INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
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2020
·
IF 3.573
Guangyue Xu,Chuang Li,Tianyu Deng,Chenguang Wang,Ying Zhang,Yao Fu
The conversion of levulinic acid (LA) to γ-valerolactone (GVL) is one of the most important reactions from biomass-derived platform chemicals to value-added chemicals. In this work, bimetallic PdRu/TiO2 catalyst compared to monometallic Ru/TiO2 was designed for the conversion of LA to GVL at ambient H2 pressure. The highly dispersed Pd affected the reaction by two antagonistic effects: (I) increasing the reaction rate by promoting the activation of H2; (II) decreasing the reaction rate by lowering the activation ability of carbonyl group over Ru. The kinetic analysis refined by H2 concentration showed much lower apparent activation energy over 0.2Pd1Ru/TiO2 than that over Ru/TiO2. Finally, the catalysts were evaluated by both GVL productivity and catalyst cost to show increasing benefit of Pd addition at lower H2 pressure. This study offers both theoretical foundation and application instructions for high efficiency conversion of LA to GVL under mild conditions, especially ambient H2 pressure.
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高影响因子
Materials Today Sustainability
·
2023
·
IF 7.8
B. Putrakumar,Prem Kumar Seelam,G.S. Rao,N. Pethan Rajan,P. Bhanuchander,G. Raveendra,P. Vijayanand,U. Lassi,E.M. Bakhsh,S.B. Khan,S. Kim
This research work introduces highly dispersed Cu nanoparticles encapsulated into a nanoporous carbon (Cu@C) structure as an efficient catalytic system in selective hydrogenation of γ-valerolactone (GVL) to 1,4-pentanediol. The nanoporous carbon support and the catalysts were synthesized by sequential novel methods and characterized extensively by using a combination of different analytical techniques to determine the phase, textural, morphology, nanoparticles size, and distribution analysis, and redox behavior. The designed Cu@C embedded catalysts show moderately high activity in GVL hydrogenation with different Cu loadings. The effect of copper loadings was found to be a significant parameter in gaining the best performance in GVL conversion. The copper nanoparticles were uniformly distributed over the nano-scaled carbon structure with active metallic Cu(111) sites with high dispersion and promote GVL hydrogenation, efficiently. Over a 5Cu@C catalyst exhibited the highest GVL conversion (∼91%) and 1,4-pentanediol selectivity (∼97%) at 200 °C for a 5 h reaction time under a 5 MPa H 2 pressure. The dispersion of the active copper phase in combination with a smaller particle size and surface acidity is directly correlated with the catalytic performance activity. The effects of reaction parameters such as the reaction time, temperature, and H 2 pressure were systematically investigated. Overall, Cu@C is a promising non-noble metal-based catalytic system for the upgradation of biomass-based platform molecules via selective hydrogenation.
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NEW JOURNAL OF CHEMISTRY
·
2023
·Vol. 47
·期 21
·10455-10462
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IF 3.3
Mengting Chen,Qifeng Zhong,Jiao Ma,Zhiyang Zhang,Yingxin Liu,Zuojun Wei,Shuguang Deng
Hydrogenation of levulinic acid (LA) to γ-valerolactone (GVL) is a key reaction in the conversion of biomass to renewable fuels and value-added chemicals. Developing low-cost, highly efficient and reusable non-noble metal-based heterogeneous catalysts is vital but challenging. Herein, non-noble Ni–Mn/SiO2 catalysts with a low Ni loading (2.0 wt%) were designed for the selective hydrogenation of LA to GVL. The results showed that the optimal Ni–Mn/SiO2 (Ni/Mn = 2) catalyst with well-dispersed and small-sized metal nanoparticles (2.21 nm) and moderate acid sites exhibited excellent activity and selectivity and achieved a 100% yield of GVL in a 1,4-dioxane solvent under mild reaction conditions (e.g., 0.8 mol% Ni, 140 °C and 2.0 MPa H2) for 5.5 h and a 100% GVL yield at 180 °C for 2 h with a turnover frequency (TOF) of 190.2 h−1, which is better than most non-noble metal catalysts reported. Furthermore, the catalyst exhibited excellent reusability and could be recycled at least five times with only slight activity loss. This work provides new insights for the rational design of highly efficient and stable non-noble metal catalysts for the conversion of LA to GVL.
