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Structures and Stability of Metal Amidoboranes (MAB): Density Functional Calculations
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作者 李采临 吴朝铃 +4 位作者 陈云贵 周晶晶 郑欣 庞丽娟 邓刚 《Communications in Theoretical Physics》 SCIE CAS CSCD 2010年第6期1167-1171,共5页
Molecule geometry structures, frequencies, and energetic stabilities of ammonia borane (AB, NH3BH3 ) and metal amidoboranes (MAB, MNH2BH3), formed by substituting H atom in AB with one of main group metal atoms, h... Molecule geometry structures, frequencies, and energetic stabilities of ammonia borane (AB, NH3BH3 ) and metal amidoboranes (MAB, MNH2BH3), formed by substituting H atom in AB with one of main group metal atoms, have been investigated by density-functional theory and optimized at the B3LYP levels with 6-311G++ (3dr, 3pd) basic set. Their structural parameters and infrared spectrum characteristic peaks have been predicted, which should be the criterion of a successfully synthesized material. Several parameters such as binding energies, vibrational frequencies, and the energy gaps between the HOMO and the LUMO have been adopted to characterize and evaluate their structure stabilities. It is also found that the binding energies and HOMO-LUMO energy gaps of the MAB obviously change with the substitution of the atoms. MgAB has the lowest binding energy and is easier to decompose than any other substitutional structures under same conditions, while CaAB has the highest chemical activity. 展开更多
关键词 ammonia borane metal amidoboranes hydrogen storage density functional theory
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Superatom-assembled boranes,carboranes,and low-dimensional boron nanomaterials based on aromatic icosahedral B_(12)and C_(2)B_(10)
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作者 Qiao-Qiao Yan Yan-Fang Wei +2 位作者 Qiang Chen Yue-Wen Mu Si-Dian Li 《Nano Research》 SCIE EI CSCD 2024年第7期6734-6740,共7页
Using the experimentally known aromatic icosahedral superatoms I_(h)B_(12)H_(12)2−and D_(5d)1,12-C_(2)B_(10)H_(12)as building blocks and based on extensive density functional theory calculations,we predict herein a se... Using the experimentally known aromatic icosahedral superatoms I_(h)B_(12)H_(12)2−and D_(5d)1,12-C_(2)B_(10)H_(12)as building blocks and based on extensive density functional theory calculations,we predict herein a series of core–shell superpolyhedral boranes and carboranes in a bottom-up approach,including the high-symmetry Th B_(12)@B_(152)H_(72)2−(2),C2h C_(2)B_(10)@B_(152)H_(72)(3),D_(3d)B_(12)@B_(144)H_(66)(4),I_(h)B_(12)@C_(24)B_(12)0H_(72)2−(6),and D_(5d)C_(2)B_(10)@C_(24)B_(12)0H_(72)(7).More interestingly,the superatom-assembled linear D2h B_(36)H_(32)^(2−)(8),close-packed planar D_(3d)B_(84)H_(60)^(2−)(10),and nearly close-packed core−shell D_(3d)B_(12)@B144H_(6)6(4)can be extended periodically to form the one-dimensional(1D)α-rhombohedral borane nanowire B_(12)H_(10)(Pmmm)(9),two-dimensional(2D)α-rhombohedral monolayer borophane B_(12)H_(6)(P m1)(11),and the experimentally known three-dimensional(3D)α-rhombohedral boron(R m)(12)which can be viewed as an assembly of the monolayer B_(12)H_(6)(11)staggered in vertical direction,setting up a bottom-up strategy to form low-dimensional boron-based nanomaterials from their borane“seeds”via partial or complete dehydrogenations.Detailed bonding analyses indicate that the high stability of these nanostructures originates from the spherical aromaticity of their icosahedral B_(12)or C_(2)B_(10)structural units which possess the universal skeleton electronic configuration of 1S21P61D101F8 following the Wade’s n+1 rule.The infrared(IR)and Raman spectra of the most-concerned neutral B_(12)@B144H_(6)6(4)and C_(2)B_(10)@C_(24)B_(12)0H_(72)(7)are computationally simulated to facilitate their experimental characterizations. 展开更多
关键词 superatom-assembling bottom-up approach density functional theory superpolyhedral boranes superpolyhedral carboranes borophanes
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Asymmetric Hydrogenation of Phenanthridines with Chiral Boranes
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作者 Guangyu Cui Xiangqing Feng Haifeng Du 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2024年第6期631-635,共5页
