摘要
甲酸分解制氢是解决能源问题的有效途径,与Pd催化剂相比,Au催化剂不易失活,具有较好的稳定性.使用次亚磷酸钠原位还原制备了Au-P/SiO_2催化剂,并利用X射线衍射、透射电子显微镜和X射线光电子能谱等表征手段探讨其结构,并以甲酸分解为目标反应研究其催化性能.结果表明,该方法制备的催化剂中Au粒子(粒径3nm左右)均匀分散在SiO_2表面,且P掺杂进入Au的晶格形成Au-P复合物,改变了Au的电子结构.同时反应过程中产生的PⅢ被Au3+氧化生成磷酸金,提供酸性中心,使Au-P/SiO_2催化剂表现出较Au/SiO_2催化剂更加优越的催化性能.在363K,4mol/L的甲酸溶液中,Au-P/SiO_2催化剂催化甲酸分解的转化率可达51%,是未掺杂的Au/SiO_2催化剂的4倍.
Formic acid decomposition is an effective way to solve energy problem.Compared with Pd catalysts, Au catalysts have bet- ter anti-inactivation ability.In this article, Au-P/SiO2 catalysts were prepared with in situ reduction using NaH2PO2.The catalysts were characterized by X-ray diffraction, transmission electron microscope, X-ray photoelectron spectroscopy,and catalytic perform- ances of the catalysts were tested through catalytic decomposition of formic acid.The results of the catalyst characterization demon- strated that with this method, the Au particles （3 nm） highly dispersed on the surface of SiO2 ,and some P entered into the crystal lattice of Au, which contributed the formation of Au-P compound and changed the electrical property of Au.Meanwhile,in the process of reaction,PⅢ appeared,and it was oxidized into pv by Au22＋ to form gold phosphate with acid-base properties.For the reasons a- bove,Au-P/SiO2 is more active than Au/SiO2. In 363 K, 4 mol/L formic acid solution, the conversion rate of formic acid reached 51% over Au-P/SiO2 ,which is 4 times of Au/SiO2.
作者
郑潇潇
谢婷
肖玥
张鸿斌
张来英
李海燕
ZHENG Xiaoxiao XIE Ting XIAO Yue ZHANG Hongbin ZHANG Laiying LI Haiyan(State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005,China)
出处
《厦门大学学报（自然科学版）》
CAS
CSCD
北大核心
2017年第1期42-47,共6页
Journal of Xiamen University：Natural Science
基金
国家重点基础研究发展计划(973计划)项目(2011CBA00500)
福建省自然科学基金(E0510001)
关键词
次亚磷酸钠
Au—P复合物
磷酸金
甲酸分解
sodium phosphinate
Au-P compound
gold phosphate
formic acid decomposition
