GREEN CHEMISTRY
·
2020
·Vol. 23
·期 1
·552-560
·
IF 9.48
Peixuan Wu,Haiyang Cheng,Xinchao Wang,Ruhui Shi,Chao Zhang,Masahiko Arai,Fengyu Zhao
The fabrication of self-healing and recyclable CO2-based polymeric materials meets the requirement of sustainable development. By introducing reversible hydrogen bonds and heat-responsive Diels–Alder bonds, a new, environmentally friendly, self-healing and recyclable polyurethane-urea Diels–Alder adduct (PUUa-DA) was successfully synthesized using CO2 and furfuryl amine as renewable feedstocks. PUUa-DA was semi-crystalline and exhibited high thermal stability, 5% weight loss temperature being above 220 °C. Moreover, PUUa-DA with a cross-linked structure showed a tensile stress of 18.5 MPa, a modulus of 151 MPa and an elongation at break of 136%. The dynamic Diels–Alder bonds and hydrogen bonds provide the self-healing response and contribute to 94% recovery of the tensile strength upon heating. Therefore, PUUa-DA will have potential applications as a functional material in a wide range of practical fields. The synthesis of PUUa-DA using CO2 and bio-based furfuryl amine will be of importance in green and sustainable chemistry.
研究领域:
材料科学
·
绿色化学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2018
·
IF 0
Yongdi Xie,Yi Huang,Chunyan Wu,Wenwen Yuan,Yongmei Xia,Xiang Liu,Haijun Wang
A series of porphyrin type catalysts with the metal active sites of Fe were prepared and investigated in aerobic oxidation of biomass-based furfural to maleic acid (MAD) in aqueous phase. The catalytic performance of meso -tetrakis(4-bromophenyl)porphyrin iron (III) chloride (FeT( p -Br)PPCl) immobilized on different supports was evaluated. It was interesting to find that the catalytic activity varied with the supports and followed the trend: FeT( p -Br)PPCl/SBA–15 > FeT( p -Br)PPCl/meso-ZSM–5 > FeT( p -Br)PPCl/MCM-41. The effect of reaction conditions were discussed in detail over FeT( p -Br)PPCl/SBA-15 catalyst, and 56.1% yield and 73.8% selectivity of MAD were obtained from renewable furfural under the optimal conditions. Moreover, the FeT( p -Br)PPCl/SBA-15 catalyst could be reused five times without a significant decrease of activity in recycling examinations.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
RSC Advances
·
2019
·Vol. 9
·期 19
·10569-10577
·
IF 3.049
Jianru Ma,Wenzhi Li,Shengnan Guan,Qiying Liu,Qingqing Li,Chaofeng Zhu,Tao Yang,Ajibola Temitope Ogunbiyi,Longlong Ma
Sulfonated graphene (SG) was prepared and employed to convert corn stalk and xylose into furfural. Transmission electron microscopy (TEM), scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS) and Fourier transform infrared spectroscopy (FT-IR) were used to characterize SG. The effects of reaction time, temperature, substrate loading, catalyst dosage and solvents on the reaction were researched and optimized. SG exhibited high catalytic activity in the conversion of xylose and corn stalk to furfural. A fairly high furfural yield of 96% was achieved at 150 °C from xylose and a 71.9% furfural yield was obtained when using a 10.7 ratio (mass ratio: xylose to SG) at 140 °C. While a 48% furfural yield was obtained from corn stalk (based on the starting combined moles of xylan and glucan in corn stalk; yield was >100%, if based on only xylan) using a substrate loading (corn stalk to catalyst mass ratio) of 2.14 and a 19% 5-hydroxymethylfurfural (5-HMF) yield was obtained. What's more, a 43.9% yield of furfural was obtained in only 20 min. In addition, the reusability of SG was also investigated and shown to have good stability for xylose dehydration.
