FUEL
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2025
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IF 7.5
Caitao Chen,Juan Ma,Yakun Tang,Xiaohui Li,Guangbo Liu,Hanyao Song,Yingluo He,Noritatsu Tsubaki,Lang Liu,Ting Liu
Cleaving the aromatic ether C-O bonds of lignite through catalytic hydroconversion (CHC) presents a significant challenge for producing organic chemicals and clean liquid fuels, which are vital for a sustainable future. In this study, we employed a sacrificial template-self-recovery strategy to synthesize highly dispersed and carbon-coated bimetallic catalysts MCo/C (M = Fe, Cu, Ni) for the CHC of Naomaohu coal (NMHC) and lignite-related model compounds (LRMCs). The carbon-coated NiCo bimetallic alloy catalysts, benefiting from the high dispersity of the active components and the synergistic effect between Ni and Co, exhibited excellent hydrogenolysis activity towards diphenyl ether (DPE). DPE conversion reached 100 % over Ni 3 Co 1 /C under optimal conditions (120 °C, 2 MPa H 2 , 2 h). Moreover, Ni 3 Co 1 /C significantly increased the content of arenes and alkanes while reducing the content of oxygen-containing compounds in the NMHC soluble portion (SP), demonstrating its efficient catalytic hydrogenolysis and hydrodeoxygenation capabilities. Density Functional Theory (DFT) calculations revealed that the Ni 3 Co 1 /C catalyst could activate H 2 to generate hydrogen radicals and diatomic active hydrogen, which are the primary hydrogen species involved in the reaction and affect the CHC of DPE. The experimental results can provide a reference for the conversion of lignite into clean liquid fuels.
研究领域:
化学工程
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能源科学
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DOI
高影响因子
FUEL
·
2025
·
IF 7.5
Haojie Liu,Linjing Hao,Guoli Zhou,Daoguang Teng,Peng Li,Yijun Cao,Baolin Xing
Lignite serves as prefer carbon sources for preparation of composite carbon fibers, as the good reactivity of carbon units and good solubility of reaction products. However, low yield of soluble products from lignite at mild condition and high volatility of toxic organic solvent during spinning are not beneficial for the preparation of coal-based composite carbon fiber. In this work, the sodium hydroxide was introduced to enhance the thermal dissolution of lignite with methanol at mild condition. The water-soluble fraction, separated from the thermal dissolution products, was then mixed with certain amount of polyvinyl alcohol to afford a solution. The solution was treated by electrostatic spinning, pre-oxidation, carbonization, acid washing, and activation, ultimately producing the coal-based composite carbon fibers. In these treatment process, acid washing is beneficial for the removal of surface impurities, resulting an increase in the specific surface area and the exposure of active sites on the surface of the composite carbon fibers. The specific capacitance is enhanced from 73.5 F/g to 197.1 F/g at a current density of 1 A/g. The activated coal-based composite carbon fibers were assembled into a symmetric snap capacitor with an energy density of 8.5 Wh/kg at a power density of 250 W/kg. This work explored a new approach for preparation of coal-based composite carbon fibers by electrostatic spinning in aqueous solution system. It is also a value-added and environmentally friendly pathway of carbon fraction from lignite for preparation of supercapacitor electrode materials.
研究领域:
材料科学
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能源工程
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DOI
高影响因子
ACS Omega
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2020
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IF 2.87
Lulu Yan,Yahe Zhang,Hongyu Yan,Yu Fan,Xuxia Liu,Chao Ma,Quan Shi
CS2/N-methyl-2-pyrrolidone (NMP) could extract much more substance from coals than any other solvents. Investigation on the molecular composition of CS2/NMP extracts from lignite is significant for the understanding of high extraction yield and the clean utilization of coal. The methanol-soluble portions from lignites and CS2/NMP extracts of lignites were characterized by electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry. The yield of CS2/NMP extracts from lignite was quite higher than that of methanol extracts. Furthermore, the yield of methanol-soluble portions from CS2/NMP extracts was far more than that of methanol extracts from lignite. At the level of molecular composition, the relative content of heteroatom compounds with more oxygen atoms, longer side chain, and higher condensation in the CS2/NMP extract was also higher than that in the methanol extract. Despite great difference in the yield and the relative content of components, the distributions of species, molecular weight, carbon number, and double-bond equivalent were similar to those of most organic molecules for the methanol extract and methanol-soluble portions from the CS2/NMP extract. These phenomena suggested that organic molecules with similar structure but different composition, nonuniformly distributed in the coal matrix, were released more in the CS2/NMP extract compared to the single methanol extract.
