
Polycarbonate diols(PCDLs) with a number average molecular weight( M n ) of 2800 and a narrow polydispersity index(PDI=1.33) were synthesized from dimethyl carbonate(DMC) and 1,4-butanediol(BD) via a two-step process. The influences of the molar ratios of DMC to BD in the feedstock, polycondensation temperature and polycondensation time on the PCDLs preparation were studied. CH 3 COONa showed the best catalytic performance among the catalysts studied. The highest BD conversion of 73.8% and PCDLs yield of 64.7% were achieved under its optimum reaction conditions. Furthermore, based on the results of 1 H NMR, the relationships between the ratio of end groups (—OCH 3 /—OH) of oligomers, the M n and chainend constitute of resultant polycarbonates were also investigated. The results indicate that PCDLs can be synthesized when the oligomers mostly bear hydroxyl end groups. In contrast, it was impossible to prepare PCDLs when the oligomers were enriched with methyl carbonate end groups.
研究领域:
材料科学
·
化学工程
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2019
·
IF 6.97
Guochao Xu,Cheng Zhu,Aitao Li,Yan Ni,Ruizhi Han,Jieyu Zhou,Ye Ni
Cofactor regeneration using diols as “smart cosubstrates” is one of the most promising approaches, due to the thermodynamic preference and 0.5-equiv requirement. In order to establish an efficient NADPH regeneration system with 1,4-butanediol (1,4-BD), a NADP+-dependent alcohol dehydrogenase from Kluyveromyces polysporus (KpADH) was engineered to solve the kinetic imbalance. Several hotspots were identified through molecular dynamic simulation and subjected to saturation and combinatorial mutagenesis. Variant KpADHV84I/Y127M exhibited a lower KM of 15.1 mM and a higher kcat of 30.1 min–1 than WTKpADH. The oxidation of 1,4-BD to 4-hydroxybutanal was found to be the rate-limiting step, for which the kcat/KM value of double mutant KpADHV84I/Y127M was 2.00 min–1·mM–1, 11.6-fold higher than that of WTKpADH. KpADHV84I/Y127M preferred diols with a longer chain length (C5–C6). The ratio of kcat/KM toward 2-hydroxytetrahydrofuran (2-HTHF), in comparison to 1,4-BD, in KpADHV84I/Y127M was dramatically reduced by almost 100-fold compared to WTKpADH, which was advantageous for NADPH regeneration. As much as 100 mM phenylpyruvic acid could be reduced into d-phenylalanine with 99.2% conversion in 6 h using merely 0.5 equiv of 1,4-BD. Both the improved catalytic efficiency toward 1,4-BD and the balanced kcat/KM between 1,4-BD and 2-HTHF contributed to the higher NADPH regeneration efficiency. This study provides guidance for engineering alcohol dehydrogenases for cosubstrate specificity toward diols and its application in NADPH regeneration for the preparation of chiral compounds of pharmaceutical relevance.
研究领域:
生物化学
·
代谢工程
·
合成生物学
✓ 已验证
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2024
·
IF 13.3
Siying Chong,Shuang Zhao,Jiaoyan Li,Gangwei Huang,Yajing Zhang,Ruirui Liu,Kangjun Wang
Gas-phase dehydrocyclization of biomass-derived 1,4-butanediol (BDO) to γ-butyrolactone (GBL) is a sustainable and environmentally friendly process conducted at atmospheric pressure. In the present work, a series of 15Cu/xMgO-yCeO 2 catalysts with different MgO: CeO 2 ratios were prepared by the ammonia vaporization method. The gas-phase dehydrocyclization of BDO to GBL was carried out over these Cu-based catalysts synthesized in a fixed-bed reactor. The physicochemical properties of the catalysts were investigated by XRD, SEM, TEM, FTIR, N 2 isothermal adsorption–desorption, H 2 -TPR, CO 2 -TPD, Raman, XPS, and EPR. The results indicated that the 15Cu/10MgO-90CeO 2 catalyst exhibited a smaller particle size, higher specific surface area, and increased oxygen vacancies than the 15Cu/CeO 2 catalyst. Operating conditions of 240 °C reaction temperature, 2.4 mL/h space velocity, and 98.92 % GBL yield from BDO dehydrogenation were achieved under 40 mL/min N 2 flow for 4 h. Density functional theory (DFT) calculations confirmed that the 15Cu/10MgO-90CeO 2 catalyst with more oxygen vacancies was more favorable for the adsorption and activation of BDO on the catalyst surface than 15Cu/CeO 2 , and its higher catalytic activity was attributed to the synergistic interaction between Cu + and oxygen vacancies on the catalyst surface.
研究领域:
催化化学
·
材料科学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
BIOCATALYSIS AND BIOTRANSFORMATION
·
2018
·
IF 1.06
Lu Dai,Cui Tai,Yaling Shen,Yali Guo,Fei Tao
1,4-Butanediol (BDO) biosynthesis from renewable resources is of increasing interest because of global energy and environmental problems. We have previously demonstrated the production of BDO from erythritol by whole-cell catalysis. Here, the effects of several variables on BDO production were investigated, including cell density, temperature, substrate concentration and pH. It was found that the maximum BDO production was obtained at cell density (OD600) of 30. Low temperature and weak alkaline environment were beneficial for the biotransformation. Regarding substrate concentration, 80 g/L of erythritol was found to be optimum for the bioconversion. Under the optimal conditions, the highest concentration of BDO reached 34.5 mg/L, resulting in 5.8-fold increment after optimization. These results will provide useful guidance for enhancing the bioconversion of erythritol to BDO.