研究领域:
生物化学
·
材料科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2017
·
IF 2.843
Chuang Li,Guangyue Xu,Xiaohao Liu,Ying Zhang,Yao Fu
Tetrahydrofurfuryl alcohol (THFAL), as a green industrial solvent, can be obtained directly from biomass-derived furfural with 100% conversion and 100% yield over a hydroxyapatite-supported Pd catalyst (Pd-HAP) under relatively mild conditions (40 °C, 1 MPa H2, and 3 h) in 2-propanol. At room temperature and reacting for 8 h, the yield of THFAL was more than 99%. By capturing the intermediates, two pathways were proposed as follows: (1) Furfural was partially hydrogenated to furfuryl alcohol, and then, furfuryl alcohol was further hydrogenated to THFAL. (2) Furfural and 2-propanol first formed 2-(isopropoxymethyl)furan (2-IPMF) via etherification, and then, 2-IPMF was ultimately converted to THFAL. The Pd-HAP catalyst was characterized by various techniques including XRD, SEM, TEM, HAADF-STEM, XPS, and ICP-AAS. The results revealed that the outstanding catalytic performance of Pd-HAP was attributed to the quasicoordination effect between Pd and HAP, which not only contributed to highly dispersed and stable Pd nanoclusters but also led to better activation of hydrogen. The recyclability of the Pd-HAP catalyst was also investigated and proved its stability in the conversion of furfural and high selectivity toward THFAL.
研究领域:
生物化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2022
·
IF 8.047
Chuncheng Lin,Jiamin Zhou,Zhangfan Zheng,Jinzhu Chen
Tertiary amines, currently obtained from fossil resources by a multi-step synthetic method, are important compounds in both chemical industry and organic transformations. Herein, we demonstrated highly efficient and convenient strategy to various biomass-based tertiary amines in excellent yields (85–95%) by a direct and consecutive reductive amination of furfural with various amines in one-pot using rhodium phosphide (Rh 2 P) catalyst. Typically, biomass-based tris (2-furanylmethyl)amine in 92% yield was directly obtained from furfural and HCOONH 4 in one-step. Time-dependent reaction profiles suggested a consecutive amination/hydrogenation pathway with furfurylamine-derived Schiff base and secondary amine as successively detected intermediates. The superiority of Rh 2 P was ascribed to its excellent low-temperature hydrogenation activity, which is structurally attributed to an efficient electron-transfer from P atoms (on the P-terminated Rh 2 P) to their bonded and dissociated H atoms. This research thus highlights a powerful, elegant, and attractive approach to biomass-based tertiary amines for a sustainable extension of amine chemistry.
研究领域:
有机化学
·
可再生资源化学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
Biomass Conversion and Biorefinery
·
2021
·Vol. 13
·期 9
·8115-8121
·
IF 4.987
Ren Dezhang,Jiang Xuelei,Zhang Nahui,Duo Jia,Norinaga Koyo,Huo Zhibao
Production of pyridine derivatives from bio-based feedstocks instead of fossil fuels is a promising strategy. The development of effective heterogeneous catalysts and mild reaction systems for pyridinization of renewable biomass derivatives remains a huge challenge. In this article, a direct and environment-friendly method was reported to produce 3-hydroxypyridine from bio-based furfural in water over a Raney Fe catalyst. Raney Fe exhibited an efficient catalytic performance for activation of the aldehyde group of furfural and afforded an 18.2% yield of 3-hydroxypyridine at 120 °C with ammonia as N source. The polymerization of furfural on the catalyst in hot water was the main cause of deactivation, which was verified by the scanning electron microscope (SEM), X-ray diffraction (XRD), and N 2 adsorption and desorption analysis. A possible mechanism for this reaction was also proposed. This study provides a new way for academia and industry to realize the synthesis of nitrogen-containing chemicals from biomass and its derivatives.
研究领域:
催化化学
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绿色化学
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可再生资源转化
✓ 已验证
产品关联
DOI
高影响因子
APPLIED SURFACE SCIENCE
·
2022
·
IF 7.392
Zhengliang Zhang,Zhiwei Zhang,Xubin Zhang,Fumin Wang,Zheng Wang,Yongwang Li,Xingtao Wang,Rosine Ahishakiye,Xu Zhang
Exploring low-cost green catalysts to achieve green organic chemicals and fuels from biomass is one of the crucial ways to solve the energy crisis. The 20 wt% Co-CoO x /AC catalysts were prepared to achieve the one-pot conversion of furfural to 2-methylfuran under milder reaction conditions (120 °C, 2.5 MPa H 2 ), shorter reaction time (5 h) and less catalyst dosage by regulating the ratio of metal to oxide species. The yield of 2-methylfuran reached 87.4 % is achieved under 20 wt% Co-CoO x /AC catalyst conditions, and there was no significant degradation of all catalyst properties after five cycles. Characterization results showed that the active components in the catalyst were present as Co 0 species with CoO x species. The reaction mechanism was explained by combining the characterization results, experimental data and DFT calculations. The formyl group of the furfural side chain is first adsorbed on the Co 0 species, and furfuryl alcohol is produced in the presence of the Co 0 species. Subsequently, the CoO x species adsorbs the C O bond on the side chain, which is broken in the presence of the CoO x species to form 2-methylfuran. The excellent catalytic activity of the 20 wt% Co-CoO x /AC catalyst provide a promising application for preparing 2-methylfuran by hydrodeoxygenation of furfural.
