CATALYSIS LETTERS
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2024
·
IF 2.3
Liang Yongjia,Zuo Jianliang,Cai Zhaohao,Lin Jing,Liu Zili
The direct conversion of furfural (FA) from biomass to pentanediols (PeDs), including 1,2-PeD and 1,5-PeD, is important for replacing fossil resources and developing bio-based polyesters from renewable sources. However, achieving high selectivity for the C–O hydrogenation of the furan ring remains a significant challenge. In this study, we synthesized a series of trimetallic CuCoLa catalysts, using a coprecipitation method with various metal ratios. The reduced CuCoLa catalyst with a metal ratio of 1/3/1, exhibited the highest activity for the selective hydrogenolysis of FA to PeDs. Under optimal reaction conditions (160 °C, 4 MPa H 2 for 9 h), CuCoLa(1/3/1)-R achieved yields of 21.7% for 1,2-PeD and 50.1% for 1,5-PeD. Furthermore, the catalyst remained stable after five cycles of FA conversion to PeDs. The high selectivity for PeDs is attributed to the synergistic interaction between Cu and Co and the appropriate number of basic surface sites. Graphical Abstract
研究领域:
催化化学
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可再生资源化学
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生物质转化
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DOI
高影响因子
Catalysts
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2024
·Vol. 14
·期 4
·223
·
IF 3.8
Yuhao Yang,Qiaoyun Liu,Zhongyi Liu
The catalytic conversion of naturally rich and renewable biomass into high-value chemicals is of great significance for pursuing a sustainable future and a green economy. The preparation of pentanediol from furfuryl alcohol is an important means of high-value conversion of biomass. The Pt-based catalyst supported on MgO was applied to the selective hydrogenation of biomass furfuryl alcohol to prepare pentanediol. By adjusting parameters such as catalyst loading, reduction temperature, reaction temperature, and pressure, a highly active catalyst was designed and the optimal catalytic hydrogenation conditions were determined. The hydrogenation experiment results showed that the selectivity of the 2Pt/MgO-200 catalyst for 1,2-pentanediol and 1,5-pentanediol reached 59.4% and 15.2%, respectively, under 160 °C and 1 MPa hydrogen pressure. The catalyst was characterized by X-ray powder diffraction (XRD), transmission electron microscopy (TEM), X-ray photoelectron spectrometer (XPS), CO2-temperature programmed desorption (CO2-TPD), and other methods. The characterization results indicate that the reduction temperature has a significant impact on the metal Pt, and an appropriate reduction temperature is beneficial for the hydrogenation performance of the catalyst. In addition, the basic sites on the carrier are also another important factor affecting the activity of the catalyst. In addition, stability tests were conducted on the catalyst, and the reasons for catalyst deactivation were studied using methods such as thermogravimetric analysis (TGA) and Fourier transform infrared spectroscopy (FT-IR). The results showed that the activity of the catalyst decreased after five cycles, and the deactivation was due to the hydrolysis of the carrier, the increase in metal particle size, and the surface adsorption of organic matter.
研究领域:
生物质化学
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催化科学
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材料科学
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DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
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2024
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IF 13.3
Ye Tian,Wenlong Xie,Zihao Yang,Zhendong Yu,Renjie Huang,Lin Luo,Miao Zuo,Zheng Li,Lu Lin,Xianhai Zeng
Selective ring-opening hydrogenolysis of furfural (FF) to 1,5 pentanediol (1,5-PeD) is crucial for biomass valorization. However, achieving accurate bond-breaking is challenging. Herein, we report a facile method to synthesize layered double hydroxide nanoflake (ZnCo-LDH) mediated via Co 2+ etching ZIF-8 with NaBH 4 in water at ambient temperature. The structure, morphology, and chemical properties of synthesis catalysts with different concentrations of Co 2+ were characterized. The results indicated a partial ZIF-8 structure in ZnCo-LDH, with increased Co 2+ concentrations leading to catalyst agglomeration. Furthermore, the constitutive relationships between the catalyst’s properties and 1.5-PeD yields were established. Moreover, Co introduction altered the catalyst surface’s Brønsted and Lewis acids content. Density functional theory (DFT) indicated enhanced H 2 adsorption and dissociation due to electro-transfer between Co and Zn species, with a tilted configuration favoring ring opening. Finally, a possible reaction mechanism was proposed. This work provides valuable insights for preparing ultrathin nanoflake ZnCo-LDH catalysts for biomass-derived furfur compound upgrading.
