JP5170516B2 - Method for producing hydrogen gas - Google Patents
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- JP5170516B2 JP5170516B2 JP2007181827A JP2007181827A JP5170516B2 JP 5170516 B2 JP5170516 B2 JP 5170516B2 JP 2007181827 A JP2007181827 A JP 2007181827A JP 2007181827 A JP2007181827 A JP 2007181827A JP 5170516 B2 JP5170516 B2 JP 5170516B2
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- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 title claims description 32
- 238000004519 manufacturing process Methods 0.000 title claims description 15
- 239000001913 cellulose Substances 0.000 claims description 18
- 229920002678 cellulose Polymers 0.000 claims description 18
- 239000000843 powder Substances 0.000 claims description 9
- 239000002028 Biomass Substances 0.000 claims description 7
- 238000002156 mixing Methods 0.000 claims description 7
- 239000000463 material Substances 0.000 claims description 6
- AXCZMVOFGPJBDE-UHFFFAOYSA-L calcium dihydroxide Chemical compound [OH-].[OH-].[Ca+2] AXCZMVOFGPJBDE-UHFFFAOYSA-L 0.000 claims description 4
- 239000000920 calcium hydroxide Substances 0.000 claims description 4
- 229910001861 calcium hydroxide Inorganic materials 0.000 claims description 4
- 239000010794 food waste Substances 0.000 claims description 3
- 239000000203 mixture Substances 0.000 claims description 3
- BFDHFSHZJLFAMC-UHFFFAOYSA-L nickel(ii) hydroxide Chemical compound [OH-].[OH-].[Ni+2] BFDHFSHZJLFAMC-UHFFFAOYSA-L 0.000 claims description 3
- 239000010893 paper waste Substances 0.000 claims description 3
- 238000010298 pulverizing process Methods 0.000 claims description 3
- 239000010801 sewage sludge Substances 0.000 claims description 3
- 239000002699 waste material Substances 0.000 claims description 3
- 210000003608 fece Anatomy 0.000 claims 1
- 239000010871 livestock manure Substances 0.000 claims 1
- 238000005303 weighing Methods 0.000 claims 1
- CURLTUGMZLYLDI-UHFFFAOYSA-N Carbon dioxide Chemical compound O=C=O CURLTUGMZLYLDI-UHFFFAOYSA-N 0.000 description 10
- 229910052739 hydrogen Inorganic materials 0.000 description 10
- 239000001257 hydrogen Substances 0.000 description 10
- UGFAIRIUMAVXCW-UHFFFAOYSA-N Carbon monoxide Chemical compound [O+]#[C-] UGFAIRIUMAVXCW-UHFFFAOYSA-N 0.000 description 5
- 239000011575 calcium Substances 0.000 description 5
- 239000001569 carbon dioxide Substances 0.000 description 5
- 229910002092 carbon dioxide Inorganic materials 0.000 description 5
- 229910002091 carbon monoxide Inorganic materials 0.000 description 5
- 239000007789 gas Substances 0.000 description 5
- 238000000034 method Methods 0.000 description 5
- PXHVJJICTQNCMI-UHFFFAOYSA-N Nickel Chemical compound [Ni] PXHVJJICTQNCMI-UHFFFAOYSA-N 0.000 description 3
- 229910000831 Steel Inorganic materials 0.000 description 3
- 239000010959 steel Substances 0.000 description 3
- 239000002023 wood Substances 0.000 description 3
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 description 2
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 229910052799 carbon Inorganic materials 0.000 description 2
- 239000003054 catalyst Substances 0.000 description 2
- 238000006243 chemical reaction Methods 0.000 description 2
- 244000144972 livestock Species 0.000 description 2
- 239000002994 raw material Substances 0.000 description 2
- ODINCKMPIJJUCX-UHFFFAOYSA-N Calcium oxide Chemical compound [Ca]=O ODINCKMPIJJUCX-UHFFFAOYSA-N 0.000 description 1
- 238000004458 analytical method Methods 0.000 description 1
- 239000012736 aqueous medium Substances 0.000 description 1
- 230000015572 biosynthetic process Effects 0.000 description 1
- 230000003197 catalytic effect Effects 0.000 description 1
- 238000000354 decomposition reaction Methods 0.000 description 1
- 230000006866 deterioration Effects 0.000 description 1
- 230000000694 effects Effects 0.000 description 1
- 238000005516 engineering process Methods 0.000 description 1
- -1 for example Substances 0.000 description 1
- 238000000227 grinding Methods 0.000 description 1
