Catalytic Dehydrogenation of Ammonia Borane Mediated by a Pt(0)/Borane Frustrated Lewis Pair: Theoretical Design

被引：5

作者：

Zhang, Lei ^{[1
,2
]}

Oishi, Takumi ^{[3
]}

Gao, Liuzhou ^{[6
]}

Hu, Shiyu ^{[6
]}

Yang, Linlin ^{[1
,2
]}

Li, Wei ^{[6
]}

Wu, Shengjun ^{[1
,2
]}

Shang, Rong ^{[3
]}

Yamamoto, Yohsuke ^{[3
]}

Li, Shuhua ^{[6
]}

Wang, Wei ^{[4
,5
]}

Zeng, Guxiang ^{[1
,2
]}

机构：

[1] Nanjing Univ, Kuang Yaming Honors Sch, Nanjing 210023, Peoples R China

[2] Nanjing Univ, Inst Brain Sci, Nanjing 210023, Peoples R China

[3] Hiroshima Univ, Grad Sch Sci, Dept Chem, Higashihiroshima 7398526, Japan

[4] Nanjing Univ, Kuang Yaming Honors Sch, Nanjing 210023, Peoples R China

[5] Nanjing Univ, Inst Brain Sci, Inst Biophys, Sch Phys, Nanjing 210023, Peoples R China

[6] Nanjing Univ, Sch Chem & Chem Engn, Inst Theoret & Computat Chem, Nanjing 210023, Peoples R China

来源：

CHEMPHYSCHEM | 2020年 / 21卷 / 23期

基金：

国家重点研发计划; 中国国家自然科学基金;

关键词：

ammonia borane; catalysis; dehydrogenation; frustrated Lewis pair; theoretical prediction; BORON-NITROGEN BONDS; AMINE-BORANES; DENSITY FUNCTIONALS; DEHYDROCOUPLING REACTIONS; THERMOCHEMICAL KINETICS; THERMAL-DECOMPOSITION; HYDROGEN ACTIVATION; IN-SITU; COMPLEXES; MECHANISM;

D O I：

10.1002/cphc.202000661

中图分类号：

O64 [物理化学（理论化学）、化学物理学];

学科分类号：

070304 ; 081704 ;

摘要：

A new efficient metal-based frustrated Lewis pair constructed by ((PBu3)-Bu-t)(2)Pt and B(C6F5)(3) was designed through density functional theory calculations for the catalytic dehydrogenation of ammonia borane (AB). The reaction was composed by the successive dehydrogenation of AB and H-2 liberation, which occurs through the cooperative functions of the Pt(0) center and the B(C6F5)(3) moiety. Two equivalents of H-2 were predicted to be liberated from each AB molecule. The generation of the second H2 is the rate-determining step, with a Gibbs energy barrier and reaction energy of 27.4 and 12.8 kcal/mol, respectively.

引用

页码：2573 / 2578

页数：6

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