研究领域:
能源化学
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分析化学
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DOI
高影响因子
SCIENCE OF THE TOTAL ENVIRONMENT
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2018
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IF 4.61
Mengqi Zheng,Yuxing Han,Chunyan Xu,Zhengwen Zhang,Hongjun Han
This study originally investigated the selective adsorption of cyclic organics in APCPW by LAC, corresponding to the change of the bioavailability . As a product from low rank coal, LAC showed more oxygen (O)-containing groups and mesoporous structure than PAC. Adsorption mechanisms were analyzed by equilibrium isotherms and kinetics models combined with physicochemical properties of adsorbent and adsorbates. The results indicated that selectivity of LAC was dominated by chemical interaction and its mesoporous, and was enhanced by hydrophobicity of adsorbates. In addition, PAC and LAC were applied for the treatment of APCPW. Compared with PAC, LAC adsorption exhibited superior removal efficiency of Tph, TOC and TN at 85.90%, 91.15% and 51.64%, respectively. Furthermore, preferential adsorption of biotoxic and bioresistant cyclic organics by LAC was further proved by GC–MS analysis, resulting in increased bioavailability of APCPW. Specifically, LAC exerted sustained detoxication capacity until 86.50% reduction of TU by D. magna evaluation, and lowered toxicity rank (TU = 4.51, classIII) to T. pyriformis than that after PAC adsorption (TU > 10, ClassIV). Meanwhile, biodegradability was also improved by 9.17% after LAC adsorption. Lastly, LAC would exhibit great economic benefits as an alternative for PAC in subsequent process after anaerobic pretreatment .
研究领域:
环境科学
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化学工程
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生物学
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DOI
PubMed
高影响因子
Journal of Cleaner Production
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2021
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IF 9.297
Yuan-Yuan Yu,Zhong-Qiu Liu,Guo-Qiang Zhang,Yu-Jing Liu,An-Guo Ying
The selective valorization of lignite into monocyclic aromatic compounds (MCACs) is extremely challenging due to its chemical inertness and geometrical complexity. The catalytic efficiency of lignite valorization into MCACs over solid acids is significantly reduced by the presence of H 2 O resulting in the leaching and deactivation of acid sites. Moreover, the precise fabrication of poly(ionic liquid)s (PILs) containing Brønsted-Lewis acidic sites, well-defined mesoporous channels, and hydrophobicity remains a considerable challenge. Herein, a novel hydrophobic mesoporous PILs with strong Brønsted-Lewis acid sites was successfully constructed by a synergistic regulation-induced copolymerization strategy for the first time. More exotically, the resultant multifunctional PILs was found to be ultra-efficient catalyst for the selective valorization of Yiwu lignite (YL) into MCACs with 23.5 wt.% yield, which is the highest yield reported for lignite catalytic valorization by precious metal-free catalysts under mild conditions. The co-catalysis mechanisms of YL valorization into MCACs over the multifunctional PILs are confirmed by characterization methods and the synergistic catalysis mechanisms are as follows: (1) hydrophobic micro-environment: the hydrophobic micro-environment created by hydrophobic block is favorable for preventing the leaching and deactivation of Brønsted-Lewis acid sites; (2) mesoporous confinement: the well-defined mesoporous channels strengthen the adsorption amount of H 2 and increases the concentration of substrates; (3) synergistic catalytic active hydrogen transfer of Brønsted-Lewis acid sites: Brønsted-Lewis acid sites synergistically promote H 2 heterolysis to the mobile H + and immobile H − , and then the resulting mobile H + transfers to oxygen atom in lignite to produce MCACs via C–O bond cleavage . This work not only sheds some light on developing the multifunctional solid acid catalysts , but also demonstrates an efficient catalyzing method to produce lignite-based MCACs by co-catalysis of Brønsted-Lewis acidic sites, mesoporous confinement, and hydrophobic micro-environment.
