【摘要】：本研究主要涵蓋以下三個部分：第一,以石墨粉為原材料,利用Hummers的改進方法制備氧化石墨烯(GO)。對產(chǎn)物進行掃描電子顯微鏡(SEM)、透射電子顯微鏡(TEM)、X線衍射(XRD)、傅里葉紅外光譜(FTIR)、紫外可見光譜(UV)和熱重分析(TGA)。結(jié)果顯示：GO的表面有明顯的褶皺和蜷曲,且具有大量的含氧官能團,在水中分散性能良好。第二,以GO為主體材料,以鐵氰化鉀(K3[Fe(CN)6])為鐵的金屬前驅(qū)體和氮源,通過水熱法制備出摻氮還原石墨烯/α-Fe2O3納米盤復合材料(NG/α-Fe2O3)。通過SEM、TEM、XRD、X射線能譜(EDS、X射線光電子能譜(XPS)、激光拉曼FTIR以及TGA對產(chǎn)物進行表征,結(jié)果顯示：生成了盤狀的α-Fe2O3并附載在在摻氮還原石墨烯表面,且N在NG/α-Fe2O3中的摻雜量為6.13 at%。將NG/α-Fe2O3作為電極修飾材料,利用電化學手段對NG/α-Fe2O3的電催化氧還原(ORR)性能進行測試,以10.0 mL 1.5 mg·mL-1K3[Fe(CN)6]和10.0 mL 1.0 mg·mL1-GO為最佳制備條件,測試結(jié)果表明：在CV測試條件下,峰電位約為-0.201 V,峰電流密度為62.00 μA·cm2；對O2的電催化還原過程含有2電子和4電子途徑；經(jīng)過7200s的連續(xù)掃描后,電流衰減量為26.02%,與20% Pt/C相比更為穩(wěn)定(20%Pt/C衰減量為35.18%)；此外,該材料還具有優(yōu)于20% Pt/C的抗甲醇干擾性能,有望在燃料電池陰極催化劑上具備一定的應用價值。第三,以GO、氯化鈷(CoCl2·6H2O)、氨水(NH3·H2O)為原料,通過水熱法制備出摻氮還原石墨烯／四氧化三鈷復合材料(NG/Co3O4)。通過SEM、TEM、XRD、 EDS、XPS、Raman、FTIR、TGA對產(chǎn)物的組成結(jié)構(gòu)進行表征,結(jié)果顯示：生成的C0304為片層狀,生長在摻氮還原石墨烯納米層上；且N的摻雜量為10.43 at%。通過電化學測試對NG/Co3O4的ORR催化性能表征,結(jié)果顯示當加入：8.0mL NH3·H2O(含量為25-28%)、10.0 mL 1.5 mg·mL-1的GO和5.0mL 2.0 mg·mL-1的CoCl2寸,該材料具有較好的ORR催化性能。其中,峰電位約為-0.163 V,峰電流密度為73.01 μA·cm-2;氧還原反應主要以4電子途徑進行；經(jīng)過7200 s的連續(xù)掃描后,電流衰減量為28.36%,比20%Pt/C穩(wěn)定；此外,該材料的抗甲醇干擾性能也優(yōu)于20% Pt/C,在燃料電池陰極催化材料領(lǐng)域?qū)⒂袧撛诘膽脙r值。
[Abstract]:This research mainly covers the following three parts: first, using graphitic powder as raw material, using the improved method of Hummers to prepare graphene oxide (GO). The products were characterized by scanning electron microscope (SEM), (SEM), transmission electron microscope (SEM), (TEM), X line diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), UV-Vis spectrum (UV) and thermogravimetric analysis (TGA). The results show that the surface of GO has obvious folds and curls, and it has a large number of oxygen-containing functional groups, and it has good dispersion in water. Secondly, the nitrogen-doped graphene / 偽-Fe2O3 nanodisk composites (NG/ 偽-Fe2O3) were prepared by hydrothermal method using GO as the main material and potassium ferrocyanide (K3 [Fe (CN) 6] as the iron precursor and nitrogen source). The products were characterized by SEM,TEM,XRD,X X-ray photoelectron spectroscopy (EDS,X) laser Raman FTIR and TGA. The results showed that the 偽 -Fe2O3 was formed on the surface of nitrogen-doped reduced graphene. The doping amount of N in NG/ 偽-Fe2O3 is 6.13 at%.. Using NG/ 偽-Fe2O3 as electrode modification material, the electrocatalytic oxygen reduction (ORR) properties of NG/ 偽-Fe2O3 were measured by electrochemical method. The optimum preparation conditions were 10.0 mL 1.5 mg mL-1K3 [Fe (CN) 6] and 10.0 mL 1.0 mg mL1-GO. The results showed that the peak potential was about-0.201 V under the CV test condition. Peak current density of 62.00 渭 A cm2; After 7200 s of continuous scanning, the current decay is 26.02, which is more stable than 20% Pt/C (20%Pt/C attenuation is 35.18%). In addition, the material is superior to 20% Pt/C in methanol interference resistance, which is expected to have some application value on fuel cell cathode catalyst. Thirdly, nitrogen-doped reduction graphene / cobalt trioxide (NG/Co3O4) composites were prepared by hydrothermal method using GO, cobalt chloride (CoCl2 6H2O) and ammonia water (NH3 H2O) as raw materials. The structure of the product was characterized by SEM,TEM,XRD, EDS,XPS,Raman,FTIR,TGA. The results showed that the formed C0304 was lamellar and grown on the nitrogen-doped reduced graphene nanolayer, and the amount of N doping was 10.43 at%.. The ORR catalytic properties of NG/Co3O4 were characterized by electrochemical test. The results showed that when the addition of 8.0mL NH3 H2O (25-28%), GO of 10.0 mL 1.5 mg mL-1 and CoCl2 inch of 5.0mL 2.0 mg mL-1 were added, The material has good ORR catalytic performance. The peak potential is about-0.163 V, the peak current density is 73.01 渭 A cm-2; oxygen reduction is mainly by 4 electron pathway, after 7200 s continuous scanning, the current attenuation is 28.36 and is more stable than that of 20%Pt/C. In addition, the anti-methanol interference performance of this material is superior to that of 20% Pt/C, in the field of fuel cell cathode catalytic material.
【學位授予單位】：福建師范大學
【學位級別】：碩士
【學位授予年份】：2015
【分類號】：TB33;O643.36