- 238000010438 heat treatment Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-M hydroxide Chemical compound [OH-] XLYOFNOQVPJJNP-UHFFFAOYSA-M 0.000 description 1
- 238000004949 mass spectrometry Methods 0.000 description 1
- 229910052751 metal Inorganic materials 0.000 description 1
- 239000002184 metal Substances 0.000 description 1
- 230000007935 neutral effect Effects 0.000 description 1
- 229910052759 nickel Inorganic materials 0.000 description 1
- 238000004451 qualitative analysis Methods 0.000 description 1
- 238000011084 recovery Methods 0.000 description 1
- 238000004064 recycling Methods 0.000 description 1
- 238000012827 research and development Methods 0.000 description 1
- 239000007858 starting material Substances 0.000 description 1
- 238000003756 stirring Methods 0.000 description 1
- 239000000126 substance Substances 0.000 description 1
- 238000003786 synthesis reaction Methods 0.000 description 1
- 238000010792 warming Methods 0.000 description 1
- XLYOFNOQVPJJNP-UHFFFAOYSA-N water Chemical compound O XLYOFNOQVPJJNP-UHFFFAOYSA-N 0.000 description 1
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y02E50/00—Technologies for the production of fuel of non-fossil origin
- Y02E50/30—Fuel from waste, e.g. synthetic alcohol or diesel
-
- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P20/00—Technologies relating to chemical industry
- Y02P20/50—Improvements relating to the production of bulk chemicals
- Y02P20/52—Improvements relating to the production of bulk chemicals using catalysts, e.g. selective catalysts
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- Processing Of Solid Wastes (AREA)
- Treatment Of Sludge (AREA)
- Hydrogen, Water And Hydrids (AREA)
- Catalysts (AREA)
Description
本発明は、セルロースを含むバイオマスから水素ガスを製造する方法に関するものである。 The present invention relates to a method for producing hydrogen gas from biomass containing cellulose.
近年、地球温暖化など住環境が悪化する中で、「持続可能な循環型社会の実現」が人類社会に求められている。その基盤技術として、再生可能なエネルギーの創製、利用拡大に注目が集まっている。その中でも、賦存量、経済性、カーボンニュートラルの優位性などの視点で、バイオマスの果たす役割は大きい。バイオマスからのエネルギー回収については、エタノール合成などを含めて、多くの研究・技術開発が世界的に進められている。 In recent years, with the deterioration of the living environment such as global warming, “realization of a sustainable recycling society” is required of human society. Attention has been focused on creating and expanding the use of renewable energy as the fundamental technology. Among them, biomass plays a major role in terms of the existing amount, economic efficiency, and carbon neutral advantage. Regarding energy recovery from biomass, many research and technological developments are underway worldwide, including ethanol synthesis.
従来、バイオマスから水素ガスを製造する方法としては、例えば、木材を水蒸気あるいは空気と共に１０００℃の高温でガス化することで、水素と一酸化炭素との混合ガスとし、一酸化炭素を水素と二酸化炭素とに変換する方法が知られているが、１０００℃程度の高温の反応条件が必要である。 Conventionally, as a method for producing hydrogen gas from biomass, for example, wood is gasified with water vapor or air at a high temperature of 1000 ° C. to obtain a mixed gas of hydrogen and carbon monoxide, and carbon monoxide is converted to hydrogen and carbon dioxide. Although a method for converting to carbon is known, reaction conditions at a high temperature of about 1000 ° C. are necessary.
また、先行技術として、高圧力容器内で、水性媒体の存在下、水素を活性化する金属触媒を用いて、バイオマスを温度３００〜３７５度に加熱する方法が提案されている（例えば、特許文献１参照）。しかし、この方法では、高圧力容器やニッケル系触媒が必要で、水素ガス製造装置のコストが高価になるという問題点がある。 In addition, as a prior art, a method of heating biomass to a temperature of 300 to 375 degrees using a metal catalyst that activates hydrogen in the presence of an aqueous medium in a high-pressure vessel has been proposed (for example, Patent Documents). 1). However, this method requires a high-pressure vessel and a nickel-based catalyst, and there is a problem that the cost of the hydrogen gas production apparatus becomes expensive.
本発明の目的は、低コストなメカノケミカル処理を利用した、セルロースまたは高セルロース含有物からの水素ガスの製造方法を提供することにある。 An object of the present invention is to provide a method for producing hydrogen gas from cellulose or a high cellulose content using a low-cost mechanochemical treatment.
