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ACS Omega · 2023 · IF 4.1

Extraction of Humic Acids from Lignite and Its Use as a Biochar Activator

Huijin Li,Shuang Ding,Jie Yuan

Current research focuses on extracting humic acid (HA) compounds from low-rank coals to obtain high value-added products. In this study, HAs with high purity and low heavy metal content were obtained from lignite by combining acid pretreatment with hydrothermal treatment. Scanning electron microscopy, elemental analysis (EA), Fourier transform infrared (FTIR) spectroscopy, X-ray diffraction, and inductively coupled plasma optical emission spectrometry (ICP–OES) were used to analyze raw lignite and HAs. The effects of acid and hydrothermal treatments on the inorganic elements, functional groups, and yield of HAs were examined. The results showed that acid treatment reduced the ash content of lignite from 20 to 9%, and hydrothermal treatment increased the yield of HAs from 36 to 68%. The chemical properties of HAs exhibited an increase in molecular weight and improved aromaticity after acid and hydrothermal treatments. The results of ICP–OES analysis suggested that the combined method of acid and hydrothermal treatments resulted in a significant reduction of heavy metal elements in HAs. FTIR analysis confirmed the results and demonstrated that the extracted HA from nitric acid pretreated and hydrothermal generation of lignite PHA was rich in carboxyl and phenolic functional groups. PHA was applied to biochar as an activator for the adsorption of heavy metal ions. The experimental results showed that PHA was successfully loaded onto biochar and introduced a large number of functional groups, and the adsorption capacity of the modified biochar for Pb2+ was effectively improved.

研究领域: 环境科学 · 化学工程
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JOURNAL OF MOLECULAR LIQUIDS · 2023 · IF 6

Crucial role of sulfonated ionic liquids as promoter for efficient production of valuable carboxylic acids by H5PMo10V2O40-catalyzed aerobic oxidation of lignite

Chong Liang,Wei Zhao,Shangshang Ma,Dingkai Wang,Xutang Liu,Linyang Dong

To explore the effect of adding acidic ionic liquids (ILs) to the heteropoly acid/H 2 SO 4 catalytic system on the aerobic oxidation of lignite, acidic ILs functionalized with -SO 3 H were synthesized accordingly and mixed with H 5 PMo 10 V 2 O 40 (HPA-2) in various molar ratios. The optimum combination of HPA-2 and 1-methyl-3-(4-sulfobutyl) imidazolium (MIMBS) with molar ratio of 0.3 showed excellent performance for the catalytic oxidation of lignite, with the yields of carboxylic acids (CAs) (including benzene carboxylic acids, formic acid and acetic acid) reaching 326.21 ± 12.86 mg/g lignite, which considerably exceeded the 136.08 ± 6.23 mg/g lignite of pure HPA-2. Highest occupied molecular orbital energy of CAs calculated by Gaussian 09 on 6-31G(d) basis set and Hammett function analysis confirmed that the oxidative activity and acidity of the catalytic system could be moderately modulated by sulfonated ILs, thereby increasing the yield of CAs. In addition, the effect of H 2 SO 4 concentration on the oxidation of lignite was investigated via the HPA-2/H 2 SO 4 /MIMBS system with different molar ratios, and the results showed that CAs yield increased first and then decreased with increasing H 2 SO 4 concentration, but the concentration of H 2 SO 4 at the maximum yield of CAs was significantly reduced from 0.28 wt% to 0.14 wt% once MIMBS was added. A possible process for the catalytic oxidation of lignite by sulfonated ILs/HPA-2/H 2 SO 4 in aerobic aqueous solution is proposed, which generally involves the reactions of hydrolysis, oxidation and re-oxidation. Due to the good reproducibility, the robust homogeneous catalytic system of HPA-2/sulphonated ILs has the advantages of including increased yields of CAs and reduced H 2 SO 4 dosage, which will pave the way for the efficient utilization of lignite.

