Towards the Operational Window for Nitridic and Carbidic Palladium Nanoparticles for Directed Catalysis

Towards the Operational Window for Nitridic and Carbidic Palladium Nanoparticles for Directed Catalysis
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面向氮化和碳化钯纳米颗粒定向催化的操作窗口

DOI:
10.1002/cctc.202300870
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发表时间:
2023
期刊:
影响因子:
4.5
通讯作者:
Costley-Wood L
Costley-Wood L
中科院分区:
化学3区
文献类型:
--
作者:
Costley-Wood L

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Pd形成间隙结构的反应在催化中是非常重要和普遍的;Pd氢化物结构的形成和稳定性已被很好地了解,但碳化物和氮化物的间隙结构相对较少被探索。本文报道用 在Pd L3边XANES谱中系统地研究了PdCx和PdNx在高温和不同气氛下的形成和稳定性。这些研究进一步得到了14N MAS-核磁共振实验和计算密度泛函研究的应用的补充。实验证实,PdCx的稳定性明显高于PdNx;14N MAS-核磁共振直接证实了氮化物的形成,但XANES研究表明,在所用条件下的稳定性非常有限。此外,结果表明,氮化物的形成带来了一些结构变化,这些变化在这些实验所用的条件下是不完全可逆的。这项工作对钯的间隙结构的稳定性以及它们可以用于定向催化过程的条件提供了重要的见解。
The reactions under which interstitial structures of Pd form are profoundly important and prevalent in catalysis; the formation and stability of Pd hydride structures are well understood, however, interstitial structures of the carbide and nitride are relatively under explored. This work reports a systematic study of the formation and stability of PdCxand PdNxat elevated temperatures and different atmospheres usingin situPd L3edge XANES spectroscopy. These studies were further complemented by the application of14N MAS‐NMR experiments and computational DFT investigations. The experiments confirmed that PdCxwas significantly more stable than PdNx;14N MAS‐NMR provided direct confirmation on the formation of the nitride, however, the XANES studies evidenced very limited stability under the conditions employed. Moreover, the results suggest that the formation of the nitride imparts some structural changes that are not entirely reversible under the conditions used in these experiments. This work provides important insights into the stability of interstitial structures of Pd and the conditions in which they could be employed for directed catalytic processes.
选定金属硼化物、氮化物和磷化物的研究。
DOI: --
发表时间: 1951
期刊:
影响因子: --
作者:
T. Bailey;J. F. Mudd;J. B. Milwee
通讯作者: J. B. Milwee