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用于臭氧分解的层状双氢氧化物催化剂:M与M的协同作用

Layered Double Hydroxide Catalysts for Ozone Decomposition: The Synergic Role of M and M.

作者信息

Wang Zhisheng, Chen Yingfa, Li Xiaotong, He Guangzhi, Ma Jinzhu, He Hong

机构信息

State Key Joint Laboratory of Environment Simulation and Pollution Control, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.

University of Chinese Academy of Sciences, Beijing 100049, China.

出版信息

Environ Sci Technol. 2022 Jan 18;56(2):1386-1394. doi: 10.1021/acs.est.1c07829. Epub 2021 Dec 31.

Abstract

In previous work, we successfully prepared a NiFe-layered double hydroxide (LDH) with superior activity and stability for catalytic ozone decomposition, which fundamentally avoids deactivation under high-humidity conditions. However, the role of the metal elements (M and M) in LDH catalysts is not clear. Here, LDH materials containing different metals (NiFe, NiAl, NiMn, CoFe, and MgFe) were prepared by a simple co-precipitation method. It was found that the LDHs containing Ni exhibited catalytic performance far superior to that of Co and Mg for ozone elimination, and NiFe-LDH had the best activity and stability among LDH materials prepared in this study. The NiFe-LDH can maintain 78% catalytic activity within 144 h at room temperature, even under a relative humidity of 65% and a space velocity of 840 L·g·h. Physicochemical characterizations demonstrated that chemical stability in an oxidizing atmosphere and the synergic role of M and M ions are crucial. The result of density functional theory calculation showed that the synergic role of Ni and Fe weakens the interaction between O and H in the O-H bond, which effectively lowers the reaction barrier of ozone decomposition compared with MgFe-LDH.

摘要

在之前的工作中,我们成功制备了一种对催化臭氧分解具有优异活性和稳定性的镍铁层状双氢氧化物(LDH),从根本上避免了在高湿度条件下失活。然而,LDH催化剂中金属元素(M和M)的作用尚不清楚。在此,通过简单的共沉淀法制备了含有不同金属(NiFe、NiAl、NiMn、CoFe和MgFe)的LDH材料。研究发现,含镍的LDH对臭氧消除表现出远优于钴和镁的催化性能,且NiFe-LDH在本研究制备的LDH材料中具有最佳的活性和稳定性。即使在相对湿度为65%、空速为840 L·g·h的条件下,NiFe-LDH在室温下144小时内仍能保持78%的催化活性。物理化学表征表明,在氧化气氛中的化学稳定性以及M和M离子的协同作用至关重要。密度泛函理论计算结果表明,与MgFe-LDH相比,Ni和Fe的协同作用减弱了O-H键中O与H之间的相互作用,有效降低了臭氧分解的反应势垒。

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