Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles.
Demonstration of chemistry at a point through restructuring and catalytic activation at anchored nanoparticles.
复制标题
DOI：
10.1038/s41467-017-01880-y
复制
发表时间：
2017-11-30
影响因子：
16.6
通讯作者：
Metcalfe IS
中科院分区：
文献类型：
--
作者：
Neagu D;Papaioannou EI;Ramli WKW;Miller DN;Murdoch BJ;Ménard H;Umar A;Barlow AJ;Cumpson PJ;Irvine JTS;Metcalfe IS
通过在钙钛矿氧化物表面析出制备的金属纳米颗粒，由于其嵌套的、良好的锚定结构，在催化、能量转换和存储技术方面取得了新的进展。在这里，我们表明，与一般的看法相反，被溶解的颗粒在氧化后不一定会重新溶解回底层的钙钛矿中。相反，它们可能会被固定在它们最初的位置，允许人们对它们进行进一步的化学转化，从而显著地改变它们的组成、结构和功能，同时保留它们最初的空间排列。我们把这个概念称为化学，并通过跟踪各个纳米颗粒在各种化学转化过程中的变化来说明它。我们通过制备纳米结构的富土金属催化剂，证明了其卓越的实用性，该催化剂在数百小时的运行中，其重量可与铂相媲美。我们的理念能够设计出具有优异稳定性和催化活性的成分多样的受限氧化物颗粒。在钙钛矿氧化物表面溶出制备的金属纳米颗粒是催化和能源领域的关键物质。在这里，作者通过跟踪在各种化学转化过程中具有优异活性和稳定性的单个纳米颗粒，开发了一个点化学概念。
Metal nanoparticles prepared by exsolution at the surface of perovskite oxides have been recently shown to enable new dimensions in catalysis and energy conversion and storage technologies owing to their socketed, well-anchored structure. Here we show that contrary to general belief, exsolved particles do not necessarily re-dissolve back into the underlying perovskite upon oxidation. Instead, they may remain pinned to their initial locations, allowing one to subject them to further chemical transformations to alter their composition, structure and functionality dramatically, while preserving their initial spatial arrangement. We refer to this concept as chemistry at a point and illustrate it by tracking individual nanoparticles throughout various chemical transformations. We demonstrate its remarkable practical utility by preparing a nanostructured earth abundant metal catalyst which rivals platinum on a weight basis over hundreds of hours of operation. Our concept enables the design of compositionally diverse confined oxide particles with superior stability and catalytic reactivity. Metal nanoparticles prepared by exsolution at the surface of perovskite oxides are key species in catalysis and energy fields. Here, the authors develop a chemistry at a point concept by tracking individual nanoparticles with excellent activity and stability throughout various chemical transformations.
登录
查看更多内容
用于 CO 氧化的 Co3O4 纳米带和纳米立方体模型催化剂的表面活性位点
影响因子：
9.9
作者：
Hu, Linhua;Sun, Keqiang;Li, Yadong
通讯作者：
Li, Yadong
影响因子：
7.3
作者：
Jansson, J;Palmqvist, AEC;Langer, V
通讯作者：
Langer, V
影响因子：
16.6
作者：
Neagu D;Oh TS;Miller DN;Ménard H;Bukhari SM;Gamble SR;Gorte RJ;Vohs JM;Irvine JTS
通讯作者：
Irvine JTS
影响因子：
3.7
作者：
Ha, Don-Hyung;Moreau, Liane M.;Robinson, Richard D.
通讯作者：
Robinson, Richard D.
影响因子：
12.9
作者：
Dai, Sheng;Zhang, Shuyi;Pan, Xiaoqing
通讯作者：
Pan, Xiaoqing