活性炭负载Pt-Ni双金属催化剂上十氢化萘脱氢

doi:10.1016/S1872-2067(14)60178-9

催化学报 ›› 2014, Vol. 35 ›› Issue (11): 1833-1839.DOI: 10.1016/S1872-2067(14)60178-9

活性炭负载Pt-Ni双金属催化剂上十氢化萘脱氢

齐随涛, 李迎迎, 岳佳琪, 陈昊, 伊春海, 杨伯伦

西安交通大学化学工程与技术学院化工系, 陕西西安710049

收稿日期:2014-04-06 修回日期:2014-05-23 出版日期:2014-11-06 发布日期:2014-11-06
通讯作者: 齐随涛
基金资助:
国家自然科学基金(21006076); 高等学校博士学科点专项科研基金(20110201130002); 中央高校基本科研业务费专项基金(xjj2011062).

Hydrogen production from decalin dehydrogenation over Pt-Ni/C bimetallic catalysts

Suitao Qi, Yingying Li, Jiaqi Yue, Hao Chen, Chunhai Yi, Bolun Yang

School of Chemical Engineering and Technology, Xi'an Jiaotong University, Xi'an 710049, Shaanxi, China

Received:2014-04-06 Revised:2014-05-23 Online:2014-11-06 Published:2014-11-06
Supported by:
This work was supported by the National Natural Science Foundation of China (21006076), the Specialized Research Fund for the Doctoral Program of Higher Education, China (20110201130002), and the Fundamental Research Funds for the Central Universities, China (xjj2011062).

摘要/Abstract

摘要：

采用等体积浸渍法制备了活性炭负载的具有脱氢活性的Pt-Ni双金属催化剂及相应的Pt单金属催化剂, 并用X射线衍射、N₂吸附-脱附和NH₃-程序升温脱附对其进行了表征. 在290 ℃下, 研究了间歇反应条件下催化剂以过热液膜状态催化十氢化萘脱氢活性, 考察了温度、浸渍顺序和Pt/Ni摩尔比对十氢化萘脱氢活性和萘产率的影响. 结果表明, 与单金属催化剂相比, Pt-Ni双金属催化剂上产氢效率显著提高. 当Pt/Ni摩尔比为1:1, Pt首先浸渍时, 得到的催化剂上脱氢转化率和萘产率最高. 将实验结果与密度泛函理论计算的氢原子在不同催化表面的结合能关联证实, 具有更强原子氢结合能的双金属表面具有更高的脱氢活性.

关键词: 铂, 镍, 双金属, 十氢化萘, 脱氢, 密度泛函理论

Abstract:

Pt-Ni bimetallic catalysts and the corresponding monometallic Pt catalysts supported on active carbon were prepared by incipient wetness impregnation and characterized by X-ray diffraction, N₂ adsorption, and NH₃-temperature programmed desorption. Their activities for decalin dehydrogenation were investigated at a superheated liquid film state in a batch reactor. The effects of temperature, impregnation sequence, and Pt/Ni molar ratio on the dehydrogenation activity and the naphthalene yield were investigated. The results show that the Pt-Ni bimetallic catalyst significantly enhanced hydrogen evolution compared with either Ni or Pt monometallic catalyst. The highest dehydrogenation conversion and naphthalene yield were obtained when the Pt/Ni molar ratio was 1:1 and Pt was impregnated first. The experimental results were correlated with density functional theory calculations of hydrogen binding energy (HBE) on different catalytic surfaces. The correlation confirmed that bimetallic surfaces with stronger HBEs had higher dehydrogenation activities.

Key words: Platinum, Nickel, Bimetallic, Decalin, Dehydrogenation, Density functional theory

齐随涛, 李迎迎, 岳佳琪, 陈昊, 伊春海, 杨伯伦. 活性炭负载Pt-Ni双金属催化剂上十氢化萘脱氢[J]. 催化学报, 2014, 35(11): 1833-1839.

Suitao Qi, Yingying Li, Jiaqi Yue, Hao Chen, Chunhai Yi, Bolun Yang. Hydrogen production from decalin dehydrogenation over Pt-Ni/C bimetallic catalysts[J]. Chinese Journal of Catalysis, 2014, 35(11): 1833-1839.