The asymmetric hydrogenation of N-heteroarenes provides an efficient method for the synthesis of optically active cyclic secondary amines.In this paper,we described an asymmetric hydrogenation of phenanthridines using... The asymmetric hydrogenation of N-heteroarenes provides an efficient method for the synthesis of optically active cyclic secondary amines.In this paper,we described an asymmetric hydrogenation of phenanthridines using a chiral mono-alkene-derived borane.A variety of dihydrophenanthridines were furnished in high yields with up to 93%ee.The current catalytic system was very sensitive for the steric hindrance of phenanthridines.Bulky substituents at one phenyl group of phenanthridines were required to obtain the high enantioselectivity.But large substituents on the carbon of the C=N bonds would diminish the reactivity sharply. 展开更多
关键词 Asymmetric catalysis HYDROGENATION Nitrogen heterocycles PHENANTHRIDINES Frustrated Lewis pairs Chiral boranes
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Integration of morphology and electronic structure modulation on cobalt phosphide nanosheets to boost photocatalytic hydrogen evolution from ammonia borane hydrolysis 被引量:2
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作者 Chao Wan Yu Liang +5 位作者 Liu Zhou Jindou Huang Jiapei Wang Fengqiu Chen Xiaoli Zhan Dang-guo Cheng 《Green Energy & Environment》 SCIE EI CAS CSCD 2024年第2期333-343,共11页
The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for ... The controllable and safe hydrogen storage technologies are widely recognized as the main bottleneck for the accomplishment of sustainable hydrogen energy.Ammonia borane(AB)has regarded as a competitive candidate for chemical hydrogen storage.However,developing efficient yet high-performance catalysts towards hydrogen evolution from AB hydrolysis remains an enormous challenge.Herein,cobalt phosphide nanosheets are synthesized by a facile salt-assisted along with low-temperature phosphidation strategy for simultaneously modulating its morphology and electronic structure,and function as hydrogen evolution photocatalysts.Impressively,the Co_(2)P nanosheets display extraordinary performance with a record high turnover frequency of 44.9 min^(-1),outperforming most of the noble-metal-free catalysts reported to date.This remarkable performance is attributed to its desired nanosheets structure,featuring with high specific surface area,abundant exposed active sites,and short charge diffusion paths.Our findings provide a novel strategy for regulating metal phosphides with desired phase structure and morphology for energy-related applications and beyond. 展开更多
关键词 Ammonia borane Hydrogen generation HYDROLYSIS Cobalt phosphide nanosheets PHOTOCATALYSIS
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Integrating theory with the nanoreactor concept to synthesize hollow carbon sphere-encapsulated PtNi alloys for enhanced H_(2) generation
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作者 Yufeng Wu Minwei Song +3 位作者 Ziyi Zhao Guang-Hui Wang Changlong Wang Didier Astruc 《Carbon Energy》 SCIE EI CAS CSCD 2024年第7期150-162,共13页
The rational design of efficient bimetallic nanoparticle(NP)catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction.Here,we re... The rational design of efficient bimetallic nanoparticle(NP)catalysts is challenging due to the lack of theoretical understanding of active components and insights into the mechanisms of a specific reaction.Here,we report the rational design of nanoreactors comprising hollow carbon sphere-confined PtNi bimetallic NPs(PtNi@HCS)as highly efficient catalysts for hydrogen generation via ammonia borane hydrolysis in water.Using both density functional theory calculations and molecular dynamics simulations,the effects of an active PtNi combination and the critical synergistic role of a hollow carbon shell on the molecule diffusion adsorption behaviors are explored.Kinetic isotope effects and theoretical calculations allow the clarification of the mechanism,with oxidative addition of an O-H bond of water to the catalyst surface being the rate-determining step.The remarkable catalytic activity of the PtNi@HCS nanoreactor was also utilized for successful tandem catalytic hydrogenation reactions,using in situ-generated H_(2) from ammonia borane with high efficiency.The concerted design,theoretical calculations,and experimental work presented here shed light on the rational elaboration of efficient nanocatalysts and contribute to the establishment of a circular carbon economy using green hydrogen. 展开更多
关键词 ammonia borane hydrogen NANOALLOY NANOREACTOR solid catalyst
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B(C_(6)F_(5))_(3)-Catalyzed Hydroboration of Alkenes with N-Heterocyclic Carbene Boranes via B-H Bond Activation