本発明によれば、バイオマスから水素ガスを製造する方法において、セルロースまたは高セルロース含有物の粉末と水酸化カルシウムの粉末と水酸化ニッケルの粉末とを所定量秤量し、該秤量物と複数の硬質ボールとを混合容器内に入れ、前記混合容器内で前記秤量物を所定時間混合粉砕し、粉砕後、該混合粉砕物を密封容器内で、３５０℃以上、４５０℃以下の温度に加熱保持し、発生した水素ガスを導出することを、特徴とする水素ガスの製造方法が得られる。
According to the present invention, in a method for producing hydrogen gas from biomass, a predetermined amount of cellulose or high cellulose-containing powder, calcium hydroxide powder, and nickel hydroxide powder are weighed, and the weighed material and a plurality of hard materials are weighed. A ball is placed in a mixing container, and the weighed product is mixed and pulverized for a predetermined time in the mixing container. After pulverization, the mixed pulverized product is heated and held at a temperature of 350 ° C. or higher and 450 ° C. or lower in a sealed container. A hydrogen gas production method characterized by deriving the generated hydrogen gas can be obtained.
また、本発明によれば、前記高セルロース含有物は、植物、植物から生産されたもの、古紙、家畜排せつ物、食品廃棄物、建築発生木材、または、下水汚泥を含む廃棄物であることを、特徴とする水素ガスの製造方法が得られる。なお、本発明の水素ガスの製造方法で、混合容器内での混合粉砕時間は、混合粉砕原料３ｇ当り２時間以下であることが好ましい。
Further , according to the present invention , the high cellulose-containing material is a plant, a product produced from a plant, waste paper, livestock excrement, food waste, building generated wood, or waste containing sewage sludge. A characteristic method for producing hydrogen gas is obtained. In the method for producing hydrogen gas of the present invention, the mixing and pulverizing time in the mixing vessel is preferably 2 hours or less per 3 g of the mixed and pulverized raw material.
本発明によれば、高圧力容器や１０００℃の高温処理を用いずに、低コストなメカノケミカル処理を利用した、セルロースまたは高セルロース含有物からの水素ガスの製造方法が得られる。 ADVANTAGE OF THE INVENTION According to this invention, the manufacturing method of the hydrogen gas from a cellulose or a high cellulose containing material using a low-cost mechanochemical process is obtained, without using a high pressure vessel or a 1000 degreeC high temperature process.
以下、本発明の実施の形態について図面を参照しながら説明する。
セルロースと水酸化カルシウムと水酸化ニッケルとの混合試料（重量３ｇ）を、メカノケミカル処理として、遊星ミルとスチールボールとを用いて混合粉砕し、処理粉末を加熱し、質量分析装置により評価し、発生ガスの定性分析を行った。水素発生の理論的反応式を式１に示す。Ni(OH)2は、水素発生の触媒的な働きを果たしているものと考えられる。
（式１）
C6(H2O)5 + 6Ca(OH)2 + 0.5Ni(OH)2 → 11.5H2 + 0.5Ni + 6CaCO3
Hereinafter, embodiments of the present invention will be described with reference to the drawings.
A mixed sample (weight 3 g) of cellulose, calcium hydroxide and nickel hydroxide is mixed and pulverized using a planetary mill and a steel ball as a mechanochemical treatment, the treated powder is heated, and evaluated by a mass spectrometer. Qualitative analysis of the generated gas was performed. The theoretical reaction formula for hydrogen generation is shown in Formula 1. Ni (OH) 2 is considered to play a catalytic role in hydrogen generation.
(Formula 1)
C 6 (H 2 O) 5 + 6Ca (OH) 2 + 0.5Ni (OH) 2 → 11.5H 2 + 0.5Ni + 6CaCO 3
図１は、セルロースと水酸化カルシウムとの混合物を２時間メカノケミカル処理し、それを質量分析装置で評価したときの、温度による発生ガスの変化結果を示す。図１から、Ca(OH)２を用いた場合は、温度によって段階的に水素以外に異なる気体も発生していることが確認できる。すなわち、セルロースとCa(OH)２とをメカノケミカル処理し、その後熱分解すると、３５０℃から４５０℃の温度範囲内で、安定な物質であるCaCO3が生成し、水素ガスが発生する。その後、さらに高温に熱すると、CaCO3が分解し、酸化カルシウム（CaO）になり、一酸化炭素（CO）と二酸化炭素（CO2）とが発生する。このように、水素と二酸化炭素とを異なる温度で発生させて分離することができる。 FIG. 1 shows the results of changes in generated gas with temperature when a mixture of cellulose and calcium hydroxide was mechanochemically treated for 2 hours and evaluated with a mass spectrometer. From FIG. 1, when Ca (OH) 2 is used, it can be confirmed that different gases other than hydrogen are generated stepwise depending on the temperature. That is, when cellulose and Ca (OH) 2 are mechanochemically treated and then pyrolyzed, CaCO 3 which is a stable substance is generated within a temperature range of 350 ° C. to 450 ° C., and hydrogen gas is generated. Thereafter, when heated to a higher temperature, CaCO 3 is decomposed into calcium oxide (CaO), and carbon monoxide (CO) and carbon dioxide (CO 2 ) are generated. Thus, hydrogen and carbon dioxide can be generated and separated at different temperatures.