研究领域: 化学工程 · 能源化学
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FUEL · 2017 · IF 4.601

Difunctional nickel/microfiber attapulgite modified with an acidic ionic liquid for catalytic hydroconversion of lignite-related model compounds

Zhong-Qiu Liu,Xian-Yong Wei,Hai-Hong Wu,Wei-Tu Li,Yang-Yang Zhang,Zhi-Min Zong,Feng-Yun Ma,Jing-Mei Liu

Modified microfiber attapulgite (MFA)-supported nickel was prepared by thermally decomposing nickel tetracarbonyl on MFA modified with an acidic ionic liquid (AIL, 1-sulfobutyl-3-methylimidazolium trifluoromethanesulfonate). It was characterized with multiple instruments and used for catalyzing hydroconversion of lignite-related model compounds (LRMCs) oxydibenzene, benzyloxybenzene, and oxybis(methylene)dibenzene. The results indicate that Ni 15% /MFA@AIL effectively catalyzes hydroconversion of the LRMCs to afford cyclanes by inducing the formation of H + , H − , and biatomic active hydrogen.

研究领域: 催化化学 · 能源材料化学
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ENERGY CONVERSION AND MANAGEMENT · 2019 · IF 7.181

Layered uniformly delocalized electronic structure of carbon supported Ni catalyst for catalytic reforming of toluene and biomass tar

Jie Ren,Jing-Pei Cao,Fei-Long Yang,Xiao-Yan Zhao,Wen Tang,Xin Cui,Qiang Chen,Xian-Yong Wei

Lignite rich in oxygen-containing species (OCSs) was employed as perfect ion-exchange material for high activity catalyst preparation. HCl treatment Shengli lignite (HSL) selectively removed the organic salt and improved capability of ion exchange. In this paper, highly desirable and layered carbon supported Ni catalyst was prepared by modified lignite. Thanks to the excellent role of Ni (1 1 1) plane and porous layered graphene-like delocalized electronic structure, specific structure of lignite provides an exchange platform in facilitating the Ni electron transfer during the catalytic reaction process. Ni loaded on HSL (Ni/HSL) showed the great catalytic activity and stability for reforming of toluene and biomass tar. Ni/HSL prepared at 650 °C shows the great activity and stability for toluene steam reforming (TSR) and biomass tar reforming (BTR). A series of instruments (XRD, SEM, TEM, H 2 -TPR, XPS, CO pulse adsorption, etc.) were employed for characterization. Based on these significant characterizations of catalyst, calculation of turnover frequency (TOF), and results of conversion of toluene and corncob tar. The results revealed the layered delocalized electronic structure of Ni/HSL, which has lower activation energy than other reported catalysts. Uniform dispersed catalyst was synthesized successfully for reforming of toluene and biomass tar.

CAS / MDL: 108-88-3
研究领域: 催化化学 · 材料科学
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SEPARATION AND PURIFICATION TECHNOLOGY · 2024 · IF 8.1

Kill two birds with one stone: Efficient leaching of germanium and recovery of lignite from germanium-rich lignite by thionyl chloride

Zhiyuan Zhang,Guixia Fan,Guoli Zhou,Daoguang Teng,Hongyan Nan,Peng Li,Yijun Cao,Jiongtian Liu

Germanium, a critical metal, is predominantly located in lignite and lead–zinc ore. The germanium was commonly extracted from the fly ash of germanium-rich lignite (GRL), however, facing the challenges of specific combustion conditions, low lignite’s thermal efficiency and value, high CO 2 emissions, and waste acid treatment. Therefore, in this work, a novel method for directly leaching germanium from the GRL was proposed, facilitating low-carbon extraction under mild conditions, and reducing lignite loss during leaching process. Results showed that leaching germanium from the GRL using thionyl chloride achieved the goals of “kill two birds with one stone”, i.e. , leaching efficiency of germanium above 95  wt % and recovery yield of lignite over 95  wt %. Specifically, the theoretical leaching efficiency of germanium reached 99.60  wt % while the recovery yield of lignite reached 86.35  wt %, at the temperature of 20 °C, liquid–solid ratio of 4 mL/g, and leaching time of 6 h. Most of the leached germanium was remained in the aqueous phase after the leaching solution was quenched, facilitating the subsequent separation of germanium. In this study, efficient extraction of germanium from the GRL was achieved with a high recovery yield of lignite, preserving the matrix structure and main composition of lignite. Therefore, this method provides a feasible way for efficient extraction of germanium from lignite with low-carbon emission under mild condition.