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作者 Qiaotian Wang Wei Meng +1 位作者 Xiangqing Feng Haifeng Du 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2021年第4期918-926,共9页
Main observation and conclusion In this work,a novel mode for the activation of N-heterocyclic carbene boranes(NHC-boranes)was developed by generating the highly reactive zwitterion species through hydride abstraction... Main observation and conclusion In this work,a novel mode for the activation of N-heterocyclic carbene boranes(NHC-boranes)was developed by generating the highly reactive zwitterion species through hydride abstraction with Lewis acid B(C_(6)F_(5))_(3) in an frustrated Lewis pairs manner.A broad range of alkenes including stilbenes,β-methylstyrenes,styrenes,and alkyl-alkenes were suitable substrates for the B(C_(6)F_(5))_(3)-catalyzed hydroboration to furnish the desired products in good to high yields.Significantly,excellent regioselectivities were obtained in some cases.Mechanistic studies indicate that the B-H bond cleavage is likely involved in the rate-determining step.In addition,an electrophilic addition of NHC-borenium cation to alkenes and the subsequent formation of carbocation are also postulated.The current work provides a promising method for the activation of stable borane adducts,which might lead to some interesting transformations in the future. 展开更多
关键词 Frustrated Lewis pairs HYDROBORATION B-H bond activation boranes ALKENES
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Bonding of the chain structure for novel boranes B_(3k+)H_(5k+p+3)^-
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作者 ZHONG, Shi-Jun WANG, Yin-Gui ZHANG, Qian-ErState Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Science, Fuzhou, Fujian 350002, China.Department of Chemistry, and Institute of Physical Chemistry, Xiamen University, Xiamen, Fujian 361005, China 《Chinese Journal of Chemistry》 SCIE CAS CSCD 1994年第4期289-294,共6页
The molecular orbitals obtained from conventional quantum chemistry calculations, are expressed in terms of symmetrized valence bond functions of fragment, and a direct picture of chemical bonding can be drawn easily.... The molecular orbitals obtained from conventional quantum chemistry calculations, are expressed in terms of symmetrized valence bond functions of fragment, and a direct picture of chemical bonding can be drawn easily. This method is utilized, together with extended Huckel calculations, to interpret the bonding properties of a centipede-like chain structure for novel laser-producing boranes B3k+pH5k+p+3- which is constructed from the repeated unit B3H5 linked to each other by three B-H-B bonds. 展开更多
关键词 Symmetrized valence bond function bridge bond novel boranes.
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Zwitterionic Hydroboranes Stabilized by β-Diimine Framework
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作者 Jianfeng Li Hongfan Hu Chunming Cui 《Chinese Journal of Chemistry》 SCIE CAS CSCD 2017年第6期886-888,共3页
Reaction of the N-heterocyclic borane [MeCCHC(CHe)(NAr)2]Btt (1, Ar=2,6-Me2C6H3) with B(C6F5)3 af- forded the zwitterionic hydroborane [MeCCHC(CHz)B(C6F5)3(NAr)2]BH, in which the β-methyl group can be d... Reaction of the N-heterocyclic borane [MeCCHC(CHe)(NAr)2]Btt (1, Ar=2,6-Me2C6H3) with B(C6F5)3 af- forded the zwitterionic hydroborane [MeCCHC(CHz)B(C6F5)3(NAr)2]BH, in which the β-methyl group can be deprotonated with LiN(SiMe3)2 to yield an anionic zwitterionic borenium. 展开更多
关键词 BORANE CATION ZWITTERION DIIMINE DEPROTONATION
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Dehydrocoupling of boranes with amines using a scandium catalyst
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作者 Yang Wang Pengfei Xu Xin Xu 《Chinese Chemical Letters》 SCIE CAS CSCD 2021年第12期4002-4005,共4页
The scandocene alkyl complex(C_(5)Me_(5))_(2)ScCH_(2)SiMe_(3)was found to be an efficient catalyst for the dehydrocoupling of the non-cyclic boranes, dicyclohexylborane and thexylborane, with amines under mild conditi... The scandocene alkyl complex(C_(5)Me_(5))_(2)ScCH_(2)SiMe_(3)was found to be an efficient catalyst for the dehydrocoupling of the non-cyclic boranes, dicyclohexylborane and thexylborane, with amines under mild conditions. The reactions afforded the corresponding aminoboranes in high yields with good functional group tolerance. The stoichiometric reaction of scandium alkyl with amine led to the isolation of a scandium amide complex, which was shown to be an active species during the catalysis. Although a boranecoordinated scandium hydride was also obtained from the stoichiometric experiment, it was not involved in the catalytic cycle. In addition, kinetic studies provided insight into this intermolecular dehydrogenation reaction. 展开更多
