Spontaneous Formation of Asymmetric Oxygen Vacancies in Transition-Metal-Doped CeO2 Nanorods with Improved Activity for Carbonyl Sulfide Hydrolysis,ACS Catalysis

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Spontaneous Formation of Asymmetric Oxygen Vacancies in Transition-Metal-Doped CeO2 Nanorods with Improved Activity for Carbonyl Sulfide Hydrolysis
ACS Catalysis ( IF 11.3 ) Pub Date : 2020-09-14 , DOI: 10.1021/acscatal.0c02832
Shunzheng Zhao _{1,

2} , Dongjuan Kang ₁ , Yunpeng Liu ₃ , Yanfeng Wen ₁ , Xizhou Xie ₁ , Honghong Yi _{1,

2} , Xiaolong Tang _{1,

2}

Affiliation

Introducing oxygen vacancies into metal oxides is a promising strategy to promote their catalytic activity, which has been extensively studied in heterogeneous catalysis. Herein, transition metal (M = Fe, Co, and Ni) doping was used to introduce oxygen vacancies in CeO₂ and promote activity for carbonyl sulfide (COS) hydrolysis. Various techniques were performed to accurately characterize the catalyst structure and state. The transition metals successfully entered the crystal lattice of CeO₂ and formed a solid solution structure. The metal-doped CeO₂ (M/CeO₂) showed improved reduction properties, more Ce³⁺ and oxygen vacancies in comparison with pure CeO₂. The introduction of transition metal greatly enhanced activity of M/CeO₂ for COS hydrolysis. Among them, the Co/CeO₂ sample displayed the highest activity and H₂S selectivity. The roles of metal doping in improving activity were explored on the basis of DFT calculations. The strong interaction between doped metals and CeO₂ promotes the spontaneous formation of asymmetric oxygen vacancies in M/CeO₂. These asymmetric oxygen vacancies facilitate the activation and dissociation of H₂O and generation of active hydroxyls, which contributes to the enhanced activity for COS hydrolysis. This work provides an attractive method for obtaining nonprecious metal catalysts for COS hydrolysis.

中文翻译：

过渡金属掺杂的CeO ₂纳米棒中自发形成不对称氧空位，具有改进的羰基硫水解活性。

将氧空位引入金属氧化物是提高其催化活性的一种有前途的策略，已在多相催化中进行了广泛研究。此处，过渡金属（M = Fe，Co和Ni）掺杂用于在CeO _2中引入氧空位并提高羰基硫（COS）水解的活性。进行了各种技术以准确表征催化剂的结构和状态。过渡金属成功地进入CeO _2的晶格并形成固溶体结构。与纯CeO ₂相比，金属掺杂的CeO ₂（M / CeO ₂）表现出改善的还原性能，更多的Ce ³⁺和氧空位。过渡金属的引入大大提高了M / CeO ₂的COS水解活性。其中，Co / CeO ₂样品显示出最高的活性和H ₂ S的选择性。在DFT计算的基础上，探讨了金属掺杂在提高活性中的作用。掺杂金属与CeO ₂之间的强相互作用促进了M / CeO ₂中不对称氧空位的自发形成。这些不对称的氧空位促进了H ₂ O的活化和解离以及活性羟基的产生，这有助于提高COS水解的活性。这项工作为获得用于COS水解的非贵金属催化剂提供了一种有吸引力的方法。

更新日期：2020-10-17

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