研究领域: 材料科学 · 环境科学
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CHEMICAL ENGINEERING JOURNAL · 2024 · IF 13.3

Lignite-derived carbonized polymer dots for oilfield tracers

Mingjin Du,Channa Wang,Yilin Zhu,Chao Ma,Jiangtao Wang,Gang Chang,Mengyu Sun,Tongsiliu Wu,Yu Xiao,Zheng Zhao,Junwei Su,Xiangdong Ding,Changsheng Xiang

Oilfield tracers are essential chemical additives in the petroleum extraction process, aiding in understanding reservoir flow characteristics, optimizing production strategies, and ultimately increasing oil recovery rates. Carbon dots (CDs), known for their tunable photoluminescent properties, ease of detection, and low toxicity, are considered promising candidates for the next generation of oilfield tracers. However, aqueous-phase oilfield tracers require CDs to possess good water solubility, high-temperature and high-salinity tolerance, low rock adsorption and detection limit, which renders many CDs unqualified for use. Currently, reports on CDs oilfield tracers are limited, with most being restricted to blue fluorescence, which has weak resistance to background fluorescence interference. In this work, by utilizing the rich organic content (17.5 wt%) of low-value lignite as a precursor, lignite-derived carbonized polymer dots (L-CPDs) exhibit green fluorescence with an absolute quantum yield (QY) of 19.78%. Comprehensive evaluations show L-CPDs offer good salt tolerance, thermal stability, and pH stability, with a detection limit reaching 1 ppb and no significant cytotoxicity. Additionally, the tracing behavior of L-CPDs is demonstrated using a microfluidic chip, highlighting their potential as alternatives to existing tracer products.

CAS / MDL: 107-15-3
研究领域: 石油工程 · 材料科学 · 环境科学
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NEW JOURNAL OF CHEMISTRY · 2020 ·Vol. 44 ·期 32 ·13755-13763 · IF 3.288

CO2 adsorption of lignite chars after one-step KOH activation

Xia Wang,Wulan Zeng,Wenjing Liu,Xiaoyu Cao,Chunhui Hou,Qi Ding,Yaxuan Lü

The design and development of low-cost sorbents is vital for CO2 capture from flue gases. In this study, the lignite char from Ordos coal (SE) was treated by a one-step KOH activation method to prepare microporous activated carbons for CO2 adsorption. The textural pore properties, surface functional groups and element contents of SE before and after activation were characterized and discussed; the effects of the mass ratio of KOH to SE, activation temperature and time, as well as the adsorption temperature on CO2 adsorption for prepared porous sorbents were investigated and optimized; the isosteric heat of adsorption and adsorption kinetics for the optimized sorbent were further calculated and fitted. When the mass ratio of KOH to SE was 1 : 1, the activation temperature and time were 700 °C and 120 min respectively, and the sorbent of K/SE700(120) showed an adsorption capacity of 1.35 mmol g−1 at 20 °C, which dropped by 2.96% after ten regenerations. The Langmuir adsorption isotherms fitted the adsorption data of K/SE700(120) well, and the isosteric heats of adsorption were 11–13 kJ mol−1, showing the physisorption characteristic. In addition, the good fit of the adsorption data to the Avrami model suggested that there are multiple adsorption routes for K/SE700(120).

CAS / MDL: 1310-58-3
研究领域: 环境科学 · 材料科学
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APPLIED BIOCHEMISTRY AND BIOTECHNOLOGY · 2019 ·Vol. 188 ·期 4 ·965-976 · IF 2.14

