使用旋转电极技术考察了一系列碳载金纳米颗粒(颗粒平均尺寸处在3～14 nm)在碱性电解质(0.5 mol/L KOH)中对氧还原反应的催化行为,随着金纳米颗粒尺寸由14nm下降至3nm,其对氧还原反应的本征活性和质量比活性均呈现持续走高趋势;但金颗粒的纳米尺寸对氧还原反应的机理及分子氧还原过程中的电子转移数目并无显著影响,使用高分辨透射电镜技术表征了金纳米颗粒的形貌,通过对金颗粒表面不同位置原子的比例进行估算,发现金颗粒表面高能原子所占比例与金对氧还原反应的本征活性密切相关,表明高能表面原子决定着金催化剂对氧还原反应的本征活性.此外,还将金纳米颗粒对氧还原反应的本征催化活性与其表面电子结构进行了关联.
参考文献
| [1] | Bron, M .Carbon black supported gold nanoparticles for oxygen electroreduction in acidic electrolyte solution[J].Journal of Electroanalytical Chemistry,2008(1/2):64-68. |
| [2] | Stamenkovic VR;Mun BS;Arenz M;Mayrhofer KJJ;Lucas CA;Wang GF;Ross PN;Markovic NM .Trends in electrocatalysis on extended and nanoscale Pt-bimetallic alloy surfaces[J].Nature materials,2007(3):241-247. |
| [3] | Stamenkovic V;Mun B S;Mayrhofer K J J;Ross P N,Markovic N M,Rossmeisl J,Greeley J,Norskov J K .[J].Angew Chem Int gd,2006,45:2897. |
| [4] | Kuai, L.;Geng, B.;Wang, S.;Sang, Y. .A general and high-yield galvanic displacement approach to Au-M (M=Au, Pd, and Pt) core-shell nanostructures with porous shells and enhanced electrocatalytic performances[J].Chemistry: A European journal,2012(30):9423-9429. |
| [5] | Kuai, L.;Yu, X.;Wang, S.;Sang, Y.;Geng, B. .Au-Pd alloy and core-shell nanostructures: One-pot coreduction preparation, formation mechanism, and electrochemical properties[J].Langmuir: The ACS Journal of Surfaces and Colloids,2012(18):7168-7173. |
| [6] | Adzic R R;Markovic N M;Vesovic V B .[J].Journal of Electroanalytical Chemistry,1984,165:105. |
| [7] | Strbac S.;Adzic RR. .THE INFLUENCE OF OH- CHEMISORPTION ON THE CATALYTIC PROPERTIES OF GOLD SINGLE CRYSTAL SURFACES FOR OXYGEN REDUCTION IN ALKALINE SOLUTIONS[J].Journal of Electroanalytical Chemistry: An International Journal Devoted to All Aspects of Electrode Kinetics, Interfacial Structure, Properties of Electrolytes, Colloid and Biological Electrochemistry,1996(1/2):169-181. |
| [8] | Tang W;Lin H F;Kleiman-Shwarsctein A;Stucky G D McFarland E W .[J].J Phys Chem C,2008,112:10515. |
| [9] | Wang S;Kuai L;Han X;Geng B .[J].CRYSTENGCOMM,2012,14:6581. |
| [10] | Hernandez J;Solla-Gullon J;Herrero E;Aldaz A;Feliu JM .Electrochemistry of shape-controlled catalysts: Oxygen reduction reaction on cubic gold nanoparticles[J].The journal of physical chemistry, C. Nanomaterials and interfaces,2007(38):14078-14083. |
| [11] | Chen W;Chen S;Angew Chem .[J].Int Ed,2009,48:4386. |
| [12] | Lee Y;Loew A;Sun S .[J].CHEMISTRY OF MATERIALS,2009,22:755. |
| [13] | Sarapuu A;Nurmik M;Mandar H;Rosental A;Laaksonen T;Kontturi K;Schiffrin DJ;Tammeveski K .Electrochemical reduction of oxygen on nanostructured gold electrodes[J].Journal of Electroanalytical Chemistry: An International Journal Devoted to All Aspects of Electrode Kinetics, Interfacial Structure, Properties of Electrolytes, Colloid and Biological Electrochemistry,2008(1):78-86. |
| [14] | Jirkovsky J S;Halasa M;Schiffrin D J .[J].Physical Chemistry Chemical Physics,2010,12:8042. |
| [15] | Zhang G-R;Xu B-Q .[J].Nanoscale,2010,2:2798. |
| [16] | Roduner E .Size matters: why nanomaterials are different[J].Chemical Society Reviews,2006(7):583-592. |
| [17] | Phala N S;van Steen E .[J].Gold Bulletin,2007,40:150. |