×
扫码分享

导出引用管理器 EndNote|Ris|BibTeX

链接本文: https://www.cjcatal.com/CN/10.1016/S1872-2067(14)60178-9

https://www.cjcatal.com/CN/Y2014/V35/I11/1833

参考文献

[1] Eberle U, Felderhoff M, Schüth F. Angew Chem Int Ed, 2009, 48: 6608
[2] David E. J Mater Process Technol, 2005, 162-163: 169
[3] Biniwale R B, Rayalu S, Devott S, Ichikawa M. Int J Hydrogen Energy, 2008, 33: 360
[4] Zhu G L, Yang B L. Progr Chem (朱刚利, 杨伯伦. 化学进展), 2009, 21: 2760
[5] Ninomiya W, Tanabe Y, Sotowa K I, Yasukawa T, Sugiyama S. Res Chem Intermed, 2008, 34: 663
[6] Pande J V, Shukla A, Biniwale R B. Int J Hydrogen Energy, 2012, 37: 6756
[7] Kariya N, Fukuoka A, Ichikawa M. Appl Catal A, 2002, 233: 91
[8] Saito Y, Aramaki K, Hodoshima S, Saito M, Shono A, Kuwano J, Otake K. Chem Eng Sci, 2008, 63: 4935
[9] Wang Y G, Shah N, Huffman G P. Energy Fuels, 2004, 18: 1429
[10] Tien P D, Satoh T, Miura M, Nomura M. Fuel Process Technol, 2008, 89: 415
[11] Du J P, Zhao R H, Jiao G R. Int J Hydrogen Energy, 2013, 38: 5789
[12] Chen A B, Zhang W P, Li X Y, Tan D L, Han X W, Bao X H. Catal Lett, 2007, 119: 159
[13] Shukla A A, Gosavi P V, Pande J V, Kumar V P, Chary K V R, Biniwale R B. Int J Hydrogen Energy, 2010, 35: 4020
[14] Shinohara C, Kawakami S, Moriga T, Hayashi H, Hodoshima S, Saito Y, Sugiyama S. Appl Catal A, 2004, 266: 251
[15] Tien P D, Satoh T, Miura M, Nomura M. Energy Fuels, 2005, 19: 731
[16] Tien P D, Satoh T, Miura M, Nomura M. Energy Fuels, 2005, 19: 2110
[17] Wang Y G, Shah N, Huggins F E, Huffman G P. Energy Fuels, 2006, 20: 2612
[18] Jiang N Z, Rao K S R, Jin M J, Park S E. Appl Catal A, 2012, 425-426: 62
[19] Suttisawat Y, Horikoshi S, Sakai H, Abe M. Int J Hydrogen Energy, 2010, 35: 6179
[20] Yolcular S, Olgun Ö. Catal Today, 2008, 138: 198
[21] Nagaraja B M, Shin C H, Jung K D. Appl Catal A, 2013, 467: 211
[22] Patil S P, Pande J V, Biniwale R B. Int J Hydrogen Energy, 2013, 38: 15233
[23] Alhumaidan F, Tsakiris D, Cresswell D, Garforth A. Int J Hydrogen Energy, 2013, 38: 14010
[24] Aboul-Fotouh S M K, Aboul-Gheit N A K. Chin J Catal (催化学报), 2012, 33: 697
[25] Gao X F, Chen C L, Ren S Y, Zhang J, Su D S. Chin J Catal (高旭锋, 谌春林, 任士远, 张建, 苏党生. 催化学报), 2012, 33: 1069
[26] Biniwale R B, Kariya N, Ichikawa M. Catal Lett, 2005, 105: 83
[27] Qi S T, Yu W T, Lonergan W W, Yang B L, Chen J G. Chin J Catal (齐随涛, 俞伟婷, Lonergan W W, 杨伯伦, 陈经广. 催化学报), 2010, 31: 955
[28] Qi S T, Yu W T, Lonergan W W, Yang B L, Chen J G. ChemCatChem, 2010, 2: 625
[29] Chen J G, Qi S T, Humbert M P, Menning C A, Zhu Y X. Acta Phys-Chim Sin (陈经广, 齐随涛, Humbert M P, Menning C A, 朱月香. 物理化学学报), 2010, 26: 869
[30] Chen J G, Menning C A, Zellner M B. Surf Sci Rep, 2008, 63: 201
[31] Skoplyak O, Barteau M A, Chen J G. ChemSusChem, 2008, 1: 524
[32] Hansgen D A, Vlachos D G, Chen J G. Nat Chem, 2010, 2: 484
[33] Shu Y Y, Murillo L E, Bosco J P, Huang W, Frenkel A I, Chen J G. Appl Catal A, 2008, 339: 169
[34] Lima F H B, Zhang J, Shao M H, Sasaki K, Vukmirovic M B, Ticianelli E A, Adzic R R. J Phys Chem C, 2007, 111: 404