図２は、メカノケミカル処理時間を変化させた場合の、混合粉砕粉末の水素ガス発生量の温度による変化の質量分析結果を示す。メカノケミカル処理時間として、遊星ミルとスチールボールとを使用せず、かき混ぜ用の棒で混合した場合（図２中の０ｍｉｎ）、遊星ミルとスチールボールとを用いて６０分間（６０ｍｉｎ）混合粉砕した場合、１２０分間（１２０ｍｉｎ）混合粉砕した場合の水素ガス発生量を調べた。図２から、メカノケミカル処理時間が長いほど水素発生量が多くなることが分かるが、メカノケミカル処理時間を１２０分間より延長しても更なる水素ガス発生はない。混合粉砕原料３ｇの分解反応が、１２０分間程度で完了したものと考えられる。 FIG. 2 shows a mass analysis result of a change in the amount of hydrogen gas generation of the mixed pulverized powder with temperature when the mechanochemical treatment time is changed. As a mechanochemical treatment time, when a planetary mill and a steel ball are not used but mixed with a stirring rod (0 min in FIG. 2), the planetary mill and the steel ball are mixed and ground for 60 minutes (60 min). In this case, the amount of hydrogen gas generated when mixing and grinding for 120 minutes (120 minutes) was examined. FIG. 2 shows that the longer the mechanochemical treatment time is, the more hydrogen is generated. However, even if the mechanochemical treatment time is extended beyond 120 minutes, no further hydrogen gas is generated. It is considered that the decomposition reaction of 3 g of the mixed pulverized raw material was completed in about 120 minutes.
なお、Ca(OH)２以外の水酸化物を使用しても、水素ガスが発生することが確認された。しかしながら、水素と二酸化炭素とがほぼ同じ温度で発生するため、水素と二酸化炭素との分離が困難である。 It was confirmed that hydrogen gas was generated even when a hydroxide other than Ca (OH) 2 was used. However, since hydrogen and carbon dioxide are generated at substantially the same temperature, it is difficult to separate hydrogen and carbon dioxide.
本実施の形態は、セルロースを出発原料として使用した実験結果について詳細に説明したが、セルロースを主成分とする植物、植物から生産されたもの、古紙、家畜排せつ物、食品廃棄物、建築発生木材、下水汚泥などの廃棄物でも同様の効果が得られることは明らかである。 In the present embodiment, the experimental results using cellulose as a starting material have been described in detail. Plants based on cellulose, those produced from plants, waste paper, livestock excrement, food waste, building-generated wood, It is clear that the same effect can be obtained with waste such as sewage sludge.
Claims (2)
セルロースまたは高セルロース含有物の粉末と水酸化カルシウムの粉末と水酸化ニッケルの粉末とを所定量秤量し、該秤量物と複数の硬質ボールとを混合容器内に入れ、前記混合容器内で前記秤量物を所定時間混合粉砕し、粉砕後、該混合粉砕物を密封容器内で、３５０℃以上、４５０℃以下の温度に加熱保持し、発生した水素ガスを導出することを、特徴とする水素ガスの製造方法。 In a method for producing hydrogen gas from biomass,
A predetermined amount of cellulose or high cellulose-containing powder, calcium hydroxide powder and nickel hydroxide powder are weighed, and the weighed material and a plurality of hard balls are placed in a mixing container, and the weighing is performed in the mixing container. The mixture is pulverized for a predetermined time, and after pulverization, the mixed pulverized product is heated and held in a sealed container at a temperature of 350 ° C. or higher and 450 ° C. or lower, and the generated hydrogen gas is derived. Manufacturing method.
The high cellulose-containing material is a plant, those produced from plants, waste paper, manure, food waste, building lumber originating, or that the waste containing sewage sludge, according to claim 1, wherein A method for producing hydrogen gas.
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| JP5572846B2 (en) * | 2010-02-23 | 2014-08-20 | 株式会社豊田中央研究所 | Energy gas production method and energy gas storage material |
| CN108212165B (en) * | 2018-01-19 | 2019-08-02 | 清华大学 | A kind of catalyst and preparation method thereof for biomass low temperature gasification high-purity hydrogen |
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| JP4364684B2 (en) * | 2004-03-17 | 2009-11-18 | 株式会社神戸製鋼所 | Method for producing gasified fuel |
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