本文選題：生物質(zhì)油 + 乙酸自熱重整　； 參考：《成都理工大學(xué)》2017年碩士論文

【摘要】：氫能是一種清潔能源,被視為傳統(tǒng)化石能源的替代能源之一,并可通過醇類、生物質(zhì)以及纖維素等可再生原料制取。其中,生物質(zhì)來源廣泛、廉價(jià)易得,吸引了廣泛的關(guān)注。然而,生物質(zhì)能量密度較低,但經(jīng)熱裂解后可轉(zhuǎn)化為具有較高能量密度的生物質(zhì)油—一種碳中性的制氫原料。本文選擇生物質(zhì)油典型組分乙酸作為研究對(duì)象,同時(shí)在重整過程中引入氧氣,實(shí)現(xiàn)了乙酸自熱重整制取氫氣,并開發(fā)設(shè)計(jì)出生物質(zhì)油催化重整制氫的高效催化劑。針對(duì)鎳基催化劑所面臨的氧化、燒結(jié)以及積炭等問題,本文制備了La_(2-x)Ca_xNiO_(4±δ)鈣鈦礦結(jié)構(gòu)以及Ca_xNi_yAl_zO_δ類水滑石結(jié)構(gòu)(LDHs)催化劑,并通過一系列表征手段探討了助劑鈣以及制備方法對(duì)于催化劑結(jié)構(gòu)和性能的影響。采用溶膠凝膠法制備了La_(2-x)Ca_xNiO_(4±δ)催化劑�；钚詼y試結(jié)果表明:La_2NiO_(4±δ)和Ca_2NiO_(3±δ)催化劑在乙酸自熱重整反應(yīng)過程中穩(wěn)定性較差;Ca促進(jìn)的LaCaNiO_(4±δ)催化劑展現(xiàn)出高活性和穩(wěn)定性。在30 h的穩(wěn)定性測試中,LaCaNiO_(4±δ)催化劑的乙酸轉(zhuǎn)化率保持在100%,氫氣產(chǎn)率達(dá)到了2.80 mol-H_2/mol-AC。表征結(jié)果表明:用溶膠凝膠法制備出了具有鈣鈦礦結(jié)構(gòu)、分散性好以及粒徑小的LaCaNiO_(4±δ)催化劑;La被Ca部分取代后提高了催化劑的比表面積、鎳粒子的穩(wěn)定性,同時(shí)具有較強(qiáng)的抗積炭能力。采用共沉淀法制備了Ca_xNi_yAl_zO_δ-LDHs催化劑,并與Ni_xAl_yO_δ以及浸漬法制備的Ni_x/Ca_yAl_zO_δ催化劑進(jìn)行了比較。表征結(jié)果表明:用共沉淀法制備出了以CaAl-LDHs為前驅(qū)體的Ca_(2.55)Ni_(0.45)AlO_(4.5)催化劑;焙燒后,堿性載體CaO有助于抑制積炭,同時(shí)Ca_(12)Al_(14)O_(33)提高了鎳粒子的穩(wěn)定性;在ATR反應(yīng)過程中,該催化劑具有較好的抗氧化性、穩(wěn)定性以及抗積炭能力�；钚詼y試結(jié)果顯示Ca_(2.55)Ni_(0.45)AlO_(4.5)催化劑的乙酸轉(zhuǎn)化率保持在100%,氫氣產(chǎn)率穩(wěn)定在2.75mol-H_2/mol-AC。
[Abstract]:Hydrogen energy is a kind of clean energy, which is regarded as one of the alternative energy sources of traditional fossil energy, and can be made from renewable raw materials such as alcohols, biomass and cellulose. Among them, biomass has a wide range of sources, cheap and easy to obtain, attracting wide attention. However, biomass energy density is relatively low, but after pyrolysis, it can be converted into biomass oil with high energy density, which is a carbon-neutral raw material for hydrogen production. In this paper, acetic acid, a typical component of biomass oil, was selected as the research object, and oxygen was introduced into the reforming process to produce hydrogen by self-heating reforming of acetic acid, and an efficient catalyst for hydrogen production by catalytic reforming of biomass oil was developed. In this paper, La2-x CaxNiO4 鹵未 perovskite structure and CaxNiyAlzO未 hydrotalcite structure (LDHs) catalysts have been prepared to solve the problems of oxidation, sintering and coke deposition in nickel based catalysts. Through a series of characterization methods, the effects of the auxiliary calcium and the preparation method on the structure and performance of the catalyst were discussed. La2-x CaxNiO4 鹵未 catalyst was prepared by sol-gel method. The results of activity test showed that the LaCaNiO4 鹵未 and CaS _ 2NiO _ (3 鹵未) catalysts exhibited high activity and stability during the autothermal reforming of acetic acid with poor stability and Ca promoted LaCaNiO4 鹵未 catalyst. In the 30 h stability test, the acetic acid conversion of LaCaNiO4 鹵未 catalyst was kept at 100 and the hydrogen yield reached 2.80 mol-Hstack 2 / mol-AC. The results showed that LaCaNiO _ (4 鹵未) catalyst with perovskite structure, good dispersion and small particle size was prepared by sol-gel method, and La _ (4 鹵未) catalyst was partially replaced by Ca, which improved the specific surface area of the catalyst and the stability of nickel particles. At the same time, it has strong resistance to carbon deposition. Castax NixNixAlzO未 -LDHs catalysts were prepared by coprecipitation method, and compared with NixAlyO未 and Nix / CayAlzO未 catalysts prepared by impregnation method. The results showed that Ca2.55 Ni0.45 AlO4.5 catalyst was prepared by co-precipitation method, and Ca2.55Ni0.45AlO4.5 catalyst was prepared by coprecipitation method, and Cao can help to inhibit coke deposition, while Ca12Al14O33 can improve the stability of nickel particles during ATR reaction. The catalyst has good oxidation resistance, stability and resistance to carbon deposition. The results of activity test showed that the acetic acid conversion of Ca2.55 Ni0.45 AlO4.5 catalyst was kept at 100 and the hydrogen yield was stable at 2.75mol-H2pmol-AC.
【學(xué)位授予單位】：成都理工大學(xué)
【學(xué)位級(jí)別】：碩士
【學(xué)位授予年份】：2017
【分類號(hào)】：O643.36;TQ116.2

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相關(guān)期刊論文 前8條

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本文編號(hào)：2098474