Hydrodesulfurization Mechanisms of Thiophene Catalyzed by Au/Pd(111) Bimetallic Surfa _Acta Phys Chim Sin
ISSN CN 11-1892/O6CODEN WHXUEU
10.3866/PKU.WHXB &&&&&&&&
THEORETICAL AND COMPUTATIONAL CHEMISTRY
Hydrodesulfurization Mechanisms of Thiophene Catalyzed by Au/Pd(111) Bimetallic Surfa
ZHANG Lian-Yang, SHI Wei, XIA Sheng-Jie,
Laboratory of Advanced Catalytic Materials, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310032, P. R. China
Full text:
The formation energy of different ensembles on Pd(111) surfaces containing N (N=1-4) Au atoms were investigated using a density functional theory model. The best model for exploring the adsorption of thiophene was selected, and the mechanism of competitive hydrodesulfurization on a Au/Pd(111) bimetallic surface was investigated. The results showed that Au/Pd(111) has the lowest formation energy, and adsorption at the hexagonal close-packed site is most stable when the thiophene plane is tilted at 30& to the Au/Pd(111) bimetallic surface with S atom. The reactions are exothermic, and desulfurization can be either direct or indirect. The direct desulfurization pathway has a low activation energy, but it is difficult to control the products. The indirect desulfurization pathway is the best fit for the cis-h C—S cleavage has the highest reaction energy barrier, and is the rate-determining step. The activation energy barrier of the rate-determining step on Au/Pd(111) is lower than those on Au(111) and Pd(111). This indicates that bimetallic AuPd is more active than single Au and Pd in the hydrodesulfurization of thiophene.
Publication Date (Web):
Corresponding Authors: NI Zhe-Ming Email: jchx@
Cite this article:
ZHANG Lian-Yang, SHI Wei, XIA Sheng-Jie, NI Zhe-Ming. Hydrodesulfurization Mechanisms of Thiophene Catalyzed by Au/Pd(111) Bimetallic Surfa[J]. Acta Phys. -Chim. Sin., 2014,30 (10): .
&& doi: 10.3866/PKU.WHXB
(1) Diaz, Y.; Sevilla, A.; M&naco, A.; M&ndez, F. J.; Rosales, P.; Garc&a, L.; Brito, J. L. Fuel 2013, 110, 235. doi:
(2) Liao, H.; Xu, X. L.; Chen,W. Q.; Shi, Q. J.; Liu,W. M.;Wang, X. Acta Phys. -Chim. Sin. 2012, 28 (12), 2924. [廖辉, 徐香兰, 谌伟庆, 石秋杰, 刘文明, 王翔. 物理化学学报, 2012, 28 (12), 2924.] doi:
(3) Villasana, Y.; Ruscio-Vanalesti, F.; Pfaff, C.; M&ndez, F. J.; Luis-Luis, M. &A.; Brito, J. L. Fuel 2013, 110, 259. doi:
(4) Zhao, D. S.; Li, F. T.; Zhou, E. P.; Sun, Z. M. Chem. Res. Chin. Univ. 2008, 24, 96. doi:
