Deciphering the alternating synergy between interlayer Pt single-atom and NiFe layered double hydroxide for overall water splitting

Single-atom catalysts (SACs) have enormous significance in heterogeneous catalysis. However, understanding how SACs function at the molecular level remains a huge challenge. Here, we report a general approach to anchor Pt single-atom intercalated in layered double hydroxide (LDH) and decipher the al...

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Bibliographic Details
Published in:Energy & environmental science 2021-12, Vol.14 (12), p.6428-644
Main Authors: Chen, Wei, Wu, Binbin, Wang, Yanyong, Zhou, Wang, Li, Yingying, Liu, Tianyang, Xie, Chao, Xu, Leitao, Du, Shiqian, Song, Minglei, Wang, Dongdong, liu, Yanbo, Li, Yefei, Liu, Jilei, Zou, Yuqin, Chen, Ru, Chen, Chen, Zheng, Jianyun, Li, Yafei, Chen, Jun, Wang, Shuangyin
Format: Article
Language:English
Subjects:
Catalysis
Catalysts
Charge transport
Chemical reactions
Electrochemical impedance spectroscopy
Electrochemistry
Hydroxides
Interlayers
Intermetallic compounds
Iron compounds
Nickel base alloys
Nickel compounds
Oxygen evolution reactions
Phase transitions
Spectroscopy
Water splitting
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Summary:Single-atom catalysts (SACs) have enormous significance in heterogeneous catalysis. However, understanding how SACs function at the molecular level remains a huge challenge. Here, we report a general approach to anchor Pt single-atom intercalated in layered double hydroxide (LDH) and decipher the alternating synergy between Pt single-atom and Ni 3 Fe LDH support for overall water splitting. Aided with Tafel slope, interface species evolution and control experiments, operando electrochemical impedance spectroscopy (EIS) can distinguish interface charge transport and elementary reactions during hydrogen and oxygen evolution reactions (HER and OER). For HER, interlayer Pt single-atom vastly enhances electron transferability of LDH support, and Ni 3 Fe LDH support accelerates water dissociation, thus resulting in a mixture of mechanisms (Heyrovsky-Volmer and Tafel-Volmer) in 1 M KOH. For OER, interlayer Pt single-atom not only prompts active phase transition from NiFe LDH to Ni 2+ δ Fe 3+ ζ O x H y , but also optimizes OER intrinsic activity of Ni 2+ δ -O-Fe 3+ ζ in Ni 2+ δ Fe 3+ ζ O x H y . Overall, we provide a referential paradigm for SACs synthesis strategy and unscrambling its alternating synergy. Single-atom catalysts (SACs) have enormous significance in heterogeneous catalysis.
ISSN:1754-5692
1754-5706
DOI:10.1039/d1ee01395e