Language：Japanese   Publishing type：Research paper (scientific journal)  

DOI： 10.1627/jpi.67.52

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Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cattod.2023.114408

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Publishing type：Research paper (scientific journal)   Publisher：Informa UK Limited  

DOI： 10.1080/00219592.2023.2269226

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Language：Japanese   Publishing type：Research paper (scientific journal)   Publisher：東京 : 石油学会 ; 1978-  

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Authorship：Lead author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/acs.iecr.3c00536

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Authorship：Lead author,　Corresponding author   Publishing type：Research paper (scientific journal)  

DOI： 10.1007/s10563-022-09377-5

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1007/s10563-022-09379-3

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Authorship：Corresponding author   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cattod.2022.06.042

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Authorship：Lead author   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.jcou.2021.101707

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Authorship：Lead author   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cattod.2020.04.007

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Authorship：Last author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.apcata.2021.118152

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Authorship：Lead author   Publishing type：Research paper (scientific journal)  

DOI： 10.1627/jpi.63.297

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Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cej.2018.10.140

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Authorship：Corresponding author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cej.2018.10.213

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Authorship：Lead author,　Corresponding author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1252/jcej.18we251

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1627/jpi.62.319

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.cattod.2017.08.018

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Other Link： http://orcid.org/0000-0002-1191-4874

Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/ef402484u

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Other Link： http://orcid.org/0000-0002-1191-4874

Language：Japanese   Publishing type：Doctoral thesis  

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Authorship：Lead author   Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1016/j.fuel.2012.12.010

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Other Link： http://orcid.org/0000-0002-1191-4874

Language：English   Publishing type：Research paper (scientific journal)  

DOI： 10.1021/ie1005564

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Other Link： http://orcid.org/0000-0002-1191-4874

Authorship：Lead author   Publishing type：Article, review, commentary, editorial, etc. (scientific journal)  

J-GLOBAL

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Language：Japanese   Publisher：一般社団法人 日本エネルギー学会  

DOI： 10.20550/jietaikaiyoushi.29.0_86

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J-GLOBAL

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J-GLOBAL

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Authorship：Lead author   Language：Japanese   Publishing type：Article, review, commentary, editorial, etc. (scientific journal)  

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Language：Japanese   Publishing type：Article, review, commentary, editorial, etc. (scientific journal)  

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J-GLOBAL

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Language：Japanese  

CiNii Books

J-GLOBAL

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Language：Japanese   Publisher：The Japan Institute of Energy  

<p>Hydrogenolysis reaction is one of the important reactions to convert lignin into valuable aromatic chemicals. High-pressure hydrogen atmosphere is usually required for hydrogenolysis reaction, which causes high cost of hydrogen transportation and difficulty in handling. Thus we have focused on &quot;in-situ hydrogenolysis&quot; in which both hydrogen production by decomposition of alcohol solvent and hydrogenolysis of the reactant with the hydrogen produced in-situ occur simultaneously. We performed in-situ hydrogenolysis of benzofuran, which is a model compounds of decomposed lignin, in methanol solvent over Pt/Al₂O₃ catalyst. It was found that only furan moiety of benzofuran was hydrogenated and aromatic compounds like phenol were selectively obtained.</p>

DOI： 10.20550/jiebiomassronbun.12.0_135

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Language：Japanese   Publisher：日本エネルギー学会  

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

Low rank coals are susceptible to spontaneous combustion, but they must be heated over a critical temperature of around 70 ℃ before spontaneous combustion starts. This work focused on the adsorption of water vapor as a possible mechanism of the temperature increase up to the critical temperature. When the coals pre-dried and cooled to 38 ℃ were exposed to a saturated air at 38℃, the coal temperatures increased up to over 60℃ in a minute or so. This work showed that the rapid adsorption of water vapor will be a cause of temperature increase leading to the spontaneous combustion of low rank coals.

DOI： 10.20550/jiesekitanronbun.52.0_80

CiNii Books

J-GLOBAL

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Language：Japanese   Publisher：The Japan Institute of Energy  

Low rank coals including an Australian coal, Loy Yang, and biomass wastes were treated in solvents at 350℃. The solvent treatment deoxygenates the raw materials to produce upgraded solid products (abbreviated to STC or STB) containing 74 to 78 % C (d.a.f.) and hence having over 30 MJ value. In this work pyrolysis and gasification characteristics of STC/STB were examined by using the temperature programmed reaction (TPR) technique using TGA with detailed gas analysis. Pyrolysis of STC/STB was found to effective to obtain low oxygen content products. Gasification of STC/STB was effective to enhance the gasification rate of Soluble fraction constituting STC/STB.

