What Elements Really Intercalate into Pd Lattice When Heated in Dimethylformamide?

化学 纳米晶 亚稳态 化学物理 纳米尺度 催化作用 扫描透射电子显微镜 纳米技术 电催化剂 透射电子显微镜 化学工程 分析化学(期刊) 物理化学 有机化学 电极 材料科学 电化学 工程类
作者
Xianmeng Song,Delun Chen,Yanyan Jia,Zhiyi Wang,Zi‐Ang Nan,Yuhao Hong,Daliang Chen,Qiuyue Zhang,Jiahong Jiang,Yanping Zheng,Jiajia Xu,Zufeng Qiu,Qiaorong Jiang,Yan-Jie Wang,Qiuxiang Wang,Sheng Dai,Haixin Lin,Zipeng Zhao,Mingshu Chen,Zhaoxiong Xie,Zhong‐Qun Tian,Feng Ru Fan
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (22): 15320-15330 被引量:2
标识
DOI:10.1021/jacs.4c03046
摘要

Palladium hydrides (PdHx) are pivotal in both fundamental research and practical applications across a wide spectrum. PdHx nanocrystals, synthesized by heating in dimethylformamide (DMF), exhibit remarkable stability, granting them widespread applications in the field of electrocatalysis. However, this stability appears inconsistent with their metastable nature. The substantial challenges in characterizing nanoscale structures contribute to the limited understanding of this anomalous phenomenon. Here, through a series of well-conceived experimental designs and advanced characterization techniques, including aberration-corrected scanning transmission electron microscopy (AC-STEM), in situ X-ray diffraction (XRD), and time-of-flight secondary ion mass spectrometry (TOF-SIMS), we have uncovered evidence that indicates the presence of C and N within the lattice of Pd (PdCxNy), rather than H (PdHx). By combining theoretical calculations, we have thoroughly studied the potential configurations and thermodynamic stability of PdCxNy, demonstrating a 2.5:1 ratio of C to N infiltration into the Pd lattice. Furthermore, we successfully modulated the electronic structure of Pd nanocrystals through C and N doping, enhancing their catalytic activity in methanol oxidation reactions. This breakthrough provides a new perspective on the structure and composition of Pd-based nanocrystals infused with light elements, paving the way for the development of advanced catalytic materials in the future.
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