关键词 BORANE Aminoborane DEHYDROCOUPLING SCANDIUM β-H elimination
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From Prediction to Realization:Synthesis and X-Ray Characterization of 15-and 16-Vertex closo-Carboranes
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作者 CUI Pengfei JIN Guoxin 《Chemical Research in Chinese Universities》 SCIE CAS CSCD 2021年第1期183-184,共2页
In order to solve the problem of the synthesis and structural characterization of 15-and 16-vertex closo-carboranes,Xie et al.introduce the method of using silyl groups to both cage carbons,stabilizing the correspondi... In order to solve the problem of the synthesis and structural characterization of 15-and 16-vertex closo-carboranes,Xie et al.introduce the method of using silyl groups to both cage carbons,stabilizing the corresponding nido-carborane dianions and promoting the capitation reaction with HBBr2·SMe2.This work demonstrates the exist of carboranes with more than 14 vertices and may open the door for further studying supercarborane chemistry. 展开更多
关键词 chemistry. BORANE VERTEX
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Anomalous metastable hcp Ni nanocatalyst induced by non-metal N doping enables promoted ammonia borane dehydrogenation 被引量:1
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作者 Ping Li Yuqi Huang +3 位作者 Quhua Huang Ran Chen Jixin Li Shuanghong Tian 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2023年第4期72-82,共11页
Developing high-performing non-noble transition metal catalysts for H_(2) evolution from chemical hydrogen storage materials is of great significance for the hydrogen economy system, yet challenging. Herein,we present... Developing high-performing non-noble transition metal catalysts for H_(2) evolution from chemical hydrogen storage materials is of great significance for the hydrogen economy system, yet challenging. Herein,we present for the first time that anomalous metastable hexagonal close-packed Ni nanoparticles induced by heteroatom N doping encapsulated in carbon(N-hcp-Ni/C) can exhibit admirable catalytic performance for ammonia borane(AB) dehydrogenation, prominently outperforming conventional fcc Ni counterpart with similar morphology and favorably presenting the state-of-the-art level.Comprehensive experimental and theoretical studies unravel that unusual hcp phase engineering of Ni together with N doping could induce charge redistribution and modulate electronic structure, thereby facilitating H_(2)O adsorption and expediting H_(2)O dissociation(rate-determining step). As a result, AB dehydrogenation can be substantially boosted with the assistance of N-hcp-Ni/C. Our proposed strategy highlights that unconventional crystal phase engineering coupled with non-metal heteroatom doping is a promising avenue to construct advanced transition metal catalysts for future renewable energy technologies. 展开更多
关键词 Hcp Ni Non-metal doping Phase engineering Electronic regulation Ammonia borane dehydrogenation
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Ammonia borane-enabled hydrogen transfer processes:Insights into catalytic strategies and mechanisms 被引量:1
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作者 Wenfeng Zhao Hu Li +2 位作者 Heng Zhang Song Yang Anders Riisager 《Green Energy & Environment》 SCIE EI CAS CSCD 2023年第4期948-971,共24页
Transfer hydrogenation(TH) with in situ generated hydrogen donor is of great importance in reduction reactions, and an alternative strategy to traditional hydrogenation processes involving pressurized molecular hydrog... Transfer hydrogenation(TH) with in situ generated hydrogen donor is of great importance in reduction reactions, and an alternative strategy to traditional hydrogenation processes involving pressurized molecular hydrogen. Ammonia borane(NH3BH3, AB) is a promising material of hydrogen storage, and it has attracted much attention in reductive organic transformations owing to its high activity, good atom economy, nontoxicity, sustainability, and ease of transport and storage. This review focuses on summarizing the recent progress of AB-mediated TH reactions of diverse substrates including nitro compounds, nitriles, imines, alkenes, alkynes, carbonyl compounds(ketones and aldehydes), carbon dioxide,and N-and O-heterocycles. Syntheses protocols(metal-containing and metal-free), the effect of reaction parameters, product distribution, and variation of reactivity are surveyed, and the mechanism of each reaction involving the action mode of AB as well as structure-activity relationships is discussed in detail. Finally, perspectives are presented to highlight the challenges and opportunities for AB-enabled TH reactions of unsaturated compounds. 展开更多
