JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
·
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.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2017
·
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
·
催化化学
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DOI
高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
IF 5.9
Bo Wang,Kai Li,Cheng-bo Zhang,Ting Huang,Ti-peng Wang,Qiang Lu
A series of regenerated cellulose (RC) were prepared by a H 3 PO 4 -H 2 O system with different H 3 PO 4 concentrations. The effects of H 3 PO 4 concentrations on the physicochemical properties of RCs were studied, including crystallinity index (CrI), hydrogen bond energy (E H ), accessibility, and degree of polymerization (DP). The catalytic pyrolysis experiments of RCs were executed with a pyrolysis-gas chromatography/mass spectrometry (Py-GC/MS) instrument and a lab-scale device, to investigate the regulatory function of cellulose structure on the LGO formation. The results indicated that the H 3 PO 4 -H 2 O system could transform the cellulose crystal form from Ⅰ to amorphous form, reduce its CrI and E H significantly, improve its accessibility, while had slight effects on the DP. These changes made RC more appropriate for the selective preparation of LGO, and the corresponding optimal catalyst loading and pyrolytic temperature were also decreased significantly. With phosphoric acid activated carbon as the catalyst, the highest yield of LGO from RC in Py-GC/MS experiments reached 21.50 wt% at catalyst/cellulose (Cat/Cel) ratio of 1/5 and 270 °C, which was much higher than the 18.16 wt% of LGO gained from untreated cellulose at Cat/Cel ratio of 1/3 and 300 °C. In the lab-scale device, the maximum LGO yield from RC was 17.09 wt% at 270 °C and Cat/Cel ratio of 1/6.
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高影响因子
Journal of Energy Chemistry
·
2019
·
IF 5.162
Bin Hu,Qiang Lu,Yu-ting Wu,Wen-luan Xie,Min-shu Cui,Ji Liu,Chang-qing Dong,Yong-ping Yang
The catalytic fast pyrolysis of cellulose impregnated with phosphoric acid (H 3 PO 4 ) offers a promising method for the selective production of levoglucosenone (LGO), a valuable anhydrosugar product. However, the fundamental mechanism for selective LGO formation is unclear. Herein, quantum chemistry calculations and catalytic fast pyrolysis experiments were performed to reveal the formation mechanism of LGO in H 3 PO 4 -catalyzed cellulose pyrolysis. H 3 PO 4 significantly decreased the energy barriers of the pyrolytic reactions and altered the competitiveness of the LGO formation pathways, promoting LGO formation. Through different pathways in the non-catalytic and H 3 PO 4 -catalyzed conditions, LGO is mainly produced from the primary decomposition of glucose units of cellulose and secondary conversion of levoglucosan. The major catalytic formation pathways of LGO comprise similar reactions, with dehydration at the 3-OH + 2-H site as the rate-determining step. Importantly, secondary conversion of 1,4;3,6-dianhydro-α- d -glucopyranose is not feasible for LGO formation, in contrast to previous reports. In addition, a high degree of polymerization is beneficial for the selectivity of LGO formation in the catalytic process, because the glycosidic bond is important for the formation of the bicyclic structure (1,5- and 1,6-acetal rings).
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高影响因子
INDUSTRIAL CROPS AND PRODUCTS
·
2023
·
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.
