JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Kai Li,Wan-zhao Huang,Shi-guan Yang,Jia-hao Yu,Qi Niu,Li Zhao,Ying Mo,Yu-han Fan,Qiang Lu
This study developed an innovative method for directional degradation and valorization of waste cellulose acetate (CA) through pretreatment followed with catalytic pyrolysis, enabling the efficient and high-value recovery of CA. A synergistic pretreatment with ethanol and NaOH was employed to modify the molecular structure of CA feedstock. Coupled with phosphoric acid-activated carbon (PAC) catalyzed pyrolysis, the pretreatment-dependent alternation in CA’s physicochemical properties and their effects on pyrolysis to prepare levoglucosenone (LGO) were systematically investigated. The results indicated that the ethanol-NaOH synergistic pretreatment selectively removed the acetyl substituents in CA, exposing more cellulose characteristics, and facilitated the swelling of CA. These modifications enhanced the suitability of CA for selective LGO production. In pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments, the highest yield of LGO from pretreated CA reached 17.84 wt%, significantly exceeding the 2.67 wt% yield gained from untreated CA. This study laid a solid foundation for the efficient and high-value recycling of waste CA.
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2022
·
IF 6.437
Haoran Yuan,Chengyu Li,Rui Shan,Jun Zhang,Lingjun Zhu,Yong Chen
In the present study, a series of municipal sludge derived solid acids, synthesized through hydrothermal pre-carbonization coupled with secondary pyrolysis method, were developed for levoglucosenone (LGO) production via cellulose fast pyrolysis . Specific physico-chemical characterizations such as XRD, FTIR, N 2 adsorption-desorption, NH 3 -TPD, etc., were undertaken to reveal the structural properties of as-prepared solid acids. Phosphoric acid and sulfuric acid decorated municipal sludge derived carbon-based materials containing abundant Brønsted acid sites remarkably facilitated the selective formation of LGO. Particularly, high LGO yield (~20 wt%) were achieved using both phosphoric and sulfonic acid functionalized municipal sludge derived porous carbon. The as-prepared municipal sludge derived solid acids could be reused for multiple cycles in LGO preparation without significant decline in pyrolysis performance. This research will provide good reference for the resource utilization of lignocellulosic biomass and municipal sludge, particularly in the aspect of valuable chemicals manufacture.
研究领域:
生物质能
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废弃物资源化
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催化化学
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2022
·
IF 6.449
Bo Wang,Kai Li,Cheng-bo Zhang,Bin Hu,Yan-qin Huang,Ti-peng Wang,Qiang Lu
This study was dedicated to enhancing the generation of levoglucosenone (LGO) from catalytic pyrolysis of cellulose by optimizing its ultrastructure. Cellulose was pretreated by Na 2 CO 3 solutions with different concentrations and Amberlyst-15 (A-15) under different temperatures, respectively. The influences of pretreatment on the cellulose ultrastructure, especially its degree of polymerization (DP) and crystallinity index (CrI), were characterized. The catalytic pyrolysis experiments of pretreated cellulose were conducted with activated carbon as the catalyst to clarify the regulatory functions of ultrastructure on the LGO formation. Na 2 CO 3 pretreatment could decrease CrI of cellulose remarkably and DP slightly. At the low Na 2 CO 3 concentration, the decrease of CrI could promote the generation of LGO, but the high Na 2 CO 3 concentration was detrimental to LGO formation because of the almost full transformation of cellulose I β to II. With the raising of temperature, A-15 pretreatment could increase the CrI and decrease the DP significantly, and the corresponding LGO yield showed a trend of gradual decrease. Moreover, the low CrI could lower the pyrolysis temperature, while the low DP could decrease the catalyst dosage for maximal LGO formation. The cellulose pretreated with 1 % Na 2 CO 3 solution was most appropriate for producing LGO, and the maximum LGO yield was 19.76 wt. %, higher than that of 18.04 wt. % from raw cellulose, while the corresponding pyrolysis temperature of 285 °C and catalyst/sample of 1/5 were lower than those of 300 °C and 1/3 from raw cellulose.
研究领域:
生物质能
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化学工程
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材料科学
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DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2020
·
IF 3.905
Kai Li,Bo Wang,Dana Bolatibieke,Dong-Hong Nan,Zhen-Xi Zhang,Min-Shu Cui,Qiang Lu
Levoglucosenone (LGO) is a valuable chiral synthon and can be produced from pyrolysis of cellulose and biomass. In the present study, Ni-P-MCM-41 catalysts with various P-to-Ni ratios were prepared and employed for selective production of LGO from biomass. Both analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) and lab-scale experiments were conducted to explore the effects of several factors on the formation of LGO, including P-to-Ni ratio in Ni-P-MCM-41, catalyst/sample ratio and pyrolysis temperature. The results revealed that all the Ni-P-MCM-41 catalysts, especially the one with a P-to-Ni ratio of 5, exhibited excellent catalytic capability and selectivity for LGO production. For Py-GC/MS, the maximal LGO yields of 27.34 wt% and 14.30 wt% were achieved from cellulose and pine at 350 °C with catalyst/cellulose ratio of 3 and catalyst/pine ratio of 2, respectively. While in lab-scale experiments, the highest LGO yields from cellulose and pine were 21.37 wt% and 10.71 wt%, with the corresponding selectivity of 78.31% and 53.75%, respectively. The Ni-P-MCM-41 catalyst possessed much better catalytic efficiency on the LGO production than previously reported catalysts, including H 2 SO 4 , H 3 PO 4 , solid superacid, solid phosphoric acid and activated carbon.