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Journal of Energy Chemistry
·
2019
·
IF 5.162
Shuqi Fang,Zhibing Cui,Yuting Zhu,Chenguang Wang,Jing Bai,Xinghua Zhang,Ying Xu,Qiying Liu,Lungang Chen,Qi Zhang,Longlong Ma
Herein, we reported in situ synthesis of biomass-derived Ni/C catalyst by self-reduction with pomelo peel. Compared with the conventional method, which includes carbonization , activation, impregnation and reduction, the entire preparation process was simplified to two steps, which was more straightforward. This synthesis method was green as Ni/C can be prepared without any additional chemical and the self-reduction process was realized in N 2 , which can avoid using H 2 thus averting some problems such as storage, transportation and safety of H 2 . Meanwhile, the size and dispersion of Ni particles can be controlled by changing carbonization temperature. The synthesis mechanism of Ni/C catalyst with self-reduction was investigated, which was mainly attributed to the carbon and reducing gas produced during the carbonization process. For the catalytic performance of GVL synthesis, a high yield (94.5%) can be obtained and it exhibited good stability up to 5 cycles without obvious loss of catalytic activity .
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APPLIED CATALYSIS B-ENVIRONMENTAL
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2024
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IF 20.2
Jianfeng Shan,Zheng Chen,Dengfeng Wang,Guangyu Zhang,Sheng Li,Chuan Sun,Dongchao Wang,Caixia Ju,Xuelan Zhang,Lei Li
Catalytic conversion of ethyl levulinate (EL) to γ-valerolactone (GVL) is a pivotal reaction in biomass conversion. Here, Pd/CoO x was studied and showed much higher EL hydrogenation reactivity than other Pd based catalysts. Further investigation revealed that EL conversion increased linearly with PdCo alloying degree elevating, indicating that PdCo alloy is ascribed to the superior reactivity of Pd/CoO x . Interestingly, Pd/CoO x with low Pd loading also exhibited excellent hydrogenation performance, and surface enrichment of Pd was identified as the main reason. Additionally, employing HZSM-5 as a co-catalyst not only accelerated ethyl 4-hydroxypentanoate lactonization, but also dramatically improved the stability of Pd/CoO x . As a result, a 99.1 % yield of GVL was achieved by the synergistic catalysis of HZSM-5 and Pd/CoO x containing 0.58 wt% Pd, which is comparable with the best catalyst ever reported in alkyl levulinate hydrogenation to GVL. Furthermore, the insights gained from this work have broad potential applications in biomass hydrogenation.
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JOURNAL OF MOLECULAR LIQUIDS
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2025
·
IF 5.2
Zi-Quan Wang,Ya-Peng Du,Xiao-Ping Zheng,Yu Chai,Yu-Cang Zhang,Yan-Zhen Zheng
The direct conversion of raw lignocellulosic waste into specialty chemicals such as levulinic acid (LA) has the potential to significantly enhance biorefinery profitability. Here, we demonstrated that incorporating γ-valerolactone (GVL) as a co-solvent during the SO 3 H-functionalized ionic liquid-catalyzed conversion of bagasse in water markedly enhanced reaction rates and catalytic activity, achieving a LA yield as high as 76.1 % with a 1:1 vol ratio of GVL to water. This catalytic system also effectively converted other lignocellulosic waste to LA. Reaction constants and activation energies for the bagasse dehydration process to LA were obtained. Comprehensive characterization via Fourier transform infrared spectroscopy (FTIR), scanning electron microscopy (SEM), and X-ray diffraction (XRD) elucidated significant changes in functional groups, surface morphology, and crystallinity index of solid residues over extended reaction times. Notably, hemicellulose and cellulose were converted within 4 h, with lignin remaining in the solid residues and forming by-products after prolonged reaction times. This efficient one-pot conversion method showed promise as a sustainable approach to transform agricultural waste into LA, offering new opportunities for eco-friendly resource utilization.