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高影响因子
ACS Sustainable Chemistry & Engineering
·
2021
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IF 8.198
Yafu Tang,Yuechao Yang,Shanmin Hou,Dongdong Cheng,Yuanyuan Yao,Shugang Zhang,Jiazhuo Xie,Xiaoqi Wang,Xiaoxiao Ma,Zhen Yu,Shan Li
Iron (Fe) chelated by water-soluble humic substances can effectively overcome plant micronutrient deficiencies. However, the traditional synthesis methods are often complex, expensive, and thus not applicable to large-scale industrial productions. In this work, an ecofriendly and multifunctional Fe–humic acid (HA) complex was successfully prepared through simply ball milling lignite with double-shelled Fe–N hollow mesoporous carbon microspheres (DS–Fe–N–HC). The novel DS–Fe–N–HC was synthesized using a simple strategy and was first applied in activating HA from lignite by solid-phase ball milling to attain the water-soluble HA–iron fertilizer (WHIF). The physicochemical properties of the DS–Fe–N–HC nanocomposites and WHIF were systematically characterized by a series of techniques. A traditional Fe–HA complex is mainly obtained by mixing HA and iron ions, which has poor water solubility because HA is not activated. In comparison to samples prepared with other methods, WHIF contained more stable water-soluble HA. Furthermore, the as-obtained WHIF had higher amounts of proteins and amino sugar tannin as evidenced in FT-ICR MS analysis. Moreover, WHIF contributed to higher activities in chlorophyll content, height, steam diameter, and biomass of peanuts than other samples. The results demonstrate that WHIF is effective in reducing symptoms of iron deficiency in peanuts, which can be attributed to its iron-based compounds and water-soluble HA. The findings of this study provide a promising, cost-effective, and environmentally friendly solution to mitigate iron deficiency and promote the growth of peanuts for large-scale agriculture production.
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高影响因子
ACS Sustainable Chemistry & Engineering
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2017
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IF 5.951
Yafu Tang,Yuechao Yang,Dongdong Cheng,Bin Gao,Yongshan Wan,Yuncong C. Li
Soil, air, and water pollution caused by lignite is considered a serious environmental problem. Activation methods thus have been developed to extract humic acid from lignite to support the agricultural production as the soil amendment or fertilizer synergist. The traditional activation methods of humic acid from lignite, however, are not environmentally friendly. As the first study, this work developed a novel solid-phase activation method with a Pd/CeO2 nanocatalyst for lignite-derived humic acid. This study analyzed the morphology and structures of the as-synthesized Pd/CeO2 nanocatalyst with various characterization tools. The mechanisms of the Pd/CeO2 nanocatalyst for lignite activation were determined. The Pd/CeO2 catalyst effectively promoted the production of water-soluble humic acids from lignite via KOH solid-phase activation at room temperature. It increased the amount of small molecular active groups and the corresponding small molecules of humic acid. The existence of a strong synergistic effect at the interface sites between Pd/CeO2 nanoparticles and lignite was one of the key factors for the outstanding catalytic performance. In conclusion, this study has great application perspectives for reducing lignite pollution and increasing humic acid utilization by crops, which can improve the sustainability of the environment and agricultural systems.
研究领域:
环境科学
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催化化学
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土壤科学
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纳米技术
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农业化学
✓ 已验证
DOI
高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2026
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IF 6.2
Zong-Pin Fu,Yun-Peng Zhao,Yu-Fa Wu,Qi-Jie Zhou,Shu-Ting Hu,Le-Le Qiu,Fang-Jing Liu,Mei Zhong,Jing Liang,Jing-Pei Cao
Mild thermal dissolution is an effective method for the clean, low-carbon conversion of lignite. However, the resulting products still contain numerous oxygen-bridged bonds and heavy molecular compounds, requiring further upgrading to serve as suitable feedstocks for fuels and chemicals. In this study, a supported Cu-Ni bimetallic catalyst was synthesized via a co-precipitation method and applied to the catalytic hydroconversion (CHC) of thermal dissolution portions from Zhaotong lignite (ZT) and lignite-related model compounds (LRMCs). Catalyst characterization revealed that metal particles were uniformly dispersed on the surface of the Cu-Ni/CoOx-CeO 2 catalyst, along with the formation of defect sites. The CoOx-CeO 2 support promoted surface oxygen vacancy formation. Furthermore, the incorporation of Ni altered the local coordination environment of Cu species through multicomponent interactions. The synergy between interfacial oxygen vacancies and Cu-Ni bimetallic sites significantly enhanced catalytic activity. Tests with LRMCs indicated that the Cu-Ni/CoOx-CeO 2 catalyst selectively cleaves C-O ether bonds under mild conditions, exhibiting both high selectivity and strong hydrogenation activity in the CHC of phenolic compounds. The catalyst also effectively promoted the CHC of macromolecular species in the soluble portion from ZT thermal dissolution, thereby converting phenolic compounds into cycloalkanol. These finding provides valuable insights for developing staged conversion routes and achieving value-added utilization of lignite.