(5) Ma, C. Y.; Li, X. H.; Jin, M. S.; Liao,W. P.; Guan, R. G.; Suo, Z. H. Chin. J. Catal. 2007, 28 (6), 535. [麻春艳, 李新华, 金明善, 廖卫平, 管仁贵, 索掌怀. 催化学报, 2007, 28 (6), 535.] (6) Parola, V. L.; Testa, M. L.; Venezia, A. M. Appl. Catal. B: Environ. 2012, 119 -120, 248. (7) Evangelisti, C.; Schiavi, E.; Aronica, L. A.; Caporusso, A. M.; Vitulli, G.; Bertinetti, L.; Martra, G.; Balerna, A.; Mobilio, S. J. Catal. 2012, 286, 224. doi:
(8) Boscoboinik, J. A.; Plaisance, C.; Neurock, M.; Tysoe,W. T. Phys. Rev. B 2008, 77 (4), 045422. doi:
(9) Gu, H. Z.; Xu, X. S.; Chen, A. A.; Ao, P.; Yan, X. H. Catal. Commun. 2013, 41, 65. doi:
(10) Pongthawornsakun, B.; Fujita, S.; Arai, M.; Mekasuwandumrong, O.; Panpranot, J. Appl. Catal. A-Gen. 2013, 467 (2), 132. (11) Suo, Z. H.; Ma, C. Y.; Liao,W. P.; Jin, M. S.; Lv, H. Y. Fuel Pro. Tech. 2011, 92, 1549. doi:
(12) Zhang, J.; Jin, H. M.; Sullivan, M. B.; Chiang, F.; Lim, H.;Wu, P. Phys. Chem. Chem. Phys. 2009, 11 (9), 1441. doi:
(13) Chen, Z. H.; Ding, K. N.; Xu, X. L.; Li, J. Q. Chin. J. Struct. Chem. 2010, 29 (1), 93. (14) Zhu, H. Y.; Lu, X. Q.; Guo,W. Y.; Li, L. F.; Zhao, L. M.; Shan, H. H. J. Mol. Catal. A-Chem. 2012, 363-364, 18. (15) Ni, Z. M.; Shi,W.; Xia, M. Y.; Xue, J. L. Chem. J. Chin. Univ. 2013, 34 (10), 2353. [倪哲明, 施炜, 夏明玉, 薛继龙. 高等学校化学学报, 2013, 34 (10), 2353.] (16) Peyghan, A. A.; Baei, M. T.; Torabi, P.; Hashemian, S. Phosphorus Sulfur Silicon Relat. Elem. 2013, 188, 1172. doi:
(17) Zheng, X. Z.; Zhang, Y. H.; Huang, S. P.; Liu, H.;Wang, P.; Tian, H. P. Comput. Theor. Chem. 2012, 979, 64. doi:
(18) Zhu, H. Y.; Guo,W. Y.; Li, M.; Zhao, L. M.; Li, S. R.; Li, Y.; Lu, X. Q.; Shan, H. H. ACS Catal. 2011, 1, 1498. doi:
(19) Moses, P. G.; Hinnemann, B.; Topsoe, H.; Norskov, J. K. J. Catal. 2009, 268 (2), 201. doi:
(20) Delley, B. J. Chem. Phys. 2000, 113 (18), 7756. doi:
(21) Perdew, J. P.; Burke, K.; Ernzerhof, M. Phys. Rev. Lett. 1996, 77 (18), 3865. doi:
(22) Ge, Q.; Jenkins, S. J.; King, D. A. Chem. Phys. Lett. 2000, 327(3/4), 125. (23) Delley, B. J. Phys. Chem. 1996, 100 (15), 6107. doi:
(24) Chen, Z. H.; Ding, K. N.; Xu, X. L.; Li, J. Q. Chin. J. Struct. Chem. 2010, 29 (3), 365. (25) Besenbacher, F.; Brorson, M.; Clausen, B. S.; Helveg, S.; Hinnemann, B.; Kibsgaard, J.; Lauritsen, J. V.; Moses, P. G.; Norskov J. K.; Tops&e, H. Catal. Today 2008, 130 (1), 86. doi:
(26) Moses, P. G.; Hinnemann, B.; Tops&e, H.; N&rskov, J. K. J. Catal. 2007, 248 (2), 188. doi:
(27) Yao, X. Q.; Li, Y.W.; Jiao, H. J. J. Mol. Struct. &Theochem 2005, 726 (1-3), 81. doi:
(28) Huang, Y. L.; Liu, Z. P. Acta Phys. -Chim. Sin. 2008, 24 (9), 1662. [黄永丽, 刘志平. 物理化学学报, 2008, 24 (9), 1662.] doi:chen111@|chongqing的基本资料
性别:保密
现所在城市:
所在城市:
人生阶段:
注册时间:
TA的标签:
马上注册,关注TA,支持TA,和TA一起分享生活、分享喜怒哀乐。
&已有账号?