Biological Modification of Montan Resin from Lignite by Bacillus benzoevorans

Wang Huanhong,Qin Yi,Li Baocai,Xiang Cheng,Dai Weifeng,Jiao Shiyun,Zhang Mi

The montan resin (MR) is a solid waste produced during the industrial process of refined montan wax from lignite, and usually disposed by landfill and incineration, which easily cause environmental pollution and resource waste. Based its physicochemical properties, our study attempted to modify MR by Bacillus benzoevorans to achieve ecological utilization of MR. As results, the weight loss rate of MR, expressed as modification degree, was found to increase with the increase of B. benzoevorans -incubated time. The apparent oil–water partition coefficient ( K ow), used to evaluate the improvement on hydrophilicity of MR, significantly increased ( P  < 0.01) after modification. IR analysis showed the functional groups of –OH and C=O in modified MR were more than those in MR. Meanwhile, comparison of the chemical changes between MR and modified MR by relatively quantitative analysis of gas chromatography–mass spectrometry (GC-MS) revealed that the content of some chemical components in the latter decreased, and the newly appeared chemical components all had more oxygen-containing functional groups. The bioactivity of the modified MR in agricultural application was evaluated regarding germination and seedling growth of maize seed preliminarly. Compared with the original MR-treated group, the modified MR showed an obvious effect on promoting the growth and germination of maize .

CAS / MDL: 629-59-4
研究领域: 环境科学 · 微生物学 · 农业科学
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FUEL · 2019 · IF 5.128

Catalytic hydroconversion of Yinggemajianfeng lignite over difunctional Ni-Mg2Si/γ-Al2O3

Xue-Ke Li,Zhi-Min Zong,Yi-Feng Chen,Zheng Yang,Guang-Hui Liu,Fang-Jing Liu,Xian-Yong Wei,Bao-Jun Wang,Feng-Yun Ma,Jing-Mei Liu

A highly active difunctional Ni-Mg 2 Si/γ-Al 2 O 3 was prepared by thermally decomposing nickel tetracarbonyl onto γ-Al 2 O 3 impregnated with Mg 2 Si. The non-catalytic hydroconversion (NCHC) and catalytic hydroconversion (CHC) of the extract ( E ) and extraction residue (ER) from Yinggemajianfeng lignite were investigated over Ni-Mg 2 Si/γ-Al 2 O 3 at 240 °C in n -hexane. Benzyloxybenzene and oxybis(methylene)dibenzene were used as lignite-related model compounds to speculate the possible mechanisms for the catalytic hydrocracking and hydrogenation over Ni-Mg 2 Si/γ-Al 2 O 3 . As a result, more organic matter in ER was converted to soluble portion (SP) by the CHC than by the NCHC. The main SP from the CHC are chain alkanes and cyclanes, while that from the NCHC is rich in arenes and oxygen-containing organic compounds. The results indicate that Ni-Mg 2 Si/γ-Al 2 O 3 effectively catalyze the hydrocracking of >C alk –O– linkages and the hydrogenation of aromatic rings in E and ER.

CAS / MDL: 22831-39-6
研究领域: 化学工程 · 能源科学
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INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH · 2012 · IF 2.237

Production of Benzene Polycarboxylic Acids from Lignite by Alkali-Oxygen Oxidation

Wenhua Wang,Yucui Hou,Weize Wu,Muge Niu,Weina Liu

The oxidation of coal to produce high-valued benzene polycarboxylic acids (BPCAs), which are obtained currently from diminishing petroleum reserves, is a promising industrial process of the future. Up to now, the yield distribution of BPCAs has not been studied in detail and the mechanism of coal oxidation to BPCAs remains unclear. In this study, Huolinhe lignite was oxidized in a batch reactor by alkali-oxygen oxidation. All 12 kinds of BPCAs obtained were quantified by a new established method. Effects of alkali/coal mass ratio, reaction temperature, initial oxygen pressure, and reaction time on the yield distribution of BPCAs were studied for the first time. The results indicate that BPCAs with four or five carboxyls are the predominant products, and BPCAs with one or two carboxyls are formed in a relatively short time; moreover, the formation of BPCAs with more carboxyls is relatively more sensitive to the salting out effect. CP/MAS 13C NMR spectra and oxidation of model compounds show that phenolic, ether-substituted aromatic, ether, and aldehyde groups are easily converted and that water-soluble acids (WSA) are formed rapidly and largely due to the breakage of these bonds. The step from WSA to BPCAs is relatively slow mainly due to the inertia of the aromatic clusters with attached carboxyls or carboxylate. On the whole, the BPCAs are derived from aromatic clusters through the oxidation of condensed benzene rings, bridges, or peripheral groups that are attached to the aromatic clusters. Possible mother units for BPCAs in the lignite are suggested based on the generally agreed lignite structure.