研究领域:
化学工程
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可再生能源
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催化
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分析化学
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DOI
高影响因子
ACS Sustainable Chemistry & Engineering
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2017
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IF 5.951
Xiao-ning Ye,Qiang Lu,Xin Wang,Hao-qiang Guo,Min-shu Cui,Chang-qing Dong,Yong-ping Yang
Activated carbon (AC) prepared by chemical activation with H3PO4 (named AC-P) was employed for catalytic fast pyrolysis of cellulose and biomass to selectively produce levoglucosenone (LGO). The catalytic pyrolysis behaviors and product distributions were revealed via both analytical pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) and lab-scale experiments. Moreover, the performance of AC-P catalyst was compared with previously reported strong acid catalysts and other ACs prepared by different activation methods. In addition, reusability and stability of the AC-P catalyst have been examined via recycling experiments. The results indicated that the AC-P catalyst was effective for selectively preparing LGO from both cellulose and biomass and performed better than other catalysts. Among the three biomass materials (pine wood, poplar wood, and bagasse), pine wood showed the best selectivity for producing LGO. The maximal LGO yields of 18.1 and 9.1 wt % were obtained from cellulose and pine wood, respectively, in Py-GC/MS experiments under a catalyst-to-feedstock ratio of 1:3 at 300 °C, whereas the lab-scale setup obtained the highest LGO yields of 14.7 and 7.8 wt % from cellulose and pine wood with selectivities of 76.3 and 43.0%, respectively, based on organic liquid products. Furthermore, granular AC-P catalyst exhibited good reusability and stability in the recycling experiments. Stable yields of LGO above 12.5 wt % from cellulose were obtained in six consecutive runs without any regeneration of the recycled granular AC-P catalyst.
研究领域:
能源与燃料化学
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催化化学
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
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2023
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IF 5.9
Ji Liu,Hao Fu,Bin Hu,Wan-yu Fu,Kai Li,Li Zhao,Bing Zhang,Qiang Lu
Catalytic fast pyrolysis of biomass/cellulose is a promising way for the production of levoglucosenone (LGO) and other value-added anhydrosugars. Herein, ammonium dihydrogen phosphate (NH 4 H 2 PO 4 ) modified mesoporous niobium pentoxide (P-Nb 2 O 5 ) was first applied to selectively produce LGO. The catalyst had a stable amorphous mesoporous structure with abundant activity species (Nb-O-Nb, Nb-O-P, P-OH, and PO 4 3- ), which affected the dehydration and depolymerization reactions of cellulose to alter the competing relationship between levoglucosan (LG) and LGO. Micro-scale pyrolysis experiments demonstrated that the yield of LGO reached 19.6 wt% under the optimized condition (P loading of 50 wt%, pyrolysis temperature of 400 °C, and catalyst-to-cellulose mass ratio of 7). In lab-scale experiments, the highest yield of LGO attained 16.5 wt%, and the catalytic activity could maintain over 80% after five recycles. Overall, the P-Nb 2 O 5 has been proven to be a promising catalyst to produce LGO from cellulose.
研究领域:
催化
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化学工程
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可再生能源
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材料科学
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DOI
高影响因子
BioEnergy Research
·
2015
·Vol. 8
·期 3
·1263-1274
·
IF 3.541
Zhang Zhi-bo,Lu Qiang,Ye Xiao-ning,Wang Ti-peng,Wang Xian-hua,Dong Chang-qing
Solid phosphoric acid (SPA) catalysts with different carriers were prepared and used for catalytic fast pyrolysis of poplar wood to produce levoglucosenone (LGO), a valuable anhydrosugar derivative that can be used in various organic synthesis applications. Pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) experiments were performed to evaluate the catalytic capabilities of these catalysts under different reaction conditions. The results indicated that SPA catalyst prepared with the SBA-15 carrier exhibited the best catalytic capability for selectively producing LGO. Both the catalytic pyrolysis temperature and catalyst-to-biomass ratio affected the pyrolytic products greatly. The maximal LGO yield reached as high as 8.2 wt% from poplar wood, obtained at the pyrolysis temperature of 300 °C and the catalyst-to-biomass ratio of 1. The by-products during the catalytic pyrolysis process were mainly acetic acid (AA) and furfural (FF). In addition, the SPA catalyst possessed better catalytic capability than the liquid phosphoric acid (H 3 PO 4 ) catalyst to produce LGO.
