用化学还原法制备了Ni-La-B非晶态合金催化剂,并采用X射线衍射、透射电镜、差热分析、X射线光电子能谱、电感耦合等离子光谱和H2程序升温脱附技术对催化剂进行了表征,研究了La含量对催化剂微观结构及其催化二硝基甲苯(DNT)加氢制二氨基甲苯(DAT)性能的影响.结果表明,随着助剂La含量的增加,Ni-La-B催化剂中非晶态结构的长程无序程度增大,催化剂平均粒径逐渐由70 nm左右减小至10 nm左右,分布更加均匀；同时降低了Ni吸附H2的强度,使H2吸附物种更易于在催化剂表面流动并参与反应.另外,La助剂还显著提高了催化剂的热稳定性和抗氧化性.在二硝基甲苯加氢反应中,催化剂性能随着La加入量提高至6％(摩尔分数)时,l MPa低压条件下DNT转化率和DAT选择性均达100％.当La加入量为8％时,催化剂的Ni活性中心数明显减少,其活性下降.
参考文献
| [1] | 李辉;李和兴;张静;LiH X Zhang J) .[P].CN 1850 330,2006. |
| [2] | 傅骐 .[P].CN 1465 433,2004. |
| [3] | 李琳,梁群芳,张爱清.Ni-B非晶态合金催化苯丙酮酸加氢合成苯丙氨酸[J].催化学报,2007(12):1031-1033. |
| [4] | 王文静,严新焕,许丹倩,孙军庆,房永彬,徐振元.Ni-B非晶态合金催化剂用于卤代硝基苯液相加氢制卤代苯胺[J].催化学报,2004(05):369-372. |
| [5] | 孔令启,李玉刚,韩方煜,郑世清.2,4-二硝基甲苯无外加溶剂的加氢表观动力学[J].化学反应工程与工艺,2009(03):244-249. |
| [6] | 阿巴斯·哈桑;易卜拉西姆·巴盖尔扎德;雷福德·G;安东尼,格雷戈里·博尔西格,阿齐兹·哈桑 .[P].CN 101687 767,2010. |
| [7] | R.H.玛查多;D.J.帕里洛;R.P.贝姆;R.R.布鲁克赫伊斯 .[P].CN 1 245 163,2000. |
| [8] | 王明辉,李和兴.Ni-B/SiO2非晶态催化剂应用于硝基苯液相加氢制苯胺[J].催化学报,2001(03):287-290. |
| [9] | 武美霞,李伟,张明慧,陶克毅.壳聚糖表面修饰的SiO2负载Ni-B非晶态合金的制备及催化性能[J].物理化学学报,2007(09):1311-1315. |
| [10] | 刘迎新,陈吉祥,张继炎.Ni/SiO2催化剂上间二硝基苯液相加氢制间苯二胺[J].催化学报,2003(03):224-228. |
| [11] | Neri G;Musolino M G;Rotondo E;Galvagno S .[J].Journal of Molecular Catalysis A:Chemical,1996,111:257. |
| [12] | Neri G;Musolino M G;Milone C;Visco A M Di Mario A .[J].Journal of Molecular Catalysis A:Chemical,1995,95:235. |
| [13] | Musolino M G;Neri G;Milone C;Minico S Galvagno S .[J].Journal of Chromatography A,1998,818:123. |
| [14] | Neri G.;Rizzo G.;Milone C.;Galvagno S.;Musolino MG.;Capannelli G. .Microstructural characterization of doped-Pd/C catalysts for the selective hydrogenation of 2,4-dinitrotoluene to arylhydroxylamines[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2003(2):303-311. |
| [15] | Neri G;Musolino M G;Milone C;Pietropaolo D Galvagno S .[J].Applied Catalysis A:General,2001,208:307. |
| [16] | 李贵贤;杨磊;马建军;司海娟 董宇航 .[J].聚氨酯工业,2009,24(01):30. |
| [17] | Zysler R D;Romero H;Ramos C A;De Biasi E Fiorani D .[J].Journal of Magnetism and Magnetic Materials,2003,266:233. |
| [18] | Wu Zh J;Zhang M H;Li W;Mu Sh Ch Tao K Y .[J].Journal of Molecular Catalysis A:Chemical,2007,273:277. |
| [19] | Guo J;Hou Y J;Yang C H;Wang Y Q He H Q Li W .[J].Catalysis Communications,2011,16:86. |
| [20] | Xie G W;Sun W;Li W B .[J].Catalysis Communications,2008,10:333. |