研究领域: 化学工程 · 煤炭化学
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FUEL · 2018 · IF 4.908

Catalytic hydroconversion of Yiwu lignite over solid superacid and solid superbase

Zhong-Qiu Liu,Xian-Yong Wei,Fang-Jing Liu,Guang-Hui Liu,Zhi-Min Zong

Trifluoromethanesulfonic acid supported on attapulgite powder (TFMSA/AP) and Mg 2 Si/γ-Al 2 O 3 were facilely prepared by impregnating TFMSA onto AP and Mg 2 Si onto γ-Al 2 O 3 . The extraction residue from Yiwu lignite (YL ER ) was subjected to non-catalytic hydroconversion (NCHC) and catalytic hydroconversion (CHC) over TFMSA/AP and Mg 2 Si/γ-Al 2 O 3 , respectively. Detailed molecular compositions of the soluble portions from the NCHC (SP NCHC ) and CHC over TFMSA/AP (SP CHC-A ) and Mg 2 Si/γ-Al 2 O 3 (SP CHC-B ) were characterized with a gas chromatograph/mass spectrometer. As a result, the yields of SP CHC-A and SP CHC-B are 19.6% and 17.5%, respectively, which are much higher than that of SP NCHC (1.04%), suggesting that both TFMSA/AP and Mg 2 Si/γ-Al 2 O 3 show excellent activity for the CHC of YL ER . Arenes and arenols are predominant in SP CHC-A and SP CHC-B , respectively, while large amounts of alkanoates were detected in SP NCHC . The results indicate that TFMSA/AP effectively catalyzes the cleavage of C ar –C alk and C alk –O bridged bonds (BBs) in YL ER , while Mg 2 Si/γ-Al 2 O 3 significantly promotes the cleavage of C–O BBs in YL ER . Di(1-naphthyl)methane, 1-methylnaphthalene, oxydibenzene, and benzyloxybenzene were used as coal-related model compounds (CRMCs) for the CHC to further explore the catalysis of TFMSA/AP and Mg 2 Si/γ-Al 2 O 3 . The results show that TFMSA/AP not only releases mobile H + but also heterolytically splits H 2 to form an immobile H − and a mobile H + , leading to the cleavage of C alk –C ar and C alk –O BBs in the CRMCs. In contrast, Mg 2 Si/γ-Al 2 O 3 facilitates heterolytically splitting H 2 to an immobile H + and a mobile H − , resulting in the cleavage of C–O BBs in the CRMCs.

CAS / MDL: 1344-28-1 1493-13-6
研究领域: 化学工程 · 煤炭化学
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FUEL · 2025 · IF 7.5

Efficient conversion of cellulose to glucose using lignite-derived solid acid catalyst

Renjie Yang,Genmao Guo,Pengfei Chen,Yang Yang,Fangming Jin

Cellulosic biomass, as the most abundant renewable resource on Earth, holds great potential for achieving carbon neutrality through efficient valorization, where its hydrolysis to glucose represents a critical initial step. Conventional methods relying on homogeneous acids face limitations such as poor catalyst recycling and significant environmental issues. Carbon-based solid acids (CSAs) for cellulose hydrolysis have emerged as promising alternative, yet, their synthesis often requires high-temperature calcination to construct stable aromatic frameworks, leading to complex and energy-intensive processes. In this study, we propose a novel approach of utilizing the inherent aromatic structure of lignite for synthesizing lignite-derived solid acids (LSAs). We found that lignite was successfully sulfonated directly at low temperature without prior calcination. The synthesized LSAs which possess abundant sulfonic and weak acid sites, proved rapid and efficient hydrolysis of cellulose, resulting in high glucose yield of 57.4 % in just 45 min at 190 °C. In situ Fourier-transform infrared (FTIR) analysis further revealed the weakening of hydrogen bonds and cleavage of glycosidic bonds in cellulose facilitated by LSAs. This work provides a sustainable and low-carbon way for the integrated valorization of lignite and cellulosic biomass.

CAS / MDL: 7664-38-2 9005-25-8
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