本文主要研究内容
作者李发达（2019）在《非晶态合金催化剂的理性构筑及其加氢性能研究》一文中研究指出：1,4-环己二醇是重要的化工原料,在多个领域有着广泛应用。对苯二酚催化加氢制1,4-环己二醇路线具有原子经济、生产量大及绿色环保等诸多优势,成为1,4-环己二醇的主要生产方法,所用催化剂大多为雷尼镍和贵金属催化剂,但雷尼镍的使用存在污染环境、反应条件苛刻及活性较低等不足,贵金属催化剂又存在制备成本较高且制备过程复杂等缺点,已无法满足对苯二酚加氢制1,4-环己二醇的新要求。非晶态合金催化剂具有远高于相应晶态催化剂的催化活性,因此研发高效的非晶态合金催化剂成为提高1,4-环己二醇产率的关键。近年来,Ru基催化剂和Ni基催化剂因催化加氢性能优越而深受广大学者的青睐,然而大多数Ru催化剂活性组分含量过高,制备过程复杂从而导致催化剂的生产成本高昂,而Ni催化剂又存在稳定性较差等缺点,这严重阻碍其工业化应用。本文旨在制备高活性、低成本、制备过程简单的新型非晶态合金催化剂,为对苯二酚催化加氢技术的升级提供一定的理论依据。本文以NaY分子筛为载体,采用化学还原法制备出系列低负载量Ru基与系列Ni基负载型非晶态合金催化剂,采用XPS、H2-TPD、NH3-TPD、XRD、SEM、ICP-OES对催化剂物相结构、组成、形貌进行表征。Ru基催化剂的研究结果表明,采用反加法、添加W、超声波辅助、使用PEG对载体NaY进行涂覆等手段制备的Ru催化剂活性粒子分散更均匀,活性位点更多;Ni基催化剂,活性成分Ni作为电子受体,而B作为电子供体,引入助剂Sr可对Ni-B/NaY二元催化剂的电子结构进行适宜修饰,促进电子转移。同时,NH3-TPD和TEM表征结果证明,助剂Sr还可对Ni催化剂酸性进行调控;另外,三元Ni基催化剂和四元Ni基催化剂的XPS和NH3-TPD表征结果表明,添加适量Cu会部分覆盖Ni粒子,这种覆盖对催化活性的影响较小,却能明显提高催化剂稳定性。将本文制备的两个系列催化剂应用于对苯二酚加氢制1,4-环己二醇,Ru-W-B/NaY-IUP（1500）0.6催化剂（I代表反加法,U代表在制备过程中使用超声波,P代表制备过程中使用了PEG,M为PEG相对分子质量,m为PEG用量）在最佳反应条件下,对应的苯二酚转化率达到99.7%,1,4-环己二醇选择性达92.3%,而该催化剂中Ru负载量仅为0.45 wt%。相同条件下,使用Ni-Sr-B/NaY-U催化剂催化对苯二酚加氢制1,4-环己二醇时,对苯二酚转化率为99.6%,1,4-环己二醇选择性高达99.2%。而Ni-Sr-Cu-B/NaY-U用于该反应时,对苯二酚转化率达到99.4%,1,4-环己二醇选择性达到98.6%,说明添加适量Cu后,催化性能未受明显影响,但Ni-Sr-Cu-B/NaY-U催化剂的稳定性显著提高,重复使用多次后,其催化活性未见明显下降。
Abstract
1,4-huan ji er chun shi chong yao de hua gong yuan liao ,zai duo ge ling yu you zhao an fan ying yong 。dui ben er fen cui hua jia qing zhi 1,4-huan ji er chun lu xian ju you yuan zi jing ji 、sheng chan liang da ji lu se huan bao deng zhu duo you shi ,cheng wei 1,4-huan ji er chun de zhu yao sheng chan fang fa ,suo yong cui hua ji da duo wei lei ni nie he gui jin shu cui hua ji ,dan lei ni nie de shi yong cun zai wu ran huan jing 、fan ying tiao jian ke ke ji huo xing jiao di deng bu zu ,gui jin shu cui hua ji you cun zai zhi bei cheng ben jiao gao ju zhi bei guo cheng fu za deng que dian ,yi mo fa man zu dui ben er fen jia qing zhi 1,4-huan ji er chun de xin yao qiu 。fei jing tai ge jin cui hua ji ju you yuan gao yu xiang ying jing tai cui hua ji de cui hua huo xing ,yin ci yan fa gao xiao de fei jing tai ge jin cui hua ji cheng wei di gao 1,4-huan ji er chun chan lv de guan jian 。jin nian lai ,Ruji cui hua ji he Niji cui hua ji yin cui hua jia qing xing neng you yue er shen shou an da xue zhe de qing lai ,ran er da duo shu Rucui hua ji huo xing zu fen han liang guo gao ,zhi bei guo cheng fu za cong er dao zhi cui hua ji de sheng chan cheng ben gao ang ,er Nicui hua ji you cun zai wen ding xing jiao cha deng que dian ,zhe yan chong zu ai ji gong ye hua ying yong 。ben wen zhi zai zhi bei gao huo xing 、di cheng ben 、zhi bei guo cheng jian chan de xin xing fei jing tai ge jin cui hua ji ,wei dui ben er fen cui hua jia qing ji shu de sheng ji di gong yi ding de li lun yi ju 。