研究领域:
化学工程
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催化科学
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DOI
高影响因子
GREEN CHEMISTRY
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2016
·Vol. 18
·期 12
·3607-3613
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IF 8.506
Guangyi Li,Ning Li,Mingyuan Zheng,Shanshan Li,Aiqin Wang,Yu Cong,Xiaodong Wang,Tao Zhang
A new route for the selective synthesis of renewable 1,3-cyclopentanediol was developed by the aqueous phase rearrangement of furfuryl alcohol to 4-hydroxycyclopent-2-enone followed by hydrogenation. The presence of a small amount of base catalysts is beneficial for the aqueous phase rearrangement of furfuryl alcohol to 4-hydroxycyclopent-2-enone. Such a promotion effect of base catalysts can be rationalized by restraining the generation of levulinic acid which may catalyze the polymerization of furfuryl alcohol. In the hydrogenation of 4-hydroxycyclopent-2-enone to 1,3-cyclopentanediol, an evident solvent effect was noticed. Higher carbon yields of 1,3-cyclopentanediol were obtained when tetrahydrofuran was used as the solvent. In the large scale tests with high initial concentrations of feedstocks, a high overall carbon yield (72.0%) of 1,3-cyclopentanediol was achieved over cheap catalysts (MgAl-HT and RANEY® Ni). As a potential application, 1,3-cyclopentanediol as obtained was successfully used as a monomer in the synthesis of polyurethane.
研究领域:
化学工程
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可再生资源
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工业催化
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DOI
高影响因子
ACS Nano
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2022
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IF 18.027
Jiawei Wang,Yan Yang,Yingyu Wang,Shuai Dong,Liwei Cheng,Yanmei Li,Zhenya Wang,Levent Trabzon,Hua Wang
Reliable power supplies at extremely high temperatures are urgently needed to broaden the application scenarios for electric devices. Aqueous zinc metal batteries (ZMBs) with intrinsic safety are a promising alterative for high-temperature energy storage. However, the reversibility and long-term cycling stability of aqueous ZMBs at extremely high temperatures (≥100 °C) have rarely been explored. Herein, we reveal that spontaneous Zn corrosion and severe electrochemical hydrogen evolution at high temperature are vital restrictions for traditional aqueous ZMBs. To address this, a crowding agent, 1,5-pentanediol, was introduced into an aqueous electrolyte to suppress water reactivity by strengthening O–H bonds of H2O and decreasing H2O content in the Zn2+ solvation sheath, while maintaining flame resistance of the electrolyte. Importantly, this electrolyte enabled reversible Zn deposition with a Coulombic efficiency of 98.1% and a long cycling life of Zn//Zn batteries for over 500 cycles (at 1 mA cm–2 and 0.5 mAh cm–2) at 100 °C. Moreover, stable cycling of Zn//Te full batteries at 100 °C was demonstrated.
