催化学报
催化學報
최화학보
CHINESE JOURNAL OF CATALYSIS
2014年
6期
952-959
,共8页
伍颖斯%余皓%王红娟%彭峰
伍穎斯%餘皓%王紅娟%彭峰
오영사%여호%왕홍연%팽봉
颗粒尺寸%石墨烯%金属氧化物%过氧化氢%苯甲醇氧化
顆粒呎吋%石墨烯%金屬氧化物%過氧化氫%苯甲醇氧化
과립척촌%석묵희%금속양화물%과양화경%분갑순양화
Particle size%Graphene%Metal oxide%Hydrogen peroxide%Benzyl alcohol
采用直接浸渍法、过氧化氢均相氧化沉积法和氨水催化水解法制备了石墨烯负载的铁、钴、镍金属氧化物纳米颗粒。研究了三种沉积方法对颗粒尺寸分布的影响;采用透射电子显微镜、傅里叶变换红外光谱、X射线衍射和X射线光电子能谱表征了催化剂的形貌与结构。用过氧化氢均相氧化沉淀法可制得粒径分布最均匀的纳米颗粒。过氧化氢的氧化作用可使石墨烯表面的氧化基团含量最大化,为纳米颗粒提供了足够的吸附与成核点。氨水加速了金属离子的水解与成核,导致纳米颗粒的粒径增大与不均。以苯甲醇氧化为探针反应考察了催化剂的性能。催化剂的活性按以下顺序逐渐下降:过氧化氢辅助沉积法>直接浸渍法>氨水催化水解法,与纳米颗粒尺寸增长趋势一致。纳米催化剂颗粒尺寸与其活性的良好关联性显示,发展石墨烯负载尺寸可控的纳米催化剂的方法具有重要意义。
採用直接浸漬法、過氧化氫均相氧化沉積法和氨水催化水解法製備瞭石墨烯負載的鐵、鈷、鎳金屬氧化物納米顆粒。研究瞭三種沉積方法對顆粒呎吋分佈的影響;採用透射電子顯微鏡、傅裏葉變換紅外光譜、X射線衍射和X射線光電子能譜錶徵瞭催化劑的形貌與結構。用過氧化氫均相氧化沉澱法可製得粒徑分佈最均勻的納米顆粒。過氧化氫的氧化作用可使石墨烯錶麵的氧化基糰含量最大化,為納米顆粒提供瞭足夠的吸附與成覈點。氨水加速瞭金屬離子的水解與成覈,導緻納米顆粒的粒徑增大與不均。以苯甲醇氧化為探針反應攷察瞭催化劑的性能。催化劑的活性按以下順序逐漸下降:過氧化氫輔助沉積法>直接浸漬法>氨水催化水解法,與納米顆粒呎吋增長趨勢一緻。納米催化劑顆粒呎吋與其活性的良好關聯性顯示,髮展石墨烯負載呎吋可控的納米催化劑的方法具有重要意義。
채용직접침지법、과양화경균상양화침적법화안수최화수해법제비료석묵희부재적철、고、얼금속양화물납미과립。연구료삼충침적방법대과립척촌분포적영향;채용투사전자현미경、부리협변환홍외광보、X사선연사화X사선광전자능보표정료최화제적형모여결구。용과양화경균상양화침정법가제득립경분포최균균적납미과립。과양화경적양화작용가사석묵희표면적양화기단함량최대화,위납미과립제공료족구적흡부여성핵점。안수가속료금속리자적수해여성핵,도치납미과립적립경증대여불균。이분갑순양화위탐침반응고찰료최화제적성능。최화제적활성안이하순서축점하강:과양화경보조침적법>직접침지법>안수최화수해법,여납미과립척촌증장추세일치。납미최화제과립척촌여기활성적량호관련성현시,발전석묵희부재척촌가공적납미최화제적방법구유중요의의。
The size of nanoparticles plays a crucial role in their performance. In this article, three methods, i.e., direct impregnation, homogeneous oxidative precipitation with hydrogen peroxide, and ammo-nia-catalyzed hydrolysis, were applied to synthesize iron, cobalt, and nickel metal oxide nanoparti-cles supported on graphene. The influence of the three deposition methods on particle size distribu-tion was investigated. Transmission electron microscopy, Fourier transform infrared spectroscopy, X-ray diffraction, and X-ray photoelectron spectroscopy were used to characterize the morphology and structure of the catalysts. The highest dispersion and the most uniform particle size distribution were obtained by the hydrogen peroxide homogeneous oxidative precipitation method. Hydrogen peroxide favors the maximization of the oxygen-containing groups on graphenes, thereby providing sufficient absorption and nucleation sites to give a high dispersion of nanoparticles. In contrast, ammonia accelerates the nucleation speed and results in the largest particle size and inhomogenei-ty. The catalytic properties of the graphene-supported metal oxide nanoparticles were tested with the oxidation of benzyl alcohol as a probe reaction. The reaction activity decreased in the following order:catalysts prepared by hydrogen peroxide-assisted deposition>direct impregnation>am-monia-catalyzed hydrolysis. The decrease in reaction activity was consistent with the order of in-creasing catalyst particle sizing shown in transmission electron microscopy images. The catalytic relevance of the particle size showed a necessity for the development of effective methods for size-controlled nanocatalyst synthesis on graphenes.