微乳液法合成纳米金催化剂及催化对硝基酚还原
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- 英文论文题名：Gold Nanoparticles Synthesized in Reverse Microemusion for Catalytic Reduction of 4-Nitrophenol
- 论文作者：王翠 ; 吕荣文 ; 张淑芬
- 英文论文作者：Cui Wang ; Rongwen Lu ; Shufen Zhang ; State Kay Laboratory of Fine chemicals ; Dalian University of Technology
- 年：2016
- 作者机构：大连理工大学精细化工国家重点实验室;
- 论文关键词：纳米金 ; 对硝基酚 ; 催化还原
- 会议召开时间：2016-07-01
- 会议录名称：中国化学会第30届学术年会摘要集-第三十七分会：纳米催化
- 语种：中文
- 分类号：O643.36
- 学会代码：ZGHY
- 会议名称：中国化学会第30届学术年会-第三十七分会 ; 纳米催化
- 会议地点：中国辽宁大连
- 主办单位：中国化学会
- 学会名称：中国化学会
- 页数：1
- 文件大小：198k
- 原文格式：D
- 会议级别：全国
摘要
金的化学性质历来被认为是惰性的,其催化潜力一直未能引起足够的重视。直到1987年,Haruta等~([1])报道了高分散金纳米颗粒能够催化一氧化碳氧化,使得金纳米颗粒的催化作用获得了广泛关注。本文通过优化传统的溶胶-凝胶法,在反相微乳液体系中制备出负载在二氧化硅上高分散的的纳米金催化剂,并对其催化对硝基酚还原性能进行研究。纳米金催化对硝基酚还原生成对氨基酚,室温即可达到转化率99%,TOF值9.9min~(-1)。利用UV-vis对反应动力学进行研究,确认该还原反应为准一级动力学反应,表观反应速率系数k_A=-0.145 min~(-1)。原位红外光谱仪与液相色谱-质谱联用仪检测到反应中间体羟胺的存在,结合文献报道~([2])证明反应过程遵循如下路径(如Fig.1)。
Gold has been considered chemical inert in catalytic reactions for a long period of time. Until 1987, Haruta et al.~([1]) reported highly dispersed gold nanoparticles for catalytic oxidation of CO, the gold catalyst received wide attention from then. In this paper, silica supported highly dispersed gold nanoparticles were prepared by reverse microemulsion and showed high activity for catalytic reduction of 4-nitrophenol at room temperature. The reaction was proved to follow a pseudo first-order reaction, and the apparent rate constant(k_A) could reach -0.145 min~(-1). More importantly, the in-situ IR and HPLC-MS were conducted to investigate the mechanism of the reduction, the formation of hydroxylamine proved the correctness of direct route(nitro →hydroxylamine →amine).
Gold has been considered chemical inert in catalytic reactions for a long period of time. Until 1987, Haruta et al.~([1]) reported highly dispersed gold nanoparticles for catalytic oxidation of CO, the gold catalyst received wide attention from then. In this paper, silica supported highly dispersed gold nanoparticles were prepared by reverse microemulsion and showed high activity for catalytic reduction of 4-nitrophenol at room temperature. The reaction was proved to follow a pseudo first-order reaction, and the apparent rate constant(k_A) could reach -0.145 min~(-1). More importantly, the in-situ IR and HPLC-MS were conducted to investigate the mechanism of the reduction, the formation of hydroxylamine proved the correctness of direct route(nitro →hydroxylamine →amine).
引文
[1]Haruta M.,Kobayashi T.,Sano H.,et al.Chem.Lett.1987,16:405.
[2]She Z.W.,Liu S.,Zhang S.Y.Chem.Commun.,2011,47:6689.
[2]She Z.W.,Liu S.,Zhang S.Y.Chem.Commun.,2011,47:6689.