研究领域:
生物能源
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催化化学
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生物质转化
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热解化学
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绿色化学
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可再生资源利用
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DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
2025
·
IF 6.2
Kai Li,Jia-hao Yu,Bo Wang,Yong-sheng Ma,Qi Niu,Bin Hu,Xin-hua Yuan,Qiang Lu
The selective pyrolysis of cellulose to levoglucosenone (LGO) remains challenging, primarily due to the lack of catalysts with tailored active sites and appropriate modification of cellulose microstructures, both critically determining reaction pathways and product selectivity. To realize the high-selectivity conversion of cellulose to LGO, this study synthesized metal-organic frameworks (MOFs) with tunable channel structures using ZIF-67 as the precursor, which were subsequently subjected to partial phosphidation to prepare MOF-derived phosphorized porous carbon (CoP/N-C) catalysts for the catalytic pyrolysis of amorphous cellulose (AMC). The effects of catalyst characteristics on the product distribution and LGO yield during AMC pyrolysis were systematically investigated using pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) and a lab-scale setup, while the catalytic pyrolysis mechanisms under the coupled effects of catalyst properties and reaction conditions were comprehensively elucidated. Results revealed that CoP/N-C significantly enhanced LGO yield from AMC pyrolysis. Particularly, the CoP (100) /N-C catalyst (synthesized with a Co:P ratio of 9:100) demonstrated optimal performance, achieving maximum LGO yields of 24.76 wt% in Py-GC/MS experiments and 18.89 wt% in lab-scale tests under optimized conditions (pyrolysis temperature: 320℃, catalyst:AMC ratio: 4:1). This study systematically revealed the structure-activity relationship between catalyst characteristics and LGO formation mechanisms, providing critical insights for further catalyst optimization and LGO yield enhancement.
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高影响因子
ENERGY & FUELS
·
2022
·
IF 4.654
Yang Li,Bin Hu,Hao Fu,Yu-long Wu,Zhen-xi Zhang,Ji Liu,Bing Zhang,Qiang Lu
Cellulose can be selectively converted into levoglucosenone (LGO), a high-value anhydrosugar, through fast pyrolysis with acidic catalysts. Herein, phosphorus molybdenum tin mixed metal oxides (P-Mo/SnO2) were prepared for the selective production of LGO from the in situ catalytic fast pyrolysis (CFP) of cellulose, where the PO43–, P-support, and Mo6+ species in P-Mo/SnO2 played the determining role in promoting depolymerization, dehydration, and deoxygenation reactions. Pyrolysis-chromatography/mass spectrometry (Py-GC/MS) tests were carried out to explore the influence of catalyst-to-cellulose (CA-to-CL) ratio, phosphomolybdic acid (PMA) loading, and pyrolytic reaction temperature on LGO preparation. The results demonstrated the maximal LGO yield could reach 17.98 wt % via using P-Mo/SnO2 with the PMA loading of 50 wt % at the pyrolysis temperature of 300 °C and the CA-to-CL ratio of 1:1. Moreover, the highest LGO yield could be up to 12.70 wt % in lab-scale CFP tests at 300 °C and the CA-to-CL ratio of 2:1, and the LGO yield could remain above 10 wt % after five runs of catalyst calcination regeneration.
研究领域:
化学工程
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催化
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生物化学工程
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可再生能源
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DOI
高影响因子
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
·
2026
·
IF 3.9
Feifan Yu,Xin Huang,Tianlong Liu,Chuan Ma,Yunlin Shao,Jingyu Ran
Levoglucosenone (LGO) holds great promise for sustainable chemical production. This study demonstrates the enhanced production of LGO from cellulose via solvothermal catalysis over sulfonated carbon (SC), enabled by tailored pretreatments. Air plasma modification of the catalyst introduced nitrogen doping and additional oxygen-containing groups (−COOH, −OH), which facilitated cellulose adsorption and promoted glycosidic bond cleavage. This boosted the LGO yield to 22.5 wt %, a significant increase from the 16.4 wt % obtained with the untreated system. Alternatively, ball milling pretreatment of cellulose dramatically reduced its crystallinity and particle size, achieving an even higher LGO yield to 24.7 wt % (31.8% mole yield) at 200 °C for 4 h with a cellulose to catalyst mass ratio of 3, which increased by 50% compared to the untreated system. Interestingly, applying both plasma and ball milling pretreatments simultaneously did not yield a synergistic effect, indicating that the observed enhancements are predominantly governed by single-mode modifications. Furthermore, the sulfonated carbon catalyst exhibited excellent stability, retaining high activity over five consecutive cycles. This work provides efficient pretreatment strategies and insight into their distinct roles, highlighting a practical pathway for valorizing cellulose into high-value chemicals.
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高影响因子
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