聚合物稳定的金簇合物上卤素吸附质:质谱检测及其对催化的影响

doi:10.1016/S1872-2067(16)62501-9

催化学报 ›› 2016, Vol. 37 ›› Issue (10): 1656-1661.DOI: 10.1016/S1872-2067(16)62501-9

聚合物稳定的金簇合物上卤素吸附质:质谱检测及其对催化的影响

Ryo Ishida^a, Setsuka Arii^a, Wataru Kurashige^b, Seiji Yamazoe^a,c, Kiichirou Koyasu^a,c, Yuichi Negishi^b, Tatsuya Tsukuda^a,c

a 东京大学理学院化学系, 东京113-0033, 日本;
b 东京理科大学理学部应用化学系, 东京162-8601, 日本;
c 京都大学触媒 & #183;电池元素战略研究基地, 京都615-8520, 日本

收稿日期:2016-05-06 修回日期:2016-06-15 出版日期:2016-10-21 发布日期:2016-10-22
通讯作者: Tatsuya Tsukuda

Halogen adsorbates on polymer-stabilized gold clusters: Mass spectrometric detection and effects on catalysis

Ryo Ishida^a, Setsuka Arii^a, Wataru Kurashige^b, Seiji Yamazoe^a,c, Kiichirou Koyasu^a,c, Yuichi Negishi^b, Tatsuya Tsukuda^a,c

a Department of Chemistry, School of Science, The University of Tokyo, 7-3-1 Hongo, Bunkyoku, Tokyo 113-0033, Japan;
b Department of Applied Chemistry, Faculty of Science, Tokyo University of Science, 1-3 Kagurazaka, Shinjuku-ku, Tokyo 162-8601, Japan;
c Elements Strategy Initiative for Catalysts and Batteries(ESICB), Kyoto University, Katsura, Kyoto 615-8520, Japan

Received:2016-05-06 Revised:2016-06-15 Online:2016-10-21 Published:2016-10-22
Contact: Tatsuya Tsukuda
Supported by:
This work was supported by the Elements Strategy Initiative for Catalysts and Batteries (ESICB) and a Grant-in-Aid for Scientific Research (26248003, 15H01042) from the Ministry of Education, Culture, Sports, Science and Technology (MEXT) of Japan.

摘要/Abstract

摘要：

聚（N-乙烯基-2-吡咯烷酮）稳定的金簇合物（Au：PVP）的质谱结果表明，来源于合成前驱体的Cl吸附质主要存在于Au₃₄和Au₄₃簇合物上.金簇合物上Cl吸附质的数量不影响其催化有氧苯甲醇氧化性能，表明Cl原子与Au簇合物间存在较弱的键合作用.相反，用Br替代Au₃₄和Au₄₃簇合物上Cl显著抑制了其催化活性，但对其电子结构没有任何影响.这表明，Br原子与金簇合物的键合较强，在空间上堵塞了活性位.因Br吸附质而导致活性显著下降表明，Au₃₄和Au₄₃簇合物对Au：PVP催化活性起主要贡献.

关键词: 金簇合物, 聚(N-乙烯基-2-吡咯烷酮), 卤素吸附质, 有氧醇氧化, 质谱

Abstract:

The mass spectrometry of gold clusters stabilized by poly(N-vinyl-2-pyrrolidone) (Au:PVP) revealed the presence of Cl adsorbates derived from synthetic precursors, mainly on the Au₃₄ and Au₄₃ clusters. Changes in the amount of Cl adsorbates on the Au clusters did not affect the catalytic properties for the aerobic oxidation of benzyl alcohol, suggesting that the Cl atoms were only weakly bound to the Au clusters. In contrast, the replacement of Cl with Br on the Au₃₄ and Au₄₃ clusters significantly suppressed activity, without any influence on the electronic structure. This result indicated that the Br atoms were strongly bound to the Au clusters and sterically blocked their active sites. The substantial reduction of the catalytic activity by the Br adsorbates suggested that the Au₃₄ and Au₄₃ clusters made a major contribution to the catalytic activity of the Au:PVP.

Key words: Gold cluster, Poly(N-vinyl-2-pyrrolidone), Halogen adsorbates, Aerobic alcohol oxidation, Mass spectrometry

Ryo Ishida, Setsuka Arii, Wataru Kurashige, Seiji Yamazoe, Kiichirou Koyasu, Yuichi Negishi, Tatsuya Tsukuda. 聚合物稳定的金簇合物上卤素吸附质:质谱检测及其对催化的影响[J]. 催化学报, 2016, 37(10): 1656-1661.

Ryo Ishida, Setsuka Arii, Wataru Kurashige, Seiji Yamazoe, Kiichirou Koyasu, Yuichi Negishi, Tatsuya Tsukuda. Halogen adsorbates on polymer-stabilized gold clusters: Mass spectrometric detection and effects on catalysis[J]. Chinese Journal of Catalysis, 2016, 37(10): 1656-1661.

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聚合物稳定的金簇合物上卤素吸附质:质谱检测及其对催化的影响

Halogen adsorbates on polymer-stabilized gold clusters: Mass spectrometric detection and effects on catalysis

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