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CHEMICAL ENGINEERING JOURNAL
·
2025
·
IF 13.2
Mengli Zhou,Sichan Li,Haojie Tian,Xinyu Liu,Zhimin Wu,Qiying Liu,Jianchun Jiang
Levlinic acid (LA) and its derived γ-valerolactone (GVL) are the two important biomass derived platform molecules, which showed wide application in the fields of fine chemicals, drug and liquid fuel industrials. Considering the coupling of sequential steps for glucose to LA and GVL, selective production of LA and GVL via glucose one-pot conversion in water is an open challenge. Herein, we used metal chlorides as the acidic catalyst for glucose conversion to LA, obtaining the high yield of 77.8 C-mol% over SnCl 4 . Moreover, using the SnCl 4 and Ru/C as the combined catalyst, glucose or cellulose could be converted to GVL with the high yield of 60.1 or 57.9 C-mol% in the case of in situ hydrogenation by formic acid (the by-products during LA formation) decomposition. The formation of LA was responsible for the cooperative effect of BAS (Bronsted acid sites) and LAS (Lewis acid sites) of SnCl 4 for accelerating glucose isomerization, fructose dehydration followed by 5-hydroxymethyl furfural (HMF) rehydration, while the GVL production is relative to the highly efficient formic acid decomposition to H 2 followed by LA hydrogenation to GVL over Ru/C. This study provided an avenue for facile and highly efficient conversion of biomass and the derivatives to LA and GVL using commercial catalysts.
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Journal of Cleaner Production
·
2025
·
IF 10
Hongguang Zhang,Zi Yu,Yongxin Liang,Tao Gan,Zuqiang Huang,Huayu Hu,Yanjuan Zhang
The utilization of organic molecules as in-situ hydrogen donors for producing γ-valerolactone (GVL) biofuel from biomass-derived levulinic acid (LA) represents one of the promising sustainable approaches. However, this process still faces challenges, including the difficult activation of the hydrogen source and the transport limitations of active hydrogen species. Herein, a Co-MnO/spontaneously polarized ceramic-carbon (Co-MnO/SPCE-C) composite catalyst, featuring a unique spontaneous polarization effect, was developed for catalytic transfer hydrogenation (CTH) of LA to GVL in the isopropanol/H 2 O (volume ratio = 1/19) cosolvent system. Co-MnO/SPCE-C contributed to an outstanding LA conversion of 99.9% and a favorable GVL yield of 93.5%, surpassing the performance achieved by comparative catalysts. Various characterization techniques demonstrate that SPCE with far-infrared emission and surface electric field increased the oxygen vacancies, thereby promoting hydrogen spillover and enhancing the properties of CoO x –MnO acidic sites. The 17 O NMR spectra reveal that SPCE activated water clusters by weakening the hydrogen bonding network. Moreover, D 2 O experiments show that SPCE facilitated the participation of water in the reaction. This work provides valuable insights into the development of an efficient strategy for producing GVL from LA. Before the catalyst can be considered for commercial applications, the focus in the future should be on a comprehensive computational analysis, long-term evaluation of catalyst stability, and additional industrial-scale testing.
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CELLULOSE
·
2020
·Vol. 27
·期 7
·3581-3590
·
IF 4.21
Yang Xue,Song Yanliang,Ma Sen,Zhang Xu,Tan Tianwei
A method for isolating components of lignocellulose in hybrid poplar by using an organic solvent (γ-valerolactone) in combination with a solid organic acid ( p -toluenesulfonic acid) is studied here. The combined hydrolysis factor (CHF) was used to measure the severity of the pretreatment conditions and to find the optimal reaction conditions (CHF = 54.99) by judging enzymatic saccharification and characterization of lignin residual. At this pretreatment strength, 91.67% hemicellulose and 86.14% lignin in lignocellulose were effectively removed, and the enzymatic hydrolysis of cellulose residue reached 84.84%. Hemicellulose was hydrolyzed to 4.39 g L −1 of xylose, and a portion was converted to 2.95 g L −1 of furfural and 3.59 g L −1 of acetic acid. The molecular weight, polydispersities and phenolic hydroxyl groups content of the isolated lignin were 1587 g mol −1 , 1.04 and 3.64 mmol g −1 respectively, which indicated that the lignin had the potential to be a phenolic resin material and wood polyurethane foam. In summary, this method effectively separated three components of lignocellulose and obtained high purity cellulose and lignin.