关键词 Transfer hydrogenation Ammonia borane Hydrogen donor Reaction mechanism Catalytic strategies
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Engineering Vacancy-Atom Ensembles to Boost Catalytic Activity toward Hydrogen Evolution 被引量:1
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作者 Ruofan Shen Yanyan Liu +8 位作者 Hao Wen Xianli Wu Zhikun Peng Sehrish Mehdi Tao Liu Huanhuan Zhang Shuyan Guan Erjun Liang Baojun Li 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第1期325-332,共8页
The dissociation of water is the rate-determining step of several energy-relating reactions due to high energy barrier in homolysis of H-O bond.Herein,engineering vacancy-atom ensembles via injecting oxygen vacancy(V ... The dissociation of water is the rate-determining step of several energy-relating reactions due to high energy barrier in homolysis of H-O bond.Herein,engineering vacancy-atom ensembles via injecting oxygen vacancy(V O)into single facet-exposed TiO_(2)-Pd catalyst to form V_(O)-Pd ensemble is proposed and implemented.The outstanding activity of as-prepared catalyst,1.5-PdTV_(O),toward water dissociation is established with a turnover frequency of 240 min^(−1) in ammonia borane hydrolysis at 298 K.Density functional theory simulation suggests that the V_(O)-Pd ensemble is responsible for the high intrinsic catalytic activity.Water molecules tend to be dissociated on V_(O) sites and ammonia borane molecules on Pd atoms.Those H atoms from water dissociation on V_(O) combine with H atoms from ammonia borane on Pd atoms to generate H_(2).This insights into engineering vacancy-atom ensembles catalysis provide a new avenue to design catalytic materials for important energy chemical reactions. 展开更多
关键词 ammonia borane hydrogen evolution PALLADIUM vacancy-atom ensembles water dissociation
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A step‐growth strategy to grow vertical porous aromatic framework nanosheets on graphene oxide:Hybrid material‐confined Co for ammonia borane methanolysis
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作者 Xiugang Li Qilu Yao +2 位作者 Rongwei Shi Minsong Huang Zhang‐Hui Lu 《Carbon Energy》 SCIE EI CAS CSCD 2023年第10期64-76,共13页
The rational synthesis of a two-dimensional(2D)porous aromatic framework(PAF)with a controllable growth direction remains a challenge to overcome the limitation of traditional stacked 2D materials.Herein,a step-growth... The rational synthesis of a two-dimensional(2D)porous aromatic framework(PAF)with a controllable growth direction remains a challenge to overcome the limitation of traditional stacked 2D materials.Herein,a step-growth strategy is developed to fabricate a vertically oriented nitrogen-rich porous aromatic framework on graphene oxide(V-PAF-GO)using monolayer benzidine-functionalized GO(BZ-GO)as a molecular pillar.Then,the confined Co nanoparticle(NP)catalysts are synthesized by encapsulating ultra-small Co into the slit pores of V-PAF-GO.Due to the high nitrogen content,large specific surface area,and adequate slit pores,the optimized vertical nanocomposites V-PAF-GO provide abundant anchoring sites for metal NPs,leading to ultrafine Co NPs(1.4 nm).The resultant Co/V-PAF-GO catalyst shows an extraordinary catalytic activity for ammonia borane(AB)methanolysis,yielding a turnover frequency value of 47.6 min−1 at 25°C,comparable to the most effective non-noble-metal catalysts ever reported for AB methanolysis.Experimental and density functional theory studies demonstrate that the electron-donating effect of N species of PAF positively corresponds to the low barrier in methanol molecule activation,and the cleavage of the O–H bond in CH3OH has been proven to be the rate-determining step for AB methanolysis.This work presents a versatile step-growth strategy to prepare a vertically oriented PAF on GO to solve the stacking problem of 2D materials,which will be used to fabricate other novel 2D or 2D–2D materials with controllable orientation for various applications. 展开更多
关键词 2D-2D materials ammonia borane graphene oxide METHANOLYSIS porous aromatic frameworks
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A Catalytic Copper/Cobalt Oxide Interface for Efficient Hydrogen Generation
