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Promotion effect of iron addition on the structure and CO2 hydrogenation performance of Attapulgite/Ce0.75Zr0.25O2 nanocomposite supported Cu-ZnO based catalyst
Guo, Haijun1,2,4,5; Ding, Shuai2,3; Zhang, Hairong1,2,4,5; Wang, Can1,2,4,5; Peng, Fen1,2,4,5; Yao, Shimiao1,2,4,5; Xiong, Lian1,2,4,5; Chen, Xinde1,2,4,5
刊名MOLECULAR CATALYSIS
2021-08-01
卷号513页码:12
关键词CO2 hydrogenation Attapulgite Ce0.25Zr0 .25O2 solid solution Fe promoter In-situ DRIFTS
ISSN号2468-8231
DOI10.1016/j.mcat.2021.111820
通讯作者Chen, Xinde(cxd_cxd@hotmail.com)
英文摘要A series of CZF(x)K/ATP-CZO catalysts (x= 0, 0.3, 0.5, 1.0, 1.5 and 2.0) are applied to clarify the effects of the iron addition on the catalytic performance of CO2 hydrogenation to CH3OH. The physicochemical properties and catalytic mechanism were investigated by N-2 adsorption/desorption, XRD, TEM, N2O chemisorption, XPS, H-2-TPR, CO2-TPD and in-situ DRIFT techniques. The best catalytic performance is achieved over CZF(0.5)K/ATP-CZO catalyst, exhibiting X-CO2 = 17.5%, STYCH3OH = 0.108 g/gcat.h and STYCO = 0.146 g/gcat.h (T = 320 degrees C, P = 6 MPa). The formation of dispersed surface metallic Cu species and larger number of surface adsorbed and lattcie oxygen species and ZnO-CZO interfaces are detected over CZF(0.5)K/ATP-CZO due to stronger interaction between dispersed metallic Cu particles on ZnO-Fe nano-cluster and ATP-CZO composite, resulting in the superior activation ability for H-2 and CO2 respectively. Additionally, the evidence is provided by in-situ DRIFTS under the activity test temperature (320 degrees C) that HCOO* and CO* species are preferable for accumulating over CZK/ATP-CZO catalyst without Fe addition while medium Fe-modified CZF(x)K/ATP-CZO catalysts (CZF(0.3)K/ATP-CZO, CZF(0.5)K/ATP-CZO) catalysts are benefitial to promote the transformation of HCOO* species to CH3OH. These excessive Fe-modified CZFxK/ATP-CZO catalysts (CZF(1.0)K/ATP-CZO, CZF(2.0)K/ATP-CZO) are more easily to produce CH4 via formate pathway (CO2* -> HCOO* -> HCO* -> CH* -> CH4*). The abundant population and high transformation activity of formate intermediate species over CZF(0.5)K/ATP-CZO give a strong positive effect on the CO2 hydrogenation to methanol performance.
资助项目Guangdong Basic and Applied Basic Research Foundation[2020A1515010516] ; Project of Guangdong Provincial Natural Science Foundation[2018A030310126] ; Project of Guangdong Provincial Natural Science Foundation[2018A030313150] ; Project of Jiangsu Province Science and Technology[BE2018342] ; Key-Area Research and Development Program of Jiangsu Province[BE2020394] ; Project of Key Laboratory Foundation of Renewable Energy, Chinese Academy of Science (CAS)[E1290104]
WOS关键词MIXED ALCOHOLS SYNTHESIS ; GAS SHIFT REACTION ; METHANOL-SYNTHESIS ; CU-ZNO/ZRO2 CATALYSTS ; NI/ZRO2 CATALYST ; CARBON-DIOXIDE ; OXIDE CARRIERS ; ACTIVE-SITE ; FUNCTIONALITY ; ADSORPTION
WOS研究方向Chemistry
语种英语
出版者ELSEVIER
WOS记录号WOS:000694709600002
资助机构Guangdong Basic and Applied Basic Research Foundation ; Project of Guangdong Provincial Natural Science Foundation ; Project of Jiangsu Province Science and Technology ; Key-Area Research and Development Program of Jiangsu Province ; Project of Key Laboratory Foundation of Renewable Energy, Chinese Academy of Science (CAS)
内容类型期刊论文
源URL[http://ir.giec.ac.cn/handle/344007/33875]  
专题中国科学院广州能源研究所
通讯作者Chen, Xinde
作者单位1.CAS Key Lab Renewable Energy, Guangzhou 510640, Peoples R China
2.Chinese Acad Sci, Guangzhou Inst Energy Convers, Guangzhou 510640, Peoples R China
3.Univ Sci & Technol China, Nano Sci & Technol Inst, Suzhou 215123, Peoples R China
4.R&D Ctr Xuyi Attapulgite Energy & Environm Mat, Xuyi 211700, Peoples R China
5.Guangdong Prov Key Lab New & Renewable Energy Res, Guangzhou 510640, Peoples R China
推荐引用方式
GB/T 7714
Guo, Haijun,Ding, Shuai,Zhang, Hairong,et al. Promotion effect of iron addition on the structure and CO2 hydrogenation performance of Attapulgite/Ce0.75Zr0.25O2 nanocomposite supported Cu-ZnO based catalyst[J]. MOLECULAR CATALYSIS,2021,513:12.
APA Guo, Haijun.,Ding, Shuai.,Zhang, Hairong.,Wang, Can.,Peng, Fen.,...&Chen, Xinde.(2021).Promotion effect of iron addition on the structure and CO2 hydrogenation performance of Attapulgite/Ce0.75Zr0.25O2 nanocomposite supported Cu-ZnO based catalyst.MOLECULAR CATALYSIS,513,12.
MLA Guo, Haijun,et al."Promotion effect of iron addition on the structure and CO2 hydrogenation performance of Attapulgite/Ce0.75Zr0.25O2 nanocomposite supported Cu-ZnO based catalyst".MOLECULAR CATALYSIS 513(2021):12.
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