Metal–organic framework immobilized RhNi alloy nanoparticles for complete H2 evolution from hydrazine borane and hydrous hydrazine†,Inorganic Chemistry Frontiers

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Metal–organic framework immobilized RhNi alloy nanoparticles for complete H2 evolution from hydrazine borane and hydrous hydrazine†
Inorganic Chemistry Frontiers ( IF 6.1 ) Pub Date : 2017-11-27 00:00:00 , DOI: 10.1039/c7qi00555e
Zhujun Zhang _{1,

2,

3,

4,

5} , Shiliang Zhang _{1,

2,

3,

4,

5} , Qilu Yao _{1,

2,

3,

4,

5} , Gang Feng _{5,

6,

7,

8} , Meihua Zhu _{1,

2,

3,

4,

5} , Zhang-Hui Lu _{1,

2,

3,

4,

5}

Affiliation

Metal–organic framework (MOF) immobilized Rh–Ni alloy nanoparticles (NPs) with a mean size of 2.8 nm have been facilely and successfully fabricated via a reduction rate controlled method. Bimetallic NP/MOF composites with uniform tiny RhNi alloy NPs immobilized on MOFs, high surface areas (1970 m² g⁻¹), and accessible porous structure have been obtained. The resulting RhNi/MOF catalysts show high catalytic activity and robust durability for complete H₂ evolution from hydrazine borane (N₂H₄BH₃) and hydrous hydrazine (N₂H₄·H₂O). The optimized Rh_0.8Ni_0.2/MIL-101 catalyst exhibits excellent catalytic performance for the dehydrogenation of N₂H₄BH₃ and N₂H₄·H₂O in aqueous solution with 100% conversion and hydrogen selectivity, high total turnover frequencies (TOF), up to 1200 and 428.6 mol_(H₂) mol_(Rh+Ni)⁻¹ h⁻¹, respectively, the highest over Rh-based catalysts. The high activity and prominent durability of Rh_0.8Ni_0.2/MIL-101 are highly dependent on the features of the MOF immobilized tiny RhNi alloy NPs, the strong interaction between the MOF crystal and RhNi alloy NPs, the optimized surface and electronic structure of RhNi alloy with an atomic ratio of 8 : 2, and the accessible open porous structure for free mass transfer.

中文翻译：

金属-有机骨架固定化RhNi合金纳米颗粒，可从肼硼烷和含水肼中完全释放出H ₂†

金属-有机骨架（MOF）固定化的平均尺寸为2.8 nm的Rh-Ni合金纳米粒子（NPs）已通过还原速率控制方法简便而成功地制备。已经获得了具有固定在MOF上的均匀细小RhNi合金NP的双金属NP / MOF复合材料，高表面积（1970 m ² g ^-1）和可及的多孔结构。所得RhNi / MOF催化剂对于从肼基硼烷（N ₂ H ₄ BH ₃）和含水肼（N ₂ H ₄ ·H ₂ O）完全释放H ₂表现出高催化活性和强大的耐久性。优化的Rh _0.8 Ni_0.2 / MIL-101催化剂对N₂ H₄ BH₃和N₂ H₄ ·H₂ O在水溶液中的脱氢表现出优异的催化性能，具有100％的转化率和氢选择性，高总周转频率（TOF），最高可达分别为1200和428.6 mol_{（H ₂）} mol_{（Rh + Ni）}^-1 h^-1，高于Rh基催化剂。Rh_0.8 Ni_0.2的高活性和出色的耐久性/ MIL-101高度依赖于固定MOF的微小RhNi合金NP的特性，MOF晶体与RhNi合金NP之间的强相互作用，原子比为8：2的RhNi合金的优化表面和电子结构以及可访问的开放式多孔结构，可进行自由质量转移。

更新日期：2017-11-27

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