版权所有 ICP证:渝B2- 渝ICP备
&&&&&&&&&& &&&&&&&&&&温馨提示!由于新浪微博认证机制调整,您的新浪微博帐号绑定已过期,请重新绑定!&&|&&
模块内容加载中...
this.p={b:2,maxb:5,maxp:6}
{if !defined('b')} 日志更新列表加载中... {elseif !b.length} 没有日志更新! {else} {list b as x}·{/list} {/if}
{if !defined('p')} 相片更新列表加载中... {elseif !p.length} 没有相片更新! {else} {list p as x}{/list} {/if}
{list 0..6 as x}${dv[x]}{/list} {list 1..6 as x}{list 1..7 as y}{/list}{/list}
{list df..dt as x}{/list}
&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&&
歌曲:太多 歌手: 专辑:
电视剧:穿越时空的爱恋片头曲 将爱情肆无忌惮的挥霍 心都碎了还要计较些什么 无论你想要什么都让你带走 如果你觉得自由是快乐 爱是犯了软弱陈旧的差错 又何必在乎别人怎么看怎么说 太多的借口太多的理由 为了爱情我也背叛了所有 如果你想离开我就别再畏畏缩缩 太多的借口太多的理由
&追梦人 &曲:罗大佑 词:罗大佑 &唱:凤飞飞 &出自专辑:《告别的年代-情歌专辑》 &让青春吹动了你的长发让它牵引你的梦 &不知不觉这红尘的历史已记取了你的笑容 &红红心中蓝蓝的天是个生命的开始 &春雨不眠隔夜的你曾空独眠的日子 &让青春娇艳的花朵绽开了深藏的红颜 &飞去飞来的满天的飞絮是幻想你的笑颜 &秋来春去红尘中谁在宿命里安排 &冰雪不语寒夜的你那难隐藏的光彩 &看我看一眼吧 莫让红颜守空枕 &青春无悔不死 永远的爱人 &让流浪的足迹在荒漠里写下永久的回忆
来了就是好 没事干的 我 &
今天第一次
我要留言 & &
& 留言列表加载中...
this.p={b:2,nv:false,cn:5,ct:5};
this.p={b:2,s:8,a:true};
{if !defined('ml')||!ml.length} 专辑 ${an|escape} 没有音乐! {else} {list ml as x}{/list} {/if}
{if !defined('ll')||!ll.length} 网易博客音乐盒 {else} {list ll as x}${x.v|default:'&'}{/list} {/if}
{if !defined('al')||!al.length} 没有专辑! {else} {list al as x}{/list} {/if}
最后登录加载中...
this.p={b:2,ua:-1, ub:'http://img.bimg.126.net/photo/NziorYsc9EUeSBftadH1yA==/802372.jpg',us:'他', friendstatus:'none',followstatus:'unFollow',hmcon:'',aShowT:'0',guideId:2};
积分 ${data.totalScore} 分,距离下一等级还有 ${data.nextGradeNeedScore}分
心情随笔列表加载中...
this.p={b:2,n:5,r:'http://chenyachuan235./blog/#m=1&c=',mset:'000',mcon:'',srk:-100};
{if defined('fl')&&fl.length>0} {list fl as x}
${x.content|xescape:x.id,x.moveFrom} ${x.publishTime|xtime}
{if x.moveFrom&&x.moveFrom=='wap'} && {/if} {if x.moveFrom&&x.moveFrom=='mobile'} && {/if}
{/list} {else} 暂无心情随笔记录! {/if}
模块内容加载中...
this.p={b:2,cv:'http://b.bst.126.net/newpage/images/album/cover75.gif'};
{if ps<0} {if ps==-1}博主相册被封禁,您无法查看!{else}博主尚未激活相册,您暂时无法查看!{/if} {elseif !ha} 目前没有相片! {elseif al.length<=0}
暂时无法加载相册数据,请稍后再试!
停止 上一个 下一个 相册列表
{if defined('al')&&al.length>0} {list al as x}
${x.name|escape} ${x.count|default:0}张相片 ${x.t|format:'MM-dd HH:mm'}
{/list} {/if}
博友列表加载中...
this.p={b:2,m:0};
列表加载中...
this.p={b:2,cn:15};
& & & & & &
网易公司版权所有&&
{list x.l as y}
{/list} {/list}
{if defined('wl')} {list wl as x}{/list} {/if}