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第 6 期 苏 炜,等: Fe-多级孔 Hβ 的制备及催化合成二苯甲烷性能 ·1123·
中心数量减少,从而降低催化活性。这也与 BET 表 catalytic properties for benzylation of benzene by benzyl chloride[J].
Chinese Journal of Catalysis (催化学报), 2003, 24(8): 579-584.
征结果相一致。而二苯甲烷的选择性增大是因为介 [3] Kun Y L, Zhang C, Li X L, et al. Iron-containing MIL-101 (Cr) as
highly active and stable heterogeneous catalysts for the benzylation
孔的产生,提高了二苯甲烷的扩散性能,降低了深 of a romatics with benzyl chloride[J]. Reaction Kinetics Mechanisms
& Catalysis, 2016, 120(1): 1-13.
度苄基化的发生。 [4] Ji Min (纪敏), Wu Haiwei (吴海鸣), He Min (贺民), et al. Kinetic
study on catalytic synthesis of diphenylmethane by immobilized
2.4 催化剂重复使用性测试 AlCl 3[J]. Journal of Dalian University of Technology (大连理工大
Fe-Hβ-B 0.10 催化苯-氯化苄反应重复使用性结 学学报), 2008, 48(2): 168-172.
[5] Arafat A, Alhamed Y. Catalytic activity of mesoporous catalysts in
果见图 9。 Friedel-Crafts benzylation of benzene[J]. Journal of Porous
Materials, 2009, 16(5): 565-572.
[6] Chuabe V D. Benzylation of benzene to diphenylmethane using
zeolite catalysts[J]. Catalysis Communications, 2004, 5(6): 321-326.
[7] Liu Hui (刘惠), Zhang Shuang (张爽), Xie Sujuan (谢素娟), et al.
Synthesis characterization and catalytic performance of hierarchical
ZSM-11 zeolite synthesized via dual-template route[J]. Chinese
Journal of Catalysis (催化学报), 2018, 39(1): 167-180.
[8] Liu Dongmei (刘冬梅), Jiang Hanbo (蒋涵博), Qu Shengtao (曲圣
涛 ), et al. Study on the alkylation of thiophene and catalyst
deactivation and regeneration with modified HZSM-5 zeolite[J].
Journal of Fuel Chemistry and Technology (燃料化学学报), 2018,
46(3): 355-364.
[9] Liu Wanrong (刘万荣), Liu Xinmei (刘欣梅), Xin Ying (辛颖), et al.
Preparation of hierarchical Y/ZrO 2 composite[J]. Acta Petrolei Sinica
(Petroleum Processing Section) (石油学报: 石油加工), 2018, 34(4):
689-695.
[10] Tarach K, Gora-marek K, Tekla J, et al. Catalytic cracking
performance of acid sites properties and their accessibility[J]. Journal
图 9 Fe-Hβ-B 0.10 催化苯-氯化苄反应重复使用性 of Catalysis, 2014, 312(2): 46-57.
[11] Guo Yongle (郭永乐), Zhang Yu (张钰), Zhao Zhongkui (赵忠奎), et
Fig. 9 Reusability of benzene-benzyl chloride reaction al. Ceria-modified hierarchical Hβ zeolite as a robust solid acid
catalyzed by Fe-Hβ-B 0.10 catalyst for alkenylation of p-xylene with phenylacetylene[J].
Chinese Journal of Catalysis (催化学报), 2018, 39(1): 181-189.
由图 9 可知,催化剂使用次数增加后,氯化苄 [12] Bi Y, Lei X, Xu G, et al. Catalytic fast pyrolysis of kraft lignin over
hierarchical HZSM-5 and Hβ zeolites[J]. Catalysts, 2018, 8(2):
82-95.
的转化率略有降低,二苯甲烷的选择性有所提升。 [13] Zhang Kongyuan (张孔远), Zhao Xingtao (赵兴涛), Shi Shijie (史世
这可能是因为随着反应次数的增加,催化剂的活性 杰), et al. Hydroisomerization of n-hexane over Pt/Hβ-HZSM-5
catalyst[J]. Acta Petrolei Sinica (Petroleum Processing Section) (石
组分流失,催化剂活性降低,从而降低了反应物的 油学报: 石油加工), 2017, 33(2): 204-209.
[14] Khan A, Chen P, Boolchand P, et al. Modified nano-crystalline
转化率。活性组分的流失在一定程度上降低了二苯 ferrites for high-temperature WGS membrane reactor applications[J].
Journal of Catalysis, 2008, 253(1): 91-104.
