Deciphering the alternating synergy between interlayer Pt single-atom and NiFe layered double hydroxide for overall water splitting
Deciphering the alternating synergy between interlayer Pt single-atom and NiFe layered double hydroxide for overall water splitting
复制标题
解读层间 Pt 单原子和 NiFe 层状双氢氧化物之间的交替协同作用以实现整体水分解
DOI：
10.1039/d1ee01395e
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发表时间：
2021-10-13
影响因子：
32.5
通讯作者：
Wang, Shuangyin
中科院分区：
文献类型：
--
作者：
Chen, Wei;Wu, Binbin;Wang, Shuangyin
单原子催化剂在多相催化中具有重要意义。然而，了解SAC如何在分子水平上发挥作用仍然是一个巨大的挑战。在这里，我们报告了一个通用的方法来锚铂单原子插入层状双氢氧化物（LDH）和破译之间的交替协同作用Pt单原子和Ni 3Fe LDH支持整体水裂解。借助Tafel斜率、界面物种演化和控制实验，操作电化学阻抗谱（EIS）可以区分析氢和析氧反应（HER和OER）中的界面电荷传输和基元反应。对于HER，层间Pt单原子极大地增强了LDH载体的电子转移能力，并且Ni 3Fe LDH载体加速了水解离，从而导致在1 M KOH中的混合机制（Heyrovsky-Volmer和Tafel-Volmer）。对于OER，层间Pt单原子不仅促进了NiFe LDH向Ni 2 + δ Fe 3 +zeta OxHy的活性相变，而且优化了Ni 2 + δ Fe 3 +zeta OxHy中Ni 2 + δ-O-Fe（3+zeta）的本征OER活性。总的来说，我们提供了一个可供参考的范式，为SAC的综合战略和解读其交替协同作用。
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 Ni3Fe 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 Ni3Fe 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 Ni2+delta Fe3+zeta OxHy, but also optimizes OER intrinsic activity of Ni2+delta-O-Fe(3+zeta )in Ni2+delta Fe3+zeta OxHy. Overall, we provide a referential paradigm for SACs synthesis strategy and unscrambling its alternating synergy.