Gu Jia-Nan, Liang Jianxing, Wang Lijun, Xue Yixin, Li Kan, Guo Mingming, Sun Tonghua, Jia Jinping
School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai 200240, PR China.
School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dong Chuan Road, Shanghai 200240, PR China; Shanghai Engineering Research Center of Solid Waste Treatment and Resource Recovery, Shanghai 200240, PR China.
J Hazard Mater. 2025 Aug 15;494:138714. doi: 10.1016/j.jhazmat.2025.138714. Epub 2025 May 25.
The regulation of lattice oxygen mobility on metal oxide-based catalysts holds great significance for balancing the conversion and selectivity in the selective catalytic oxidation of HS (HS-SCO). Herein, we successfully suppress the lattice oxygen mobility of iron oxide-based catalyst via Ag loading to realize the high HS removal effect and high sulfur selectivity simultaneously. The Ag-loaded FeO catalyst synthesized by simple precipitation and impregnation method exhibits an outstanding sulfur capacity of 3344.9 mgS g and a high sulfur selectivity of 93.0 % at 120 °C, which is superior to those of FeO catalyst (771.1 mgS g and 86.4 %). The X-ray photoelectron spectroscopy (XPS), extended X-ray absorption fine structure (EXAFS) and hydrogen temperature programmed reduction (H-TPR) characterization results reveal that the bond energy of Fe-O is enhanced via Ag loading, resulting in the reduced lattice oxygen mobility. Furthermore, oxygen temperature programmed desorption (O-TPD) result shows that the amount of lattice oxygen is decreased after Ag loading. These regulations of lattice oxygen prevent the over-oxidation of HS and improve sulfur selectivity, thereby delaying the catalyst poisoning and prolonging the lifespan of catalyst. Meanwhile, the Ag loading reduces the alkaline environment on the catalyst surface, which avoids the accumulation of sulfur. This work provides a new insight into designing desulfurizers with high conversion and selectivity for HS-SCO process.
调节基于金属氧化物的催化剂上晶格氧的迁移率对于平衡硫化氢选择性催化氧化(HS-SCO)中的转化率和选择性具有重要意义。在此,我们通过负载银成功抑制了氧化铁基催化剂的晶格氧迁移率,从而同时实现了高硫化氢去除效果和高硫选择性。通过简单沉淀和浸渍法合成的负载银的FeO催化剂在120°C时表现出3344.9 mgS g的出色硫容量和93.0%的高硫选择性,优于FeO催化剂(771.1 mgS g和86.4%)。X射线光电子能谱(XPS)、扩展X射线吸收精细结构(EXAFS)和氢气程序升温还原(H-TPR)表征结果表明,通过负载银增强了Fe-O的键能,导致晶格氧迁移率降低。此外,氧程序升温脱附(O-TPD)结果表明,负载银后晶格氧的量减少。这些晶格氧的调节防止了硫化氢的过度氧化并提高了硫选择性,从而延迟了催化剂中毒并延长了催化剂寿命。同时,负载银降低了催化剂表面的碱性环境,避免了硫的积累。这项工作为设计用于HS-SCO过程的具有高转化率和选择性的脱硫剂提供了新的见解。