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氮化银和氮化铜协同作用实现将一氧化碳电还原为丙醇。

Silver and Copper Nitride Cooperate for CO Electroreduction to Propanol.

作者信息

Phong Duong Hong, Rivera de la Cruz Jose Guillermo, Tran Ngoc-Huan, Louis Jacques, Zanna Sandrine, Portehault David, Zitolo Andrea, Walls Michael, Peron Deizi Vanessa, Schreiber Moritz W, Menguy Nicolas, Fontecave Marc

机构信息

Laboratoire de Chimie des Processus Biologiques, CNRS UMR 8229, Collège de France, Sorbonne Université, 11 Place Marcelin Berthelot, 75231, Paris Cedex 05, France.

Laboratoire de Chimie du Solide et Energie, CNRS UMR 8260, Collège de France, Sorbonne Université, 1 Place Marcelin Berthelot, 75231, Paris Cedex 05, France.

出版信息

Angew Chem Int Ed Engl. 2023 Dec 4;62(49):e202310788. doi: 10.1002/anie.202310788. Epub 2023 Oct 31.

Abstract

The need of carbon sources for the chemical industry, alternative to fossil sources, has pointed to CO as a possible feedstock. While CO electroreduction (CO R) allows production of interesting organic compounds, it suffers from large carbon losses, mainly due to carbonate formation. This is why, quite recently, tandem CO R, a two-step process, with first CO R to CO using a solid oxide electrolysis cell followed by CO electroreduction (COR), has been considered, since no carbon is lost as carbonate in either step. Here we report a novel copper-based catalyst, silver-doped copper nitride, with record selectivity for formation of propanol (Faradaic efficiency: 45 %), an industrially relevant compound, from CO electroreduction in gas-fed flow cells. Selective propanol formation occurs at metallic copper atoms derived from copper nitride and is promoted by silver doping as shown experimentally and computationally. In addition, the selectivity for C liquid products (Faradaic efficiency: 80 %) is among the highest reported so far. These findings open new perspectives regarding the design of catalysts for production of C compounds from CO .

摘要

化学工业对替代化石燃料来源的碳源的需求,使一氧化碳成为一种可能的原料。虽然一氧化碳电还原(COR)能够生产出有价值的有机化合物,但它存在大量的碳损失,主要是由于碳酸盐的形成。这就是为什么最近人们考虑采用串联式一氧化碳电还原,这是一个两步过程,首先使用固体氧化物电解池将一氧化碳还原为一氧化碳,然后进行一氧化碳电还原(COR),因为在这两个步骤中都没有碳以碳酸盐的形式损失。在此,我们报道了一种新型的铜基催化剂——银掺杂氮化铜,在气体进料流动池中由一氧化碳电还原生成丙醇(法拉第效率:45%)时具有创纪录的选择性,丙醇是一种与工业相关的化合物。实验和计算结果表明,选择性丙醇的形成发生在氮化铜衍生的金属铜原子上,并且银掺杂对其有促进作用。此外,C液体产物的选择性(法拉第效率:80%)是迄今为止报道的最高值之一。这些发现为设计从一氧化碳生产碳化合物的催化剂开辟了新的前景。

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