New route toward building active ruthenium nanoparticles on ordered mesoporous carbons with extremely high stability.
New route toward building active ruthenium nanoparticles on ordered mesoporous carbons with extremely high stability.
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在有序介孔碳上构建具有极高稳定性的活性钌纳米粒子的新途径
DOI：
10.1038/srep04540
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发表时间：
2014-04-01
影响因子：
4.6
通讯作者：
Jiang D
中科院分区：
文献类型：
--
作者：
Yang Y;Sun C;Ren Y;Hao S;Jiang D
创造高活性和稳定的金属催化剂是多相催化领域的一个持久目标。然而，由于活性位点和载体设计的限制，真正的催化剂很少能同时实现这两种品质。解决这个问题的一种方法是在同时形成的介孔载体的空隙上制造牢固附着的金属物质。在这项研究中，我们开发了一种新型钌催化剂，通过在热解和去除二氧化硅之前制造立方Ia3d壳聚糖-钌-二氧化硅中间相，该催化剂被有序介孔碳牢牢限制。这种简便的方法可生成均匀分散在介孔碳质框架上的细钌纳米颗粒（约 1.7 nm）。这种钌催化剂可以循环使用22次而不会损失任何反应活性，表现出所有金属催化剂中最高的稳定性；当金属负载量为 6.1 wt% 时，该催化剂在乙酰丙酸 (LA) 催化加氢过程中表现出高活性 (23.3 molLAh−1gmetal−1)。即使在超低负载量 (0.3 wt%) 下，该催化剂的性能仍然优于已知的最具活性的 Ru/C 催化剂。这项工作揭示了通过同时创建金属位点和介孔载体来设计和制造高度稳定和活性的金属催化剂的新可能性。
Creating highly active and stable metal catalysts is a persistent goal in the field of heterogeneous catalysis. However, a real catalyst can rarely achieve both of these qualities simultaneously due to limitations in the design of the active site and support. One method to circumvent this problem is to fabricate firmly attached metal species onto the voids of a mesoporous support formed simultaneously. In this study, we developed a new type of ruthenium catalyst that was firmly confined by ordered mesoporous carbons through the fabrication of a cubicIa3dchitosan-ruthenium-silica mesophase before pyrolysis and silica removal. This facile method generates fine ruthenium nanoparticles (ca.1.7 nm) that are homogeneously dispersed on a mesoporous carbonaceous framework. This ruthenium catalyst can be recycled 22 times without any loss of reactivity, showing the highest stability of any metal catalysts; this catalyst displays a high activity (23.3 molLAh−1gmetal−1) during the catalytic hydrogenation of levulinic acid (LA) when the metal loading is 6.1 wt%. Even at an ultralow loading (0.3 wt%), this catalyst still outperforms the most active known Ru/C catalyst. This work reveals new possibilities for designing and fabricating highly stable and active metal catalysts by creating metal sites and mesoporous supports simultaneously.
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影响因子：
7.3
作者：
Gallo, J. M. R.;Pastore, H. O.;Schuchardt, U.
通讯作者：
Schuchardt, U.
影响因子：
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作者：
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通讯作者：
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影响因子：
3.9
作者：
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影响因子：
19
作者：
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影响因子：
8.4
作者：
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通讯作者：
Palkovits, Regina