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学科主题: 物理化学
题名: Sustainable Synthesis of Zeolites without Addition of Both Organotemplates and Solvents
作者: Wu, Qinming1;  Wang, Xiong1;  Qi, Guodong2;  Guo, Qiang;  Pan, Shuxiang1;  Meng, Xiangju1;  Xu, Jun2;  Deng, Feng2;  Fan, Fengtao3;  Feng, Zhaochi3;  Li, Can3;  Maurer, Stefan4;  Mueller, Ulrich4;  Xiao, Feng-Shou1
通讯作者: 孟祥举 ;  李灿 ;  肖丰收
刊名: JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
发表日期: 2014-03-12
DOI: 10.1021/ja500098j
卷: 136, 期:10, 页:4019-4025
收录类别: SCI
文章类型: Article
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Multidisciplinary
研究领域[WOS]: Chemistry
英文摘要: The development of sustainable and environmentally friendly techniques for synthesizing zeolites has attracted much attention, as the use of organic templates and solvents in the hydrothermal synthesis of zeolites is a major obstacle for realizing green and sustainable synthesis ways. Recently, the introduction of the organotemplate-free synthesis method allowed avoiding the use of organic templates, but water as solvent was still required; solvent-free routes on the other hand beared the potential to significantly reduce the amount of polluted wastewater, but organic templates were still present. In this work, we have demonstrated a combined strategy of both organotemplate- and solvent-free conditions to synthesize aluminosilicate zeolites Beta and ZSM-5 (S-Beta and S-ZSM-5), two of the most important zeolites relevant for industry. The samples are thoroughly characterized by XRD patterns, SEM images, N-2 sorption isotherms, UV-Raman spectra, and Si-29 and Al-27 MAS NMR spectra. The results demonstrate that S-Beta and S-ZSM-5 zeolites exhibit almost the same textural parameters (e.g., BET surface area and pore volume) and catalytic performance in cumene cracking and m-xylene isomerization as those of conventional Beta and ZSM-5 zeolites synthesized under hydrothermal conditions (C-Beta and C-ZSM-5). The organotemplate- and solvent-free syntheses of S-Beta and S-ZSM-5 take place at a low-pressure regime and are free of harmful gases as well as give high product yields together with highly efficient consumption of the starting raw materials. These advantages plus the very simple procedures opened the pathway to a highly sustainable zeolite synthesis protocol compared to conventional methods currently employed for C-Beta and C-ZSM-5. Very interestingly, this simple synthesis is a good model for understanding zeolite crystallization. The detail characterizations indicate that the S-Beta crystals are formed from the assembly of zeolite building units, mainly 4MRs, while the SMRs in the framework are just formed in the crystallization of S-ZSM-5, rather than existence in the starting solid mixture. During the crystallization processes, small traces of water play an important role for the hydrolysis and condensation of silica and/or aluminosilicate species.
关键词[WOS]: SEED-ASSISTED SYNTHESIS ;  TEMPLATE-FREE SYNTHESIS ;  OSDA-FREE SYNTHESIS ;  SDA-FREE SYNTHESIS ;  MTW-TYPE ZEOLITE ;  IONOTHERMAL SYNTHESIS ;  MOLECULAR-SIEVE ;  BETA-ZEOLITE ;  HYDROTHERMAL SYNTHESIS ;  EMERGING APPLICATIONS
语种: 英语
WOS记录号: WOS:000332922600047
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/143857
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Zhejiang Univ, Key Lab Appl Chem Zhejiang Prov, Dept Chem, Hangzhou 310007, Zhejiang, Peoples R China
2.Chinese Acad Sci, Wuhan Inst Phys & Math, State Key Lab Magnet Resonance & Atom & Mol Phys, Wuhan Ctr Magnet Resonance, Wuhan 430071, Peoples R China
3.Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
4.BASF SE, D-67056 Ludwigshafen, Germany

Recommended Citation:
Wu, Qinming,Wang, Xiong,Qi, Guodong,et al. Sustainable Synthesis of Zeolites without Addition of Both Organotemplates and Solvents[J]. JOURNAL OF THE AMERICAN CHEMICAL SOCIETY,2014,136(10):4019-4025.
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