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作者 Wenjing Xu Sheli Zhang +5 位作者 Ruofan Shen Zhikun Peng Baozhong Liu Jun Li Zhanying Zhang Baojun Li 《Energy & Environmental Materials》 SCIE EI CAS CSCD 2023年第2期1-7,共7页
Metal nanoparticles and metal oxides promisingly provide different catalytic active sites at their interfaces.Constructing high-density interfaces is essential to maximize synergies.Herein,a Cu-Co_(3)O_(4) nanoparticl... Metal nanoparticles and metal oxides promisingly provide different catalytic active sites at their interfaces.Constructing high-density interfaces is essential to maximize synergies.Herein,a Cu-Co_(3)O_(4) nanoparticles interfacial structure produced via pyrolysis and moderate oxidation from metal-organic frameworks has been designed to boost the intrinsic activity.The Cu-Co_(3)O_(4) nanoparticles composites exhibit a turnover frequency of 57.5 min−1 for ammonia borane hydrolysis,far higher than those of monometallic Cu and Co_(3)O_(4) nanoparticles,showing the synergistic effect of Cu and Co_(3)O_(4) nanoparticles at their interface.Density functional theory calculations and in situ Raman spectroscopy reveal the catalytic mechanism of dual active sites,in which Co_(3)O_(4) nanoparticles at Cu-Co_(3)O_(4) interface efficiently bind and activate water molecules and Cu nanoparticles easily activate NH3BH3 molecules.This study opens up a new pathway for achieving high-efficiency noble metal-free catalysts for hydrogen generation and other heterogeneous catalysis. 展开更多
关键词 ammonia borane METAL metal oxide metal-organic framework synergistic effect
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Production of Nanopowders of Platinum Metals Using the Chemical Reduction Method
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作者 PYATAKHINA E. S. BUSLAYEVA T. M. +2 位作者 VOLCHKOVA E. V. KHRISTICH E. A. ERGEYEVA T. Yu. 《贵金属》 CAS CSCD 北大核心 2012年第A01期267-268,共2页
The literary data on the application of various methods for the production of nanopowders of platinum metals and alloys have been summarized, and the selection of the method of chemical reduction from salt solutions h... The literary data on the application of various methods for the production of nanopowders of platinum metals and alloys have been summarized, and the selection of the method of chemical reduction from salt solutions has been substantiated as the simplest and most affordable. The optimum conditions for the production of nanoparticles of metal palladium and platinum/cobalt alloy, using the effect of boranes with various structures, have been selected. 展开更多
关键词 platinum metals POWDERS double complex salts REDUCTION boranes
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Gold-containing metal nanoparticles for catalytic hydrogen generation from liquid chemical hydrides 被引量:5
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作者 杨新春 徐强 《Chinese Journal of Catalysis》 SCIE EI CAS CSCD 北大核心 2016年第10期1594-1599,共6页
Liquid chemical hydrides, which store hydrogen in the form of chemical bonds, are considered one of the most promising classes of hydrogen storage materials. Their application depends heavily on the development of eff... Liquid chemical hydrides, which store hydrogen in the form of chemical bonds, are considered one of the most promising classes of hydrogen storage materials. Their application depends heavily on the development of efficient catalytic systems. Gold‐containing metal nanoparticles have exhibited excellent catalytic performance for hydrogen generation from liquid chemical hydrides. The present mini‐review focuses on recent developments in hydrogen generation from liquid chemical hydrides using gold‐nanoparticle and gold‐containing heterometallic nanoparticle catalysts. 展开更多
关键词 Gold catalysts Hydrogen generation Formic acid Ammonia borane Heterogeneous catalysis
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Bimetallic RuM(M=Co,Ni)Alloy NPs Supported on MIL-110(AI):Synergetic Catalysis in Hydrolytic Dehydrogenation of Ammonia Borane 被引量:2
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作者 宁红辉 鲁迪 +5 位作者 周立群 陈锰寰 李悦 周高建 彭薇薇 王峥 《Chinese Journal of Chemical Physics》 SCIE CAS CSCD 2018年第1期99-110,I0002,共13页
