Synergistic Pd-Au Catalyst for Selective Electrosynthesis of Dimethyl Carbonate in Conjunction with High-Rate Redox System,Advanced Functional Materials

当前位置： X-MOL 学术 › Adv. Funct. Mater. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

Synergistic Pd-Au Catalyst for Selective Electrosynthesis of Dimethyl Carbonate in Conjunction with High-Rate Redox System
Advanced Functional Materials ( IF 18.5 ) Pub Date : 2024-09-18 , DOI: 10.1002/adfm.202412402
Naohiro Fujinuma ₁ , Natalie Page ₂ , Anna G Boddy ₃ , Joshua Rivkind ₃ , Lindsey Tomlinson ₃ , Erik P Hoy ₃ , Samuel E Lofland ₂

Affiliation

This study reports ambient electrosynthesis of dimethyl carbonate with a palladium–gold catalyst. Material screening identifies a region of intermediate-catalyst binding energy that facilitates interfacial electron and proton transfers for selective carbonylation, achieving a distinct maximum of 92% faradaic efficiency to dimethyl carbonate. Structural and electrochemical analyses suggest that the alloying of palladium and gold effectively modulates the CO* binding energy to the catalytic surface, in accord with subsequent computational studies. With an extended heterogeneous–homogeneous catalytic environment with a halide redox mediator, a remarkable partial current density of 52 mA cm⁻² is observed for dimethyl carbonate for 100 h of continuous operation.

中文翻译：

协同 Pd-Au 催化剂与高速氧化还原系统联合用于碳酸二甲酯选择性电合成

本研究报道了碳酸二甲酯与钯-金催化剂的环境电合成。材料筛选确定一个中间催化剂结合能区域，该区域有助于界面电子和质子转移以进行选择性羰基化，从而达到对碳酸二甲酯 92% 法拉第效率的明显最大值。结构和电化学分析表明，钯和金的合金化有效地调节了催化表面的 CO* 结合能，这与随后的计算研究一致。在具有卤化物氧化还原介质的扩展非均相-均相催化环境中，在连续运行 100 小时期间，观察到碳酸二甲酯的显着部分电流密度为 52 mA ^cm-2。

更新日期：2024-09-18

点击分享查看原文

点击收藏

公开下载

阅读更多本刊新发论文本刊介绍/投稿指南