DOI： 10.20550/jietaikaiyoushi.24.0_4

CiNii Books

J-GLOBAL

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Language：Japanese   Publisher：The Japan Institute of Energy  

Development of effective methods suppressing spontaneous combustion is one of biggest issues for utilizing abundant and valuable fossil fuels, low rank coals, more effectively all over the world. In this review report, a large number of works performed to evaluate the spontaneous combustion susceptibility of coals and to elucidate the mechanism by which spontaneous combustion take places were briefly reviewed. Progress of various sophisticated methods such as adiabatic calorimetry, cross point temperature method, pulse flow calorimetry, etc. have made it possible to predict the spontaneous combustion susceptibility of a specified coal rather accurately. Detailed studies utilizing modern analytical instruments including FTIR, XPS, ESR, and NMR have almost clarified the oxidation reaction path leading to the spontaneous combustion. It has been clarified that the formation of hydroperoxides from aliphatic C-H moiety and active radicals is the initial step of the spontaneous combustion. Decomposition of the hydro- peroxides and COOH functional groups are believed to be the following steps. Various factors such as humidity of air, oxidation history, and pyrolysis conditions in addition to inherent coal properties have been reported to affect the spontaneous combustion. Finally, the present status of several processes developed for suppressing the spontaneous combustion of low rank coals was introduced briefly.

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

We have developed a new effective method which realizes both dewatering and upgrading of low carbonaceous materials including biomass, peat, brown coals, and lignites by treating them in a non-polar solvent at temperatures below 350℃. For practical use, it is required to reduce energy for recovering solvent-soluble fraction, which we call "Soluble", from the solvent and to reduce the amount of solvent used. Then we have recently proposed an idea to overcome these problems, which users the solvent saturated with Soluble. It is necessary to understand the reactivity of Soluble at the temperatures around 350℃ for examining the validity of the idea. In this study, the pyrolysis of Soluble was carried out by using tubular autoclave and the thermal behavior of the solid product was investigated. It was found that decompostion of oxygen-containing functional groups and polymerization occured even at 350℃, which was caused by the high concentration of aliphatic carbons in Soluble. The thermal behavior of the solid product pyrolyzed at 400℃ was significantly different from Soluble.

DOI： 10.20550/jiesekitanronbun.51.0_6

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

The authors have recently proposed an upgrading method of low-rank coals in which low-rank coals are treated in a non-polar solvent at around 350℃ to produce upgraded coals containing a large amount of low-molecular-weight compounds with less oxygen content. In this study the solvent treatment method was applied to various types of low-grade carbonaceous resources such as biomass waste, peat, brown coal, and sub-bituminous coal. The method was effective for any of the low-grade resources, and the carbon contents of the upgraded products all converged on around 80% (daf). To further upgrade the coals, heat-treatments at around 400℃ under either mechanical or gaseous pressure were investigated. It was found that heat-treatment under mechanical pressure could alter the structural and thermal properties of a sub-bituminous coal (C: 79.6%-daf) to the properties which were close to coking coals'.

DOI： 10.20550/jietaikaiyoushi.22.0_8

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

The purposes of this study are to examine the mechanism in detail and to formulate the rate of the low temperature oxidation of coal. To do so, weight change, gas formation rates, and heat generation rates were measured respectively by using a sensitive thermobalance, a micro gas chromatograph, and a differential scanning calorimeter during the oxidation of low rank coals below 300 ℃. Furthermore, the fate of the functional groups on the coal surface was also observed by using an in-situ FT-IR spectrometer. In-situ FT-IR measurement clearly showed that the aliphatic carbons were first oxidized to form carboxyl groups above 140 ℃, further oxidized to form esters below 260 ℃, and then converted to anhydrides below 300 ℃. Based on the thermogravimetric data and heat generation rate measurements, both the oxidation rate constants and the enthalpy of reaction at the initial stage of oxidation were successfully formulated, and the possibility of estimating the initiation of self-ignition using the rate constants and the enthalpy of reaction was examined.

DOI： 10.20550/jietaikaiyoushi.22.0_2

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

To use low grade carbonaceous resources, such as brown coal and biomass, efficiently, dewatering, increasing heating value, and suppressing self-ignition tendency are required. We have found that the low-molecular-weight compounds obtained by treating low rank coal in non-polar solvent at around 350℃ had the low self-ignition tendency because of their small pore surface area. However, the self-ignition tendency of the entire solvent treated coal(STC)was still slightly higher than that of raw coal. In this study, hot-press briquetting method was employed to reduce pore surface area of low rank coal and STC. It was found that the samples prepared by hot-press briquetting from raw coal had small pore surface area than the raw coal and the coal pyrolyzed under normal pressure, and the self-ignition tendency decreased with the increase of treatment pressure. The samples prepared by hot-press briquetting from the STC at around 250℃ also had small pore surface area and low self-ignition tendency than the STC.

