本文主要研究内容
作者任宏伟（2019）在《CuZn基催化剂的完全液相-溶剂热法制备及合成气制乙醇研究》一文中研究指出：合成气一步催化法制乙醇是C1化学中极具挑战性的课题,由于目标产物选择性低,目前仍处于实验室研究阶段,开发经济适用且性能优良的催化剂是各方研究的重点。课题组自主开创的完全液相法制备的Cu基催化剂在用于CO加氢制低碳醇方面有着良好的性能。前期研究表明,流动气氛高压热处理和密闭环境溶剂热处理制得的催化剂,其催化产物中乙醇选择性最高可达38.7%。本文在此基础上做了进一步研究。本文采用完全液相-溶剂热法制备CuZnAl催化剂,先考察了前驱体结晶度的变化对催化剂的影响;然后针对乙醇选择性较高的催化剂活性却较低的问题,提出采用掺杂的方式,在前驱体制备过程中引入SBA-15分子筛和碳纳米管作为结构助剂对催化剂进行改性。分别考察了SBA-15在前驱体制备阶段中的加入位置和加入量,含羧基的短碳纳米管和硝酸处理后的长碳纳米管用量对催化剂的影响,采用多种方法对催化剂进行表征,在浆态床中评价催化剂的CO加氢性能,结果显示:1、采用完全液相-溶剂热法制备CuZnAl催化剂,前驱体结晶度较高时,Cu物种较为分散,有利于甲醇的生成和催化活性的提高;结晶度较低时,自生压较高,有利于尖晶石和较大颗粒Cu的形成,且易形成Cu+和Cu0共存的状态,有利于C2+OH的生成。2、与CuZnAl催化剂相比,加入SBA-15制备的催化剂中有一定量碱式盐存在。SBA-15先与CuZn盐的乙醇溶液混合,利于CuZn组分与SBA-15表面产生相互作用,促进了大颗粒Cu和中强酸位的生成。3、随着SBA-15加入量增多,催化剂中Cu晶粒尺寸增大,难还原Cu+含量增多,生成一定的弱酸和中强酸中心,促进了乙醇的生成。催化剂Cat0.2、Cat0.6在活性测试期内乙醇平均选择性分别为42.7%和66.4%。4、羧基化短碳纳米管与CuZn盐乙醇溶液混合加入,利于生成难还原Cu+和较多数量的弱酸以及中强酸。适量含羧基的短碳纳米管辅助制备CuZn基催化剂有利于乙醇生成。5、长碳纳米管与Al的醇解液混合加入,利于Cu和Cu2O晶粒的生长;难还原Cu+的量增多;催化剂中生成较多含量的弱酸以及部分中强酸,利于乙醇的生成。CatL15%的催化产物中乙醇平均选择性为36.0%。6、催化剂的织构参数性质与催化剂活性、产物选择性没有较为明显的关联。
Abstract
ge cheng qi yi bu cui hua fa zhi yi chun shi C1hua xue zhong ji ju tiao zhan xing de ke ti ,you yu mu biao chan wu shua ze xing di ,mu qian reng chu yu shi yan shi yan jiu jie duan ,kai fa jing ji kuo yong ju xing neng you liang de cui hua ji shi ge fang yan jiu de chong dian 。ke ti zu zi zhu kai chuang de wan quan ye xiang fa zhi bei de Cuji cui hua ji zai yong yu COjia qing zhi di tan chun fang mian you zhao liang hao de xing neng 。qian ji yan jiu biao ming ,liu dong qi fen gao ya re chu li he mi bi huan jing rong ji re chu li zhi de de cui hua ji ,ji cui hua chan wu zhong yi chun shua ze xing zui gao ke da 38.7%。ben wen zai ci ji chu shang zuo le jin yi bu yan jiu 。ben wen cai yong wan quan ye xiang -rong ji re fa zhi bei CuZnAlcui hua ji ,xian kao cha le qian qu ti jie jing du de bian hua dui cui hua ji de ying xiang ;ran hou zhen dui yi chun shua ze xing jiao gao de cui hua ji huo xing que jiao di de wen ti ,di chu cai yong can za de fang shi ,zai qian qu ti zhi bei guo cheng zhong yin ru SBA-15fen zi shai he tan na mi guan zuo wei jie gou zhu ji dui cui hua ji jin hang gai xing 。fen bie kao cha le SBA-15zai qian qu ti zhi bei jie duan zhong de jia ru wei zhi he jia ru liang ,han suo ji de duan tan na mi guan he xiao suan chu li hou de chang tan na mi guan yong liang dui cui hua ji de ying xiang ,cai yong duo chong fang fa dui cui hua ji jin hang biao zheng ,zai jiang tai chuang zhong ping jia cui hua ji de COjia qing xing neng ,jie guo xian shi :1、cai yong wan quan ye xiang -rong ji re fa zhi bei CuZnAlcui hua ji ,qian qu ti jie jing du jiao gao shi ,Cuwu chong jiao wei fen san ,you li yu jia chun de sheng cheng he cui hua huo xing de di gao ;jie jing du jiao di shi ,zi sheng ya jiao gao ,you li yu jian jing dan he jiao da ke li Cude xing cheng ,ju yi xing cheng Cu+he Cu0gong cun de zhuang tai ,you li yu C2+OHde sheng cheng 。2、yu CuZnAlcui hua ji xiang bi ,jia ru SBA-15zhi bei de cui hua ji zhong you yi ding liang jian shi yan cun zai 。SBA-15xian yu CuZnyan de yi chun rong ye hun ge ,li yu CuZnzu fen yu SBA-15biao mian chan sheng xiang hu zuo yong ,cu jin le da ke li Cuhe zhong jiang suan wei de sheng cheng 。3、sui zhao SBA-15jia ru liang zeng duo ,cui hua ji zhong Cujing li che cun zeng da ,nan hai yuan Cu+han liang zeng duo ,sheng cheng yi ding de ruo suan he zhong jiang suan zhong xin ,cu jin le yi chun de sheng cheng 。cui hua ji Cat0.2、Cat0.6zai huo xing ce shi ji nei yi chun ping jun shua ze xing fen bie wei 42.7%he 66.4%。4、suo ji hua duan tan na mi guan yu CuZnyan yi chun rong ye hun ge jia ru ,li yu sheng cheng nan hai yuan Cu+he jiao duo shu liang de ruo suan yi ji zhong jiang suan 。kuo liang han suo ji de duan tan na mi guan fu zhu zhi bei CuZnji cui hua ji you li yu yi chun sheng cheng 。5、chang tan na mi guan yu Alde chun jie ye hun ge jia ru ,li yu Cuhe Cu2Ojing li de sheng chang ;nan hai yuan Cu+de liang zeng duo ;cui hua ji zhong sheng cheng jiao duo han liang de ruo suan yi ji bu fen zhong jiang suan ,li yu yi chun de sheng cheng 。CatL15%de cui hua chan wu zhong yi chun ping jun shua ze xing wei 36.0%。6、cui hua ji de zhi gou can shu xing zhi yu cui hua ji huo xing 、chan wu shua ze xing mei you jiao wei ming xian de guan lian 。
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标签：完全液相法论文; 溶剂热法论文; 加氢论文; 乙醇论文; 太原理工大学2019-07-26论文;