As<sub>2</sub>O<sub>3</sub>与Cu-ZSM-5催化剂的相互作用机理

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Abstract The adsorption properties of NO and As₂O₃ over Cu-ZSM-5surface were calculated based on density functional theory in this paper. By determining the optimum adsorption site of As₂O₃ over Cu-ZSM-5, the reaction pathway of As³⁺ adsorbed on its active site was investigated, and the activation energy barriers and decisive speed steps of As adsorption reaction on the catalyst were calculated, to reveal the bonding and interaction mechanisms of the reaction between As₂O₃ and Cu-O-Cu. The results show that the non-oxygen sites of NO and As₂O₃ are adsorbed on the lattice oxygen sites of active site Cu-O-Cu and the adsorption energies are -218.515kJ/mol and -206.422kJ/mol, respectively. The loss of charge suggests that they interact strongly during adsorption process. The oxidation of As₂O₃ on lattice oxygen of Cu-O-Cu is divided into two steps. As³⁺, as Lewis base, is easy to react with Cu-O-Cu as Lewis acid center, and the oxidation product of the first stage, As₂O₄, undergoes a secondary oxidation reaction at the adjacent active site. As₂O₅ becomes the main form after As³⁺ adsorption. The reaction pathway to produce As₂O₄ has to overcome energy barrier of 242.75kJ/mol, which becomes the decisive speed step of the whole oxidation process.

Key words： Cu-ZSM-5 As₂O₃ adsorption oxidation reaction energy barrier

Received: 20 September 2023

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X511

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	ZHANG Huan
	SHI Yi-lin
	LIU Liang
	WANG Chen-xing
	SUN Rui-bin
	JIA Li
	JIN Yan

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ZHANG Huan,SHI Yi-lin,LIU Liang等. Adsorption mechanism of As₂O₃ and Cu-ZSM-5catalysts[J]. CHINA ENVIRONMENTAL SCIENCECE, 2024, 44(4): 2003-2010.

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http://www.zghjkx.com.cn/EN/ OR http://www.zghjkx.com.cn/EN/Y2024/V44/I4/2003

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