DOI： 10.20550/jietaikaiyoushi.21.0_22

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

Low rank coals are abundantly deposited and widely distributed, although they have not been used on a large scale except at the mining sites because of their high water content and oxygen content, and because of the high possibility of self-ignition when dewatered. Therefore, treatment for both dewatering low rank coals and suppressing their self-ignition tendency as well as increasing their heating value is essential. In this study, the possibility of the degradative solvent treatment, which treats coals in a non-polar solvent at 350℃, was examined as the method for self-ignition suppression, and the factors influencing self-ignition tendency was discussed.

DOI： 10.20550/jiesekitanronbun.49.0_6

CiNii Books

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Language：Japanese   Publisher：The Japan Institute of Energy  

We have recently presented a novel method which can not only dewater but upgrade low rank coals under mild conditions. This method consists of treatment of coals in non-polar solvents, such as 1-methylnaphthalene, at temperatures below 350℃. One of the remaining problems to be solved for this method is whether it can suppress self-ignition of low rank coals. In this study, self-ignition tendencies were examined for the samples prepared from an Australian brown coal by the proposed method. It was found that the treated coal obtained from this method contained little water and had the heating value corresponding to high rank coal. The self-ignition tendency of the extracted fractions was remarkably suppressed due to their small pore surface area which minimizes oxygen access to them. The self-ignition tendency of the solvent treated coal was smaller than the pyrolyzed coal, which was caused by the coating of the extracted fractions. However, the self-ignition tendency of the solvent treated coal was still slightly higher than that of raw coal.

DOI： 10.20550/jietaikaiyoushi.20.0_22

CiNii Books

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Language：English  

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Language：Japanese   Publisher：The Japan Institute of Energy  

Mild oxidation of brown coal at relatively low temperature was examined as one of the methods to suppress the spontaneous combustibility of the brown coal. Two brown coals were heated up to 260, 280 or 300 °C in a helium stream containing 22 % oxygen and kept for 0 - 120 min. Pyrolysis was also tested for comparison purpose, in which the coals were heated to 300, 400 or 500 °C in a helium stream and kept for 10 min. The spontaneous combustibility of the treated coals was evaluated by gasification rate of the coals measured in 22 % oxygen-containing helium at elevated temperature or the amount of oxygen adsorbed on the coals from gaseous oxygen at 100 °C. The gasification rate of the coals treated by low temperature oxidation was lowered with the increase of gaseous oxygen consumption during the treatment, suggesting that spontaneous combustibility of the coals was successfully suppressed by the treatment. Pyrolysis treatment, on the other hand, had little effect on spontaneous combustibility. In-situ FT-IR analysis showed that aliphatic C-H groups of the coal were selectively oxidized to form esters, anhydrides, or CO_2 during low temperature oxidation.

DOI： 10.20550/jiesekitanronbun.47.0_122

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Language：Japanese   Publisher：公益社団法人 化学工学会  

DOI： 10.11491/scej.2010f.0.111.0

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Event date： 2021.8

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Low rank coals are abundantly deposited and widely distributed, although they have not been used on a large scale except at the mining sites because of their high water content and oxygen content, and because of the high possibility of self-ignition when dewatered. Therefore, treatment for both dewatering low rank coals and suppressing their self-ignition tendency as well as increasing their heating value is essential. In this study, the possibility of the degradative solvent treatment, which treats coals in a non-polar solvent at 350℃, was examined as the method for self-ignition suppression, and the factors influencing self-ignition tendency was discussed.

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Language：Japanese   Presentation type：Oral presentation (general)  

To use low grade carbonaceous resources, such as brown coal and biomass, efficiently, dewatering, increasing heating value, and suppressing self-ignition tendency are required. We have found that the low-molecular-weight compounds obtained by treating low rank coal in non-polar solvent at around 350℃ had the low self-ignition tendency because of their small pore surface area. However, the self-ignition tendency of the entire solvent treated coal(STC)was still slightly higher than that of raw coal. In this study, hot-press briquetting method was employed to reduce pore surface area of low rank coal and STC. It was found that the samples prepared by hot-press briquetting from raw coal had small pore surface area than the raw coal and the coal pyrolyzed under normal pressure, and the self-ignition tendency decreased with the increase of treatment pressure. The samples prepared by hot-press briquetting from the STC at around 250℃ also had small pore surface area and low self-ignition tendency than the STC.