【參考文獻】

相關(guān)期刊論文 前10條

1 朱振峰;程莎;董曉楠;;石墨烯的制備和應用[J];功能材料;2013年21期

2 李賞;趙偉;王家堂;錢柳;王坤;潘牧;;薄紙狀氧化石墨和石墨烯的制備與表征[J];武漢理工大學學報;2013年01期

3 鄭龍珍;陶X;熊樂艷;葉丹;韓奎;紀憶;;堿性介質(zhì)中Fe/N/C催化劑的氧氣還原反應催化性能研究[J];化學學報;2012年22期

4 ;Synthesis of graphene on a Ni film by radio-frequency plasma-enhanced chemical vapor deposition[J];Chinese Science Bulletin;2012年23期

5 楊偉;陳勝洲;鄒漢波;林維明;;氮摻雜碳載鈷催化劑制備及其TG-FTIR和XRD光譜分析[J];光譜學與光譜分析;2012年04期

6 孫艷紅;趙家昌;唐博合金;唐敖民;廖晨敏;徐菁利;;石墨烯復合材料的研究進展[J];上海工程技術(shù)大學學報;2011年03期

7 趙遠;黃偉九;;石墨烯及其復合材料的制備及性能研究進展[J];重慶理工大學學報(自然科學);2011年07期

8 ;The synthesis and characterization of a Co-N/C composite catalyst for the oxygen reduction reaction in acidic solution[J];Chinese Science Bulletin;2011年11期

9 謝普;呂晴;王麗娥;于杰;羅筑;黃浩;許國楊;鄧青;秦軍;;石墨烯的制備和改性及其與聚合物復合的研究進展[J];材料導報;2010年S2期

10 呂鵬;馮奕鈺;張學全;李t@;封偉;;功能化石墨烯的應用研究新進展[J];中國科學:技術(shù)科學;2010年11期

相關(guān)碩士學位論文 前2條

1 鐘軼良;電化學剝離制備石墨烯及其石墨烯用作燃料電池催化劑載體的研究[D];華南理工大學;2013年

2 肖瑋;鋰離子電池Fe_2O_3/石墨烯復合負極材料的水熱制備及性能研究[D];中南大學;2013年

，

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