<br>二维氮化碳作为单 Cu、Ag 和 Au 原子的载体用于二氧化碳还原反应,Physical Chemistry Chemical Physics

当前位置： X-MOL 学术 › Phys. Chem. Chem. Phys. › 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.)

二维氮化碳作为单 Cu、Ag 和 Au 原子的载体用于二氧化碳还原反应
Physical Chemistry Chemical Physics ( IF 2.9 ) Pub Date : 2023-02-23 , DOI: 10.1039/d3cp00392b
Sergio Posada-Pérez ₁ , Anna Vidal-López _{1,

2} , Miquel Solà ₁ , Albert Poater ₁

Affiliation

将CO ₂电化学转化为增值化学品是回收CO _{2 的}重要途径。在这项工作中，我们结合了该反应最有效的金属催化剂，即Cu、Ag和Au，作为分散在二维氮化碳载体上的单原子颗粒，旨在探索它们在CO ₂中的性能。还原反应。在这里，我们报告了密度泛函理论计算，显示了单个金属原子颗粒对载体的影响。我们发现，裸碳氮化物需要高过电势来克服第一次质子-电子转移的能垒，而第二次转移是放能的。尽管在 Cu 和 Au 单原子上发现 CO 吸附具有强结合能，但单金属原子的沉积增强了系统的催化活性，因为在能量方面有利于第一次质子-电子转移。我们的理论解释与实验证据一致，即由于强CO结合能，竞争性H ₂生成受到青睐。我们的计算研究为寻找合适的金属铺平了道路，这些金属可以催化二氧化碳还原反应中的第一次质子-电子转移，并产生具有中等结合能的反应中间体，促进溢出到氮化碳载体上，从而充当双功能电催化剂。

"点击查看英文标题和摘要"

2D carbon nitride as a support with single Cu, Ag, and Au atoms for carbon dioxide reduction reaction

The electrochemical conversion of CO₂ into value-added chemicals is an important approach to recycling CO₂. In this work, we have combined the most efficient metal catalysts for this reaction, namely Cu, Ag, and Au, as single-atom particles dispersed on a two-dimensional carbon nitride support, with the aim of exploring their performance in the CO₂ reduction reaction. Here, we report density functional theory computations showing the effect of single metal-atom particles on the support. We found that bare carbon nitride needed a high overpotential to overcome the energy barrier for the first proton–electron transfer, while the second transfer was exergonic. The deposition of single metal atoms enhances the catalytic activity of the system as the first proton–electron transfer is favored in terms of energy, although strong binding energies were found for CO adsorption on Cu and Au single atoms. Our theoretical interpretations are consistent with the experimental evidence that the competitive H₂ generation is favored due to the strong CO binding energies. Our computational study paves the road to finding suitable metals that catalyze the first proton–electron transfer in the carbon dioxide reduction reaction and produce reaction intermediates with moderate binding energies, promoting a spillover to the carbon nitride support and thereby serving as bifunctional electrocatalysts.

更新日期：2023-02-23

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南