Stick-like mesoporous titania loaded Pd as highly active and cost effective catalysts for hydrodebenzylation of hexabenzylhexaazaisowurtzitane (HBIW)

doi:10.1016/j.mcat.2019.110556

	Stick-like mesoporous titania loaded Pd as highly active and cost effective catalysts for hydrodebenzylation of hexabenzylhexaazaisowurtzitane (HBIW)
	Liu, Shuang 1; Ji, Fei 1; Li, Xiaoyu 2; Pan, Xiaoli 2; Chen, Shuyuan 1; Wang, Xuefei 1; Zhang, Yanhua 3; Men, Yong 1
刊名	MOLECULAR CATALYSIS
	2019-10-01
卷号	477 页码:12
关键词	Catalytic hydrogenolysis Debenzylation CL-20 Pd catalyst Titania
ISSN号	2468-8231
DOI	10.1016/j.mcat.2019.110556
通讯作者	Men, Yong(men@sues.edu.cn)
英文摘要	Hydrodebenzylation of hexabenzylhexaazaisowurtzitane (HBIW) is one key step for the synthesis of High Energy Density Compound CL-20 (hexanitrohexaazaisowurtzitane). Design of a "high atom economy" debenzylation catalyst to promote the industry production and massive use in the fields of aerospace and military has attracted great attentions. Herein, we designed a catalyst of stick-like mesoporous titania supported ultrafine Pd nanoparticles with low loading 2 wt.% using a hydrothermal and then deposition-precipitation method. The supports and catalysts were thoroughly characterized by N-2 physisorption, X-ray diffraction (XRD), scanning electron microscopy (SEM), high resolution transmission electron microscopy (HRTEM), Raman, ultraviolet-visible absorption (UV-vis), in situ diffuse reflectance infrared Fourier transform (DRIFT), H-2 chemisorption to determine their physical and chemical properties. The results revealed that stick-like titania (ST) treated at low temperature showed rutile crystalline structure, large interplanar spacing (3.2394 angstrom) and surface area (53 m(2)/g), small average crystallite size (63 nm) with mesoporous. The Pd can deposit into the interstices and lattice of ST and displayed ultrafine and even sub-nanometer sizes (average value 1.2 nm), and high dispersion. The Pd/ST-2 exhibited particularly high activity for hydrodebenzylation of HBIW. The product TADBIW was obtained in a high turnover number (TON) 107, which is 2 (similar to) 5 times higher than those of conventional Pd/C catalysts. This work paves a promising way to develop highly efficient catalysts with low loading of Pd and high atomic utilization for cost-effective synthesis of CL-20.
资助项目	National Natural Science Foundation of China[21503264] ; National Natural Science Foundation of China[21503133] ; Science and Technology Commission of Shanghai Municipality[18030501100] ; Shanghai Talent Development Foundation[2017076] ; Natural Science Foundation of Hebei Province of China[B2017202182] ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Talent Program of Shanghai University of Engineering Science
WOS关键词	REDUCTIVE DEBENZYLATION ; NANOCOMPOSITE CATALYSTS ; HETEROGENEOUS REDUCTION ; PALLADIUM CATALYST ; CARBON SUPPORTS ; N-DEBENZYLATION ; PARTICLE-SIZE ; KEY STEP ; EFFICIENT ; HYDROGENATION
WOS研究方向	Chemistry
语种	英语
出版者	ELSEVIER
WOS记录号	WOS:000487172800011
资助机构	National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Commission of Shanghai Municipality ; Science and Technology Commission of Shanghai Municipality ; Shanghai Talent Development Foundation ; Shanghai Talent Development Foundation ; Natural Science Foundation of Hebei Province of China ; Natural Science Foundation of Hebei Province of China ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Talent Program of Shanghai University of Engineering Science ; Talent Program of Shanghai University of Engineering Science ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Commission of Shanghai Municipality ; Science and Technology Commission of Shanghai Municipality ; Shanghai Talent Development Foundation ; Shanghai Talent Development Foundation ; Natural Science Foundation of Hebei Province of China ; Natural Science Foundation of Hebei Province of China ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Talent Program of Shanghai University of Engineering Science ; Talent Program of Shanghai University of Engineering Science ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Commission of Shanghai Municipality ; Science and Technology Commission of Shanghai Municipality ; Shanghai Talent Development Foundation ; Shanghai Talent Development Foundation ; Natural Science Foundation of Hebei Province of China ; Natural Science Foundation of Hebei Province of China ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Talent Program of Shanghai University of Engineering Science ; Talent Program of Shanghai University of Engineering Science ; National Natural Science Foundation of China ; National Natural Science Foundation of China ; Science and Technology Commission of Shanghai Municipality ; Science and Technology Commission of Shanghai Municipality ; Shanghai Talent Development Foundation ; Shanghai Talent Development Foundation ; Natural Science Foundation of Hebei Province of China ; Natural Science Foundation of Hebei Province of China ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Program for Professor of Special Appointment (Eastern Scholar) at Shanghai Institutions of Higher Learning ; Talent Program of Shanghai University of Engineering Science ; Talent Program of Shanghai University of Engineering Science
内容类型	期刊论文
源URL	[http://cas-ir.dicp.ac.cn/handle/321008/172852]
专题	大连化学物理研究所_中国科学院大连化学物理研究所
通讯作者	Men, Yong
作者单位	1.Shanghai Univ Engn Sci, Coll Chem & Chem Engn, Shanghai 201620, Peoples R China 2.Chinese Acad Sci, Dalian Inst Chem Phys, Dalian 116023, Peoples R China 3.Hebei Univ Technol, Tianjin 300401, Peoples R China
推荐引用方式 GB/T 7714	Liu, Shuang,Ji, Fei,Li, Xiaoyu,et al. Stick-like mesoporous titania loaded Pd as highly active and cost effective catalysts for hydrodebenzylation of hexabenzylhexaazaisowurtzitane (HBIW)[J]. MOLECULAR CATALYSIS,2019,477:12.
APA	Liu, Shuang.,Ji, Fei.,Li, Xiaoyu.,Pan, Xiaoli.,Chen, Shuyuan.,...&Men, Yong.(2019).Stick-like mesoporous titania loaded Pd as highly active and cost effective catalysts for hydrodebenzylation of hexabenzylhexaazaisowurtzitane (HBIW).MOLECULAR CATALYSIS,477,12.
MLA	Liu, Shuang,et al."Stick-like mesoporous titania loaded Pd as highly active and cost effective catalysts for hydrodebenzylation of hexabenzylhexaazaisowurtzitane (HBIW)".MOLECULAR CATALYSIS 477(2019):12.