| [21] | 王威燕,杨运泉,罗和安,彭会左,张小哲,胡韬.Ni-Co-W-B非晶态催化剂的制备及其加氢脱氧性能[J].催化学报,2011(10):1645-1650. |
| [22] | Wu Zh J;Zhang M H;Zhao Z F;Li W Tao K Y .[J].Journal of Catalysis,2008,256:323. |
| [23] | Li H X;Xu Y P;Li H;Deng J F .[J].Applied Catalysis A:General,2001,216:51. |
| [24] | 戴维林,曹勇,范康年,邓景发.纳米Ni-Co-B非晶态合金抗氧化行为的原位XPS研究[J].高等学校化学学报,2003(03):473-476. |
| [25] | 郭延红,郭丽,赵峭梅.Ni-B/SiO2非晶态催化剂在二硝基苯催化加氢合成苯二胺中的应用[J].延安大学学报（自然科学版）,2005(03):54-56. |
| [26] | 严新焕,孙军庆,李波,吕翔,孙孟飞.Ni-Ce-P非晶态合金催化剂用于氯代硝基苯液相加氢制氯代苯胺[J].催化学报,2006(02):178-182. |
| [27] | Li HX;Wu YD;Zhang J;Dai WL;Quao MH .Liquid phase acetonitrile hydrogenation to ethylamine over a highly active and selective Ni-Co-B amorphous alloy catalyst[J].Applied Catalysis, A. General: An International Journal Devoted to Catalytic Science and Its Applications,2004(1/2):199-206. |
| [28] | Wang W Y;Yang Y Q;Luo H A;Liu W Y .[J].Catalysis Communications,2010,11:803. |
| [29] | Wen M;Li L J;Liu Q Y;Qi H Q Zhang T .[J].Journal of Alloys and Compounds,2008,455:510. |
| [30] | Liu Sh Ch;Liu Zh Y;Wang Zh;Wu Y W Yuan P .[J].Chemical Engineering Journal,2008,139:157. |
| [31] | Li H X;Zhang S Y;Luo H Sh .[J].Materials Letters,2004,58:2741. |
| [32] | 石秋杰,雷经新,张宁.糠醛液相加氢用Mo改性Ni-B/TiO2-Al2O3（S）非晶态合金催化剂[J].物理化学学报,2007(01):98-102. |
| [33] | 郑一雄,姚士冰,周绍民.Ni-Mo-B非晶态合金纳米颗粒的抗氧化性能研究[J].物理化学学报,2004(11):1352-1356. |
| [34] | Li H;Zhao Q F;Li H X .[J].Journal of Molecular Catalysis A:Chemical,2008,285:29. |
| [35] | Li H;Li H X;Deng J F .[J].Catalysis Today,2002,74:53. |
| [36] | Bai G Y;Niu L B;Qiu M D;He F Fan X X Dou H Y Zhang X F .[J].Catalysis Communications,2010,12:212. |
| [37] | Zhang R B;Li F Y;Shi Q J;Luo L T .[J].Applied Catalysis A:General,2001,205:279. |
| [38] | Zhang R B;Li F Y;Zhang N;Shi Q J .[J].Applied Catalysis A:General,2003,239:17. |
| [39] | Hou Y J;Wang Y Q;He F;Mi W L Li Zh H Mi Zh T Wu W Min E Z .[J].Applied Catalysis A:General,2004,259:35. |
| [40] | 严新焕,孙军庆,徐颖华,杨建峰.Ni-Co-B非晶态合金催化剂用于氯代硝基苯液相加氢制氯代苯胺[J].催化学报,2006(02):119-123. |
| [41] | 武美霞,李伟,张明慧,陶克毅.以壳聚糖为介质的Ni-B非晶态合金/膨胀石墨的制备及其催化加氢性能[J].催化学报,2007(04):351-356. |
| [42] | 武美霞,李伟,张明慧,陶克毅.壳聚糖修饰的NiB非晶态合金的制备及表征[J].物理化学学报,2011(04):953-958. |
| [43] | Walter J L .[J].Materials Science and Engineering,1981,50:137. |
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