Unraveling Excellent Performance in NH3–SCR over Cr-Doped NiMn-LDO Catalysts: A Combined Experimental and Computational Study

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-05-13 DOI:10.1021/acs.nanolett.5c0019710.1021/acs.nanolett.5c00197

Xinru Luan, Yujia Zhai, Yingying Guo, Wei Liu, Jian Zhang, Liguo Wang and Zhongpeng Wang*,

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Abstract

A sequence of Cr-doped NiMnO_x layered double oxide catalysts was synthesized through coprecipitation and applied in selective catalytic reduction of NO with ammonia (NH₃–SCR). The catalytic performance for NO reduction was enhanced by tuning the Ni/Mn/Cr molar ratios of the Ni₁Mn₁Cr_x-LDO precursors (x = 1, 2, 3); notably, Ni₁Mn₁Cr₂-LDO achieved over 90% NO conversion and N₂ selectivity within the temperature range of 150–300 °C. Moreover, Ni₁Mn₁Cr₂-LDO demonstrated significant resistance to SO₂ and H₂O along with exceptional stability. From the results of the characterization of the physicochemical properties of the catalysts, the presence of Cr species in Ni₁Mn₁Cr_x-LDO may enhance the surface acidity and reducibility. Additionally, higher amounts of Mn⁴⁺, Ni³⁺, Cr³⁺, and surface-adsorbed oxygen species were detected on the Ni₁Mn₁Cr₂-LDO catalyst. Through in situ DRIFTS experiments, the promotion of the NH₃–SCR process on Ni₁Mn₁Cr₂-LDO was confirmed to involve a combination of Langmuir–Hinshelwood and Eley–Rideal mechanisms.

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NH3-SCR在cr掺杂NiMn-LDO催化剂上的优异性能：实验与计算相结合的研究

通过共沉淀法合成了一系列掺cr的NiMnOx层状双氧化物催化剂，并将其应用于氨（NH3-SCR）选择性催化还原NO。通过调整Ni1Mn1Crx-LDO前驱体的Ni/Mn/Cr摩尔比（x = 1,2,3），提高了NO还原的催化性能；值得注意的是，Ni1Mn1Cr2-LDO在150-300℃的温度范围内实现了90%以上的NO转化率和N2选择性。此外，Ni1Mn1Cr2-LDO表现出对SO2和H2O的显著抗性以及优异的稳定性。从催化剂的理化性质表征结果来看，Ni1Mn1Crx-LDO中Cr的存在可能会增强其表面酸度和还原性。此外，在Ni1Mn1Cr2-LDO催化剂上检测到更高数量的Mn4+、Ni3+、Cr3+和表面吸附的氧。通过原位DRIFTS实验，证实了NH3-SCR过程对Ni1Mn1Cr2-LDO的促进涉及Langmuir-Hinshelwood和ley - rideal机制的组合。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

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