本文主要研究内容
作者高丽慧（2019）在《粘土矿物催化生物质热解机理及生物炭吸附特性研究》一文中研究指出：生物质是我国储量丰富的绿色能源,生物质的高效利用是近年来广大科研工作者研究的热点问题。但目前生物质热解技术存在气体产率低、热解液体氧含量高及酸性大等问题。催化热解是增加气体产率,提高热解液体中高附加值产物的有效途径。常规合成类催化剂存在易失活、价格昂贵的问题,天然粘土矿物以其特有的层间结构及表面酸性位点受到了国内外学者的广泛关注。鉴于此,本课题提出利用天然粘土矿物作为催化剂开展生物质催化热解行为及机理研究。选取组分单一的纤维素和组分复杂的橡树叶作为热解生物质原料,采用自然界最常见、不同层状结构的高岭石和蒙脱石作为催化剂,以具有化学惰性的石英作为对照矿物,围绕粘土矿物原位催化热解生物质的关键科学问题,研究了粘土矿物对生物质热解过程的影响规律,基于粘土矿物表面活性位点的分析与探讨,揭示了粘土矿物对生物质的催化热解机理;并通过对热解生物炭的物化性质表征,开展基于生物炭脱除模拟废水中亚甲基蓝和重金属离子性能研究,揭示了污染物脱除过程生物炭的作用机制。围绕上述研究内容,本文主要研究工作如下:（1）首先利用TGA-DSC研究了生物质热解过程失重行为,对热解气体产物进行红外在线分析,采用多步反应的分布活化能模型（DAEM）对负载粘土矿物的生物质进行热解动力学分析,揭示了高岭石、蒙脱石对生物质催化热解温度迁移、热解行为及热解活化能的影响规律。研究表明:在相同加热速率下,蒙脱石-橡树叶和高岭石-橡树叶的最大失重峰温度Tmax较石英-橡树叶降低;而蒙脱石-纤维素和高岭石-纤维素的最大分解速率较石英-纤维素高。粘土矿物的负载对生物质的热解平均活化能未表现出明显影响,但蒙脱石的负载改变了纤维素的热解路径,促进了初始时刻β-消除路径的进行,使活化能E随转化率X呈现出先轻微升高后递减的趋势。TG-FTIR结果表明,粘土矿物的负载对橡树叶和纤维素热解过程中产物的种类以及最大分解速率对应温度未产生影响,只对热解产物产量产生一定影响。（2）利用自行设计的管式炉热解系统进行了生物质热解实验,计算了气、液、固三种热解产物产率,并对热解轻质气体及重质液体进行了定性和定量分析,结合粘土矿物表面性质,揭示了生物质热解过程粘土矿物催化热解机理。研究结果表明:粘土矿物遵循“破碎”的催化机理,使生物质产生更多轻质小分子气体以及高附加值化工中间体。粘土矿物可“消耗”生物油进行二次分解,增加轻质非冷凝气体产品产率,降低重质液体产率,而对固体产率无明显影响。管式炉热解试验表明,CO2、CH4和H2是两种生物质热解的主要气体产物,且粘土矿物的负载可改变生物质的热解路径,使热解气体的产量和产气速率得到提高。同时,气体增量随着酸性位点总数增加而增大。橡树叶样品热解液体产物主要为糠醛类、羧酸类、酮类、酚类以及少量烃类物质;纤维素样品热解液体产物主要为呋喃类和酮类物质。粘土矿物的负载改变了生物质油的成分,降低了橡树叶油中三种羧酸类物质（醋酸、丁酸和乙酸酐）、愈创木酚和对甲酚的含量。而糠醛,作为一种高附加值的中间化学品,在粘土矿物表面及层间Lewis酸和Br?nsted酸的协同催化下,随着催化剂总酸性位点数增加而呈现增加趋势。当负载量为10 wt%时,蒙脱石-橡树叶和高岭石-橡树叶与石英-橡树叶相比,糠醛的含量可分别增大86%和39%;在纤维素热解油中,左旋葡聚糖（LG）和1,4:3,6-二脱水α-D-吡喃葡萄糖（DGP）含量呈现出下降趋势,而作为手性合成底物的左旋葡聚糖酮（LGO）在粘土矿物的催化作用下含量得到显著提高,且随着催化剂总酸性位点数增加含量逐渐增大。（3）对生物质热解固体产物生物炭进行物化性质表征,开展基于生物炭脱除模拟废水中亚甲基蓝和重金属离子的吸附性能研究,探讨了不同污染物在不同生物炭表面的吸附行为,揭示了污染物脱除过程生物炭的作用机制。研究结果表明:生物炭均为富碳固体,在粘土矿物催化作用下生物炭中C含量升高,而失去碳原子“束缚”的H和O元素降低。粘土矿物负载的生物炭BET比表面积高于石英负载的生物炭,由于蒙脱石-生物炭孔径的坍塌和蒙脱石对孔径的堵塞,导致BET比表面积减小。FTIR分析结果表明,粘土矿物的负载使热解生物炭的芳香性结构增强,同时还形成脱氢羧基、羰基和羟基等含氧官能团。5 wt%矿物负载的生物炭吸附有机物和金属离子的研究表明,生物炭对亚甲基蓝（MB）的吸附为单分子层化学吸附,且颗粒内扩散不是生物炭吸附MB的唯一限速步骤。生物炭对五种金属离子的吸附均为化学吸附,总吸附容量为400-600 mg/g,其中吸附离子的性质在吸附过程中占主导作用。Cd2+、Co2+、Mn2+和Zn2+在生物炭上的吸附既有单分子层又有多分子层吸附,而Cu2+在橡树叶生物炭上为单分子层吸附,在纤维素生物炭上为多分子层吸附。生物炭的阳离子交换容量（CEC）和比表面积在生物炭的最大吸附容量中起主导作用,而重金属离子的电负性影响着吸附速率的大小。综上,上述研究为粘土矿物催化热解生物质的工业化应用提供理论依据,也为生物炭基材料的应用提供了方向,具有很好的实践意义。本论文图75幅,表21个,参考文献214篇。
Abstract
