氧化铁负载铂纳米簇催化卤代硝基苯本体氢化性质研究

引用本文: 连超, 张垲, 王远. 氧化铁负载铂纳米簇催化卤代硝基苯本体氢化性质研究[J]. 物理化学学报, 2017, 33(5): 984-992. doi: 10.3866/PKU.WHXB201702084 shu

Citation: LIAN Chao, ZHANG Kai, WANG Yuan. Catalytic Properties of Platinum Nanoclusters Supported on Iron Oxides for the Solvent-Free Hydrogenation of Halonitrobenzene[J]. Acta Physico-Chimica Sinica, 2017, 33(5): 984-992. doi: 10.3866/PKU.WHXB201702084 shu

氧化铁负载铂纳米簇催化卤代硝基苯本体氢化性质研究

连超 ^1,2, ,
张垲 ^2, ,
王远 ^2,

1.
北京交通大学理学院化学系, 北京 100044;
2.
北京大学化学与分子工程学院, 分子动态与稳态结构国家重点实验室, 北京分子科学国家实验室, 北京 100871
基金项目:
国家自然科学基金（21573010），科技部国家重点研发计划项目（2016YFE0118700）和北京交通大学人才基金（2015RC070）资助

摘要: 复相金属催化剂中的载体效应研究具有重要意义。我们以结构不同的氧化铁载体吸附“非保护型”Pt金属纳米簇制备了具有相同Pt 纳米簇的Pt/Fe₃O₄、Pt/γ-Fe₂O₃和Pt/α-Fe₂O₃催化剂，考察了其在无溶剂条件下（本体条件）催化邻氯硝基苯（o-CNB）选择性氢化反应的性能，发现三种铂/氧化铁催化剂的催化选择性远高于商购铂/碳催化剂，Pt/γ-Fe₂O₃和Pt/α-Fe₂O₃的催化选择性明显高于Pt/Fe₃O₄，而Pt/Fe₃O₄的催化活性较Pt/α-Fe₂O₃高50%。铂/氧化铁对不同卤代硝基苯的本体选择性氢化反应表现出优良的催化性能，相应卤代苯胺产物的选择性均可达到99%以上。考察了温度、氢气压力对Pt/Fe₃O₄催化o-CNB本体氢化性能的影响。本工作为理解氧化铁负载金属纳米簇催化剂的特殊催化性质，进而发展高效金属纳米簇基催化体系提供了新的基础。

关键词:

English

Catalytic Properties of Platinum Nanoclusters Supported on Iron Oxides for the Solvent-Free Hydrogenation of Halonitrobenzene

1.
Department of Chemistry, School of Science, Beijing Jiaotong University, Beijing 100044, P. R. China;
2.
Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P. R. China
Received Date: 28 November 2016
Revised Date: 23 January 2017
Available Online: 08 February 2017
Fund Project:
The project was supported by the National Natural Science Foundation of China (21573010), MOST, China (2016YFE0118700), and Fundamental Research Funds for the Central Universities, China (2015RC070).

Abstract: It is of significance to investigate the support effect in heterogeneous metal catalysts. Pt/Fe₃O₄, Pt/ γ-Fe₂O₃, and Pt/α-Fe₂O₃ nanocomposites with the same Pt nanoclusters were prepared by adsorbing Pt colloidal particles stabilized with simple ions and solvent molecules on different iron oxide supports. The catalytic performances over the as-prepared catalysts for the selective hydrogenation of o-chloronitrobenzene (o-CNB) in the absence of solvent were evaluated. It was found that the catalytic activity and selectivity over the prepared iron oxide-supported Pt nanocluster catalysts were higher than those of a commercial Pt/C catalyst. The selectivity towards o-chloroaniline over Pt/γ-Fe₂O₃ or Pt/α-Fe₂O₃ was higher than that over Pt/Fe₃O₄, while the catalytic activity over Pt/Fe₃O₄ was 50% higher than that over Pt/α-Fe₂O₃. The Pt/iron oxide catalysts also exhibited excellent catalytic properties for the solvent-free selective hydrogenation of other tested halonitrobenzenes, with the selectivity to corresponding haloanilines being > 99%. In addition, the influences of temperature and hydrogen pressure on the solvent-free selective hydrogenation of o-CNB over Pt/Fe₃O₄ were studied. This work is helpful in understanding the superior properties of iron oxide-supported metal nanocluster catalysts and provides a foundation for further developing highly efficient catalytic systems based on metal nanoclusters.

Key words:

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1.
沈阳化工大学材料科学与工程学院沈阳 110142

氧化铁负载铂纳米簇催化卤代硝基苯本体氢化性质研究

English

Catalytic Properties of Platinum Nanoclusters Supported on Iron Oxides for the Solvent-Free Hydrogenation of Halonitrobenzene

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通讯作者: 陈斌, bchen63@163.com

中国化学会秘书处

氧化铁负载铂纳米簇催化卤代硝基苯本体氢化性质研究

English

Catalytic Properties of Platinum Nanoclusters Supported on Iron Oxides for the Solvent-Free Hydrogenation of Halonitrobenzene

CCS Chemistry：嵌段共聚物自组装成 “三明治”二维有机材料，实现纳米级压力传感功能

CCS Chemistry：颜徐州、鲍哲南： 你的皮肤可能是一片SPMs

CCS Chemistry：工作高效不疲劳，只须让催化剂动起来

CCS Chemistry：静电组装导向聚合- 聚电解质纳米凝胶量化制备新策略

CCS Chemistry：金黄色葡萄球菌醛基脱氢酶是如何识别特异性底物的？

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