This paper reports the reactions of a monomeric aluminum dihydride LAlH2(L=HC[C(Me)N(Ar)]2,Ar=2,6-i-Pr2C6H3)with diazo,azido,and terminal alkyne compounds.The reaction of LAlH2 with N2CH(SiMe3)and N3(1-Ad)occurred thr...This paper reports the reactions of a monomeric aluminum dihydride LAlH2(L=HC[C(Me)N(Ar)]2,Ar=2,6-i-Pr2C6H3)with diazo,azido,and terminal alkyne compounds.The reaction of LAlH2 with N2CH(SiMe3)and N3(1-Ad)occurred through an Al-H addition to end-on nitrogen to yield respective compounds LAl[N(H)N=CH(SiMe3)]2(1)and LAl[N(H)N=N(1-Ad)]2(2),while the reaction of LAlH2 with PhC≡CH occurred through a stepwise deprotonation to yield LAlH(C≡CPh)(5)and LAl-(C≡CPh)2(6),respectively.2 further reacted by N2-release to yield LAl[NH(1-Ad)][N(H)N=N(1-Ad)](3)and LAl[NH-(1-Ad)]2(4)upon the increased temperature treatment.Compounds 1-6 have been fully characterized,revealing novel reactivity patterns of LAlH2 toward different substrates under the steric influence from the bulky L ligand at Al.展开更多
In this work,Ni-Bi-B alloy has been synthesized via chemical synthesis method.A new kind of Al-InCl3-(Ni-Bi-B)composite has been prepared by high energy mechanical ball grinding A1 powder with additives.Results show t...In this work,Ni-Bi-B alloy has been synthesized via chemical synthesis method.A new kind of Al-InCl3-(Ni-Bi-B)composite has been prepared by high energy mechanical ball grinding A1 powder with additives.Results show that the doped Ni-Bi-B alloy can significantly improve the hydrogen generation performance of Al-InCl3 and the catalytic activity is enhanced with the increasing content of Bi in Ni-Bi-B alloy.Under optimal conditions,the hydrogen generation yield and conversion yield of Al-InCl3-(Ni-Bi-B)reached1196.8 mL g^-1 and 100.0%at room temperature,respectively.Mechanism study shows five kinds of active sites,such as the fresh surface/defect of Al particle,Al-AlCl3,Al-In,Al-Bi/B and Al-Ni/B produced during the ball milling process.Their synergistic effect enhances the hydrogen generation performance of AlInCl3-(Ni-Bi-B)remarkably.In general,the proposed Al-InCl3-(Ni-Bi-B)composite is possible to serve as hydrogen generation material for fuel cells.展开更多
基金supported by the National Natural Science Foundation of China(20842006,20972129,and 20902112)China Postdoctoral Science Foundation(20090460748)+1 种基金the Fund for New Teacher of Higher Education(200803841012)the Project Sponsored by SRF for ROCS,SEM(2009060011500466)
文摘This paper reports the reactions of a monomeric aluminum dihydride LAlH2(L=HC[C(Me)N(Ar)]2,Ar=2,6-i-Pr2C6H3)with diazo,azido,and terminal alkyne compounds.The reaction of LAlH2 with N2CH(SiMe3)and N3(1-Ad)occurred through an Al-H addition to end-on nitrogen to yield respective compounds LAl[N(H)N=CH(SiMe3)]2(1)and LAl[N(H)N=N(1-Ad)]2(2),while the reaction of LAlH2 with PhC≡CH occurred through a stepwise deprotonation to yield LAlH(C≡CPh)(5)and LAl-(C≡CPh)2(6),respectively.2 further reacted by N2-release to yield LAl[NH(1-Ad)][N(H)N=N(1-Ad)](3)and LAl[NH-(1-Ad)]2(4)upon the increased temperature treatment.Compounds 1-6 have been fully characterized,revealing novel reactivity patterns of LAlH2 toward different substrates under the steric influence from the bulky L ligand at Al.
基金supported by the National Key R&D Program of China(2018YFB1501200,MOST)the National Natural Science Foundation of China(5187011196,U1501242 and 51671062)+4 种基金the Guangxi Collaborative Innovation Centre of Structure and Property for New Energy and Material(2012GXNSFGA06002)Guangxi Science and Technology Project(AD17195073)Guangxi Major Science and Technology Special Project(AA17202030-1)the Guangxi Key Laboratory of Information Laboratory Foundation(161002-Z,161002-K and 161003-K)the financial support of Guangxi Advanced Functional Materials Foundation and Application Talents Small Highlands
文摘In this work,Ni-Bi-B alloy has been synthesized via chemical synthesis method.A new kind of Al-InCl3-(Ni-Bi-B)composite has been prepared by high energy mechanical ball grinding A1 powder with additives.Results show that the doped Ni-Bi-B alloy can significantly improve the hydrogen generation performance of Al-InCl3 and the catalytic activity is enhanced with the increasing content of Bi in Ni-Bi-B alloy.Under optimal conditions,the hydrogen generation yield and conversion yield of Al-InCl3-(Ni-Bi-B)reached1196.8 mL g^-1 and 100.0%at room temperature,respectively.Mechanism study shows five kinds of active sites,such as the fresh surface/defect of Al particle,Al-AlCl3,Al-In,Al-Bi/B and Al-Ni/B produced during the ball milling process.Their synergistic effect enhances the hydrogen generation performance of AlInCl3-(Ni-Bi-B)remarkably.In general,the proposed Al-InCl3-(Ni-Bi-B)composite is possible to serve as hydrogen generation material for fuel cells.