sheng wu zhi shi wo guo chu liang feng fu de lu se neng yuan ,sheng wu zhi de gao xiao li yong shi jin nian lai an da ke yan gong zuo zhe yan jiu de re dian wen ti 。dan mu qian sheng wu zhi re jie ji shu cun zai qi ti chan lv di 、re jie ye ti yang han liang gao ji suan xing da deng wen ti 。cui hua re jie shi zeng jia qi ti chan lv ,di gao re jie ye ti zhong gao fu jia zhi chan wu de you xiao tu jing 。chang gui ge cheng lei cui hua ji cun zai yi shi huo 、jia ge ang gui de wen ti ,tian ran nian tu kuang wu yi ji te you de ceng jian jie gou ji biao mian suan xing wei dian shou dao le guo nei wai xue zhe de an fan guan zhu 。jian yu ci ,ben ke ti di chu li yong tian ran nian tu kuang wu zuo wei cui hua ji kai zhan sheng wu zhi cui hua re jie hang wei ji ji li yan jiu 。shua qu zu fen chan yi de qian wei su he zu fen fu za de xiang shu xie zuo wei re jie sheng wu zhi yuan liao ,cai yong zi ran jie zui chang jian 、bu tong ceng zhuang jie gou de gao ling dan he meng tuo dan zuo wei cui hua ji ,yi ju you hua xue duo xing de dan ying zuo wei dui zhao kuang wu ,wei rao nian tu kuang wu yuan wei cui hua re jie sheng wu zhi de guan jian ke xue wen ti ,yan jiu le nian tu kuang wu dui sheng wu zhi re jie guo cheng de ying xiang gui lv ,ji yu nian tu kuang wu biao mian huo xing wei dian de fen xi yu tan tao ,jie shi le nian tu kuang wu dui sheng wu zhi de cui hua re jie ji li ;bing tong guo dui re jie sheng wu tan de wu hua xing zhi biao zheng ,kai zhan ji yu sheng wu tan tuo chu mo ni fei shui zhong ya jia ji lan he chong jin shu li zi xing neng yan jiu ,jie shi le wu ran wu tuo chu guo cheng sheng wu tan de zuo yong ji zhi 。wei rao shang shu yan jiu nei rong ,ben wen zhu yao yan jiu gong zuo ru xia :（1）shou xian li yong TGA-DSCyan jiu le sheng wu zhi re jie guo cheng shi chong hang wei ,dui re jie qi ti chan wu jin hang gong wai zai xian fen xi ,cai yong duo bu fan ying de fen bu huo hua neng mo xing （DAEM）dui fu zai nian tu kuang wu de sheng wu zhi jin hang re jie dong li xue fen xi ,jie shi le gao ling dan 、meng tuo dan dui sheng wu zhi cui hua re jie wen du qian yi 、re jie hang wei ji re jie huo hua neng de ying xiang gui lv 。yan jiu biao ming :zai xiang tong jia re su lv xia ,meng tuo dan -xiang shu xie he gao ling dan -xiang shu xie de zui da shi chong feng wen du Tmaxjiao dan ying -xiang shu xie jiang di ;er meng tuo dan -qian wei su he gao ling dan -qian wei su de zui da fen jie su lv jiao dan ying -qian wei su gao 。nian tu kuang wu de fu zai dui sheng wu zhi de re jie ping jun huo hua neng wei biao xian chu ming xian ying xiang ,dan meng tuo dan de fu zai gai bian le qian wei su de re jie lu jing ,cu jin le chu shi shi ke β-xiao chu lu jing de jin hang ,shi huo hua neng Esui zhuai hua lv Xcheng xian chu xian qing wei sheng gao hou di jian de qu shi 。