Optimizing low-temperature CO2 methanation through frustrated Lewis pairs on Ni/CeO2 catalysts

被引：24

作者：

Chen, Xiaohan ^{[1
,2
]}

Ye, Runping ^{[1
]}

Sun, Chunyan ^{[1
]}

Jin, Chengkai ^{[1
]}

Wang, Yuan ^{[2
,3
]}

Arandiyan, Hamidreza ^{[4
,5
]}

Lim, Kang Hui ^{[2
]}

Song, Guoqiang ^{[2
]}

Hu, Feiyang ^{[1
]}

Li, Claudia ^{[2
]}

Lu, Zhang-Hui ^{[6
]}

Feng, Gang ^{[1
]}

Zhang, Rongbin ^{[1
]}

Kawi, Sibudjing ^{[2
]}

机构：

[1] Nanchang Univ, Sch Chem & Chem Engn, Key Lab Jiangxi Prov Environm & Energy Catalysis, Nanchang 330031, Jiangxi, Peoples R China

[2] Natl Univ Singapore, Dept Chem & Biomol Engn, 4 Engn Dr 4, Singapore 117585, Singapore

[3] Univ Melbourne, Dept Chem Engn, Parkville, Vic 3010, Australia

[4] Univ Sydney, Sch Chem, Lab Adv Catalysis Sustainabil, Sydney, NSW 2006, Australia

[5] RMIT Univ, Ctr Appl Mat & Ind Chem CAM, Sch Sci, Melbourne, Vic 3000, Australia

[6] Jiangxi Normal Univ, Inst Adv Mat IAM, Coll Chem & Chem Engn, Nanchang 330022, Jiangxi, Peoples R China

来源：

CHEMICAL ENGINEERING JOURNAL | 2024年 / 484卷

基金：

新加坡国家研究基金会;

关键词：

Ni/CeO2; Morphological control; Frustrated Lewis pair; Oxygen vacancy; CO2methanation; Reaction pathways; COKING RESISTANCE; PERFORMANCE; HYDROGENATION; MORPHOLOGY; CEO2; MECHANISM; OXIDATION; KINETICS;

D O I：

10.1016/j.cej.2024.149471

中图分类号：

X [环境科学、安全科学];

学科分类号：

08 ; 0830 ;

摘要：

The promising realm of carbon dioxide (CO2) conversion offers a compelling avenue to advance environmental sustainability. This study introduces a novel approach by utilizing frustrated Lewis pairs (FLPs) for efficient lowtemperature CO2 methanation. Through a tailored ammonium bicarbonate (AB) precipitation method, we engineered Ni/CeO2 catalysts abundant in FLPs. Various morphologies, including aggregated flakes, broom -like structures, and irregular granules, were achieved by modulating the AB -to -cerium molar ratio. The distinctive broom -like Ni/(0.06AB)CeO2 catalyst, comprised of nanorods with abundant FLPs, exhibited outstanding lowtemperature CO2 methanation performance: 67.5 % CO2 conversion, 99.6 % CH4 selectivity, and 0.27 s-1 CO2 turnover frequency (TOFCO2) at 240 C-degrees, with excellent stability in a 100-h test at 300 C-degrees. Furthermore, leveraging in -situ DRIFTS and in -situ Raman techniques, and DFT study, we unraveled CO2 hydrogenation pathways and found a dual interplay of CO and formate pathways in the low -temperature methanation over Ni/(0.06AB)CeO2 catalyst.

引用

页数：15

共 75 条

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