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APPLIED ORGANOMETALLIC CHEMISTRY
·
2022
·Vol. 36
·期 5
·e6646
·
IF 4.072
Yanyun Wang,Yuming Zhou,Jiehua Bao,Jiajia Wang,Yiwei Zhang,Xiaoli Sheng,Yuzhong Huang
Pt nanocatalysts have received enthusiastic attention in the field of clean energy technologies due to their high catalytic activity and selectivity. The growth size and dispersion of Pt particles play significant effects on the reaction activity, especially in high temperature catalytic reactions where catalysts are prone to deactivation due to agglomeration and sintering of Pt particles. Herein, the Pt nanoparticles were effectively stabilized on AIPO-18 molecular sieve by a biomolecule-mediated green synthesis method. Based on the biocompatibility and electrostatic synergy of carboxymethyl chitosan (CMC), a high degree of Pt nanoclusters dispersion in AIPO-18 zeolites was achieved. The hydroconversion of levulinic acid (LA)was carried out at 160°C and 2 MPa hydrogen pressure, and the LA conversion of Pt/AIPO-18 (5CMC) reached 95.2% and the selectivity of γ-valerolactone (GVL) was 97.9% after 2 h. Pt/AIPO-18 (5CMC) exhibited satisfactory results that superior to the initial reactivity of Pt/AIPO-18 (0CMC) after five runs.
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INDUSTRIAL CROPS AND PRODUCTS
·
2021
·
IF 5.645
Qiong Wang,Yunyun Liu,Yi Zhang,Yang Chen,Qifa Feng,Wen Wang,Cuiyi Liang,Yunzi Hu,Wei Qi
The conventional pretreatment method of poplar comprises multiple steps, including different procedures for fractionating hemicellulose and lignin separately. In our study, hemicellulose and lignin were removed simultaneously by a one-step method. In the γ-valerolactone (GVL)–water environment, the cellulose retention, hemicellulose removal, and lignin removal rates of 84.94%, 89.08%, and 72.28%, respectively, were achieved over a magnetic carbon-based solid acid (MMCSA) catalyst, under best conditions (160 °C, 30 min, 2 g of poplar, 2 g of MMCSA, 35 mL of GVL, and 15 mL of water). The pretreatment of fresh poplar in the reused MMCSA–GVL–water environment showed similar fractionation results as the first time. Scanning electron microscopy characterization of the cellulosic residue revealed the presence of noticeable structural fragmentation. Brunauer–Emmett–Teller characterization showed that the total pore volume of the residue was 2.13 times that of the raw material. The above features of the residue confirmed the high enzymatic hydrolysis potential of the pretreated residue. The enzymatic hydrolysis efficiency of the poplar residue was 67% at a cellulase loading of 20 FPU/g cellulose in dry matter, and it increased to 77.02% at 40 FPU/g cellulose in dry matter. Interestingly, the addition of Tween 80 did not improve the enzymatic hydrolysis efficiency at high cellulase loadings (30 and 40 FPU/g cellulose in dry matter) compared to the case at low cellulase loadings. The relative mechanisms were also analyzed. In this study, a one-step pretreatment method comprising the MMCSA–GVL system for the catalytic depolymerization of poplar wood was developed. The system was verified to be very effective for the subsequent enzymatic hydrolysis of the residues.
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Molecular Catalysis
·
2021
·
IF 5.062
Weile Li,Mengzhu Li,Huai Liu,Wenlong Jia,Xin Yu,Shuai Wang,Xianhai Zeng,Yong Sun,Junnan Wei,Xing Tang,Lu Lin
The economic and highly efficient synthesis of γ-valerolactone (GVL) is being increasingly focused due to its wide applications in solvent, chemical, and fuel. Herein, a range of SAPO-34 supported zirconium phosphate (ZPS-X) catalysts were prepared for a facile one-pot conversion of furfural (FF) to GVL through a series of cascaded reactions involving transfer hydrogenation, etherification, alcoholysis and esterification. The introduction of zirconium phosphate renders the formation of relatively strong Lewis acid sites, and the amount of Lewis (L) and Brønsted (B) acid sites of ZPS-X catalysts could be modified by adjusting the molar ratio of Zr to P (Zr/P ratio). Specifically, ZPS-1.0 having an appropriate Zr/P ratio with relatively strong L acid sites exhibited superior activity and selectivity for the production of GVL from FF.
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