活性炭负载Pt-Ni双金属催化剂上十氢化萘脱氢

Hydrogen production from decalin dehydrogenation over Pt-Ni/C bimetallic catalysts

PDF

可视化

被引次数

摘要/Abstract

引用本文

使用本文

扫码分享

参考文献

相关文章 15

编辑推荐

Metrics

[1]	胡金念, 田玲婵, 王海燕, 孟洋, 梁锦霞, 朱纯, 李隽. MXene负载3d金属单原子高效氮还原电催化剂的理论筛选[J]. 催化学报, 2023, 52(9): 252-262.
[2]	孙嘉辰, 陈赛, 付东龙, 王伟, 王显辉, 孙国栋, 裴春雷, 赵志坚, 巩金龙. 氧扩散与表面反应在VO_x-Ce_1‒_xZr_xO₂催化丙烷脱氢反应中的影响[J]. 催化学报, 2023, 52(9): 217-227.
[3]	程璐, 陈许宁, 胡培君, 曹宵鸣. 双氧水对于单核铜分子筛催化甲烷直接氧化制甲醇反应性能的利弊[J]. 催化学报, 2023, 51(8): 135-144.
[4]	尹春, 杨甫林, 王书莉, 冯立纲. 异质结构NiSe₂/MoSe₂用于高效尿素辅助电解水制氢[J]. 催化学报, 2023, 51(8): 225-236.
[5]	刘赵春, 宗雪, Dionisios G. Vlachos, Ivo A. W. Filot, Emiel J. M. Hensen. 金属掺杂SnO₂电化学还原CO₂制甲酸的计算研究[J]. 催化学报, 2023, 50(7): 249-259.
[6]	周波, 石建巧, 姜一民, 肖磊, 逯宇轩, 董帆, 陈晨, 王特华, 王双印, 邹雨芹. 强化脱氢动力学实现超低电池电压和大电流密度下抗坏血酸电氧化[J]. 催化学报, 2023, 50(7): 372-380.
[7]	耿仕鹏, 陈利明, 陈海鑫, 王毅, 丁朝斌, 蔡丹丹, 宋树芹. 揭示层状晶态CoMoO₄的水裂解电催化机制: 从晶面选择到活性位点设计的理论研究[J]. 催化学报, 2023, 50(7): 334-342.
[8]	刘诗瑶, 巩玉同, 杨晓, 张楠楠, 刘会斌, 梁长海, 陈霄. 具有富电子镍位点的耐酸金属间化合物CaNi₂Si₂催化剂用于不饱和有机酸酐/酸的水相加氢[J]. 催化学报, 2023, 50(7): 260-272.
[9]	李显泉, 庞纪峰, 赵于嘉, 吴鹏飞, 于文广, 颜佩芳, 苏扬, 郑明远. Cu-MFI催化剂上Cu^δ⁺催化乙醇脱氢制乙醛[J]. 催化学报, 2023, 49(6): 91-101.
[10]	张功, 张炜松, 王小雨, 杨洋, 季定纬, 万伯顺, 陈庆安. 镍催化杂芳烃的非天然戊烯基化及环状单萜化反应[J]. 催化学报, 2023, 49(6): 123-131.
[11]	张锋伟, 郭河芳, 刘萌萌, 赵阳, 洪峰, 李静静, 董正平, 乔波涛. 表面应力介导的碳基Pt纳米催化剂用于硝基芳烃的高选择性加氢[J]. 催化学报, 2023, 48(5): 195-204.
[12]	黄正清, 贺姝玥, 班涛, 高新, 许云华, 常春然. Pt-Cu合金催化剂上甲烷无氧偶联的机理与微观动力学研究: 从单原子位点到单团簇位点[J]. 催化学报, 2023, 48(5): 90-100.
[13]	李静静, 张锋伟, 詹新雨, 郭河芳, 张涵, 昝文艳, 孙振宇, 张献明. 酞菁镍分子结构的精确设计: 优化电子和空间效应用于CO₂电还原[J]. 催化学报, 2023, 48(5): 117-126.
[14]	井会娟, 龙军, 李欢, 傅笑言, 肖建平. 电催化硝酸盐还原合成氨电势相关性的计算见解[J]. 催化学报, 2023, 48(5): 205-213.
[15]	邢亚楠, 康磊磊, 马静远, 蒋齐可, 苏杨, 张盛鑫, 徐晓燕, 李林, 王爱琴, 刘智攀, 马思聪, 刘晓艳, 张涛. Sn₁Pt单原子合金催化剂在丙烷脱氢反应中的应用[J]. 催化学报, 2023, 48(5): 164-174.