独特的 Pd/WO3 3D 空心球纳米催化剂对 CO 氧化具有显着的抗 SO2 和 H2S 能力：关联 SO2 暴露的结构-活性关系,ACS Applied Energy Materials

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独特的 Pd/WO3 3D 空心球纳米催化剂对 CO 氧化具有显着的抗 SO2 和 H2S 能力：关联 SO2 暴露的结构-活性关系
ACS Applied Energy Materials ( IF 5.4 ) Pub Date : 2024-01-24 , DOI: 10.1021/acsaem.3c02664
Vijayakrishnan Jeyavani _{1,

2} , Deepali Kondhekar ₃ , Meema Bhati _{1,

2} , Sahil Dev _{1,

2} , Kavita Joshi _{1,

2} , R. Nandini Devi _{2,

3} , Shatabdi Porel Mukherjee _{1,

2}

Affiliation

我们报道了一种合成 Pd/WO ₃ 3D 空心球纳米催化剂的简单无机路线，其中 Pd 纳米颗粒被封装并良好地分布在多孔氧化钨纳米球上。该合成方案具有优点，因为它不需要表面活性剂或稳定剂，Pd负载量易于调整，并且合成的纳米材料可以直接用作CO氧化反应的催化剂。合成的纳米催化剂在260℃下表现出100%的CO到CO _{2的转化效率。}此外，纳米催化剂在 CO 氧化反应过程中表现出显着的 SO ₂ (3 ppm) 耐受性，可在 260–400 °C 下进行 1–21 小时的长时间 SO _{2硫酸化。}这代表了迄今为止报道的基于单一金属Pd/载体的纳米催化剂的最长SO _{2暴露时间。}_{基于单一金属Pd基纳米催化剂，即使在SO 2} (3 ppm)处理21小时后也没有观察到CO转化效率的下降，这是首次。此外，合成的纳米催化剂表现出H ₂ S（4 ppm），甚至在260℃下CO氧化反应1-3小时期间原位H ₂ S耐受性，并且对长期和严格的硫暴露表现出较低的敏感性，具有最高的H据我们所知，基于 Pd 基纳米催化剂，首次在 H ₂ S 处理后获得了₂ S 浓度和最大 100% CO 至 CO _{2转化效率。}通过废催化剂分析证实，即使在CO氧化反应过程中长时间暴露于SO ₂和H _{2 S之后，R-Pd/WO}₃纳米催化剂的组成和结构也没有受到太大影响。最后，我们基于 DFT 的模型通过分析潜在的电子结构，为理解 Pd/WO ₃上观察到的抗硫性提供了见解。因此，我们的战略合成方法将为选择Pd/金属氧化物基纳米材料来设计高效、稳定且耐SO ₂ /H ₂ S的纳米复合催化剂提供许多机会。

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Remarkable SO2 and H2S Resistant Ability on CO Oxidation by Unique Pd/WO3 3D Hollow Sphere Nanocatalyst: Correlating Structure–Activity Relationships on SO2 Exposure

We report a simple inorganic route for synthesizing a Pd/WO₃ 3D hollow sphere nanocatalyst, where Pd nanoparticles are encapsulated and well distributed on porous tungsten oxide nanospheres. The synthesis protocol has advantages, as it requires no surfactant or stabilizing agent, Pd loading is easily tuned, and the as-synthesized nanomaterials can be directly used as catalysts for the CO oxidation reaction. The synthesized nanocatalyst exhibited 100% CO to CO₂ conversion efficiency at 260 °C. In addition, the nanocatalyst demonstrated remarkable SO₂ (3 ppm) tolerance during the CO oxidation reaction for prolonged SO₂ sulfation of 1–21 h at 260–400 °C. This represents the longest SO₂ exposure time reported to date based on a single metal Pd/support-based nanocatalyst. No decrement in CO conversion efficiency was observed even after SO₂ (3 ppm) treatment for 21 h for the first time based on a single metal Pd-based nanocatalyst. Moreover, the synthesized nanocatalyst shows H₂S (4 ppm), even in situ H₂S tolerance during the CO oxidation reaction at 260 °C for 1–3 h and exhibited less sensitivity to prolonged and stringent sulfur exposure, with the highest H₂S concentration and maximum 100% CO to CO₂ conversion efficiency obtained after H₂S treatment for the first time based on a Pd-based nanocatalyst to the best of our knowledge. The composition and structure of the R-Pd/WO₃ nanocatalyst were not much influenced, even after the prolonged SO₂ and H₂S exposure during the CO oxidation reaction, as verified from spent catalyst analysis. Finally, our DFT-based model provides insights into understanding the observed sulfur resistance on Pd/WO₃ by analyzing the underlying electronic structure. Therefore, our strategic synthesis methodology will open up many opportunities to select Pd/metal oxide-based nanomaterials for designing highly efficient, stable, and SO₂/H₂S-resistant nanocomposite catalyst.

更新日期：2024-01-24

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