By adjusting various Ru/M (M=Co, Ni) molar ratios, a series of highly dispersed bimetallic RuM alloy nanoparticles (NPs) anchored on MIL-110(Al) have been successfully prepared via a conventional impregnation-re... By adjusting various Ru/M (M=Co, Ni) molar ratios, a series of highly dispersed bimetallic RuM alloy nanoparticles (NPs) anchored on MIL-110(Al) have been successfully prepared via a conventional impregnation-reduction method. And they are first used as heterogeneous catalysts for the dehydrogenation reaction of AB at room temperature. The results reveal that the as-prepared RulCo1@MIL-110 and RulNi1@MIL-110 exhibit the highest catalytic activities in different RuCo and RuNi molar ratios, respectively. It is worthy of note that the turnover frequency (TOF) values of Ru1Co1@MIL-110 and Ru1Ni1@MIL-110 catalysts reached 488.1 and 417.1 mol H2 min-1 (mol Ru)-1 and the activation energies (Ea) are 31.7 and 36.0 k J/tool, respectively. The superior catalytic performance is attributed to the bimetallic synergistic action between Ru and M, uniform distribution of metal NPs as well as bi-functional effect between RuM alloy NPs and MIL-110. Moreover, these catalysts exhibit favorable stability after 5 consecutive cycles for the hydrolysis of AB. 展开更多
关键词 RuCo@MIL-110 RuNi@MIL-110 Ammonia borane Hydrogen production
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Interface electron collaborative migration of Co–Co3O4/carbon dots:Boosting the hydrolytic dehydrogenation of ammonia borane 被引量:8
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作者 Han Wu Min Wu +5 位作者 Boyang Wang Xue Yong Yushan Liu Baojun Li Baozhong Liu Siyu Lu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2020年第9期43-53,I0002,共12页
Ammonia borane(AB)is an excellent candidate for the chemical storage of hydrogen.However,its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein,we re... Ammonia borane(AB)is an excellent candidate for the chemical storage of hydrogen.However,its practical utilization for hydrogen production is hindered by the need for expensive noble-metal-based catalysts.Herein,we report Co-Co3O4 nanoparticles(NPs)facilely deposited on carbon dots(CDs)as a highly efficient,robust,and noble-metal-free catalyst for the hydrolysis of AB.The incorporation of the multiinterfaces between Co,Co3O4 NPs,and CDs endows this hybrid material with excellent catalytic activity(rB=6816 mLH2 min^-1 gCo^-1)exceeding that of previous non-noble-metal NP systems and even that of some noble-metal NP systems.A further mechanistic study suggests that these interfacial interactions can affect the electronic structures of interfacial atoms and provide abundant adsorption sites for AB and water molecules,resulting in a low energy barrier for the activation of reactive molecules and thus substantial improvement of the catalytic rate. 展开更多
关键词 Ammonia borane Hydrogen evolution Co-Co3O4 interface Carbon dots Nanoparticles
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Carbon dots-confined CoP-CoO nanoheterostructure with strong interfacial synergy triggered the robust hydrogen evolution from ammonia borane 被引量:3
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作者 Han Wu Yaojia Cheng +5 位作者 Boyang Wang Yao Wang Min Wu Weidong Li Baozhong Liu Siyu Lu 《Journal of Energy Chemistry》 SCIE EI CAS CSCD 2021年第6期198-205,I0006,共9页
Ammonia borane(NH_(3)BH_(3),AB) is promising for chemical hydrogen sto rage;however,current systems for rapid hydrogen production are limited by the expensive noble metal catalysts required for AB hydrolysis.Here we r... Ammonia borane(NH_(3)BH_(3),AB) is promising for chemical hydrogen sto rage;however,current systems for rapid hydrogen production are limited by the expensive noble metal catalysts required for AB hydrolysis.Here we report the design and synthesis of a highly efficient and robust non-noble-metal catalyst for the hydrolysis of AB at 298 K(TOF=89.56 molH_(2) min^(-1) molCo^(-1)).Experiments and density functional theory calculations were performed to explore the catalyst’s hybrid nanoparticle heterostructure and its catalytic mechanism.The catalyst comprised nitrogen-doped carbon dots confining CoO and CoP,and exhibited strong interface-induced synergistic catalysis for AB hydrolysis that effectively decreased the energy barriers for the dissociation of both AB and water molecules.The co-doping of N and P introduced numerous defects,and further regulated the reactivity of the carbon layers.The heterogeneous interface design technique presented here provides a new strategy for developing efficient and inexpensive non-noblemetal catalysts that may be applicable in other fields related to energy catalysis. 展开更多
关键词 Nano-heterostructure Interface engineering Ammonia borane Hydrolysis mechanism Hydrogen
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