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Yuan-Yuan Dong1, Chun-Yu Liu2, Wan-Qi Shi1
1Department of Chemistry, Engineering Research Center of Advanced Rare Earth Materials (Ministry of Education), Tsinghua University, Beijing, 100084, P.R. China.
一个新的黄金纳米集群,Au26,利用松散的协调策略来创建可访问的开放金属站点. 这种稳定,开的催化剂在选择性醇氧化中表现出卓越的性能.
科学领域:
- * 纳米催化剂的使用
- * 有机金属化学
- * 材料科学 材料科学
背景情况:
- * 开放的金属位点对于催化活性至关重要.
- * 设计具有可访问活性位点的催化剂仍然是一个挑战.
- *金纳米集群具有独特的电子和催化性能.
研究的目的:
- * 开发一种采用松散协调策略,预先组织开放金属位点的金纳米团催化剂.
- * 为了研究产生的黄金纳米团的电子结构和稳定性.
- * 评估新型催化剂在选择性氧化反应中的催化性能.
主要方法:
- * 黄金纳米集群的一合成 [Au26(3,4-Me2-Ph-形式) 9(iPr2-imy) 3(Me2S) ](BF4) 2.2.
- *电子喷雾电离飞行时间质谱 (ESI-TOF-MS) 验证连接体脱离和开放部位形成.
- *用2-纳夫他乙醇进行发光定位,以量化可访问的金原子.
- * 超导量子干扰装置 (SQUID) 和电子磁共振 (EPR) 用于确认未配对电子的存在.
主要成果:
- * 一个稳定的,开的金纳米集群 (Au26) 与可访问的开放金属位点被成功合成.
- *ESI-TOF-MS证实了Me2S连接体的分离,形成了活性位点.
- *发光定位量化验证了暴露的黄金原子的可访问性.
- * SQUID和EPR分析证实Au26具有15个价值电子和一个未配对的电子.
- * Au26催化剂表现出了显著的稳定性和高的催化活性,用于选择性氧化醇到甲,周转率高达100670.
结论:
- * 松散协调策略有效地预先组织黄金集群催化剂中的开放金属位点.
- * 开放的,富含电子的Au26纳米集群表现出卓越的稳定性和催化效率.
- * 这项研究为选择性氧化反应提供了一个有前途的新黄金催化剂.
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