研究领域:
化学工程
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催化科学
·
生物质转化
✓ 已验证
产品关联
DOI
高影响因子
Reaction Chemistry & Engineering
·
2022
·Vol. 8
·期 2
·377-388
·
IF 5.2
Tiefu Li,Jiaming Liu,Zipeng Li,Peng Zhang,Yunlong Yao,Zhichao Sun,Yao Wang,Ying-Ya Liu,Anjie Wang
A monolith reactor was fabricated by growing carbonaceous fibers in a copper tube (i.d. 2 mm) via copper-catalyzed acetylene polymerization. The fibers were oxidized with air to convert CC bonds to CO bonds and to improve hydrophilicity. –SO3H groups were anchored on the surface by amination. Cu species were introduced by deposition and subsequent reduction. The resultant Cu/CF-SO3H monolith reactor was used to continuously and selectively convert furfural to furfuryl alcohol. At 180 °C, the monolith catalytic reactor performed significantly and stably in a 500 h run, maintaining a 100% conversion with a >99% selectivity. Additionally, the monolith reactor also performed well in continuous transfer hydrogenation of other α,β-unsaturated compounds, including 5-hydroxymethyl-2-furaldehyde, benzaldehyde, and cyclohexanone.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
ACS Sustainable Chemistry & Engineering
·
2023
·
IF 8.4
Kun Yuan,Wen Zhao,Yaohong Zhou,Xiaohua Zhang,Shangxing Chen,Jing Chen,Changxiang Liu,Wanming Xiong
A novel strategy for preparing 1,13-tridecanediol by valorization of furfural was proposed, involving aldol condensation to build C13 intermediates and further hydrodeoxygenation. During this process, Raney Ni exhibited excellent catalytic performance for the initial hydrogenation (C═C and C═O) with a yield of 98.30%, while Pd/TiO2–ZrO2 showed promising de–OH and ring opening performance. Results showed that ZrO2 was necessary for de–OH and ring opening, and the catalytic performance could be improved by incorporating with TiO2 to form TiO2–ZrO2 due to the increase in weak acid sites. Also, the introduction of Pd could further promote the reaction oriented toward obtaining 1,13-tridecanediol. After optimization, 1,13-tridecanediol yield could be straightforwardly up to 57.93% in water, and it would improve to 76.51% (69.64% based on furfural) by introducing trace amounts of methanol, and even the reaction parameters (time, pressure, temperature, etc.) contributed to the distribution of products. Additionally, mechanistic investigation revealed that there were multiple simultaneous or sequential reaction steps in the hydrodeoxygenation reaction, and the superior catalytic performance of Pd/TiO2–ZrO2 for oriented upgrading of furfural into 1,13-tridecanediol could be attributed to the synergistic effect of TiO2–ZrO2 and Pd. Overall, this work may provide some insights for the utilization of biomass resources in the future.
