原子精确的(AgPd)27团簇用于硝酸盐电还原制氨：一种配体诱导策略来调控金属核

doi:10.3866/PKU.WHXB202403008

物理化学学报 >> 2025, Vol. 41 >> Issue (1): 100008.doi: 10.3866/PKU.WHXB202403008

原子精确的(AgPd)₂₇团簇用于硝酸盐电还原制氨：一种配体诱导策略来调控金属核

秦露冰¹^,†, 孙芳²^,†, 李美银³, 范浩¹, 王立开³, 唐青²^,*(), 王春栋⁴, 唐正华¹^,⁵^,*()

¹ 华南理工大学环境与能源学院新能源研究所, 广州 510006
² 重庆大学化学化工学院重庆市理论与计算化学重点实验室, 重庆 401331
³ 山东理工大学化学与化工学院, 山东淄博 255049
⁴ 华中科技大学集成电路学院武汉光电子国家实验室, 武汉 430074
⁵ 黑龙江大学功能无机材料化学教育部重点实验, 哈尔滨 150001

收稿日期:2024-03-11 修回日期:2024-04-25 录用日期:2024-04-25 发布日期:2024-11-27
通讯作者: Email: zhht@scut.edu.cn (唐正华)qingtang@cqu.edu.cn (唐青)
作者简介:
^†Lubing Qin and Fang Sun contributed equally to this work.
基金资助:
功能无机材料化学教育部重点实验室(黑龙江大学)开放基金; 广东省自然科学基金(2023A0505050107); 重庆市科学技术委员会(cstc2020jcyj-msxmX0382)

Atomically Precise (AgPd)₂₇ Nanoclusters for Nitrate Electroreduction to NH₃: Modulating the Metal Core by a Ligand Induced Strategy

Lubing Qin¹, Fang Sun², Meiyin Li³, Hao Fan¹, Likai Wang³, Qing Tang²^,*(), Chundong Wang⁴, Zhenghua Tang¹^,⁵^,*()

¹ New Energy Research Institute, School of Environment and Energy, South China University of Technology, Guangzhou 510006, China
² School of Chemistry and Chemical Engineering, Chongqing Key Laboratory of Theoretical and Computational Chemistry, Chongqing University, Chongqing 401331, China
³ School of Chemistry and Chemical Engineering, Shandong University of Technology, Zibo 255049, Shandong Province, China
⁴ School of Integrated Circuits, Wuhan National Laboratory for Optoelectronics, Huazhong University of Science and Technology, Wuhan 430074, China
⁵ Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, Harbin 150001, China

Received:2024-03-11 Revised:2024-04-25 Accepted:2024-04-25 Published:2024-11-27
Contact: Email: zhht@scut.edu.cn (Zhenghua Tang)qingtang@cqu.edu.cn (Qing Tang)
Supported by:
the Open Funds of Key Laboratory of Functional Inorganic Material Chemistry (Heilongjiang University), Ministry of Education, China; the funding from Guangdong Natural Science Funds(2023A0505050107); the Chongqing Science and Technology Commission(cstc2020jcyj-msxmX0382)

摘要/Abstract

摘要：

电化学硝酸根还原反应(eNO₃^–RR)合成氨是一种可持续的将环境污染物转化为高附加值产品的方法。钯基双金属纳米催化剂作为高效催化剂已显示出巨大的前景，但调控其组成和构型以提高催化性能并实现深入的机理理解仍然很有挑战。通过使用不同供/吸电子官能团的两个配体，我们成功地制备了两个原子精确的(AgPd)₂₇双金属团簇，即Ag₁₈Pd₉(C₈H₄F)₂₄ (简称Ag₁₈Pd₉)和Ag₂₂Pd₅(C₉H₁₀O₂)₂₆ (简称Ag₂₂Pd₅)。两个团簇的金属核具有明显不同组成和构型，其中Ag₁₈Pd₉为中间层是9个Pd原子的“三明治”型金属核结构，Ag₂₂Pd₅为M₁₃构型组成的棒状金属核结构，而5个钯原子位于M₁₃构型的顶点和中心位置。出乎意料的是，Ag₂₂Pd₅表现出明显优于Ag₁₈Pd₉的eNO₃⁻RR性能。具体表现来说，Ag₂₂Pd₅在−0.6 V时NH₃的法拉第效率和产生速率达到最高，分别为94.42%和1.41 mmol·h⁻¹·mg⁻¹，但Ag₁₈Pd₉的NH₃的最高法拉第效率和产生速率只有在−0.5 V时的43.86%和0.41 mmol·h⁻¹·mg⁻¹。原位衰减全反射表面增强红外光谱(ATR-SEIRAS)测试提供了反应中间体的实验证据，从而揭示了反应途径，也表明Ag₂₂Pd₅比Ag₁₈Pd₉具有更强的NO₃^–吸附和NH₃脱附能力。理论计算表明，配体脱落的团簇可以暴露AgPd双金属位点，Ag-Pd位点为协同催化活性位点，不同构型的AgPd活性位点有显著差异，其中Ag₂₂Pd₅中的活性位点更有利于NO₃⁻吸附和NH₃脱附，从而加速催化过程。

