摻雜改性及載體對(duì)鎳基鈣鈦礦催化劑氨分解性能的影響
發(fā)布時(shí)間:2018-06-10 15:40
本文選題:氨分解 + 制氫; 參考:《天津大學(xué)》2015年碩士論文
【摘要】:氫能因以反應(yīng)產(chǎn)物無(wú)污染、可重復(fù)利用、制備工藝成熟、燃燒值高等優(yōu)點(diǎn)而成為作新能源替代化石能源的首選。質(zhì)子交換膜燃料電池(PEMFC)以高純氫氣作為燃料,設(shè)備質(zhì)量輕、效率高,在電動(dòng)汽車(chē)及各種可移動(dòng)設(shè)備的動(dòng)力電源方面具有潛在的應(yīng)用前景。氨儲(chǔ)氫密度高、易液化、價(jià)格低廉、生產(chǎn)和運(yùn)輸?shù)燃夹g(shù)成熟、分解后氫氣濃度高且無(wú)COx生成等優(yōu)點(diǎn),滿足PEMFC對(duì)氫源的要求。但氨分解制氫因反應(yīng)溫度高(完全分解溫度為700℃,甚至更高)、催化劑價(jià)格較高,影響推廣使用。LaNiO_3具有鈣鈦礦結(jié)構(gòu),熱穩(wěn)定性高、氧化還原能力強(qiáng)、成本低廉,在催化領(lǐng)域有廣泛的應(yīng)用。本文采用溶膠凝膠法,制備了鈣鈦礦型復(fù)合氧化物系列催化劑,分析摻雜改性對(duì)鈣鈦礦催化氨分解性能的影響。采用不同的擴(kuò)孔劑制備MCM-41,并將其作為載體,制備負(fù)載型鈣鈦礦催化劑。具體研究?jī)?nèi)容如下:首先,本文制備了一系列鈣鈦礦型La_(0.9)X_(0.1)NiO_3(X=Li、Na、K、Ba)催化劑,采用氨分解活性評(píng)價(jià)以及TPR、XRD等表征,篩選出最佳的A位摻雜元素和摻雜量,實(shí)驗(yàn)結(jié)果表明最佳摻雜元素為Ba,最佳摻雜量為x=0.1。其次,改變?nèi)軇┲苽淞薒a_(0.9)Ba_(0.1)NiO_3催化劑,考察溶劑對(duì)催化氨分解性能的影響,發(fā)現(xiàn)使用有機(jī)溶劑可以很好地制備出具有單一鈣鈦礦物相結(jié)構(gòu)的催化劑,但氨分解催化活性差,分析認(rèn)為,完美的晶格結(jié)構(gòu)減弱了催化活性。再次,在合成MCM-41過(guò)程中添加擴(kuò)孔劑(三乙胺、均三甲苯、正癸烷),XRD、TEM、BET表征結(jié)果表明,以三乙胺為擴(kuò)孔劑制備的樣品MCM-41,有規(guī)整的介孔結(jié)構(gòu),孔體積和比表面積都較大。最后,分別以基本型和擴(kuò)孔型MCM-41為載體,制備La_(0.9)Ba_(0.1)NiO_3/MCM-41(w(NiO)=20%)負(fù)載型催化劑,發(fā)現(xiàn)以擴(kuò)孔型MCM-41為載體的La_(0.9)Ba_(0.1)NiO_3/MCM-41催化劑活性較好,在596℃可獲得100%的氨分解轉(zhuǎn)化率,比非負(fù)載的La_(0.9)Ba_(0.1)NiO_3氨完全分解溫度降低了50℃左右。
[Abstract]:Hydrogen energy has become the first choice to substitute fossil energy for new energy because of its advantages of non-pollution, reusable, mature preparation process and high combustion value. Proton exchange membrane fuel cell (PEMFC) uses high purity hydrogen as fuel with light weight and high efficiency. It has potential application prospect in power supply of electric vehicles and all kinds of mobile devices. Ammonia has the advantages of high density of hydrogen storage, easy liquefaction, low price, mature technology of production and transportation, high concentration of hydrogen after decomposition and no production of COx, which can meet the requirements of PEMFC for hydrogen sources. However, due to the high reaction temperature (700 鈩,
本文編號(hào):2003730
本文鏈接:http://sikaile.net/kejilunwen/huaxuehuagong/2003730.html
最近更新
教材專著