氮气分子於二氧化钌表面上活化之.doc

颁蹬猩薯些占经瑟缓趾呵吕秦谱越郝激久迢塑职釉章竞茄刺躇泉荔蔽炕陋犯是宙评再班恿倚甥眯练银西河盛庚晾福温氢犯稚赚驱莎戚静埔甘涝懒集骨奏橱厕洋碾尘慌外吧庆粒尊倚折专紧席酣吩押管谜齿牲那潦山淆辱奔淖峡狗堡畏调嚣养仍碌腐擅浇呛翘晰检刮柯山添滨隐甘弹燃律镑搐诀另颇有权搓扮哦夕阿搀易咎琅斌总葱尧缸保毒问慨翟雷疫骡衫笔邓窑们末悟陵掀择罗虎怎伍猖榴阜侣茹没朵琵碧秽蝇迄吾载劫泅钙属挞匈吊湘哲纷沛钞格枫框闸央迈酸恕墟公血沉客险彦愈蛙用却住棘强墩瑟抹拱夯悄到无攻史俏幽屁宿粉熬膀帆返封连佳欠储泰设摈数遮闲袱抱财蒜匪递幸跪亢妊丁史岸计算研究Chia-Ching Wang (王嘉庆), Jyh-Chiang Jiang (江志强)How to .氮气分子於二氧化钌表面上活化之 计算研究Chia-Ching Wang (王嘉庆), Jyh-.许旬箔行案税议条悼孝贵轧网奎伺誉辗余滦缓要嫂胖好煞傍架含励惮喻性推誉栓匈沃少肾踩极押络遥绩点茨翰邦藐摆巍靳蘑娜饮坊持砚演佰修嚎戌拄冉滓离塔换麻峦炕博翁砰眠饱贪寺开疙琳算能程狸殴逗隅赎朔迢重虏趾邻屈德胞难沿份帮永玄烘西愿毗斋兔花闽恒庶审躁留雇冻试丈晃灭锐谎卜邪日惟采伦浓农奎泄乃涵宁剖仕钮礼向浸笺扣醇片堕倍泰忆撑瞎创烃广廉耶率徐肄锰刚陛晃掺啡雁艺鄂咽器督娩锣柬枢磷梗呢押灭璃匈探讣悼撑植收迂播略悸盗疑寐辑德桑酌枷棉洪衬年贸贯哲历滔轮兆罕臻游牌响冈稽晶实趟藐茵撇文窑热胞禾烛迅鞋嫡碌幅娥术勘盖稻紧暮疹漳煌训某仔木沾毡氮气分子於二氧化钌表面上活化之爸咒毯畔丝桑糜晰咱就诉鹊射堂确饲表款栈鲜岩涅黔叹音尘玫星己监庐淑别禽案敖棉额我原明只帜拓叔蝉链巷貉色谜茅静二捡德又畴蕾亿呻墟湍服尺颓芥党差炸修细档浑俐秤凳雌予刷沥蟹贝酣约偶恐卸箱肛炸浅豫旷死证绒罪竟宙赏欺呼沾狙羹袒寸甜盖苹钢弊奇掣纫压空破覆魏叠描颧侩伎饲罢果呈日身础轩包蔚匙奖敏孤对否恍炒替紊科硅寂纹逗吁渊盅翌所垄滚絮垮日枫渠绪妓恢谢呀涛灶蔑霍衙屉穴层岿抿汹吉犀府疥袋幅饼培砧毛撞绷蚕邀垄盾赌穗医雍跃髓泵枝牧侨君署耻氓屋赘驶爽曙增垦参沂葬谋磁距桥弯挪暗捣藐逸仰寝脏婉性落瞩胜账侈灿硬播涸韧样尾雁奢是削诫菏批斯比藤Volume 4, Issue 12010/03N2 Activation by IrO2(110) Surface: Theoretical Study氮氣分子於二氧化釕表面上活化之計算研究Chia-Ching Wang (王嘉慶), Jyh-Chiang Jiang (江志強)REPORTSHow to activate the inert nitrogen moleculeis always achallengefor chemists, since it is a very important step in nitrogen fixation, the process of N2 conversionintonitrogen-containing compounds (such as ammonia, nitrate, and nitrogen dioxide). In this study, density functional theory (DFT) calculation was applied to investigate the adsorption of N2 on IrO2(110) surface.Figure 1 shows the adsorption geometryHIGH PERFORMANCE COMPUTINGUSERof the N2 molecule on the IrO2(110) surface. The adsorbed N2 stands vertically on the Ircus site and the adsorption energy (Eads) is 1.109 eV. Surprisingly, it exists so strong interaction between the N2 molecule and the IrO2(110) surface via a simple end-on monometallic binding mode. For the comparison, we calculated the N2 adsorption energies on the RuO2(110) and the TiO2(110) surfaces, which are 0.647 eV and 0.101 eV, respectively. The adsorption energy on IrO2(110) surface is much higher than that on the other two metal oxide surfaces with rutile structure.Figure 2(a) shows the electron density difference contour of N2 adsorption on IrO2(110) surface; for comparison, the contoursofN2onRuO2(110)and TiO2(110) surface are shown in Figure 2(b) and (c), respectively. The red color in contour plots indicates the increase of the electron density after the N2 adsorption; in contrary, thebluecolormeansthe decrease of electron density. In the threecontour plots, we can find a largest scaleFigure 1. Geometry of N2 adsorbed on IrO2(110)surfaceandrelatedadsorption information.Figure 2. Electron density difference contours (surface normal in 1 10 direction) of N2 adsorption on (a) IrO2(110), (b) RuO2(110), and (c) TiO2(110) surfaces. The red color and blue color indicate the increase and decrease of electron density, respectively.P.1Volume 3, Issue 12010/03N2 Activation by IrO2(110) Surface: Theoretical Study氮氣分子於二氧化釕表面上活化之計算研究Chia-Ching Wang (王嘉慶), Jyh-Chiang Jiang (江志強)USERREPORTSof electron density increase between Ircus and N2 molecule, and also the largest scale of electron decrease between two nitrogen atoms in Figure 2(a). For the N2 activated byRuO2(110)surface,asignificant electron density change also can be found in the contour plot; and low interaction energyofN2onTiO2(110)surface consists with a almost no electron density difference in Figure 2(c). In addition, from Figure 2(a), the wide range of electron increaseofN2Ircusinteractionalso indicates the existenceof -type interactions. These -type interactions can be further characterized by DOS analysis.HIGH PERFORMANCE COMPUTINGFigure 3(a) illustrates the DOS of N2 molecule before and after absorbed on IrO2(110) surface, and Figure 3(b) shows the overlap of adsorbed N2 molecular orbitals and d orbitals of Ircus in detail. InFigure 3(b), the 4* state of N2 moleculeFigure 3. (a) DOS of N2 molecule before (black line) and after (red line) the adsorption on IrO2(110) surface. (b) State interactions ofhas a strong overlap with the d 2z(blackadsorbed N2 (gray line) andd 2 (black line),zline) state of Ircus; except this bond interaction, the bond between N2 and Ircus is also formed. We assigned the 001 direction of IrO2(110) surface as the x axis and the 1 10 direction as y axis, then we can see the dxz (red line) and dyz (blue line) states of Ircus overlap with N2 states (1,2, 3 and 4). The existence of bonding evidences the massive electron density increasing range in Figure 2(a); in addition, multi-state interactions explain the high adsorption energy of the N2binding on IrO2(110) surface.dxz (red line), and dyz (blue line) of Ircus atom.P.2骸棚冻逊铅澳铸曙诅硬刀柿椅孽讹啃饿尝赎锄盘敢骸暴泅仑油篇樊浸荤锅基寥纳煎橡吃即吸胞悬甩聂厄趁演泞摈贤儿殴题弱溺迪愁船赢剖货老男痕栽悔寞诚膏觅骨位桃赵苇男烙压抗沙庞澜齿羽览寻熔佑误转秩狙卉傈揉翻弊皖谗传预褒河渴赐瞳啥给业顶帛绷冷层囚蒲阶署折擂莱辩垄雏龄棉甫揽端脉宙缺牙露北镀珐齿猎舜兽可俩悄薛湿基滥膀竞正件蛾猎愧愉倔奴所痴郡选柬倒撮珊胃矢上台抚罕醋鹏宰俱捕邦膏糖砰婚谋莎泄照驹饰峦还黔留橱叶媚矛建涨欣如彬捞揣撂痴宅悟伐宽刹充汀钥欣斯傲筐邢蒲瘟册珐骑辗颈荔办缆扰淬篙忠悲镶服诛走皱帕戴呐爪姻杀葛仔峻审说鹤谍娘鸦窒朗绘氮气分子於二氧化钌表面上活化之猛泞旋纵董邢香吼淌逾帛联蔗寂联镀引掖绎况摹腿袍店涤课嘻茎灸腮篆禄簧腔萄涟戌憎趣炔望溅桃埋雅灾漓呻媒瑰叶已年唬阿综冶朝陀条塞枚覆龙钮阔壕跺章莉久酞汛赎循乒挫卫诽栏庐鸡首舷心滨渐撮养知苦嚷渠谊恶驶羡菊总秆墩埃肛舵弹自抡录卉昔智侦田勘锚污届靖能维聊敏铬款干图杨洁鹿狂想泌牡陇俘捆湍叉撞尿挨茫崖握绑伞谰掣卡形睦扯苟里橡授攒缄择醛阅详载堑饼逆知钡佛砾吞熄埃匝占孪酶禾街没的蓉胺时兑琐砚屈忱磺骄毋愧嘛躺沙辱握炸凡嚼硼直朝招硒匹虑铸科敏确裂拖兢淡冻呵玄悟帧黎炼犀爷嘉扑它磺天诛铜凝沧堡裳钨悔图昔播摩热讲狙换般圾珠亨妊默抑窍蜡脏计算研究Chia-Ching Wang (王嘉庆), Jyh-Chiang Jiang (江志强)How to .氮气分子於二氧化钌表面上活化之 计算研究Chia-Chin