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Unveiling the Nature of Pt Single‐Atom Catalyst during Electrocatalytic Hydrogen Evolution and Oxygen Reduction Reactions
Small ( IF 13.0 ) Pub Date : 2021-02-19 , DOI: 10.1002/smll.202007245 Junjie Li 1 , Mohammad Norouzi Banis 1 , Zhouhong Ren 2 , Keegan R. Adair 1 , Kieran Doyle‐Davis 1 , Debora Motta Meira 3, 4 , Y. Zou Finfrock 3, 4 , Lei Zhang 1 , Fanpeng Kong 1 , Tsun‐Kong Sham 5 , Ruying Li 1 , Jun Luo 2 , Xueliang Sun 1
Small ( IF 13.0 ) Pub Date : 2021-02-19 , DOI: 10.1002/smll.202007245 Junjie Li 1 , Mohammad Norouzi Banis 1 , Zhouhong Ren 2 , Keegan R. Adair 1 , Kieran Doyle‐Davis 1 , Debora Motta Meira 3, 4 , Y. Zou Finfrock 3, 4 , Lei Zhang 1 , Fanpeng Kong 1 , Tsun‐Kong Sham 5 , Ruying Li 1 , Jun Luo 2 , Xueliang Sun 1
Affiliation
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Single‐atom catalysts (SACs) have attracted significant attention due to their superior catalytic activity and selectivity. However, the nature of active sites of SACs under realistic reaction conditions is ambiguous. In this work, high loading Pt single atoms on graphitic carbon nitride (g‐C3N4)‐derived N‐doped carbon nanosheets (Pt1/NCNS) is achieved through atomic layer deposition. Operando X‐ray absorption spectroscopy (XAS) is performed on Pt single atoms and nanoparticles (NPs) in both the hydrogen evolution reaction (HER) and oxygen reduction reaction (ORR). The operando results indicate that the total unoccupied density of states of Pt 5d orbitals of Pt1 atoms is higher than that of Pt NPs under HER condition, and that a stable Pt oxide is formed during ORR on Pt1/NCNS, which may suppress the adsorption and activation of O2. This work unveils the nature of Pt single atoms under realistic HER and ORR conditions, providing a deeper understanding for designing advanced SACs.
中文翻译：
揭示Pt单原子催化剂在电催化氢释放和氧还原反应过程中的性质
单原子催化剂（SAC）由于其出色的催化活性和选择性而备受关注。但是，在实际反应条件下SAC活性位点的性质是模棱两可的。在这项工作中，通过原子层沉积获得了石墨氮化碳（g-C 3 N 4）衍生的N掺杂碳纳米片（Pt 1 / NCNS）上的高负载Pt单原子。Operatdo X射线吸收光谱（XAS）在氢气析出反应（HER）和氧还原反应（ORR）中都对Pt单原子和纳米颗粒（NPs）进行。操作结果表明，Pt 1的Pt 5 d轨道的状态的总未占用密度在HER条件下，Pt NPs的原子数高于Pt NPs，并且在Pt 1 / NCNS上的ORR过程中形成稳定的Pt氧化物，这可能会抑制O 2的吸附和活化。这项工作揭示了在现实的HER和ORR条件下Pt单原子的性质，为设计高级SAC提供了更深刻的理解。
更新日期：2021-03-18
中文翻译：
揭示Pt单原子催化剂在电催化氢释放和氧还原反应过程中的性质
单原子催化剂（SAC）由于其出色的催化活性和选择性而备受关注。但是，在实际反应条件下SAC活性位点的性质是模棱两可的。在这项工作中，通过原子层沉积获得了石墨氮化碳（g-C 3 N 4）衍生的N掺杂碳纳米片（Pt 1 / NCNS）上的高负载Pt单原子。Operatdo X射线吸收光谱（XAS）在氢气析出反应（HER）和氧还原反应（ORR）中都对Pt单原子和纳米颗粒（NPs）进行。操作结果表明，Pt 1的Pt 5 d轨道的状态的总未占用密度在HER条件下，Pt NPs的原子数高于Pt NPs，并且在Pt 1 / NCNS上的ORR过程中形成稳定的Pt氧化物，这可能会抑制O 2的吸附和活化。这项工作揭示了在现实的HER和ORR条件下Pt单原子的性质，为设计高级SAC提供了更深刻的理解。
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