Silver Single‐Atom Catalyst for Efficient Electrochemical CO2 Reduction Synthesized from Thermal Transformation and Surface Reconstruction,Angewandte Chemie International Edition

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Silver Single‐Atom Catalyst for Efficient Electrochemical CO2 Reduction Synthesized from Thermal Transformation and Surface Reconstruction
Angewandte Chemie International Edition ( IF 16.1 ) Pub Date : 2020-12-04 , DOI: 10.1002/anie.202014718
Ningqiang Zhang ₁ , Xinxin Zhang ₂ , Lei Tao ₃ , Peng Jiang ₁ , Chenliang Ye ₁ , Rui Lin ₁ , Zhiwei Huang ₄ , Ang Li ₅ , Dawei Pang ₅ , Han Yan ₁ , Yu Wang ₆ , Peng Xu ₇ , Sufeng An ₈ , Qinghua Zhang ₆ , Licheng Liu ₆ , Shixuan Du ₆ , Xiaodong Han ₅ , Dingsheng Wang ₉ , Yadong Li ₁

Affiliation

We report an Ag₁ single‐atom catalyst (Ag₁/MnO₂), which was synthesized from thermal transformation of Ag nanoparticles (NPs) and surface reconstruction of MnO₂. The evolution process of Ag NPs to single atoms is firstly revealed by various techniques, including in situ ETEM, in situ XRD and DFT calculations. The temperature‐induced surface reconstruction process from the MnO₂ (211) to (310) lattice plane is critical to firmly confine the existing surface of Ag single atoms; that is, the thermal treatment and surface reconstruction of MnO₂ is the driving force for the formation of single Ag atoms. The as‐obtained Ag₁/MnO₂ achieved 95.7 % Faradic efficiency at −0.85 V vs. RHE, and coupled with long‐term stability for electrochemical CO₂ reduction reaction (CO₂RR). DFT calculations indicated single Ag sites possessed high electronic density close to Fermi Level and could act exclusively as the active sites in the CO₂RR. As a result, the Ag₁/MnO₂ catalyst demonstrated remarkable performance for the CO₂RR, far surpassing the conventional Ag nanosized catalyst (Ag_NP/MnO₂) and other reported Ag‐based catalysts.

中文翻译：

通过热转化和表面重建合成的银单原子催化剂，可有效降低电化学CO2排放

我们报告了一种Ag ₁单原子催化剂（Ag ₁ / MnO ₂），它是通过Ag纳米颗粒（NPs）的热转化和MnO _2的表面重构合成的。首先通过多种技术揭示了银纳米颗粒向单原子的演化过程，包括原位ETEM，原位XRD和DFT计算。从MnO ₂（211）到（310）晶格表面的温度诱导表面重建过程对于牢固地限制Ag单原子的存在表面至关重要。即，MnO _2的热处理和表面重构是形成单个Ag原子的驱动力。所得的Ag ₁ / MnO ₂相对于RHE，在-0.85 V时可达到95.7％的法拉第效率，并具有电化学CO ₂还原反应（CO ₂ RR）的长期稳定性。DFT计算表明，单个Ag位点具有接近费米能级的高电子密度，并且可以仅充当CO ₂ RR中的活性位点。结果，Ag ₁ / MnO ₂催化剂表现出了出色的CO ₂ RR性能，远远超过了传统的Ag纳米催化剂（Ag _NP / MnO ₂）和其他已报道的基于Ag的催化剂。

更新日期：2020-12-04

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