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CuNi NPs supported on MIL-101 as highly active catalysts for the hydrolysis of ammonia borane

机译:MIL-101上担载的CuNi NPs作为氨硼烷水解的高活性催化剂

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摘要

The catalysts containing Cu, Ni bi-metallic nanoparticles were successfully synthesized by in-situ reduction of Cu2+ and Ni2+ salts into the highly porous and hydrothermally stable metal-organic framework MIL-101 via a simple liquid impregnation method. When the total amount of loading metal is 3 x 10(-4) mol, Cu2Ni1@MIL-101 catalyst shows higher catalytic activity comparing to CuxNiy@MIL-101 with different molar ratio of Cu and Ni (x, y = 0, 0.5, 1.5, 2, 2.5, 3). Cu2Ni1@MIL-101 catalyst has the highest catalytic activity comparing to mono-metallic Cu and Ni counterparts and pure bi-metallic CuNi nanoparticles in hydrolytic dehydrogeneration of ammonia borane (AB) at room temperature. Additionally, in the hydrolysis reaction, the Cu2Ni1@MIL-101 catalyst possesses excellent catalytic performances, which exhibit highly catalytic activity with turn over frequency (TOF) value of 20.9 mol H-2 min(-1) Cu mol(-1) and a very low activation energy value of 32.2 kJ mol(-1). The excellent catalytic activity has been successfully achieved thanks to the strong bi-metallic synergistic effects, uniform distribution of nanoparticles and the bi-functional effects between CuNi nanoparticles and the host of MIL-101. Moreover, the catalyst also displays satisfied durable stability after five cycles for the hydrolytically releasing H-2 from AB. The non-noble metal catalysts have broad prospects for commercial applications in the field of hydrogen-stored materials due to the low prices and excellent catalytic activity. (C) 2017 Elsevier B.V. All rights reserved.
机译:通过简单的液体浸渍方法,通过将Cu2 +和Ni2 +盐原位还原成高度多孔和水热稳定的金属有机骨架MIL-101,成功地合成了含Cu,Ni双金属纳米粒子的催化剂。当负载金属总量为3 x 10(-4)mol时,与CuxNiy @ MIL-101相比,Cu2Ni1 @ MIL-101催化剂具有不同的Cu和Ni摩尔比(x,y = 0,0.5)。 ,1.5、2、2.5、3)。在室温下,氨硼烷(AB)水解脱氢反应中,Cu2Ni1 @ MIL-101催化剂与单金属Cu和Ni对应物以及纯双金属CuNi纳米颗粒相比具有最高的催化活性。此外,在水解反应中,Cu2Ni1 @ MIL-101催化剂具有出色的催化性能,具有很高的催化活性,转换频率(TOF)值为20.9 mol H-2 min(-1)Cu mol(-1)和极低的活化能值为32.2 kJ mol(-1)。强大的双金属协同效应,纳米粒子的均匀分布以及CuNi纳米粒子与MIL-101主体之间的双功能效应已成功实现了出色的催化活性。此外,在从AB水解释放H-2的五个循环之后,该催化剂还显示出令人满意的持久稳定性。非贵金属催化剂由于价格低廉和催化活性优异,在储氢材料领域具有广阔的商业应用前景。 (C)2017 Elsevier B.V.保留所有权利。

著录项

  • 来源
    《Applied Surface Science》 |2018年第ptab期|114-122|共9页
  • 作者单位

    Hubei Univ, Coll Chem & Chem Engn, Key Lab Synth & Applicat Organ Funct Mol, Minist Educ,Hubei Collaborat Innovat Ctr Adv Orga, Wuhan 430062, Hubei, Peoples R China;

    Hubei Univ, Coll Chem & Chem Engn, Key Lab Synth & Applicat Organ Funct Mol, Minist Educ,Hubei Collaborat Innovat Ctr Adv Orga, Wuhan 430062, Hubei, Peoples R China;

    Hubei Univ, Coll Chem & Chem Engn, Key Lab Synth & Applicat Organ Funct Mol, Minist Educ,Hubei Collaborat Innovat Ctr Adv Orga, Wuhan 430062, Hubei, Peoples R China;

    Hubei Univ, Coll Chem & Chem Engn, Key Lab Synth & Applicat Organ Funct Mol, Minist Educ,Hubei Collaborat Innovat Ctr Adv Orga, Wuhan 430062, Hubei, Peoples R China;

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  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类
  • 关键词

    CuNi@MIL-101; Heterogeneous catalysis; Ammonia-borane; Releasing hydrogen;

    机译:CuNi @ MIL-101;多相催化;氨硼烷;释放氢;

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