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高影响因子
FUEL PROCESSING TECHNOLOGY
·
2022
·
IF 8.129
Anbang Xu,Xin Huang,Guangchuan Tang,Lei Tang,Changlei Qin,Zhongqing Yang,Jingyu Ran
Levoglucosenone (LGO) has shown a promising potential in the application of the sustainable chemistry. In this work, alkali metal-doped phosphotungstic acids, M 2.5 H 0.5 PW 12 O 40 (M = Li, Na, K, Rb and Cs), were synthesized and employed for catalytic fast pyrolysis of cellulose to selectively produce LGO. The results show that levoglucosan , the main precursor of LGO, was produced with a yield of 33.5 wt% by non-catalytic pyrolysis of cellulose, while LGO by catalytic fast pyrolysis of cellulose is mainly regulated by the strong/weak acid sites of the M 2.5 H 0.5 PW 12 O 40 . Increasing the atomic radius of the alkali metals from Li to Cs doping to phosphotungstic acid led to an increase of LGO yield, attaining to 15.6 wt% at 300 °C over Cs 2.5 H 0.5 PW 12 O 40 due to a high strong/weak acid site ratio. In addition, LGO yield was further enhanced to 19.2 wt% over (NH 4 ) 2 HPO 4 modified Cs 2.5 H 0.5 PW 12 O 40 as a result of an increase of moderate strong acid sites. This study provides a potential method for LGO production by catalytic pyrolysis of cellulose.
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高影响因子
BioEnergy Research
·
2015
·Vol. 8
·期 3
·1263-1274
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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
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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.
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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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DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2025
·
IF 9
Naeun Kim,Gihoon Kwon,Minki Choi,Gigap Han,Jinsoo Kim,Kyungjung Kwon,Hocheol Song
The rapid increase of electronic waste, particularly battery waste, presents significant environmental challenges such as pollutant emissions and resource depletion, emphasizing the need for effective valorization and reuse strategies. This study introduces a novel approach for repurposing end-of-life lithium iron phosphate (LFP) batteries as catalysts in the pyrolysis of walnut shells (WS). Characterization analyses revealed that LFP provides both Lewis and Brønsted acid sites, which alter the thermal decomposition pathway of WS. As a catalyst, LFP enhanced dehydration reactions, leading to increased yields of key platform chemicals including H 2 , furfural, 2-methylfurfural, and levoglucosenone, while simultaneously reducing CO 2 emissions. Additionally, WS effectively captured fluorine species released from the volatilization of polyvinylidene fluoride (PVDF) in LFP, thereby suppressing harmful HF formation. The optimal furfural yield was achieved at a 1:2 WS to LFP blending ratio. H 2 production increased with temperature up to 800 ˚C, but higher temperature also accelerated the thermal degradation of valuable chemicals, highlighting the importance of proper temperature control to achieve optimal product yields. Life cycle assessment demonstrated that incorporating LFP into WS pyrolysis substantially reduced a broad range of environmental impacts. These findings support the potential of spent LFP batteries as catalysts for sustainable chemical production and resource recycling, contributing to the development of a circular industrial value chain.
研究领域:
环境科学
·
化学工程
·
材料科学
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能源技术
·
废弃物管理
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DOI
PubMed
高影响因子
FUEL
·
2022
·
IF 8.035
Chengyu Li,Jun Zhang,Rui Shan,Haoran Yuan,Yong Chen
In the present study, the kinetics for waste mixed cloth (WMC) pyrolysis over antibiotic residue derived carbon-based solid acids was investigated for the first time. The kinetic parameters for direct pyrolysis and WMC catalyzed pyrolysis were calculated through isoconvertional method, and different types of mechanism function models were employed to elucidate the catalytic pyrolysis process of WMC. Meanwhile, the most suitable pyrolysis mechanism model was determined by matching the apparent activation energy ( E a ). From the kinetical results, the carbon-based solid phosphoric acids significantly reduced the E a of the main reaction of WMC pyrolysis, which significantly decreased from 366.79 ∼ 434.26 kJ/mol to 141.07 ∼ 184.85 kJ/mol. The matching of mechanistic models confirmed that the catalytic reaction largely depended on both phase boundary control and diffusion control, which corresponded to the interaction of the primary pyrolysis products with the outer surface and inner acidic sites from carbon-based solid acids, respectively. The more acidic sites on the outer surface of the catalyst, the better its catalytic pyrolysis kinetic process matches the phase boundary-control model. This kinetical investigation will provide a promising reference for the rational design of carbon-based solid acids in WMC pyrolysis, with the aim of realizing the high-value utilization of organic solid wastes.
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高影响因子
危险品化学品经营许可证（带存储）