研究领域:
材料科学
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电化学
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DOI
PubMed
高影响因子
JOURNAL OF CHEMICAL TECHNOLOGY AND BIOTECHNOLOGY
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2024
·Vol. 99
·期 4
·922-930
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IF 2.8
Dingshuo Zhang,Heqian Zhang,Yue Li,Daolai Sun,Jianhua Lv
BACKGROUND Levulinic acid is an important platform chemical derivable from lignocellulosic biomass. In this work, the hydrogenolysis of levulinic acid to produce 1,4-pentanediol was performed over some Co-based non-noble catalysts. The relationship between the catalyst properties and the catalytic activity was investigated, and the effects of the reaction conditions on the catalytic activity were studied. RESULTS The Co/ZrO 2 catalyst prepared by a coprecipitation method showed a high catalytic performance in the hydrogenolysis of levulinic acid to form 1,4-pentanediol. The calcination of Co/ZrO 2 significantly affected the catalytic activity, and a high calcination temperature of 750 °C could promote the formation of 1,4-pentanediol. Meanwhile, the reduction of Co/ZrO 2 at 400 °C in an H 2 flow was beneficial for producing 1,4-pentanediol, and the Co species after the reduction existed as the forms of Co 2+ and Co 0 . A high H 2 pressure and a moderate reaction temperature of 200 °C were beneficial for producing 1,4-pentanediol, and a high 1,4-pentanediol selectivity of 85.6% with a complete conversion of levulinic acid was obtained over the Co/ZrO 2 catalyst at 200 °C under an H 2 pressure of 7 MPa. CONCLUSION The Co species in the 400 °C-reduced Co/ZrO 2 catalyst existed as the forms of Co 2+ and Co 0 . It was proposed that the synergistic effect of Co 2+ and Co 0 contributed to the effective formation of 1,4-pentanediol from levulinic acid. © 2024 Society of Chemical Industry (SCI).
研究领域:
化学工程
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可再生能源
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DOI
高影响因子
Catalysis Science & Technology
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2022
·Vol. 12
·期 19
·5879-5890
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IF 6.177
Dengfeng Dai,Chao Feng,Minmin Wang,Qingzhou Du,Dandan Liu,Yuan Pan,Yunqi Liu
Biomass-based chemicals as a renewable alternative to petroleum-based chemicals are of great significance. The conversion of biomass-based furfuryl alcohol to pentanediol, including 1,5-pentanediol and 1,2-pentanediol, is explored over a series of bifunctional Cu/MFI catalysts in a continuous-flow reactor. These catalysts are synthesized by supporting copper nanoparticles on MFI zeolites with varying molar ratios of SiO2/Al2O3. Among them, the Z60-10Cu catalyst containing balanced Cu0–Cu+ and Brønsted acid sites exhibits excellent performance, and a high furfuryl alcohol conversion of 99.5% and selectivity of 85.2% for 1,5-pentanediol (69.2%) and 1,2-pentanediol (16.0%) could be achieved (hydrogen pressure: 2.5 MPa) at 160 °C. The experimental results and the results obtained using the DFT technique revealed that the high catalytic activity realized during the processes of ring-opening and hydrogenation could be attributed to the synergistic effect between the Cu species and Brønsted acid sites. The Brønsted acid sites on the Si(OH)Al groups significantly affect the ring-opening process of furfuryl alcohol. The methoxy group on furfuryl alcohol adsorbs on the Cu+ sites, and the hydrogenation saturation of the ring-opening intermediate is realized under the influence of the activated hydrogen units on the Cu0 sites. The results reported herein could help promote the continuous production of high value-added pentanediol from biomass-based raw materials in the presence of non-noble metal catalysts. An economical and feasible path for the transformation of biomass resources into high value-added fine chemicals could also be developed.
