Mechanochemical Redox: Calcination-free Synthesis of Ceria-hybrid Catalyst with Ultra-High Surface Area,ChemCatChem

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Mechanochemical Redox: Calcination-free Synthesis of Ceria-hybrid Catalyst with Ultra-High Surface Area
ChemCatChem ( IF 3.8 ) Pub Date : 2021-03-04 , DOI: 10.1002/cctc.202100256
Siyang Nie ₁ , Shize Yang ₂ , Pengfei Zhang ₃

Affiliation

Transition metal-doped CeO₂ (MCeO_x) is of great importance in industrial catalysis. However, current synthetic methods often result in the separation of MO_x phases, which significantly decreases their catalytic activity. Toward this end, the chemistry of mechanochemical redox was introduced to prepare Ce_1-xMn_xO_2-δ catalyst. The redox behavior between MnO₄⁻ and Ce³⁺ could in situ produces atomically dispersed Ce_1-xMn_xO_2-δ solid solution without calcination. Moreover, the mechanochemical synthesis endows Ce_1-xMn_xO_2-δ a surface area (302 m²/g) that is much higher than the counterparts prepared by traditional methods, such as co-precipitation method (66 m²/g) CTAB-assisted precipitation method (122 m²/g) and sol-gel method (136 m²/g). Importantly, the well dispersed heteroatoms and high porosity afford doped ceria excellent activity and stability during CO oxidation. The reaction mechanism was finally explored by DFT calculation, which reveals that Mn and Cu dopants facilitate electron transfer and oxygen releasing.

中文翻译：

机械化学氧化还原：超煅烧二氧化铈杂化催化剂的无煅烧合成

过渡金属掺杂的CeO ₂（MCeO _x）在工业催化中非常重要。然而，当前的合成方法经常导致MO _x相的分离，这大大降低了它们的催化活性。为此，引入了机械化学氧化还原化学以制备Ce _1-x Mn _x O2 _-δ催化剂。的MnO之间的氧化还原行为₄^-和Ce ³⁺可以原位产生原子分散的Ce _1-x的Mn _X ö _2-δ固体无需煅烧溶液。此外，机械化学合成赋予Ce _1-x Mn_x O2 _-δ的表面积（302 m ² / g）比通过传统方法（如共沉淀法（66 m ² / g）CTAB辅助沉淀法（122 m ² / g）和溶胶-凝胶法（136 m ² / g）。重要的是，良好分散的杂原子和高孔隙率使掺杂的二氧化铈在CO氧化过程中具有出色的活性和稳定性。最后通过DFT计算探索了反应机理，结果表明Mn和Cu掺杂剂促进了电子转移和氧释放。

更新日期：2021-03-04

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