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高影响因子
INORGANIC CHEMISTRY COMMUNICATIONS
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2026
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IF 5.9
Zongsheng Chen,Yanxi Ma,Hui Kang,Ting Liu,Hao Song,Ludan Chen,Yingluo He
The development of highly active catalysts for the catalytic conversion of oxygen-containing aromatics in lignite under mild conditions is of crucial importance for the production of clean liquid fuels. In this study, an in situ nitrogen-doped carbon-coated Ni@C/g-C 3 N 4 catalyst was fabricated. The abundant lone-pair electrons on nitrogen atoms within the g-C 3 N 4 support can coordinate with nickel, facilitating the migration of electrons toward the nickel surface. This electron transfer process favors the formation of Ni δ+ active sites with low electron cloud density, thereby enhancing the hydrogenation catalytic activity of the catalyst. The catalyst exhibited exceptional performance in lignite hydrodeoxygenation (HDO): under conditions of 80 °C, 1.5 MPa H 2 , and a reaction time of 1.5 h, 100% conversion of the lignite model compound benzyl phenyl ether (BOB) was achieved. Furthermore, the catalyst demonstrated remarkable hydrodeoxygenation activity, with high selectivity toward various oxygen-containing model compounds, including methyl nonanoate and 2,6-dimethylphenol. The optimal catalyst was applied to the catalytic conversion of the soluble portion (SP) of Naomaohu coal (NMHC). Results indicated that, compared with the SP, the hydrogenated soluble products from catalytic hydrogenation conversion (SP CHC ) showed a significant increase in the variety and quantity of aromatic and alkane compounds, while the relative contents of phenols, alcohols, esters, and ethers were reduced. These findings fully confirm that the Ni@C/g-C 3 N 4 catalyst can effectively cleave C C and C O bonds during the hydrogenation conversion of the SP, providing theoretical guidance for the conversion of lignite into high-quality clean liquid fuels.
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高影响因子
JOURNAL OF ANALYTICAL AND APPLIED PYROLYSIS
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2024
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IF 5.8
Yang-Yang Xu,Xing Fan,Feng-Yun Ma,Hai-Xu Zou,Xian-Yong Wei
Directly converting lignite into arenes as commodity chemicals and drop-in fuels is a highly desirable target for researchers. However, this is severely limited by the presence of stable inter unit C-O linkages in lignite. Herein, a highly active catalyst, Co-MoS 2 , has been designed and prepared to be used for the selective catalytic cleavage of inter unit C-O bridged bonds (BBs) in the conversion of Naomaohu (NMH), a lignite, to yield arenes. Both catalytic hydrogenation conversion (CHC) and thermal dissolution (a non-catalytic process, named NCHC) of NMH were conducted using n-hexane as the solvent. The soluble fractions from the first stage of NCHC (SF NCHC-1 ) and CHC (SF CHC-1 ), as well as the second stage of NCHC (SF NCHC-2 ) and CHC (SF CHC-2 ) were obtained using the same solvent. After the first-stage catalytic treatment, the relative contents of arenes and alkanes in SF CHC-1 increased by 16.7 % and 9.3 %, respectively, compared to those in SF NCHC-1 , and the relative content of oxygen-containing compounds (OCCs), such as alcohols, phenols , esters, ketones , acids, and furans, decreased by 13.2 %. For the second-stage conversion, the relative contents of arenes and alkanes in SF CHC-2 were 53.5 % and 15.5 % higher than those in SF NCHC-2 , and the relative contents of OCCs was only 6.6 % in SF CHC-2 . The catalytic mechanisms of cleavage of C-O BBs and deoxygenation were proposed based on the CHC of model compounds and density functional theory (DFT) calculation. The adsorption of OCCs and the activation of released hydrogen radical (H·) by Co-MoS 2 , followed by H· addition to the carbon atom connected to oxygen in C-O BBs and oxygen-containing functional groups, are crucial for the cleavage of C-O BBs and formation of deoxygenated compounds, particularly arenes.