关键词: 电化学硝酸盐还原反应, 原子精确双金属团簇, Ag₁₈Pd₉(C₈H₄F)₂₄, Ag₂₂Pd₅(C₉H₁₀O₂)₂₆, 原位衰减全反射表面增强红外光谱, 理论计算

Abstract:

Electrochemical nitrate reduction reaction (eNO₃^–RR) to synthesize NH₃ is a sustainable method to convert environmental contaminants into valuables. Pd based bimetallic nanocatalysts have demonstrated great promise as efficient catalysts, yet modulating the composition and configuration to improve the catalytic performance and achieve comprehensive mechanistic understanding remains challenging. Herein, by employing two ligands with different electron functional groups, we successfully prepared two atomically precise (AgPd)₂₇ bimetallic clusters of Ag₁₈Pd₉(C₈H₄F)₂₄ (Ag₁₈Pd₉) and Ag₂₂Pd₅(C₉H₁₀O₂)₂₆ (Ag₂₂Pd₅). The two clusters possess markedly different metal core composition and configuration, where Ag₁₈Pd₉ has a sandwich metal core structure with 9 Pd atoms located in the middle layer and Ag₂₂Pd₅ has a rod-shaped metal core structure composed of the M₁₃ configuration with 5 Pd atoms located at the center and vertices of the M₁₃ configuration. Unexpectedly, Ag₂₂Pd₅ exhibited remarkably superior eNO₃⁻RR performance than Ag₁₈Pd₉. Specifically, the highest Faradaic efficiency of NH₃ (FE_NH3) and its yield rate can reach 94.42% and 1.41 mmol∙h⁻¹∙mg⁻¹ at −0.6 V vs. RHE for Ag₂₂Pd₅, but the largest FE_NH3 and NH₃ yield rate is only 43.86% and 0.41 mmol∙h⁻¹∙mg⁻¹ at −0.5 V vs. RHE for Ag₁₈Pd₉. The in situ attenuated total reflection surface enhanced infrared absorption spectroscopy (ATR-SEIRAS) test provides the experimental evidence of the reaction intermediates hence revealing the reaction pathway, also shows that Ag₂₂Pd₅ has stronger capability for NO₃⁻ adsorption and NH₃ desorption than that of Ag₁₈Pd₉. Theoretical calculations indicate that the de-ligated clusters can expose the available AgPd bimetallic sites, synergistically serving as effective active sites and the different configurations result in significantly different catalytic activities, where the active sites in Ag₂₂Pd₅ are more favorable for NO₃⁻ adsorption and NH₃ desorption to accelerate the catalytic process.

Key words: Electrochemical nitrate reduction reaction, Atomically precise bimetallic cluster, Ag₁₈Pd₉(C₈H₄F)₂₄, Ag₂₂Pd₅(C₉H₁₀O₂)₂₆, In situ attenuated total reflection surface enhanced infrared absorption spectroscopy, Theoretical calculations

秦露冰, 孙芳, 李美银, 范浩, 王立开, 唐青, 王春栋, 唐正华. 原子精确的(AgPd)₂₇团簇用于硝酸盐电还原制氨：一种配体诱导策略来调控金属核[J]. 物理化学学报, 2025, 41(1), 100008. doi: 10.3866/PKU.WHXB202403008

Lubing Qin, Fang Sun, Meiyin Li, Hao Fan, Likai Wang, Qing Tang, Chundong Wang, Zhenghua Tang. Atomically Precise (AgPd)₂₇ Nanoclusters for Nitrate Electroreduction to NH₃: Modulating the Metal Core by a Ligand Induced Strategy[J]. Acta Phys. -Chim. Sin. 2025, 41(1), 100008. doi: 10.3866/PKU.WHXB202403008

链接本文: https://www.whxb.pku.edu.cn/CN/10.3866/PKU.WHXB202403008

https://www.whxb.pku.edu.cn/CN/Y2025/V41/I1/100008

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