研究领域:
生物化学
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催化化学
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材料科学
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DOI
高影响因子
ChemSusChem
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2024
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IF 7.5
Shenyu Wang,Junjie Zhang,Ying Zhang
Graphical The CoO@Co core-shell catalyst, 7Co-0.2Fe/CeO 2 , efficiently catalyzes the hydrogenation and ring-opening of furfural to 1,5-pentanediol, with a high productivity of 54.76 mmol/g Co /h, representing the top activity level among the reported catalysts. The addition of Fe optimizes the Co 2+ /Co 0 ratio, improves substrate adsorption, and prevents the formation of tetrahydrofurfuryl alcohol, a saturated furan byproduct. In the conversion of furfural using non-noble metal catalysts, preferential cleavage of the C2−O bond followed by hydrogenation of the C=C bond facilitates selective access to valuable 1,5-pentanediol (1,5-PeD). Herein, we developed CeO₂ loaded core-shell CoO@Co nanoparticle catalysts. Adjusting Co loading, Fe doping, and reduction temperature improved reaction efficiency. 7Co-0.2Fe/CeO₂ catalysts reduced at 500 °C demonstrated optimal performance. 1,5-PeD produced at 54.76 mmol/g Co /h, representing the top activity levels among the reported catalysts. H₂-TPR, XRD, HAADF-STEM, FT-IR, XPS, and XANES were employed to investigate the catalyst structure-activity relationship. Co 2+ cleaves furan ring C−O bond, Co⁰ promotes double-bond hydrogenation. The CoO@Co structure favors the desired 1,5-PeD production route. Trace Fe species optimize the Co 2+ /Co⁰ ratio, enhance the substrate adsorption, and inhibit the furan ring saturation. These findings emphasize the importance of fine-tuning catalyst structure and composition for selectivity improvement.
研究领域:
化学工程
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催化科学
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可再生资源转化
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产品关联
DOI
PubMed
高影响因子
ACS Catalysis
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2025
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IF 13.1
Yang Li,Jian Zhang,Wei Zhang,Chang Zhou,Jianbin Huang,Zerui Su,Ziyuan Qiao,Xiaoyuan Qin,Pei Xiong,Feng-Shou Xiao
Direct hydrogenolysis of biomass-derived furfural to produce 1,5-pentanediol, an essential precursor for polyesters and polyurethanes, plays a significant role in biomass utilization. In this work, using the carbothermal shock strategy, 1.5PtCo1Ce1-CTS ternary metal oxides were successfully prepared, containing abundant oxygen vacancies (Ov) and Co2+ species that are favorable for hydrogen transfer and ring-opening of furan, thereby enhancing catalytic activity and 1,5-pentanediol selectivity. Under an optimized condition (170 °C, 3 MPa of H2, 4 h), the 1.5PtCo1Ce1-CTS catalyst achieved furfural conversion at 99.3% and 1,5-pentanediol selectivity at 59.2%. During recycling tests, the 1.5PtCo1Ce1-CTS catalyst exhibited high resistance to deactivation with a simple and rapid regeneration process. This work offers an alternative, versatile, and eco-friendly strategy for designing efficient heterogeneous catalysts for the hydrogenolysis of furfural into 1,5-pentanediol in the future.
研究领域:
化学工程
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催化科学
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生物质转化
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产品关联
DOI
高影响因子
CATALYSIS LETTERS
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2021
·Vol. 151
·期 9
·2513-2526
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IF 3.186
Cui Kai,Qian Wei,Shao Zhengjiang,Zhao Xiuge,Gong Honghui,Wei Xinjia,Wang Jiajia,Chen Manyu,Cao Xiaoming,Hou Zhenshan
Furfural (FFR) is one of the most important biomass-derived chemicals. Its large-scale availability calls for the exploration of new transformation methods for further valorization. Herein, we demonstrate that Ru nanoparticles (Ru NPs)-supported on a sulfonated carbon layer coated SBA-15 can be employed as an efficient bi-functional catalyst for one step conversion of FFR into 1,4-pentanediol (1,4-PeDO). The optimum bi-functional catalyst can afford the full the conversion of FFR and 86% selectivity to 1,4-PeDO. The catalysts have been characterized thoroughly by using a complementary combination of powder X-ray diffraction, N 2 adsorption–desorption, scanning/transmission electron microscopy, Fourier transform infrared spectroscopy, elemental analysis, and X-ray photoelectron spectroscopy. The characterization revealed that acidic groups (–SO 3 H) have been introduced on the surface of the carbon layer coated SBA-15 support after