研究领域:
化学工程
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催化科学
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产品关联
DOI
高影响因子
JOURNAL OF THE ENERGY INSTITUTE
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2025
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IF 6.2
Hao-Dong An,Guang-Hui Liu,Yan-Jun Li,Ling-Zhi Tuo,Yu-Hong Kang,Zhi-Ping Wang,Yong Gao,Chen Shi,Yun-Yan Gao,Xian-Yong Wei
Hydrofining of low-grade lignite liquefied oils into high-density liquid fuels is a critical pathway for their value-added utilization. However, abundant condensed aromatic rings (ARs) and O atoms in such crude oils pose significant challenges for secondary upgrading, particularly in achieving concurrent AR hydrogenation and hydrodeoxygenation in one-pot to produce alkyl cyclanes. In view of this, Co-CoN x @C 650 was constructed by a cascade preparation strategy consisting of in-situ co-pyrolysis and NH 3 nitridation. It has highly dispersed Co-CoN x dual-sites and carbon substrate with abundant defects/vacancies, and exhibits good performance in AR hydrogenation and hydrodeoxygenation. In addition, this catalyst can effectively activate H 2 and promote the synergistic transfer of H ··· H, δ+ H ··· H δ− , and H · . Good accessibility, cyclic stability, and renewability make it suitable for the hydrogenation of medium/large-sized molecules such as naphth-2-ol and aryl ethers into cyclanes. The liquefied oil (SP TD ) from Dongming lignite thermal dissolution in n -hexane is rich in aromatics (76.1 %), while refined oil (CHSP TD ) from catalytic hydrofining over Co-CoN x @C 650 is rich in saturated hydrocarbons (91.7 %), especially alkyl cyclanes (69.8 %). The efficient conversion of aromatic-oxygenated moieties demonstrated by Co-CoN x @C 650 provides a new solution for converting low-grade lignite liquefied oils into value-added cyclanes-rich liquid fuels.
研究领域:
能源化学
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催化材料科学
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高影响因子
ChemistrySelect
·
2023
·Vol. 8
·期 43
·e202303563
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IF 2.1
Chong Liang,Wei Zhao,Xutang Liu,Fei Wang,Zhijie Jiang
Graphical This attractive work examines the changes in CAs selectivity when lignite is oxidized by H 3+n [PMo 12-n V n O 40 ] (HPA-n, n=1-5) and discloses the catalytic mechanism of HPA. The catalytic process of HPA follows the electron transfer-oxygen transfer (ET-OT) mechanism, where it not only activates lignite through electron transfer, but also activates oxygen, leading to the generation of active substance ⋅OH in water. The ⋅OH promotes the breakage of lignite. Although the oxidation of lignite has been extensively studied, the factors affecting the selectivity of carboxylic acids (CAs) are unclear. This attractive work examines the changes in CAs selectivity when lignite is oxidized by H 3+n [PMo 12-n V n O 40 ] (HPA-n, n=1-5) and discloses the catalytic mechanism of HPA. The results show that the selectivity of benzene polycarboxylic acids and acetic acid (AA) increases with increasing vanadium content of HPA-n, such as mellitic acid and benzenepentacarboxylic acid from 0.8 % and 3.0 % to 5.4 % and 16.2 %, respectively. Consequently, the differences in the concentration of HPA or H 2 SO 4 used to obtain optimal formic acid and AA yields confirm that the intrinsic properties of CAs calculated by Gaussian 09 can also affect their selectivity. HPA can not only activate lignite through electron transfer, but also further activate oxygen, leading to the generation of active substance ⋅OH in water. Consequentially, ⋅OH as the key reactive substance can promote the breakage of bridge bonds, side chains and condensed aromatic rings during HPA-catalyzed oxidation of lignite. Thus, the oxidation pathway of lignite over HPA is proposed. This work constructs a relationship between oxidation capacity and CAs selectivity and discloses the lignite oxidation pathway at the molecular level, which is a significant progress in HPA-catalyzed conversion of lignite.
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高影响因子
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