铂单原子和铂原子簇在硫掺杂氮化钛纳米管上的协同作用以增强析氢反应,Small

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铂单原子和铂原子簇在硫掺杂氮化钛纳米管上的协同作用以增强析氢反应
Small ( IF 13.0 ) Pub Date : 2022-11-02 , DOI: 10.1002/smll.202205603
Jing Yan ₁ , Zichao Xi ₁ , Linlin Cong ₂ , Kun Lv ₁ , Ruiyun Xin ₁ , Bo Cao ₁ , Baocang Liu ₁ , Jinlu He ₁ , Jun Zhang _{1,

3}

Affiliation

高度分散的 Pt，如 Pt 单原子和原子团簇，由于具有高原子效率和独特的电子构型，在电催化析氢反应（HER）中具有巨大的潜力。合理地重新调整 Pt 催化剂的电子结构对于提高 HER 性能是可取的。_{在此，一种由 Pt 单原子 (Pt SAs} ) 和 Pt 原子团簇 (Pt _ACs )组成的 3D 自支撑整体电极锚定在 Ti 网格上封装在聚苯胺 (PANI) 中的硫掺杂氮化钛纳米管 (S-TiN NTs) 上 ( PANI@Pt/S-TiN NTs/Ti) 通过一种简便的电化学策略设计并合成了高效的 HER。由独特的结构和组成以及 Pt _SAs、 Pt _{ACs的协同作用所贡献}和 S-TiN NTs 相比，PANI@Pt/S-TiN NTs/Ti 电极表现出超高的 HER 活性，在酸性、碱性和中性介质中 -10 mA cm ^-2下的过电位分别仅为 12、25 和 39 mV ，并且可以25 h 性能稳定。令人印象深刻的是，质量活度分别是 Pt/C/CC 电极的 26.1、22.4 和 17.7 倍。理论计算结果表明，Pt _SAs、Pt _ACs和 S-TiN NTs 的协同作用可以优化 Pt 的电子结构并产生多个具有热力学有利的氢吸附自由能 (Δ G _H* ) 的活性位点，从而导致增强的 HER 活性。

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Synergy of Platinum Single Atoms and Platinum Atomic Clusters on Sulfur-Doped Titanium Nitride Nanotubes for Enhanced Hydrogen Evolution Reaction

Highly dispersed Pt, such as Pt single atoms and atomic clusters, has great potential in the electrocatalytic hydrogen evolution reaction (HER) due to the high atomic efficiency and unique electronic configuration. Rationally regrating the electronic structure of Pt catalysts is desirable for promoting the HER performance. Herein, a 3D self-supported monolithic electrode consisting of Pt single atoms (Pt_SAs) and Pt atomic clusters (Pt_ACs) anchored on sulfur-doped titanium nitride nanotubes (S-TiN NTs) encapsulated in polyaniline (PANI) on Ti mesh (PANI@Pt/S-TiN NTs/Ti) via a facile electrochemical strategy for efficient HER is designed and synthesized. Contributed by the unique structure and composition and the synergy of Pt_SAs, Pt_ACs and S-TiN NTs, the PANI@Pt/S-TiN NTs/Ti electrode exhibits ultrahigh HER activities with only 12, 25 and 39 mV overpotentials at −10 mA cm⁻² in acidic, alkaline and neutral media, respectively, and can maintain a stable performance for 25 h. Impressively, the mass activities are respectively up to 26.1, 22.4, and 17.7 times as that of Pt/C/CC electrode. Theoretical calculation results show that the synergistic effect of Pt_SAs, Pt_ACs, and S-TiN NTs can optimize the electronic structure of Pt and generate multiple active sites with a thermodynamically favorable hydrogen adsorption free energy (ΔG_H*), thereby resulting in an enhanced HER activity.

更新日期：2022-11-02

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