TG-FTIRjie guo biao ming ,nian tu kuang wu de fu zai dui xiang shu xie he qian wei su re jie guo cheng zhong chan wu de chong lei yi ji zui da fen jie su lv dui ying wen du wei chan sheng ying xiang ,zhi dui re jie chan wu chan liang chan sheng yi ding ying xiang 。（2）li yong zi hang she ji de guan shi lu re jie ji tong jin hang le sheng wu zhi re jie shi yan ,ji suan le qi 、ye 、gu san chong re jie chan wu chan lv ,bing dui re jie qing zhi qi ti ji chong zhi ye ti jin hang le ding xing he ding liang fen xi ,jie ge nian tu kuang wu biao mian xing zhi ,jie shi le sheng wu zhi re jie guo cheng nian tu kuang wu cui hua re jie ji li 。yan jiu jie guo biao ming :nian tu kuang wu zun xun “po sui ”de cui hua ji li ,shi sheng wu zhi chan sheng geng duo qing zhi xiao fen zi qi ti yi ji gao fu jia zhi hua gong zhong jian ti 。nian tu kuang wu ke “xiao hao ”sheng wu you jin hang er ci fen jie ,zeng jia qing zhi fei leng ning qi ti chan pin chan lv ,jiang di chong zhi ye ti chan lv ,er dui gu ti chan lv mo ming xian ying xiang 。guan shi lu re jie shi yan biao ming ,CO2、CH4he H2shi liang chong sheng wu zhi re jie de zhu yao qi ti chan wu ,ju nian tu kuang wu de fu zai ke gai bian sheng wu zhi de re jie lu jing ,shi re jie qi ti de chan liang he chan qi su lv de dao di gao 。tong shi ,qi ti zeng liang sui zhao suan xing wei dian zong shu zeng jia er zeng da 。xiang shu xie yang pin re jie ye ti chan wu zhu yao wei kang quan lei 、suo suan lei 、tong lei 、fen lei yi ji shao liang ting lei wu zhi ;qian wei su yang pin re jie ye ti chan wu zhu yao wei fu nan lei he tong lei wu zhi 。nian tu kuang wu de fu zai gai bian le sheng wu zhi you de cheng fen ,jiang di le xiang shu xie you zhong san chong suo suan lei wu zhi （cu suan 、ding suan he yi suan gan ）、yu chuang mu fen he dui jia fen de han liang 。er kang quan ,zuo wei yi chong gao fu jia zhi de zhong jian hua xue pin ,zai nian tu kuang wu biao mian ji ceng jian Lewissuan he Br?nstedsuan de xie tong cui hua xia ,sui zhao cui hua ji zong suan xing wei dian shu zeng jia er cheng xian zeng jia qu shi 。dang fu zai liang wei 10 wt%shi ,meng tuo dan -xiang shu xie he gao ling dan -xiang shu xie yu dan ying -xiang shu xie xiang bi ,kang quan de han liang ke fen bie zeng da 86%he 39%;zai qian wei su re jie you zhong ,zuo xuan pu ju tang （LG）he 1,4:3,6-er tuo shui α-D-bi nan pu tao tang （DGP）han liang cheng xian chu xia jiang qu shi ,er zuo wei shou xing ge cheng de wu de zuo xuan pu ju tang tong （LGO）zai nian tu kuang wu de cui hua zuo yong xia han liang de dao xian zhe di gao ,ju sui zhao cui hua ji zong suan xing wei dian shu zeng jia han liang zhu jian zeng da 。