研究领域:
生物化学
·
工业微生物学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS LETTERS
·
2024
·
IF 2.3
Mei Mingjie,Zhao Jiangui,Fang Hu,Sun Zuowei,Xue Weichao,Fu Haiyan,Li Ruixiang,Chen Hua,Li Chen,Yang Chunji,Zheng Xueli,Yuan Maolin
1,4-Butanediol, an important chemical raw material, especially as the monomer of engineering plastic polyethylene terephthalate (PBT), plays a pivotal role in contemporary chemicals. A promising parallel approach is the linear-selective hydroformylation of inexpensive allyl acetate, which is economical yet challenging. Herein, we describe an atom-economic approach characterized by high selectivity for synthesizing 4-oxobutyl acetate through rhodium-catalyzed hydroformylation using allyl acetate. This protocol affords the intermediate of valuable 1,4-butanediol in excellent yield (up to 95%) and exhibits excellent regioselectivity (linear/branched up to 164) under mild conditions (60 °C, 10 bar of syngas), effectively minimizing the formation of decomposed byproducts. The success of this protocol hinges on the use of a "Rh/POP-type ligand" in combination with either acetic acid or bulky anionic salts as additives. Preliminary mechanism studies show that the use of CH 3 COOH facilitates the formation of a tridentate κ 3 -P,O,P-coordination, which prevents the coordination of carbonyl with the Rh center, leading to the relatively high linear selectivity of 4-oxobutyl acetate. Furthermore, the successful application of this protocol in synthesizing 4-oxobutyl acetate at a scale of 3.8 g, employing low Rh-loading (0.05 mol%), highlights its potential for industrial applications. Graphical Abstract
研究领域:
化学工程
·
催化化学
✓ 已验证
DOI
高影响因子
VACUUM
·
2024
·
IF 3.8
Kaile Shi,Haodong Zheng,Yuze Sun,Honghai Wang,Jing Fang,Chunli Li,Jiapeng Liu
The utilization of 1,4-butanediol (BDO) spans across numerous sectors, underscoring its significance as a pivotal chemical. However, the separation of crude BDO still presents great challenges. Ethylene glycol (EG) and 3-methyl-1,5-pentanediol (MPD) are classical impurities in BDO crude products. In this paper, the pressure and temperature data of MPD components under high vacuum pressure were measured, and Antoine constant was obtained by fitting to supplement the basic data. The isobaric vapor-liquid equilibrium (VLE) data for the EG-BDO and BDO-MPD mixtures were experimentally measured at pressures of 1.0, 10.0, and 50.0 kPa. Meanwhile, the thermodynamic consistency of the experimental binary data was examined using the Herington area test. The experimental VLE data for binary systems were analyzed using the nonrandom two-liquid (NRTL) universal quasichemical (UNIQUAC) and Wilson activity coefficient models, demonstrating that the predicted outcomes showed excellent agreement with the measured data. Finally, the interaction energy between the components was calculated by molecular simulation to explain the gas-liquid equilibrium behavior. Therefore, this work provided guidance and basis for the separation of EG-BDO and BDO-MPD in high vacuum separation.
研究领域:
化学工程
·
物理化学
✓ 已验证
产品关联
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
·
2024
·
IF 8.1
Zicheng Du,Baojie Liu,Xiaoying Liu,Lu Liu,Chen Liang,Shuangquan Yao,Chengrong Qin
Separating low condensed lignin from lignocellulosic biomass is of great importance for achieving its full component conversion. This study proposed a new efficient and environmentally friendly alcohol/acid pretreatment system using 1,4-butanediol (1,4-BDO) as a solvent, combined with p -toluene sulfonic acid ( p -TsOH) to efficiently separate low condensed lignin. The results showed that the system could remove 85.55 % of hemicellulose and 84.78 % of lignin in a short time, with a high retention rate of cellulose. Based on the phenomenon of 1,4-BDO molecule protecting lignin structure, the recovered low-condensed lignin structure contains the main aliphatic hydroxyl structure, and the remaining solid surface lignin condensation grains were fewer, and the fiber crystallinity was high, which was beneficial for the preparation of high-value products. In addition, the lignin dissolution kinetics revealed that the p -TsOH/1,4-BDO pretreatment had a lower reaction activation energy, clarifying the solvation effect of 1,4-BDO on efficient lignin dissolution. Finally, combining density functional theory (DFT) from the molecular level clarified that the hydrogen bonding and conjugated effect between 1,4-BDO and lignin structure could effectively reduce the self-condensation reaction of lignin molecules. This study achieved effective separation of lignocellulosic biomass, providing a theoretical basis for the application of 1,4-BDO in biomass component separation, and promoting the development of green and efficient component separation technologies.
研究领域:
生物质化学
·
可再生资源工程
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）