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对于热催化与电催化酸盐还原反应的单原子的对比能力

Xuanhao Wu^1,2, Mohammadreza Nazemi², Srishti Gupta³

¹Department of Environmental Engineering, Zhejiang University, Hangzhou 310058, China.

ACS catalysis

|May 26, 2023

概括

单原子合金 (SAA) 在酸盐还原反应 (NRR) 中表现不同. Pd/Cu纳米合金对电催化NRR有效,实现高选择性,与热催化NRR不同.

科学领域:

环境科学环境科学
材料科学材料科学材料科学
催化剂是一种催化剂.

背景情况:

水中的高酸盐度会给环境和健康带来风险.
酸盐还原反应 (NRR) 对于水的整治至关重要.
单原子合金 (SAA) 是NRR的新兴催化剂.

研究的目的:

用Pd/Cu纳米合金研究热催化 (T-NRR) 和电催化 (E-NRR) 酸盐降解之间的性能差异.
为了确定最佳的SAA组合,以有效和选择性地去除酸盐.
阐明T-NRR和E-NRR之间的性能差异的机械起源.

主要方法:

合成和表征不同组成的Pd/Cu纳米合金.
对T-NRR和E-NRR的催化活性和选择性的评估.
密度函数理论 (DFT) 计算用于研究反应机制和中间体.

主要成果:

Pd/Cu_1:100)SAA表现出优越的活性 (TOF_Pd=2分钟-1) 和N_{2的选择性 (94%) 对于E-NRR.}
相同的Pd/Cu_(1:100)SAA在T-NRR中表现不佳,与其他纳米合金组合物相比.
DFT计算显示了增强的NO₃*稳定性和E-NRR中较低的N₂形成障碍,归因于局部的pH效应和质子可用性.

结论:

在SAA的T-NRR和E-NRR之间存在显著的绩效差异.
Pd/Cu_1:100)SAA是电催化酸盐去除的非常有前途的催化剂.
来自DFT的机制见解突出了局部pH和质子转移在E-NRR选择性中的重要性.

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