| [18] | van Bokhoven J A;Miller J T .[J].J Phys Chem C,2007,111:9245. |
| [19] | Erikson H;Juermann G;Sarapuu A;Potter R J Tammeveski K .[J].Electrochimica Acta,2009,54:7483. |
| [20] | Tsunoyama H;Ichikuni N;Sakurai H;Tsukuda T .[J].Journal of the American Chemical Society,2009,131:7086. |
| [21] | Villa A;Wang D;Su D S;Prati L .[J].ChemCatChem,2009,1:510. |
| [22] | 杨新伟,张贵荣,李永绣,徐柏庆.单分散纳米金尺寸的分步晶种生长控制[J].物理化学学报,2009(12):2565-2569. |
| [23] | Zhang, G.-R.;Zhao, D.;Feng, Y.-Y.;Zhang, B.;Su, D.S.;Liu, G.;Xu, B.-Q. .Catalytic Pt-on-Au nanostructures: Why Pt becomes more active on smaller Au particles[J].ACS nano,2012(3):2226-2236. |
| [24] | 冯媛媛,马俊红,张贵荣,赵丹,徐柏庆.界面合金化的Pt^Ag催化剂对阴极氧还原反应的电催化特点[J].催化学报,2009(08):776-779. |
| [25] | Feng, Y.-Y.;Ma, J.-H.;Zhang, G.-R.;Liu, G.;Xu, B.-Q. .Dealloyed carbon-supported PtAg nanostructures: Enhanced electrocatalytic activity for oxygen reduction reaction[J].Electrochemistry communications,2010(9):1191-1194. |
| [26] | Feng Y-Y;Zhang G-R;Ma J-H;Liu G Xu B-Q .[J].Physical Chemistry Chemical Physics,2011,13:3863. |
| [27] | Bard A J;Faulkner L R.Electrochemical Methods:Fundamentals and Applications[M].New York:Wiley,2000 |
| [28] | Trasatti S;Petrii O A .[J].Pure and Applied Chemistry,1991,63:711. |
| [29] | Gorshkov, V;Zavalov, A;Privman, V .Shape Selection in Diffusive Growth of Colloids and Nanoparticles[J].Langmuir: The ACS Journal of Surfaces and Colloids,2009(14):7940-7953. |
| [30] | Lim B;Wang J;Camargo P H C;Cobley C M,Kim M J,Xia Y .[J].AngewChem Int Ed,2009,48:6304. |
| [31] | Mohr C;Hofmeister H;Claus P .[J].Journal of Catalysis,2003,213:86. |
| [32] | Koga K.;Sugawara K. .Population statistics of gold nanoparticle morphologies: direct determination by HREM observations[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,2003(1/2):23-35. |
| [33] | Xia Y;Xiong Y;Lim B;Skrabalak S E .[J].Angew Chem Int Ed,2009,48:60. |
| [34] | Schmidt T J;Stamenkovic V;Arenz M;Markovic N M Ross P N .[J].Electrochimica Acta,2002,47:3765. |
| [35] | Varcoe J R;Slade R C T;Wright G L;Chen Y .[J].Journal of Physical Chemistry B,2006,110:21041. |
| [36] | Vielstich W;Lamm A;Gasteiger H A.Handbook of Fuel Cells Fundamentals Technology and Applications[M].New York:Wiley,2003 |
| [37] | Montejano-Carrizales J M;Aguilera-Granja F;Moran-Lopez J L .[J].Nanostructured Materials,1997,8:269. |
| [38] | Hammer B;Nielsen O H;Norskov J K .[J].Catalysis Letters,1997,46:31. |
| [39] | Pedersen MO.;Ruban A.;Stensgaard I.;Laegsgaard E.;Norskov JK.;Besenbacher F.;Helveg S. .How a gold substrate can increase the reactivity of a Pt overlayer[J].Surface Science: A Journal Devoted to the Physics and Chemistry of Interfaces,1999(3):395-409. |
| [40] | Tritsaris G A;Greeley J;Rossmeisl J;Norskov J K .[J].Catalysis Letters,2011,141:909. |
| [41] | Hammer B;Norskov J K .[J].NATURE,1995,376:238. |
| [42] | Greeley J;Norskov J K;Mavrikakis M .[J].Ann Rev Phys Chem,2002,53:319. |
| [43] | Kibler L A;El-Aziz A M;Hoyer R;Kolb D M .[J].Angew Chem Int Ed,2005,44:2080. |
| [44] | Norskov J K;Abild-Pedersen F;Studt F;Bligaard T .[J].Proceedings of the National Academy of Sciences(USA),2011,108:937. |
上一张
下一张
上一张
下一张
计量
- 下载量()
- 访问量()
文章评分
- 您的评分：
-
10%
-
20%
-
30%
-
40%
-
50%