甲烷深度苄基化的发生,从而选择性有所增加。重 [15] Yang Jing (杨静), Ming Yang (明阳), Sun Yu (孙宇), et al.
Preparation and adsorption desulfurization performance of
复使用 3 次后催化剂依然保持较高的催化能力。说 Cu-β/SBA-15 composite molecular sieves[J]. Acta Petrolei Sinica
明催化剂具有优良的稳定性。 (Petroleum Processing Section) (石油学报: 石油加工), 2017, 33(5):
919-926.
[16] Liu J, Cui L, Wang L, et al. Alkaline-acid treated mordenite and beta
3 结论 zeolites featuring mesoporous dimensional uniformity[J]. Materials
Letters, 2014, 132(10): 78-81.
[17] Li Yuping (李宇萍), Wang Tiejun (王铁军), Ma Longlong (马隆龙),
(1)采用碱处理制备了多级孔 Hβ,采用浸渍法 et al. Hβ modified Co/SiO 2 catalysts for Fischer-Tropsch synthesis of
jet fuel-range hydrocarbons[J]. Journal of Inorganic Materials (无机
制备了 Fe-多级孔 Hβ,并对其进行了表征,结果表 材料学报), 2014, 29(6): 599-604.
[18] Zeng Maorong (曾茂荣), Luo Gang (罗刚), Wang Yu (王宇), et al.
明,Hβ 经过碱处理脱除骨架硅形成介孔,Fe 的负 Quaternary ammonium surfactant assisted synthesis of hierarchical
porous Hβ zeolite for aniline catalytic condensation[J]. Journal of
载没有破坏多级孔 Hβ 的结构。 Chemical Engineering of Chinese Universities (高校化学工程学报),
2017, 31(5): 1113-1119.
(2)在反应温度 75 ℃、反应时间 20 min、苯 [19] He Jiajie (何嘉杰), Zhu Baokun (朱保昆), Wu Jiacan (吴家灿), et al.
Effect of surface modification by H 2 reduction on geranylacetone
与氯化苄物质的量比为 6∶1、催化剂用量为氯化苄 adsorption and desorption of modified Hβ zeotiles[J]. Ion Exchange
and Adsorption (离子交换与吸附), 2017, 33(5): 463-471.
质量的 2%的条件下,Fe-多级孔 Hβ 的苯-氯化苄烷 [20] Guo Haiwei (郭海纬), Fei Zhaoyan (费兆阳), Wang Yu (王宇), et al.
基化性能为:氯化苄转化率 99.7%,二苯甲烷选择 Effect of alkali treatment on the catalytic performance of Hβ zeolites
in condensation of aniline to diphenylamine[J]. Acta Petrolei Sinica
性 81.2%。 (Petroleum Processing Section) (石油学报: 石油加工), 2017, 33(1):
100-107.
(3)Fe-多级孔 Hβ 分子筛是一种良好的催化合 [21] Yang C, Xu Q H. States of aluminum in zeolite β and influence of
acidic or basic medium [J]. Zeolites, 1997, 19(5): 404-410.
成二苯甲烷的催化剂,具有较高的催化活性和较好 [22] Wang Junfeng (王俊丰), Shen Jian (沈健), Shi Weiwei (石薇薇), et
al. Experimental study on the catalytic alkylation of phenol with
的稳定性,有着广阔的应用前景。 methanol by Ce/USY modified molecular sieve[J]. Acta Petrolei
Sinica (Petroleum Processing Section) (石油学报: 石油加工), 2017,
参考文献: 33(4): 757-762.
[23] Xiang Shouhe (项寿鹤), Wang Jingzhong (王敬中), Gao Feng (高
[1] Zhan Jinyou (詹金友), Zhang Yaobing (张耀兵), Shen Jian (沈健), 峰), et al. Study on L acid on Hβ zeolite[J]. Chinese Journal of
et al. Synthesis of diphenylmethane on Sb-SBA-15[J]. Chemical Catalysis (催化学报), 1991, 12(5): 404-408.
Industry and Engineering Progress ( 化工进展 ), 2016, 35(5): [24] Yang Juhong (杨菊红), Han Xiaoxiang (韩晓祥), Chen Qing (陈青),
1460-1465. et al. Synthesis of diphenylmethane by alkylation of benzene with
[2] Zhou Chunhui (周春晖), Luo Xiping (罗锡平), Ge Zhonghua (葛忠 benzyl chloride by ionic liquid[J]. Fine Chemicals (精细化工), 2010,
华), et al. Preparation of acid-treated clay-supported ZnCl 2 and its 27(6): 610-613.