研究领域:
化学工程
·
可再生资源利用
✓ 已验证
产品关联
DOI
高影响因子
JOURNAL OF CATALYSIS
·
2023
·
IF 7.3
Yujie Wan,Pengfei Ma,Hongliang Lu,Jianping Zhang,Jie Wang,Weiping Fang,Wenjing Song,Quanxing Zheng,Weikun Lai
Hydrogen spillover had played a significant role in catalytic processes involving reducible oxide supported metal catalyst and hydrogen molecule. Herein, crystal plane regulative hydrogen spillover strategy for the effective reductive amination on Ni/Al 2 O 3 was developed. A rod-like alumina supported Ni catalyst with primarily external (1 1 1) facets was prepared. In the presence of NH 3 and H 2 , Ni/Al 2 O 3 (1 1 1) exhibited a turnover number of 30.4 h −1 , which was 136-fold higher than that of Ni/Al 2 O 3 (1 1 0) in the reductive amination of furfural to furfuryl amine. For the Ni/Al 2 O 3 (1 1 1) catalyst, Al 2 O 3 (1 1 1) facets exhibited strong Lewis acidity, resulting in an enhanced H affinity of Al 2 O 3 (1 1 1) and a positively charged of Ni through electronic interaction. It was revealed that strong H affinity of Al 2 O 3 (1 1 1) and positively charged Ni sites significantly promoted hydrogen migration from Ni surface to Al 2 O 3 (1 1 1) facets, which effectively prevented the Ni sites from hydrogen poisoning and enhanced the adsorption and activation of NH 3 and intermediates for reductive amination. Consequently, the activation energy of Schiff base reductive ammonolysis was obviously reduced, resulting in high inherent activity for furfural reductive amination to furfuryl amine. This work developed a new strategy for high efficiency reductive amination catalyst in terms of hydrogen spillover effect.
研究领域:
催化化学
·
材料科学
·
能源化学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING SCIENCE
·
2020
·
IF 3.871
Danni Li,Jun Zhang,Ying Liu,Haoran Yuan,Yong Chen
A series of boron doped magnetic zirconium catalysts were developed for the selective transfer hydrogenation of biomass-derived furfural (FFR) into furfuryl alcohol (FA) using 2-propanol as hydrogen source and solvent. Full characterizations with XRD, SEM, TG, Py-IR, NH 3 -TPD, and CO 2 -TPD techniques were undertaken to uncover structural properties of magnetic catalysts. Boron doped magnetic zirconium catalysts endowing with adjustable acid-base sites exhibited excellent performance as well as good regenerability in the transfer hydrogenation of FFR, where almost 100% FA yield was achieved in the presence of 2-propanol and the catalyst still sustained good activity after being used five times. Suitable acidity/basicity ratio of 3.8 ~ 4.0 apparently benefited the selective production of FA. Gratifyingly, the activation energy for FA formation over Zr 1 B 3 FeO was as low as 48.3 kJ/mol. In addition, plausible reaction mechanism involving two H-transfer paths for transfer hydrogenation of FFR into FA under the catalysis of active Zr/B species was proposed.
研究领域:
催化化学
·
生物质能
·
材料科学
✓ 已验证
DOI
高影响因子
CHINESE JOURNAL OF CATALYSIS
·
2021
·
IF 8.271
Shujing Zhang,Hong Ma,Yuxia Sun,Xin Liu,Meiyun Zhang,Yang Luo,Jin Gao,Jie Xu
Tandem catalysis for the hydrogenation rearrangement of furfural (FA) provides an attractive solution for manufacturing cyclopentanone (CPO) from renewable biomass resources. The CuNi/Al-MCM-41 catalyst was synthesized and afforded excellent catalytic performance with 99.0% conversion and 97.7% selectivity to CPO in a near-neutral solution under 2.0 MPa H 2 at 160 °C for 5 h, much higher than those on other molecular sieve supports including MCM-41, SBA-15, HY, and ZSM-5. A small amount of Al highly dispersed in MCM-41 plays an anchoring role and ensures the formation of highly dispersed CuNi bimetallic nanoparticles (NPs). The remarkably improved catalytic performance may be attributed to the bimetallic synergistic and charge transfer effects. In addition, the initial FA concentration and the aqueous system pH required precise control to minimize polymerization and achieve high selectivity of CPO. Fourier transform infrared spectroscopy and mass spectra results indicated that polymerization was sensitive to pH values. Under acidic conditions, FA and intermediate furfuryl alcohol polymerize, while the intermediate 4-hydroxy-2-cyclopentenone mainly polymerizes under alkaline conditions, blocking the cascade of multiple reactions. Therefore, near-neutral conditions are most suitable for minimizing the impact of polymerization. This study provides a useful solution for the current universal problems of polymerization side reactions and low carbon balance for biomass conversion .
研究领域:
催化化学
·
生物质转化
·
材料科学
✓ 已验证
DOI
高影响因子
危险品化学品经营许可证（带存储）