ben wen yi NaYfen zi shai wei zai ti ,cai yong hua xue hai yuan fa zhi bei chu ji lie di fu zai liang Ruji yu ji lie Niji fu zai xing fei jing tai ge jin cui hua ji ,cai yong XPS、H2-TPD、NH3-TPD、XRD、SEM、ICP-OESdui cui hua ji wu xiang jie gou 、zu cheng 、xing mao jin hang biao zheng 。Ruji cui hua ji de yan jiu jie guo biao ming ,cai yong fan jia fa 、tian jia W、chao sheng bo fu zhu 、shi yong PEGdui zai ti NaYjin hang tu fu deng shou duan zhi bei de Rucui hua ji huo xing li zi fen san geng jun yun ,huo xing wei dian geng duo ;Niji cui hua ji ,huo xing cheng fen Nizuo wei dian zi shou ti ,er Bzuo wei dian zi gong ti ,yin ru zhu ji Srke dui Ni-B/NaYer yuan cui hua ji de dian zi jie gou jin hang kuo yi xiu shi ,cu jin dian zi zhuai yi 。tong shi ,NH3-TPDhe TEMbiao zheng jie guo zheng ming ,zhu ji Srhai ke dui Nicui hua ji suan xing jin hang diao kong ;ling wai ,san yuan Niji cui hua ji he si yuan Niji cui hua ji de XPShe NH3-TPDbiao zheng jie guo biao ming ,tian jia kuo liang Cuhui bu fen fu gai Nili zi ,zhe chong fu gai dui cui hua huo xing de ying xiang jiao xiao ,que neng ming xian di gao cui hua ji wen ding xing 。jiang ben wen zhi bei de liang ge ji lie cui hua ji ying yong yu dui ben er fen jia qing zhi 1,4-huan ji er chun ,Ru-W-B/NaY-IUP（1500）0.6cui hua ji （Idai biao fan jia fa ,Udai biao zai zhi bei guo cheng zhong shi yong chao sheng bo ,Pdai biao zhi bei guo cheng zhong shi yong le PEG,Mwei PEGxiang dui fen zi zhi liang ,mwei PEGyong liang ）zai zui jia fan ying tiao jian xia ,dui ying de ben er fen zhuai hua lv da dao 99.7%,1,4-huan ji er chun shua ze xing da 92.3%,er gai cui hua ji zhong Rufu zai liang jin wei 0.45 wt%。xiang tong tiao jian xia ,shi yong Ni-Sr-B/NaY-Ucui hua ji cui hua dui ben er fen jia qing zhi 1,4-huan ji er chun shi ,dui ben er fen zhuai hua lv wei 99.6%,1,4-huan ji er chun shua ze xing gao da 99.2%。er Ni-Sr-Cu-B/NaY-Uyong yu gai fan ying shi ,dui ben er fen zhuai hua lv da dao 99.4%,1,4-huan ji er chun shua ze xing da dao 98.6%,shui ming tian jia kuo liang Cuhou ,cui hua xing neng wei shou ming xian ying xiang ,dan Ni-Sr-Cu-B/NaY-Ucui hua ji de wen ding xing xian zhe di gao ,chong fu shi yong duo ci hou ,ji cui hua huo xing wei jian ming xian xia jiang 。
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论文作者分别是来自兰州理工大学的李发达，发表于刊物兰州理工大学2019-07-18论文，是一篇关于非晶态合金论文,对苯二酚论文,加氢论文,环己二醇论文,兰州理工大学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，资料来自兰州理工大学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：非晶态合金论文; 对苯二酚论文; 加氢论文; 环己二醇论文; 兰州理工大学2019-07-18论文;