（3）dui sheng wu zhi re jie gu ti chan wu sheng wu tan jin hang wu hua xing zhi biao zheng ,kai zhan ji yu sheng wu tan tuo chu mo ni fei shui zhong ya jia ji lan he chong jin shu li zi de xi fu xing neng yan jiu ,tan tao le bu tong wu ran wu zai bu tong sheng wu tan biao mian de xi fu hang wei ,jie shi le wu ran wu tuo chu guo cheng sheng wu tan de zuo yong ji zhi 。yan jiu jie guo biao ming :sheng wu tan jun wei fu tan gu ti ,zai nian tu kuang wu cui hua zuo yong xia sheng wu tan zhong Chan liang sheng gao ,er shi qu tan yuan zi “shu fu ”de Hhe Oyuan su jiang di 。nian tu kuang wu fu zai de sheng wu tan BETbi biao mian ji gao yu dan ying fu zai de sheng wu tan ,you yu meng tuo dan -sheng wu tan kong jing de tan ta he meng tuo dan dui kong jing de du sai ,dao zhi BETbi biao mian ji jian xiao 。FTIRfen xi jie guo biao ming ,nian tu kuang wu de fu zai shi re jie sheng wu tan de fang xiang xing jie gou zeng jiang ,tong shi hai xing cheng tuo qing suo ji 、tang ji he qiang ji deng han yang guan neng tuan 。5 wt%kuang wu fu zai de sheng wu tan xi fu you ji wu he jin shu li zi de yan jiu biao ming ,sheng wu tan dui ya jia ji lan （MB）de xi fu wei chan fen zi ceng hua xue xi fu ,ju ke li nei kuo san bu shi sheng wu tan xi fu MBde wei yi xian su bu zhou 。sheng wu tan dui wu chong jin shu li zi de xi fu jun wei hua xue xi fu ,zong xi fu rong liang wei 400-600 mg/g,ji zhong xi fu li zi de xing zhi zai xi fu guo cheng zhong zhan zhu dao zuo yong 。Cd2+、Co2+、Mn2+he Zn2+zai sheng wu tan shang de xi fu ji you chan fen zi ceng you you duo fen zi ceng xi fu ,er Cu2+zai xiang shu xie sheng wu tan shang wei chan fen zi ceng xi fu ,zai qian wei su sheng wu tan shang wei duo fen zi ceng xi fu 。sheng wu tan de yang li zi jiao huan rong liang （CEC）he bi biao mian ji zai sheng wu tan de zui da xi fu rong liang zhong qi zhu dao zuo yong ,er chong jin shu li zi de dian fu xing ying xiang zhao xi fu su lv de da xiao 。zeng shang ,shang shu yan jiu wei nian tu kuang wu cui hua re jie sheng wu zhi de gong ye hua ying yong di gong li lun yi ju ,ye wei sheng wu tan ji cai liao de ying yong di gong le fang xiang ,ju you hen hao de shi jian yi yi 。ben lun wen tu 75fu ,biao 21ge ,can kao wen suo 214pian 。
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论文作者分别是来自中国矿业大学的高丽慧，发表于刊物中国矿业大学2019-07-18论文，是一篇关于粘土矿物论文,生物质论文,催化热解论文,生物炭论文,水处理论文,吸附论文,中国矿业大学2019-07-18论文的文章。本文可供学术参考使用，各位学者可以免费参考阅读下载，文章观点不代表本站观点，资料来自中国矿业大学2019-07-18论文网站，若本站收录的文献无意侵犯了您的著作版权，请联系我们删除。
标签：粘土矿物论文; 生物质论文; 催化热解论文; 生物炭论文; 水处理论文; 吸附论文; 中国矿业大学2019-07-18论文;