Highly Poison-Resistant Single-Atom Co–N4 Active Sites with Superior Operational Stability over 460 h for H2S Catalytic Oxidation,Small

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Highly Poison-Resistant Single-Atom Co–N4 Active Sites with Superior Operational Stability over 460 h for H2S Catalytic Oxidation
Small ( IF 13.0 ) Pub Date : 2021-10-19 , DOI: 10.1002/smll.202104939
Ganchang Lei ₁ , Yawen Tong ₂ , Lijuan Shen _{1,

3} , Yong Zheng _{1,

4} , Shijing Liang _{1,

4} , Wei Lin ₂ , Fujian Liu _{1,

4} , Yanning Cao _{1,

4} , Yihong Xiao _{1,

4} , Lilong Jiang _{1,

4}

Affiliation

Efficient catalytic elimination of hydrogen sulfide (H₂S) with high activity and durability in nature gas and blast-furnace gas is very critical for both fundamental catalytic research and applied environmental chemistry. Herein, atomically dispersed Co atom catalysts with Co–N₄ sites that can transform H₂S into S with conversion rate of ≈100% are designed and prepared. The representative 4Co-N/NC achieves a sulfur yield of nearly 100% and TOF_(Co) of 869 h^–1 at 180 °C. Importantly, remarkable long-term durability is achieved as well, with no obvious loss of catalytic activity in the run of 460 h, outperforming most of the reported catalysts. The short bond length and strong cooperation of Co–N are beneficial to improve the structural stability of the Co–N₄ centers, and significantly enhanced resistance of water and sulfation over single-atom Co-catalyst. The present mechanism involves the stepwise hydrogen transfer process via the adsorbed *HOO and *HS intermediates.

中文翻译：

高抗毒单原子 Co-N4 活性位点，在 460 小时内对 H2S 催化氧化具有卓越的运行稳定性

在天然气和高炉煤气中以高活性和耐久性有效催化消除硫化氢 (H ₂ S) 对于基础催化研究和应用环境化学都非常关键。在此，设计并制备了具有 Co-N ₄位点的原子分散 Co 原子催化剂，可以将 H ₂ S 转化为 S，转化率约为 100%。代表性的 4Co-N/NC 实现了近 100% 的硫产率和869 h ^{–1 的}TOF _(Co)在 180°C。重要的是，还实现了显着的长期耐久性，在 460 小时的运行中没有明显的催化活性损失，优于大多数报道的催化剂。Co-N 的短键长和强协同作用有利于提高 Co-N ₄中心的结构稳定性，并显着提高了单原子助催化剂的抗水和硫酸盐化能力。目前的机制涉及通过吸附的 *HOO 和 *HS 中间体的逐步氢转移过程。

更新日期：2021-11-18

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