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作 者:郑潇潇[1] 谢婷[1] 肖玥[1] 张鸿斌[1] 张来英[1] 李海燕[1] 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)
机构地区:[1]厦门大学化学化工学院,固体表面物理化学国家重点实验室,醇醚酯化工清洁生产国家工程实验室,福建厦门361005
出 处:《厦门大学学报(自然科学版)》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)
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.
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