Noble metal modified copper-exchanged mordenite zeolite (Cu-ex-MOR) catalysts for catalyzing the methane efficient gas-phase synthesis methanol

被引：1

作者：

Xie, Xuanlan ^{[1
,2
]}

Li, Chang ^{[1
,2
]}

Lu, Zhiheng ^{[1
,2
]}

Wang, Yishuang ^{[1
,2
]}

Yang, Wenqiang ^{[4
]}

Chen, Mingqiang ^{[1
,2
]}

Li, Wenzhi ^{[2
,3
]}

机构：

[1] Anhui Univ Sci & Technol, Analyt & Testing Ctr, Sch Chem & Blasting Engn, Huainan 232001, Peoples R China

[2] Hefei Comprehens Natl Sci Ctr, Inst Energy, Hefei 230031, Peoples R China

[3] Univ Sci & Technol China, Lab Clean Low Carbon Energy, Hefei 230023, Peoples R China

[4] Univ South Carolina, Chem Engn, 301 S Main St, Columbia, SC 29208 USA

来源：

ENERGY | 2024年 / 300卷

关键词：

Partial oxidation; Methane to methanol; Mordenite; Copper-based catalyst; Noble metal; PARTIAL OXIDATION; DIRECT CONVERSION; PROPIONIC-ACID; SURFACE; SITES; STEAM; DRY; HYDRODEOXYGENATION; MECHANISM;

D O I：

10.1016/j.energy.2024.131595

中图分类号：

O414.1 [热力学];

学科分类号：

摘要：

Copper mordenite catalysts are key for methane oxidation to methanol, yet lack sufficient activity. In this paper, noble metal (Au, Ru, Pt and Pd) modified copper ion-exchanged mordenite catalysts were prepared by the ionexchange method for further improving the methanol yield in the gas-phase continuous catalytic direct partial oxidation of methane to methanol reaction, and the role of noble metal doping on Cu-ex-MOR catalysts was investigated. Experimental results showed that the doping of Ru resulted in a significant increase in the methanol yield of Ru/Cu-ex-MOR catalyst to 157.36 mu mol/g cat /h compared to that of Cu-ex-MOR catalyst (12.89 mu mol/ g cat /h). SEM, XRD, FT -IR, N 2 adsorption-desorption, XPS, NH 3 -TPD and H 2 -TPR results showed that Ru/Cu-exMOR had uniformly dispersed Ru elements and the largest number of surface acidic and oxidation sites, which facilitated the adsorption and activation of methane. Additionally, it was found by TEM, in situ FT -IR and DFT characterization that Ru played a role in stabilizing the Cu active sites, the adsorptive activation of water on the Ru site and the H-transfer process reduced the energy required for breaking C - H bond of CH 4 at the Cu active site, which significantly improved the methane activation capacity of the Ru/Cu-ex-MOR catalysts, resulting in higher methanol yields.

引用

页数：14