Pressure-induced generation of heterogeneous electrocatalytic metal hydride surfaces for sustainable hydrogen transfer.
Laihao LuoXinyan LiuXinyu ZhaoXinyan ZhangHong-Jie PengKe YeKun JiangQiu JiangJie ZengTingting ZhengChuan XiaPublished in: Nature communications (2024)
Metal hydrides are crucial intermediates in numerous catalytic reactions. Intensive efforts have been dedicated to constructing molecular metal hydrides, where toxic precursors and delicate mediators are usually involved. Herein, we demonstrate a facile pressure-induced methodology to generate a cost-effective heterogeneous electrocatalytic metal hydride surface for sustainable hydrogen transfer. Taking carbon dioxide (CO 2 ) electroreduction as a model system and zinc (Zn), a well-known carbon monoxide (CO)-selective catalyst, as a model catalyst, we showcase a homogeneous-type hydrogen atom transfer process induced by heterogeneous hydride surfaces, enabling direct hydrogenation pathways traditionally considered "prohibited". Specifically, the maximal Faradaic efficiency for formate is enhanced by ~fivefold to 83% under ambient conditions. Experimental and theoretical analyses reveal that unlike the distal hydrogenation route for CO 2 to CO over pristine Zn, the Zn hydride surface enables direct hydrogenation at the carbon site of CO 2 to form formate. This work provides a promising material platform for sustainable synthesis.
Keyphrases
- carbon dioxide
- reduced graphene oxide
- visible light
- metal organic framework
- heavy metals
- high glucose
- diabetic rats
- highly efficient
- ionic liquid
- air pollution
- room temperature
- biofilm formation
- minimally invasive
- high throughput
- risk assessment
- electron transfer
- genome wide
- heart rate
- molecular dynamics
- escherichia coli
- single cell
- oxidative stress
- pseudomonas aeruginosa
- dna methylation