文献类型：期刊文献

英文题名：What Elements Really Intercalate into Pd Lattice When Heated in Dimethylformamide?

作者：Song, Xianmeng[1];Lu, Linzhe[1];Jia, Yanyan[2];Wang, Zhiyi[1];Nan, Zi-Ang[5];Hong, Yu-Hao[1];Chen, Daliang[1];Zhang, Qiuyue[1];Jiang, Jiahong[1];Zheng, Yanping[1];Xu, Jiajia[1];Qiu, Zufeng[1];Jiang, Qiaorong[1];Wang, Yanjie[1];Wang, Qiuxiang[3];Dai, Sheng[2];Lin, Haixin[1];Zhao, Zipeng[4];Chen, Mingshu[1];Xie, Zhaoxiong[1];Tian, Zhong-Qun[1];Fan, Feng Ru[1]

机构：[1]Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces, Innovat Lab Sci & Technol Energy Mat Fujian Prov I, Xiamen 361005, Peoples R China;[2]East China Univ Sci & Technol, Inst Fine Chem, Frontiers Sci Ctr Materiobiol & Dynam Chem, Feringa Nobel Prize Scientist Joint Res Ctr,Key La, Shanghai 200237, Peoples R China;[3]Huaqiao Univ, Instrumental Anal Ctr, Xiamen 361021, Peoples R China;[4]Beijing Inst Technol, Sch Mat Sci & Engn, Beijing 100081, Peoples R China;[5]Chinese Acad Sci, Fujian Inst Res Struct Matter, State Key Lab Struct Chem, Fuzhou 350002, Peoples R China

年份：2024

卷号：146

期号：22

起止页码：15320

外文期刊名：JOURNAL OF THE AMERICAN CHEMICAL SOCIETY

收录：;EI(收录号：20241916037054);WOS:【SCI-EXPANDED(收录号:WOS:001239723600001)】；

基金：This work was supported by and the National Natural Science Foundation of China (22222305, 22021001, 21931009, 22202082, 22202163, and 22109043) and the Natural Science Foundation of Xiamen, China (3502Z202371030).

语种：英文

外文关键词：Catalyst activity - Catalytic oxidation - Crystalline materials - Dimethylformamide - Electrocatalysis - High resolution transmission electron microscopy - Nanocrystals - Organic solvents - Organometallics - Palladium compounds - Scanning electron microscopy - Thermodynamic stability

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.