Boosting Interfacial Electron Transfer between Pd and ZnTi-LDH via Defect Induction for Enhanced Metal–Support Interaction in CO Direct Esterification Reaction

• Published in: ACS applied materials & interfaces Vol. 13; no. 21; pp. 24856 - 24864
• Main Authors: Jing, Kai-Qiang, Fu, Yu-Qing, Chen, Zhe-Ning, Zhang, Teng, Sun, Jing, Xu, Zhong-Ning, Guo, Guo-Cong
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 02.06.2021
• Subjects: Energy, Environmental, and Catalysis Applications; layered double hydroxide; electron transfer; metal−support interaction; CO direct esterification; defects
• ISSN: 1944-8244; 1944-8252
• DOI: 10.1021/acsami.1c04523

Strong metal–support interaction is crucial to the stability of catalysts in heterogeneous catalysis. However, reports on boosting interfacial electron transfer between metal and support via defect induction for enhanced metal–support interaction are limited. In this work, ultrathin reducible ZnTi-layered double hydroxide (LDH) nanosheets with rich oxygen defects were synthesized to stabilize Pd clusters, and the rich oxygen defects promoted Pd cluster bonding with Zn and Ti atoms in supports, thereby forming a metal–metal bond. Electron spin resonance (ESR), X-ray absorption fine spectra (XAFS), and density functional theory (DFT) calculations demonstrate remarkable interfacial electron transfer (0.62 e). The Pd/ZnTi-LDH catalyst shows superior catalytic stability for CO direct esterification to dimethyl oxalate. By contrast, the nonreducible Pd/ZnAl-LDH catalyst with a few oxygen defects shows minimal interfacial electron transfer (0.08 e), which leads to relatively poor catalytic stability. This work provides a deep insight into promoting the stability of catalysts by boosting interfacial electron transfer via defect induction.