sulfonation with 98% H 2 SO 4 and the surface acidity can be tuned facilely by the sulfonating time. Meantime, Ru(0) sites was highly dispersed via an impregnation and sequential reduction and directly adjacent to the surface –SO 3 H group. There existed an electronic interaction between Ru(0) sites and sulfonic groups, in which the electronic transfer from sulfonic sites to Ru(0) sites occurred. Brönsted acid sites (–SO 3 H) have a significant influence on the FFR conversion and the selectivity to 1,4-PeDO. The ordered mesoporous structure, the appropriate density of acid sites and the electron-rich Ru(0) sites accounted for the the excellent performance of the catalyst for an efficient production of 1,4-PeDO from FFR. Graphic Abstract
研究领域:
催化化学
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生物质转化
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材料科学
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DOI
高影响因子
ACS Applied Polymer Materials
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2025
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IF 4.7
ZhangHe Wang,Chao Zeng,YuHao Wu,ChaoChen Xu,ShengMing Zhang,Peng Ji,ChaoSheng Wang,HuaPing Wang
Polyester (PET) has become the focus of research in the shrink film industry due to its good heat resistance, high transparency, and excellent mechanical properties. In order to improve the shrinkage rate of the film, amorphous PET (PETG) is usually obtained by copolymerization modification using some flexible diols and so on. However, introducing flexible structures reduces the glass transition temperature (Tg) and mechanical strength, and importantly, the gas barrier properties of most PETGs are weak. Here, a series of poly(terephthalic acid-naphthalene dicarboxylic acid-ethylene glycol-neopentyl glycol) (PENTN) were prepared by melt polymerization using different contents of 1,4-naphthalene dicarboxylic acid (1,4-NDA) or 2,6-naphthalene dicarboxylic acid (2,6-NDA). The results show that the introduction of 1,4-NDA does not enhance the Tg of the copolyesters significantly, whereas the Tg of the copolyesters increases linearly with the increase in the content of 2,6-NDA. The Tg of 2,6-PENTNs ranges from 82.2 to 90.5 °C. The crystallization is inhibited effectively due to the neopentyl glycol and exhibits good transparency (>85%) and low haze value (<4%), which results in the preparation of copolyesters that are all amorphous polymers. The differences in the effects of 2,6-NDA and 1,4-NDA on the thermal properties of the copolyesters were analyzed. Meanwhile, the copolyesters were prepared into films, and the gas barrier properties were analyzed in detail. The rheological analysis reveals the free volume of the copolyester is rapidly decreasing with the introduction of the naphthalene group structure. The gas barrier property of the copolyesters can be improved to a high level. This work provides an idea for the functionalized modification of packaging materials.
研究领域:
材料科学
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高分子化学
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DOI
高影响因子
Catalysts
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2024
·Vol. 14
·期 7
·428
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IF 3.8
Weiying Wang,Changlin Chen
Tetrahydrofurfuryl alcohol, a cost-effective biomass derivative, offers a sustainable path for synthesizing 1,5-pentanediol through hydrogenolysis. To develop the efficient production of 1,5-pentanediol from this alcohol, we have prepared a series of MgAl2O4-modified Pt/WOx/γ-Al2O3catalysts with varying compositions via impregnation–calcination methods. The physicochemical properties of these catalysts were subsequently characterized using diverse techniques. Characterization revealed that magnesia–alumina spinel modification enhanced Pt particle dispersion, CO adsorption on Pt/WOx/γ-Al2O3, reduced Pt particle reduction temperature, diminished the acid content in the catalysts, and increased the surface oxygen vacancy concentration. These alterations appear to influence the catalyst performance, though other factors cannot be ruled out. Catalytic activity tests demonstrated that magnesia–alumina spinel modification improved tetrahydrofurfuryl alcohol hydrogenolysis activity and the 1,5-pentanediol selectivity of Pt/WOx/γ-Al2O3. Optimal performance was achieved at 12% magnesia–alumina spinel loading, with a tetrahydrofurfuryl alcohol conversion of 47.3% and 1,5-pentanediol selectivity of 88.4%.
研究领域:
化学工程
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催化科学
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生物质转化
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产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）