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Although the deposits of low rank coals such as brown coal or lignite are huge and widely distributed in the world, they have been just utilized only near coal mines for power generation. This is because the heating value of the coal is very low due to high moisture and oxygen contents and because the coal can neither be stored nor transported due to its high self-ignition tendency especially when dewatered. It is therefore essential to suppress the self-ignition tendency as well as to dewater and upgrade for effective utilization of the low rank coal. We have been proposing a new method effective for simultaneous dewatering and upgrading of brown coal. The method treats the coal in a non-polar solvent at around 350°C and separates the coal into upgraded, clean, and low-molecular extract and residue. We call this method degradative solvent extraction of brown coal. In this work the possibility of the application of the method for suppressing the self-ignition tendency was examined from fundamental aspects. It was found that the self-ignition tendency of an extract from a brown coal was much smaller than that of the raw coal. This was mainly because the extract softens and melts wh

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Language：English   Presentation type：Oral presentation (general)  

Recently, we proposed degradative solvent extraction at around 350°C as an efficient upgrading method of low rank coals. In this study, eight low rank coals including lignites and sub-bituminous coals were thermally treated and fractionated by using 1-methylnaphthalene as solvent at 350°C. The coals were partly decomposed and were separated into three fractions having different molecular weights. The yields of the three fractions respectively ranged from 17wt% to 27wt% (soluble), 4 wt% to 17 wt% (deposit), and 47 wt% to 64 wt% (residue; upgraded coal) on d.a.f. coal basis. The total higher heating value (HHV) of the fractions (sum of HHV of soluble, deposit and residue on raw coal basis) was not lost. The carbon contents of the three fractions were much larger than those of their parent coals, suggesting that significant amount of oxygen was effectively removed from the coals during the treatment. The interesting findings were that the solubles and deopsits obtained from the eight coals were respectively very close to each other in elemental composition, chemical structure, molecular weight distribution, pyrolysis behavior, and thermal plastic behavior. Thus, the proposed degrada

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Mild oxidation of brown coal at relatively low temperature was examined as one of the methods to suppress the spontaneous combustibility of the brown coal. Two brown coals were heated up to 260, 280 or 300 °C in a helium stream containing 22 % oxygen and kept for 0 - 120 min. Pyrolysis was also tested for comparison purpose, in which the coals were heated to 300, 400 or 500 °C in a helium stream and kept for 10 min. The spontaneous combustibility of the treated coals was evaluated by gasification rate of the coals measured in 22 % oxygen-containing helium at elevated temperature or the amount of oxygen adsorbed on the coals from gaseous oxygen at 100 °C. The gasification rate of the coals treated by low temperature oxidation was lowered with the increase of gaseous oxygen consumption during the treatment, suggesting that spontaneous combustibility of the coals was successfully suppressed by the treatment. Pyrolysis treatment, on the other hand, had little effect on spontaneous combustibility. In-situ FT-IR analysis showed that aliphatic C-H groups of the coal were selectively oxidized to form esters, anhydrides, or CO_2 during low temperature oxidation.

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Language：Japanese   Presentation type：Oral presentation (general)  

Efficient utilization methods of low rank coals must realize not only dewatering and upgrading but suppressing self-ignition tendency of low rank coals. The authors have recently proposed a novel method to dewater and to upgrade low rank coals. The method treats coals in non-polar solvent, such as 1-methylnaphthalene (1-MN), at temperatures below 350℃. In this study, the possibility of this solvent treatment was examined as a method to suppress self-ignition tendency of low rank coals as well as to dewater and to upgrade them. It was found that the samples obtained from an Australian brown coal by the treatment in either 1-MN or subcritical water were almost free from water, and their heating values were higher than the heating value of the original coal. The values ware as high as 30 MJ/kg on the treated coal basis which corresponded to the heating values of subbituminous or bituminous coals. The self-ignition tendencies of the solvent treated coal and the water treated coal were slightly higher or almost same as the self-ignition tendency of the raw coal. These treated coals were separated into the extracted fraction and the residue at the treatment temperature to investigate t

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Language：Japanese   Presentation type：Oral presentation (general)  

We have recently presented a novel method which can not only dewater but upgrade low rank coals under mild conditions. This method consists of treatment of coals in non-polar solvents, such as 1-methylnaphthalene, at temperatures below 350℃. One of the remaining problems to be solved for this method is whether it can suppress self-ignition of low rank coals. In this study, self-ignition tendencies were examined for the samples prepared from an Australian brown coal by the proposed method. It was found that the treated coal obtained from this method contained little water and had the heating value corresponding to high rank coal. The self-ignition tendency of the extracted fractions was remarkably suppressed due to their small pore surface area which minimizes oxygen access to them. The self-ignition tendency of the solvent treated coal was smaller than the pyrolyzed coal, which was caused by the coating of the extracted fractions. However, the self-ignition tendency of the solvent treated coal was still slightly higher than that of raw coal.

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