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Contracted Fe–N5–C11 Sites in Single-Atom Catalysts Boosting Catalytic Performance for Oxygen Reduction Reaction
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-06-28 , DOI: 10.1021/acsami.3c03982
Chao Xu 1 , Yan-Ping Zhang 2 , Tian-Long Zheng 3 , Zhi-Qiang Wang 2 , Ye-Min Zhao 1 , Peng-Peng Guo 1 , Chen Lu 1 , Kun-Zu Yang 1 , Ping-Jie Wei 1 , Qing-Gang He 3 , Xue-Qing Gong 2 , Jin-Gang Liu 1
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2023-06-28 , DOI: 10.1021/acsami.3c03982
Chao Xu 1 , Yan-Ping Zhang 2 , Tian-Long Zheng 3 , Zhi-Qiang Wang 2 , Ye-Min Zhao 1 , Peng-Peng Guo 1 , Chen Lu 1 , Kun-Zu Yang 1 , Ping-Jie Wei 1 , Qing-Gang He 3 , Xue-Qing Gong 2 , Jin-Gang Liu 1
Affiliation
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Promoting the catalyst performance for oxygen reduction reaction (ORR) in energy conversion devices through controlled manipulation of the structure of catalytic active sites has been a major challenge. In this work, we prepared Fe–N–C single-atom catalysts (SACs) with Fe–N5 active sites and found that the catalytic activity of the catalyst with shrinkable Fe–N5–C11 sites for ORR was significantly improved compared with the catalyst bearing normal Fe–N5–C12 sites. The catalyst C@PVI-(TPC)Fe-800, prepared by pyrolyzing an axial-imidazole-coordinated iron corrole precursor, exhibited positive shifted half-wave potential (E1/2 = 0.89 V vs RHE) and higher peak power density (Pmax = 129 mW/cm2) than the iron porphyrin-derived counterpart C@PVI-(TPP)Fe-800 (E1/2 = 0.81 V, Pmax = 110 mW/cm2) in 0.1 M KOH electrolyte and Zn–air batteries, respectively. X-ray absorption spectroscopy (XAS) analysis of C@PVI-(TPC)Fe-800 revealed a contracted Fe–N5–C11 structure with iron in a higher oxidation state than the porphyrin-derived Fe–N5–C12 counterpart. Density functional theory (DFT) calculations demonstrated that C@PVI-(TPC)Fe-800 possesses a higher HOMO energy level than C@PVI-(TPP)Fe-800, which can increase its electron-donating ability and thus help achieve enhanced O2 adsorption as well as O–O bond activation. This work provides a new approach to tune the active site structure of SACs with unique contracted Fe–N5–C11 sites that remarkably promote the catalyst performance, suggesting significant implications for catalyst design in energy conversion devices.
中文翻译：
单原子催化剂中的收缩 Fe-N5-C11 位点提高了氧还原反应的催化性能
通过控制催化活性位点的结构来提高能量转换装置中氧还原反应（ORR）的催化剂性能一直是一个重大挑战。在这项工作中，我们制备了具有Fe–N 5活性位点的Fe–N–C单原子催化剂（SAC），发现具有可收缩Fe–N 5 –C 11位点的催化剂对ORR的催化活性比传统催化剂显着提高。催化剂带有正常的 Fe–N 5 –C 12位点。通过热解轴向咪唑配位铁咯咯前驱体制备的催化剂C@PVI-(TPC)Fe-800表现出正移半波电位( E 1/2= 0.89 V vs RHE) 和比铁卟啉衍生对应物 C@PVI-(TPP)Fe-800 ( E 1/2 = 0.81 V, P max = 129 mW/cm 2 )更高的峰值功率密度 ( P max = 129 mW/cm 2 ) 0.1 M KOH 电解质和锌空气电池中分别为110 mW/cm 2 ）。C@PVI-(TPC)Fe-800 的 X 射线吸收光谱 (XAS) 分析揭示了收缩的 Fe–N 5 –C 11结构，其中铁的氧化态比卟啉衍生的 Fe–N 5 –C 12更高对方。密度泛函理论（DFT）计算表明，C@PVI-(TPC)Fe-800具有比C@PVI-(TPP)Fe-800更高的HOMO能级，这可以增加其给电子能力，从而有助于实现增强O 2吸附以及O-O键活化。这项工作提供了一种调整SAC活性位点结构的新方法，该SAC具有独特的收缩Fe-N 5 -C 11位点，可显着提高催化剂性能，这对能量转换装置中的催化剂设计具有重要意义。
更新日期：2023-06-28
中文翻译：
单原子催化剂中的收缩 Fe-N5-C11 位点提高了氧还原反应的催化性能
通过控制催化活性位点的结构来提高能量转换装置中氧还原反应（ORR）的催化剂性能一直是一个重大挑战。在这项工作中，我们制备了具有Fe–N 5活性位点的Fe–N–C单原子催化剂（SAC），发现具有可收缩Fe–N 5 –C 11位点的催化剂对ORR的催化活性比传统催化剂显着提高。催化剂带有正常的 Fe–N 5 –C 12位点。通过热解轴向咪唑配位铁咯咯前驱体制备的催化剂C@PVI-(TPC)Fe-800表现出正移半波电位( E 1/2= 0.89 V vs RHE) 和比铁卟啉衍生对应物 C@PVI-(TPP)Fe-800 ( E 1/2 = 0.81 V, P max = 129 mW/cm 2 )更高的峰值功率密度 ( P max = 129 mW/cm 2 ) 0.1 M KOH 电解质和锌空气电池中分别为110 mW/cm 2 ）。C@PVI-(TPC)Fe-800 的 X 射线吸收光谱 (XAS) 分析揭示了收缩的 Fe–N 5 –C 11结构，其中铁的氧化态比卟啉衍生的 Fe–N 5 –C 12更高对方。密度泛函理论（DFT）计算表明，C@PVI-(TPC)Fe-800具有比C@PVI-(TPP)Fe-800更高的HOMO能级，这可以增加其给电子能力，从而有助于实现增强O 2吸附以及O-O键活化。这项工作提供了一种调整SAC活性位点结构的新方法，该SAC具有独特的收缩Fe-N 5 -C 11位点，可显着提高催化剂性能，这对能量转换装置中的催化剂设计具有重要意义。
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